REVIEW

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Recent Advances in Spatial Self-Phase Modulation with 2D

Materials and its Applications
Yunlong Liao, Chunmei Song, Yuanjiang Xiang, and Xiaoyu Dai*

methods of nonlinear parameter

In recent years, spatial self-phase modulation (SSPM) with two-dimensional measurement mainly include the z-
(2D) materials has attracted the attention of many researchers as an emerging scan,[14–17] four wave mixing (FWM),[18,19]
and ubiquitous nonlinear optical effect. In this review, the state of the art of interferometry,[20,21] and spatial self-
2D material-based SSPM is summarized. SSPM measures or tunes the phase modulation (SSPM).[22–24] All of
these methods measuring nonlinear
nonlinearity of 2D materials, and it is also an effective approach to study the refraction have some disadvantages. For
band structure of 2D materials. Several modified forms of SSPM, such as example, the z-scan method requires
high-order, white-light-excited, vector field excited, and optically nonlinearly complex data fitting, interferometry re-
enhanced SSPM are also presented. Subsequently, the physical origin of the quires precise adjustment of the optical
SSPM formation mechanism is compared and analyzed. Furthermore, the path, and FWM requires a complex op-
tical configuration. In contrast to these,
applications of SSPM with 2D materials, including passive photonic devices,
SSPM is a simple method with a short
generation of Bessel beams, and identifying the mode of the orbital angular measurement period.
momentum, are listed. Finally, several urgent problems of the SSPM with 2D SSPM is an all light modulation
materials, potential applications, and prospects for future development are phenomenon occurring due to Kerr non-
presented. linearity of the nonlinear material.[25–29]
In 1967, Callen et al. reported this highly
interesting nonlinear effect for the first
time.[30] In 1978, Stolen et al. employed SSPM to measure the
1. Introduction
nonlinear optical response of a single-mode fiber.[31,32] SSPM
Nonlinear optics is a study of high-intensity light in nonlinear was found to cause a significant spread of the spectrum and
materials, whose polarization density is not linearly dependent achieve precise modulation of the phase. Immediately after-
on the light’s electric field. The field emerged after Mainman wards, Durbin et al. realized SSPM in liquid crystal and con-
invented the first laser in 1960.[1] Subsequently, a series of non- structed its theory of numerical research.[23] However, in the fol-
linear optical effects were reported, including second harmonic lowing 30 years, the research progress of SSPM has been devel-
generation (SHG),[2] stimulated Raman scattering,[3] optical oping slowly and was mainly concentrated in the optical fiber.
phase conjugation,[4] optical bistability,[5] saturable absorption With the discovery of graphene, 2D materials have been used as
(SA),[6] two-photon absorption (TPA),[7] and the Kerr effect.[8] carriers for studying SSPM, demonstrating countless interesting
Photonic applications based on various novel nonlinear optical applications. Although the 2D material is thin, it exhibits a strong
effects have significant advantages over electronic applications. interaction between light and matter, providing opportunities for
In fact, nonlinear effects are employed in numerous practical as- accurate observation of the behavior of SSPM. Furthermore, the
pects, including biological imaging technologies,[9] ultrafast laser diversified electronic structure of 2D materials makes some pho-
generation for laser processing,[10] optical communication,[11] all- tonic devices (all-optical switching, all-optical modulators) based
optical devices,[12] and optoelectronic devices.[13] Simultaneously, on the SSPM exhibit a broadband optical response.[33] Exploring
the third-order nonlinear susceptibility of material is a highly novel nonlinear optical effects is likewise a subject that has been
important parameter in nonlinear applications. In general, the widely studied. The novel form of SSPM promotes continuous
improvement and development of the SSPM. All-optical modu-
Dr. Y. Liao, C. Song, Prof. X. Dai
lation technology and all-optical devices have significant poten-
College of Electrical and Information Engineering tial in the application of optical communication technology and
Hunan University all-optical networks. In the dual beam SSPM, referred to as spa-
Changsha 410082, China tial cross-phase modulation (SXPM), the phase of the incident
E-mail: [email protected] light is not only modulated by its own intensity, but also by the
Prof. Y. Xiang intensity of the pump light.[34] SXPM is a typical all-optical modu-
School of Physics and Electronics
Hunan University lation technique, which has been applied to numerous photonic
Changsha 410082, China devices. Furthermore, the generation, identification, amplifica-
tion, and transmission of light beams are of great significance
The ORCID identification number(s) for the author(s) of this article for light field regulation. SSPM and SXPM also excel in light field
can be found under https://doi.org/10.1002/andp.202000322
regulation.[35]
DOI: 10.1002/andp.202000322

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2D materials typically exhibit completely different character- susceptibilities, respectively. The first term 𝜒 (1) E(t) describes the
istics in comparison to bulk materials due to quantum confine- conventional linear optical effect, the second term 𝜒 (2) E(t)2 de-
ment effects. Numerous researchers are devoted to discovering notes the second-order nonlinear optical effect (e.g., SHG [62] ),
2D materials with excellent performance and more practical ap- and the third term 𝜒 (3) E(t)3 denotes the third-order nonlinear op-
plications. For instance, graphene has ultra-high carrier mobility tical effect (e.g., third harmonic generation (THG),[63] TPA [64] ).
and thermal conductivity, as well as high optical absorption.[36–38] The optical Kerr effect refers to the birefringence of the light
Compared to zero-band-gap graphene, transition-metal dichalco- beam transmitted through the medium caused by an external
genides (TMDs) can have an adjustable band gap, which constant light field acting on the medium, and the change in the
indicates that TMDs have a broadband spectral response in refractive index of the medium is proportional to the square of the
optoelectronic or photonic device applications.[39,40] Black phos- applied light intensity. Assuming that the medium is isotropic,
phorus has a band gap range that fills the gap between graphene the total refractive index n is expressed as
and TMDs, exhibits anisotropy, and has a higher nonlinear
refractive index coefficient (≈10−5 cm2 W−1 ) than graphene.[41] √
Other 2D materials with attractive attributes include MXene, 3
n= 1 + 𝜒 (1) + 𝜒 (3) |E(t)|2 = n0 + Δn (2)
graphdiyne, tellurene, InSe, and boron. 4
In this review, first we summarize the current use of the SSPM
to investigate the third-order nonlinear optical response of 2D where n0 is the linear refractive index of the medium, and ∆n
materials. The nonlinear refractive index of 2D materials, such is change of the refractive index. Therefore, when the laser
as graphene (≈10−7 cm2 W−1 ),[22] MoS2 (≈10−9 cm2 W−1 ),[24] light passes through 2D materials, according to the optical
MoSe2 (≈10−4 cm2 W−1 ),[42] WSe2 (≈10−10 cm2 W−1 ),[43] MoTe2 Kerr effect, the refractive index is expressed as n = n0 + n2 I,
(≈10−12 cm2 W−1 ),[44] Ti3 C2 Tx (≈10−4 cm2 W−1 ),[45] graphdiyne where n2 is the nonlinear refractive index coefficient, and I
(≈10−5 cm2 W−1 ), InSe (≈10−5 cm2 W−1 ),[46] boron (≈10−6 cm2 is the incident laser light intensity. Further, a change in the
W−1 ) [47] were experimentally determined by the SSPM. The cur- refractive index of the medium will effectuate the phase change
rent research hotspots of the SSPM are discussed, such as tun- of the light wave, such the light wave propagates through the
ing of the nonlinear refractive index and investigation of the medium and receives its own intensity modulation, which is
band gap.[42,48] Second, we summarized novel forms of SSPM, self-phase modulation (SPM). In general, the fundamental mode
including SSPM with enhanced optical nonlinearity, high-order Gaussian beam (TEM00 ) is used to excite the SSPM effect. The
SSPM, SSPM excited by white light, and vector field excited Gaussian beam passes through a nonlinear medium with a
SSPM.[48,49] These different SSPM techniques may provide in- length L along the z-axis, and its electric field distribution can be
spiration for future optical solutions. Moreover, we list typical ap- described as
plications of SSPM, such as passive photonic devices [50–52] (e.g.,
optical limiting, photodiodes, all-optical modulators, and switch- ( )
𝜔0 r2
ing), beam generation [53–55] (e.g., Bessel beam, Bessel-like beam, E(r, z) = E(0, z) exp −
𝜔(z) 𝜔(z)2
Gauss–Bessel beam), optical orbital angular momentum pattern
recognition,[56] optical bistability.[57] ( [ ])
z kn0 r 2
Despite significant research performed on SSPM, consider- × exp −i kz − arctan + (3)
z0 2R(z)
able controversy remains about the physical origin of the SSPM;
two main formation mechanisms were proposed, one is pure
electronic coherence,[24] and the other is thermally induced where 𝜆 is the wavelength of the laser, k = 2𝜋/𝜆 is the wave
nonlinearity.[58] Several researchers claim that both effects are vector, z0 = 𝜋𝜔20 ∕𝜆 is the Rayleigh length (the length of the
combined. Other models, such as the saturation model, likewise beam that propagates like a plane wave), R(z) = z[1 + (z0 ∕z)2 ] is
strive to explain the physical origin of SSPM.[59] Therefore, the es- the radius of curvature of the wavefront, 𝜔0 is the beam waist
√
tablishment of a universally applicable model is an urgent mat- radius, and 𝜔(z) = 𝜔0 1 + (z∕z0 )2 is the beam radius at z.
ter for all SSPM with 2D materials effects. Finally, we present
Using the radius of the laser beam waist as the starting point for
several problems to solve the current situation of SSPM research
beam propagation, the electric field distribution at the plane of
and look forward to future development prospects.
incidence of the 2D materials (r, z0 ) is described as

2. Fundamentals of 2D Material-Based SSPM ( ) ( )

( ) ( ) r2 kn0 r 2
E r, z0 = E 0, z0 exp − ( )2 exp −i (4)
2.1. Fundamentals of SSPM 𝜔 z0 2R(z)

In the field of nonlinear optics, the optical response of a mate-

rial to an applied light field can be expressed by the polarization The light intensity distribution is expressed as I(r, z) =
intensity P(t) and optical field intensity E(t) as follows [60,61] I0 (1 + z2 ∕z20 )−1 exp(−2r 2 ∕𝜔20 ), where I0 = 2Pave ∕[𝜋𝜔(z)2 ] is the
central intensity of the Gaussian beam, and Pave is the average
P(t) = 𝜒 (1) E(t) + 𝜒 (2) E(t)2 + 𝜒 (3) E(t)3 + ⋯ (1) power of the laser. Therefore, the refractive index is corrected to
n(r) = n0 + n2 I(r). Assuming that the sample is thin enough, the
where 𝜒 (1) is the linear susceptibility, and 𝜒 (2) and 𝜒 (3) and so total phase at the output of the sample can be expressed as Δ𝜙 =
forth are second-order, third-order, and higher-order nonlinear Δ𝜓L (r) + Δ𝜓NL (r), where Δ𝜓L (r) = kn0 r 2 ∕[2R(z)] is the linear

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Figure 1. The formation and evolution of SSPM. a) Diagram of the experimental setup for measuring the third-order nonlinear response of 2D materials
through SSPM. Reproduced with permission.[41] Copyright 2016, Optical Society of America. b) The pattern of the diffraction ring received by the CCD
changes with the incident light intensity (SnS Ns). Reproduced with permission.[175] Copyright 2018, Wiley-VCH. c) In the case of 𝜆 = 457nm (①–③),
𝜆 = 532nm (④–⑥) and 𝜆 = 671nm (⑦–⑨), the evolution of the diffraction ring with time. Reproduced with permission.[50] Copyright 2018, Wiley-VCH.
The ring number of the diffraction ring changes with the incident light intensity under the d) excitation of pulse and e) continuous light. d) Reproduced
with permission.[41] Copyright 2016, Optical Society of America. e) Reproduced with permission.[42] Copyright 2016, Springer Nature. f) Spectrum
before and after excitation of SSPM. Reproduced with permission.[247] Copyright 2020, Institute of Electrical and Electronics Engineers. g) The number
of diffraction rings varies with the number of graphene layers. Reproduced with permission.[48] Copyright 2014, American Institute of Physics. i) The
value of 𝜉 at different intensities. Reproduced with permission.[41] Copyright 2016, Optical Society of America.
phase shift, and Δ𝜓NL (r) is a nonlinear phase shift. The nonlinear condition is satisfied, and an interference ring between light and
phase shift related to the light intensity is described as dark is generated in the radial direction. The basic experimental
( ) setup for exciting SSPM is shown in Figure 1a. Notably, the sam-
L
2𝜋n0 ple is usually placed before and after the focus, but not on the
Δ𝜓NL (r) = n2 I(r, z)dz (5)
𝜆 ∫0 focus.

The transverse propagation wave vector is thus expressed as 2.1.1. Formation and evolution of SSPM
( )
dΔ𝜓NL −8rkn2 I(r, z) exp −2r 2 ∕𝜔20 There are two typical evolution characteristics of the diffraction
𝛿k(r) = = (6)
dr n0 ring pattern. In one, the ring number and radius increase lin-
early with the increase in light intensity (Figure 1a). The other is
Evidently, the nonlinear phase shift has a Gaussian distribution, that the diffraction ring continues to increase at the initial time,
thus we have( dΔ𝜓 )
dr r=r1
= ( dΔ𝜓 ) . Therefore, the two transverse
dr r=r2
after which it becomes a non-axisymmetric diffraction ring and
waves (k = dΔ𝜓∕dr) at r1 and r2 are equal, such that the coherence finally stabilizes for all excitation bands (Figure 1b). In 2006, Ji

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et al. reported the thermally induced SSPM of carbon nanotubes In the case of circular aperture, at P(x, y) the light intensity
(CNTs) under the influence of gravity.[65] The distribution of car- distribution is described as
bon nanotubes obeys Boltzmann distribution law, which may
( ) ( )
also be applicable to other 2D materials. The number of carbon | ∞ r2 kn0 r 2
I = I0 || J0 (kr𝜃) exp − exp −i
nanotubes depends on the vertical height and can be expressed as
M gx | ∫0 𝜔(z)2 2R(z)
Λ = Λ0 exp( 2DM kB T
), where M2DM is the mass of 2D materials, g is
the gravity constant, kB is the Boltzmann constant, and Λ0 is the ( ) |2
× exp −iΔ𝜓NL rdr || (9)
concentration of 2D materials at the center of symmetry of the |
laser beam. When the laser power is low, the far-field intensity is
close to the Gaussian distribution. As the power increases, con- E(0,z)e−𝛼L
where I0 = 4𝜋 2 | i𝜆D |2 , J0 (kr𝜃) is the zero-order Bessel func-
centric rings begin to appear and continue to increase. In 2015, tion, and D denotes the distance from the sample to the
Xiao et al. observed dynamic SSPM effects in the MoS2 disper- screen.
sion. These effects are mainly divided into the following three
stages.[66] In the first stage, the laser beam changes from a Gaus-
sian beam to a centrally symmetric diffraction ring. The radius
2.2. Fundamentals of Optical Properties of 2D materials
of the diffraction expands, and the number of rings continues
to increase. In the second stage, the diffraction rings become
When layered material is at its thinnest limit, it exhibits extraordi-
asymmetric in the vertical direction, and their size and number
nary properties that are completely different from bulk materials.
tend to stabilize. In the third stage, the diffraction rings gradually
Generally, 2D material refers to a crystalline material, where elec-
become asymmetric in the horizontal direction. In fact, a large
trons can only move freely on two nanometer scales. Thus far,
number of subsequent studies have shown that the first and sec-
countless 2D materials have been successfully synthesized and
ond stages are ubiquitous, and the third stage is mainly due to
widely explored. Here, we mainly discuss the typical and emerg-
defects in the laser itself. The time evolution of the diffraction
ing 2D materials that have been used to study the SSPM.
ring number (N) can be fitted by an exponential decay model,
N = Ae−t∕𝜏rise , where 𝜏rise is the rise time for ring formations,
and A denotes a constant.[44] According to the wind chime model
proposed by Zhao et al., the formation time of the diffraction ring 2.2.1. Graphene
𝜀r 𝜋𝜂𝜉Rc
is described as  = 1.72(𝜀 , where 𝜖 r is the relative dielectric
r −1)Ih
Graphene, as the first successfully prepared 2D material,[70] has
constant of the 2D material, 𝜂 is the viscosity coefficient of the
excellent properties in terms of electrical, thermal, mechanical,
solvent, 𝜉 is the fluid property of the 2D material, R is the average
and particularly optical. For instance, it exhibits ultra-high
radius of the nanosheet disk, and I is the laser intensity.[24] The
carrier mobility (15 000 cm2 V−1 S−1 ),[36] electrical conductivity
SSPM effect of most materials is almost instantaneous; however,
(106 S m−1 ),[71] thermal conductivity (5 × 103 W m−1 K),[37] high
this is not the case in some photopolymers (e.g., organ siloxanes).
flexibility (elastic modulus up to 1.1 T Pa), robustness (strength
The refractive index change at this time is expressed as [67]
limit up to 42 N m−2 ),[72] high environmental stability, and a
{ [ t−𝜏 ]} broadband optical response (from far infrared to ultraviolet).[73]
1
Δn = Δns 1 − exp − |E(t)|2 dt (7) Graphene has a hexagonal honeycomb lattice structure, where
U0 ∫0
each hexagonal unit is composed of six sp2 hybrid carbon atoms.
where Δns is the maximum refractive index change, U0 is the As a zero-bandgap semi-metal, it exhibits a conical energy band
critical exposure required to initiate the polymerization reaction, structure and massless Dirac fermions, and its conduction and
and 𝜏 is the lifetime of the monomer radical. Due to the satura- valence bands meet at point K in the Brillouin region. Conse-
tion of the lateral refractive index, the beam becomes thin and quently, it has unique optical properties and a resonant optical
self-focusing occurs.[68] Subsequently, Ana et al. found that due response over a wide range of wavelengths. Because monolayer
to the flat Gaussian distribution of the refractive index, the far- graphene has a strict absorptivity of 𝜋𝛼 ≈ 2.3% (𝛼 = e2 ∕ℏc de-
field pattern of SSPM gradually evolves from multiple diffraction notes the fine-structure constant) [38] at visible light band, it is
rings to a single ring.[27] widely used in a variety of broadband photoelectric devices (e.g.,
photodetectors, all-light modulators, ultrafast photons).[38,74–77]
In fact, weak absorption is beneficial for numerous devices,
2.1.2. Light Field Distribution of SSPM Pattern such as organic light emitting diodes and solar cells.[76,78,79]
The transmittance of monolayer graphene in the visible light
Analogous to classical optics, we can describe the light field band is 97.3%,[80] which allows to estimate the effective number
caused by SSPM as the Fraunhofer diffraction of a circular of graphene layers in the sample by measuring its total trans-
aperture.[69] First, we assume that the shape of the aperture is ar- mittance. Furthermore, graphene also has excellent nonlinear
bitrary and lies in the 𝜗𝜂z plane. According to Huygens’ principle optical properties, including nonlinear scattering,[81] excited
and the Fraunhofer approximation (z ≫ 2k (𝜗2 + 𝜂 2 )), the electric state absorption,[82] saturation absorption,[83,84] SHG,[85,86]
field distribution at P(x, y) is described as THG,[87–89] higher harmonic generation (HHG),[90] FWM,[91]
and SPM.[86] Recently, graphene derivatives such as graphene
∞ ∞
eikz 2zik (x2 +y2 ) −ik oxide,[92] graphdiyne,[93] and antimonene[94] have gradually
E(x, y) = e E(𝜁, 𝜂)e z (x𝜉+y𝜂) d𝜉d𝜂 (8)
i𝜆z ∫𝜂=0 ∫𝜉=0 attracted attention.

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2.2.2. Transition-Metal Dichalcogenides Topological insulators (TI) are a new state of quantum matter,
most of which are insulating, but the surface can conduct
TMDs with the formula of MX2 , where M represents a transition electricity. Compared with graphene, TI has some unique op-
metal element (e.g., Mo, W, Nb, Re, or Ni), and X denotes the toelectronic properties due to the combined effect of spin–orbit
chalcogen element (S, Se, or Te) is the most widely studied 2D interaction and the surface state protected by time reverse
semiconductor material beyond graphene.[95–97] Unlike graphene symmetry. In addition, TI also demonstrated fascinating optical
with zero band gap, the band gap of TMDs varies from 1 to 2.5 eV properties and applications.[140–143]
as the number of layers decreases (bulk to monolayer), and its In summary, 2D materials exhibit numerous fascinating prop-
Γ point in the Brillouin zone transitions from an indirect band erties, and in this article, we focus on SSPM with 2D materials
gap to a direct band gap at K. Generally, MX2 exhibits two crys- and its applications.
tal structures, namely the 1T phase (octahedron) and 2H phase
(triangular prism), which can be easily identified by resonance
2.3. Synthesis and Characterization of 2D materials
Raman spectroscopy. Both phases can be interconverted by an
atomic slip in the layer (e.g., 2H-MoS2 can be transformed into
The synthesis and characterization of 2D materials is a large
1T-MoS2 is embedded into Li or K,[98] and it gradually converts
premise for studying the SSPM effect, as the quality of the ma-
back to 2H-MoS2 due to thermodynamic instability [91] ). TMDs
terial directly determines the outcome of the experiment. The
also exhibit fascinating nonlinear optical responses,[91,99] and it
preparation methods of 2D materials are mainly divided into two
is interesting that even-order and even higher-order nonlinear
categories,[144–146] “top-down” (e.g., mechanical cracking,[70–148]
optical responses can also be observed in 3R-TMDs with odd
liquid exfoliation [36,149–151] ) and “bottom-up” (e.g., chemical va-
layers due to the lack of inversion symmetry.[39] TMDs have a
por deposition,[152,153] physical vapor deposition,[154,155] pulsed
very large exciton binding energy (e.g., the excitation binding of
laser deposition,[156] wet-chemical synthesis [157] ). Top-down
a monolayer MoS2 is about 0.5–0.9 eV),[40] a very small exciton
refers to peeling off the stacked layers in the bulk crystal into
Bohr radius,[96] enhanced photoluminescence (PL) (monolayer
monolayer or multi-layer 2D nanosheets by an external driving
MOS2 can be increased by four orders of magnitude),[100] and val-
force, while bottom-up refers to direct synthesis through a chem-
ley polarization.[101] This indicates broad application prospects,
ical reaction of precursors.
including solar cells, photodetectors, light-emitting diodes, sen-
sors, and phototransistors.[102–107]
3. State of the Art of 2D Material-Based SSPM
2.2.3. Black Phosphorus, Topological Insulators and Other Emerging 3.1. SSPM Measures n2 and 𝝌(3 ) of 2D Material
2D Materials
The light intensity is inserted into Equation (5) to obtain
Black phosphorus (BP) is the most stable allotrope of phos- 2𝜋n0 n2 2 2
phorus, first synthesized in 2014.[108] The band gap of BP Δ𝜓(r) = I0 Leff e−2r ∕𝜔0 (10)
𝜆
has a broad band tenability (0.3–2.0 eV) with the number
L −1 L
of layers,[109] which indicates that BP exhibits a broadband where Leff = ∫L 2 (1 + z2 ∕z20 ) dz = z0 arctan(z∕z0 )|L2 is the effec-
1 1
optical response from visible light to mid-infrared.[110] Fur- tive thickness of the medium, L1 is the distance from the front
ther, extreme conditions have a large effect on BP, such as surface of the cuvette to the focal point, and L is the width of the
exhibiting semiconductor-to-conductor transitions [111] and cuvette (L2 = L – L1 ). The brightness of the diffraction ring formed
high-temperature superconductors.[112] Compared with TMDs, by any two points r1 , r2 in the radial direction of the Gaussian
BP has higher carrier mobility (10 000 cm2 V−1 s−1 ) and optical beam is given by the following equation Δ𝜓(r1 ) − Δ𝜓(r2 ) = M𝜋
anisotropy.[113] At the same time, BP also has a large surface area- (where M is an Integer). Dark and bright stripes appear when M
volume ratio,[114] large light absorption coefficient,[115] nonlinear is odd and even, respectively. The center and infinity of the Gaus-
optical properties,[116–118] and high photothermal conversion sian beam are satisfied
efficiency, which makes it very promising in nanomedicine,
photodetectors,[119] solar cells,[120] pulse generation,[121] and pho- Δ𝜓 (0) − Δ𝜓 (∞) = 2N𝜋 (11)
tothermal treatment.[122] As 2D material that is easily oxidized in where N is the number of the diffraction ring, and
air, the stability of BP can be improved by several methods (e.g.,
ligand surface coordination,[123] fluorination,[124] and chemical 2𝜋n0 n2
Δ𝜓 (∞) = 0, Δ𝜓(0) = I0 Leff (12)
surface functionalization [125] ). However, these methods are 𝜆
usually complicated, which limits the application of BP to a large The nonlinear refractive index n2 is expressed as
extent. ( )
In the recent years, BP analogs (BPA), such as 𝜆 N
n2 = ⋅ (13)
antimoene,[126,127] bismuthene,[128] and tellurene.[45,129,130] were 2n0 Leff I
the subject of extensive studies because of their similar structure The third-order nonlinear susceptibility of the 2D material is
and properties to BP, along with higher stability. Recently, a expressed as
larger number of 2D materials have attracted attention, such
as MXene,[131–133] graphyne,[134,135] borophene,[136,137] Group (3) c𝜆n0 dN
𝜒total = ⋅ (14)
III monochalcogenide (e.g., InSe,[137] GeSe [138] ), and SnS.[139] 2.4 × 104 𝜋 2 Leff dI

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In general, dN/dI is the nonlinear optical response term, which Table 1. Summary of SSPM method for measuring n2 and𝜒 (3) of 2D mate-
may not always be accurate, as it is also affected by factors such rials.
as sample position, concentration, and effective thickness of the
cuvette.[46] SSPM hardly depends on the type of laser, as long as 2D materials n2 [cm2 W−1 ] 𝜒 (3) References
monolayer
the excitation conditions are met. Figures 1d and 1e depict the
Graphene 10−7 10−7 [22]
cases of dN/dI under pulsed light excitation and continuous light
Graphene oxide 10−6 10−10 [ 160,161]
excitation, respectively. After SSPM, the spectrum will exhibit
Graphdiyne 10−5 N/A [52]
a multi-peak structure and widen (Figure 1f), which is mainly
caused by the coherence of two light waves with the same fre- Tellurene 10−5 N/A [ 162]

quency and different phases. Bismuthene 10−6 10−9 [34,163]

Antimonene 10−5 10−9 [ 164]

Ti3 C2 Tx 10−4 10−7 [50,165]

3.1.1. Estimation of Effective Layer Number of 2D Materials
Ti2 CTx 10−11 10−10 [ 166]

For 2D materials, the effective number of layers has significant Black phosphorus 10−5 10−8 [41,167]

influence on the nonlinear optical response. Furthermore, the Bi2 Te3 10−12 10−7 [ 140]

number of layers of 2D materials prepared by various methods Bi2 Se3 10−9 10−9 [ 168]

is not necessarily the same, hence the nonlinear optical response Bi2 S3 10−7 N/A [ 169]

of monolayer 2D material has greater significance. The electric MoS2 N/A 10−9 [24]

field across the entire sample and the electric field across the MoSe2 10−4 10−9 [42]

monolayer of 2D material have the following relationship Etotal = 10−9

∑Neff MoTe2 N/A [44]

i=1
Ei ≈ Neff Emonolayer , where Neff is the effective number of lay- WSe2 10−10 10−6 [ 170]
ers of 2D materials.[22] The third-order nonlinear susceptibility
WS2 10−7 10−9 [ 158]
and nonlinear refractive index of a monolayer 2D material can be
(3) (3) TaS2 10−5 10−6 [ 171]
expressed as 𝜒monolayer ≈ 𝜒total ∕N2eff , n2monolayer ≈ n2 ∕N2eff . As men-
TaSe2 10−7 10−10 [ 172]
tioned in Section 2.1, we can estimate the effective number of
NbSe2 10−5 10−9 [ 173]
layers by the transmittance of graphene. Assume that the inci-
GeSe 10−6 10−9 [ 174]
dent light intensity is I0 , and the light intensity after passing
InSe 10−5 10−10 [46]
through the Nth layer of the 2D material is IN . The total trans-
mittance T after passing through Nth layer of 2D material is SnS 10−5 10−10 [ 175]

∏Neff IN Bi2 Se3 -Bi2 Te3 10−5 N/A [ 176]

T = N=1 TN = Ieff , where TN is the transmittance through the
0 CsPbI3 10−6 N/A [ 177]
Nth layer. In general, the monolayer transmittance of 2D mate-
Boron 10−6 10−9 [47]
rial within a certain band is fixed. For instance, the monolayer
Franckeite 10−6 10−3 [ 178]
transmittance of graphene in the visible band is 97.3%, and T1 =
T2 = T3 ⋯ ⋯ TNeff = T0 . Therefore, the effective number of layers N/A, not available
of the sample can be evaluated from the following formula

Neff INeff the density and volume of MoS2 are 0.85 × 10−3 mol L−1 and
T = T0 = (15) 4 × 10−3 L, respectively, such the total number of molecules is
I0
𝜁 = 1.71 × 1018 . The cross-sectional area of the cuvette was 1 ×
Taking the work of Wang et al as an example,[158] the transmit- 4 cm2 , and the lattice constants of MoS2 are a = 3.161 Å and c =
tance (T) of MoS2 , WS2 , and MoSe2 at 𝜆 = 488 nm are 78.26%, 12.295 Å. Thus, the number of molecules of an effective layer in
53.54%, and 44.79%, respectively. On the other hand, the mono- MoS2 is 𝛿 = 1 × 4cm2 ∕(sin60◦ ) × (3.161)2 = 4.6 × 105 . Therefore,
layer transmission (T0 ) of these three TMDs are estimated to be the effective number of layers of MoS2 is estimated to be 444.
99.70%, 99.10%, and 99.4%, respectively.[159] Consequently, Neff Based on the above discussion, the third-order nonlinear optical
values are estimated to be 82, 69, and 133 for these three TMDs, response of 2D materials can be obtained (Table 1).
respectively. However, the monolayer transmittance of 2D ma-
terials is not always easily obtained, especially in certain wave-
length bands. Although it is theoretically possible to estimate the 3.1.2. Similar Comparison Method
monolayer transmittance by the dielectric constant of monolayer
2D material, this method is not always reliable. Further, we em- To estimate the difference between the nonlinear refractive index
ploy the concentration method to estimate the effective number of the new and existing 2D materials, the similar contrast S can
|n −n | |N ∕I −N ∕I |
of layers in 2D material. The total number of molecules 𝜁 in 2D be expressed as [177] S = 1 − 21n 22 = 1 − 1 N1 ∕I 2 2 , where n21
21 1 1
material dispersion can be described as 𝜁 = C × V × NA , where is the nonlinear refractive index calculated in the forward direc-
C denotes the concentration of dispersion, V is the volume of tion, n22 is the nonlinear refractive index calculated in the reverse
the dispersion, and NA is the Avogadro constant (6.022 × 10²³). direction, N1 ∕I1 is the nonlinear optical response obtained in the
The effective number of layers of the sample can be estimated forward direction, and N2 ∕I2 is the nonlinear optical response
as Neff = 𝜁∕𝛿, where 𝛿 is the number of molecules of a mono- obtained in the reverse direction. Wu et al. measured the nonlin-
layer 2D material. In the study of Wu et al.,[24] as an example, ear optical response of CsPbI3 quantum dots (QDs) through the

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SSPM effect, and they estimated the S of the hybrid structure effect has been observed in some nonlinear materials, including
CsPbI3 QDs and Bi2 Se3 NSs. When the laser beam is incident on nitrobenzene,[182] Srx Ba1−x Nb2 O6 (SBN), BaTiO3 ,[183] hot atomic
the target (CsPbI3 QDs/Bi2 Se3 NSs), thenN1 ∕I1 = 0.3331, and vapor,[184] liquid crystal,[23,185,186] Fe2 O3 ,[187] ethanol.[188] In 2006,
when the laser is incident reversely (CsPbI3 QDs/Bi2 Se3 NSs), Ji et al. obtained a non-collapsed diffraction ring (Figure 2c)
N2 ∕I2 = 0.4631. The similar contrast is S = 0.61, which indicates through the method of laser vertical incidence (Figure 2a).
that the nonlinear optical responses of the two materials are very For comparison, Figures 2b and 2d illustrate the SSPM device
different. However, for CsPbI3 QDs and bismuthene NSs, the diagram and far-field diffraction pattern with the SSPM ring
similar contrast is S = 0.902, which indicates that the nonlinear deformation, respectively. In 2011, Wu et al. observed this
optical responses of the two materials are alike. Furthermore, the phenomenon in 2D graphene for the first time.[22] In 2012,
estimated nonlinear refractive index of bismuthene is consistent Karimzadeh argued that non-axisymmetric thermal convection
with the results measured by Lu et al.[163] Recently, Wu et al., was the cause of the SSPM ring deformation.[22,189] In 2014,
using graphdiyne as a material with a known nonlinear refractive Wang et al. proposed a nonlinear tunable method based on
index and SnS2 , Bi2 Se3 , MoS2 , Sb, and SnS as materials with un- this collapse effect in graphene.[48] Figure 2e depicts the SSPM
known nonlinear refractive indices, obtained similar contrast at ring deformation of the diffraction ring taken by the Charge
54%, 58%, 74%, 85%, and 90%,[52] respectively. This showed that Coupled Device (CCD). Taking the intersection of incident light
both graphdiyne and SnS and SnS2 , and Bi2 Se3 have similar non- and the cuvette as the origin, the angle formed by the point on
linear refractive indices of ≈10−5 and ≈10−9 cm W−1 , respectively. the outermost ring and the center point of the ring is defined
as the maximum diffraction half angle 𝜃H . The angle after sta-
′ ′
bilization is 𝜃H , and the collapse angle is given by 𝜃D = 𝜃H − 𝜃H .
′
3.2. Influencing Factors of SSPM When the diffraction distance is sufficiently large, 𝜃H and 𝜃H
are determined by the collapse distance RH (or R′H ) and the
Basically, the far-field diffraction pattern is affected by the posi- diffraction distance D, respectively, 𝜃H = sin−1 (RH ∕D) ≈ RH D,
tion of the sample relative to the beam waist, the beam profile, 𝜃H′
≈ sin−1 (R′H ∕D) ≈ R′H ∕D. Taking MXene as an example, RH
and the light intensity.[28,29,179] The number of layers of 2D mate- and R′H depend linearly on the light intensity (Figure 2f,g). In con-
rial has an almost linear effect on the SSPM pattern (Figure 1g). 𝜆
trast, 𝜃H can be expressed as 𝜃H ≈ 2𝜋n ( dΔ𝜓 ) , r ∈ [0, +∞). The
dr max
In fact, the number of layers of 2D materials essentially affects 0
maximum diffraction half angle is expressed as 𝜃H = n2 IC, where
its band gap and absorption properties. Presently, most studies 8rL 2
believe that the formation mechanism of the SSPM ring defor- C = [− 𝜔2eff exp(− 2r𝜔2 )]max , r ∈ [0, +∞) is the maximum diffrac-
0 0
mation is due to bubbles and thermal convection.[22] The laser tion constant. Therefore, the collapse angle 𝜃D is rewritten as
induces bubbles in the 2D material nanosheets, and the bubbles
′
gradually become larger and rise, which causes the upper half 𝜃D = 𝜃H − 𝜃H = Δn2 IC (16)
of the nanosheets to line up, such the nonlinear refractive index
becomes smaller. Dispersions used to stimulate the SSPM effect where Δn2 = n2 − n′2 is the change in the nonlinear refractive in-
usually contain more than ten million molecules, hence gravity dex. The relative change in the nonlinear refractive index is thus
cannot be ignored. Ji et al. obtained a highly regular diffraction expressed as
ring by perpendicularly incident the laser beam into the carbon
nanotubes.[65] Macromolecules in solution obey the Maxwell– Δn2 ∕n2 = 𝜃D ∕𝜃H = RD ∕RH (17)
Boltzmann distribution under the action of gravity. Subsequent
studies have demonstrated that this configuration is indeed ef- Based on Equation (17), in the process of the distortion of the
fective and has been used in nonlinear photonic devices.[46,172,177] diffraction ring, we can qualitatively detect the relative change
When the light intensity is low, the fluid ball performance de- of the nonlinear refractive index through the dynamic change
pends on it (Figure 1h), which also means that in this case, the of 𝜃D ∕𝜃H or RD ∕RH . Thus far, the relative change in the non-
light intensity is a complex influencing factor of the diffraction linear refractive index is mainly controlled by the light intensity,
pattern formation time. In 2013, Gu et al. investigated the effects time, and temperature (Figure 2h–j).[48,190] In 2015, Wang et al.
of sample defects, such as uneven thickness, bending, and ad- qualitatively analyzed this by means of nonlinear regulation in
hered dust, on the far-field diffraction pattern.[180] Further, the TMDs.[158] Δn2 ∕n2 of the MoSe2 , MoS2 , and WS2 dispersions
surface morphology of the sample is estimated based on the mea- can be modulated as 0.029–0.154, 0.091–0.304, and 0.012–0.240,
sured diffraction pattern. In 2015, Irivas et al. considered the ef- respectively. The amount of change in the nonlinear refractive
fects of nonlinear absorption and non-local order on the SSPM index reaches 0.09, 0.02, and 0.03, respectively, which is larger
far-field pattern.[181] than in some other methods of nonlinear change. For example,
the electric field induction method [191] and the carrier induction
method [192] only reach 0.01. In 2018, we observed the broadband
3.3. SSPM Ring Deformation and Tunable Nonlinear Refractive characteristics of this light intensity tuning of the nonlinear re-
Index fractive index.[170] At the beginning, we assumed that this tuning
was a simple linear tuning. However, in subsequent research,
When the nonlinear material is liquid or dispersed, the upper we noticed that this tuning begins to saturate, and the greater
half of the diffraction ring formed by the SSPM effect evolves into the energy of the photon, the lower the threshold of saturation
a semi-ellipse with time, which is usually referred to as SSPM intensity.[173] Thus far, there is no convincing reason to explain
ring deformation.[182] Before the advent of 2D materials, this this behavior. Recently, we explored GeSe samples at different

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Figure 2. Distortion effect of SSPM. a,b) Diagrams of the experimental setup where the laser is incident vertically and horizontally on the sample. c,d) The
far-field diffraction patterns of SSPM in (a) and (b). Reproduced with permission.[65] Copyright 2006, Optical Society of America. e) Schematic diagram
of the far-field pattern from close to the standard ring to the collapsed diffraction ring. f,g) The changes of the maximum diffraction radius of the upper
half with the incident light intensity before and after collapse. Reproduced with permission.[50] Copyright 2018, Wiley-VCH. h–j) The relative changes of
the nonlinear refractive index as a function of incident light intensity, time, and temperature. “Light intensity” reproduced with permission.[50] Copyright
2018, Wiley-VCH. “Time” reproduced with permission.[52] Copyright 2019, Wiley-VCH. “Temperature” reproduced with permission.[48] Copyright 2014,
American Institute of Physics. respectively. k) In the case of (a) and (b), the radius of the upper half of the diffraction ring changes with time. l) Evolution
of the number of diffraction rings over time. Reproduced with permission.[47] Copyright 2020, Elsevier.

concentrations and effective lengths, and found that saturation study the nonlinear enhancement of 2D material. In most stud-
effects almost always exist.[174] More recently, Wu et al. achieved ies that consider non-local electronic coherence as the physical
nonlinear tuning of the broadband nonlinear refractive index in origin of SSPM,[24,41,163] the shape and orientation of 2D mate-
the time dimension, with the maximum Δn2 ∕n2 approaching rial nanosheets are usually arbitrary. Li et al. studied the non-
90% (Figure 2i).[162] Although the formation time of the SSPM linear optical response of uniform rectangular MoS2 by exciting
effect can be changed,[44] the nonlinear tuning in the time dimen- SSPM in the excitation wavelength of 700 nm.[197] The nonlinear
sion remains difficult to control. The same effect can be achieved refractive index n2 (≈3.17 × 10−5 cm∕W) of the uniform rectan-
at the temperature scale, which may be caused by thermally in- gular MoS2 dispersion is larger than the nonlinear refractive in-
duced nonlinearity or bubble scattering (Figure 2j). Figure 2k is dex n2 (2.88 × 10−6 cm∕W) of the randomly shaped disc-shaped
the evolution of the diffraction ring radius of boron nanosheets MoS2 dispersion.[24] Enhancement of non-linear refractive index
with time in the experimental setup of Figure 2a and Figure 2b, occurs, because the long axis of the rectangle is parallel to the po-
respectively. Further, the number of boron nanoplate diffraction larization direction of the laser, establishing non-local electronic
rings also conform to the exponential decay model (Figure 2l), coherence. Coupling MoS2 with wide band gap TiO2 to adjust
which may be a common feature of SSPM with 2D materials. the absorption mechanism of 2D material is another possible
and effective method. Interestingly, compared with MoS2 disper-
sions, MoS2 /TiO2 dispersions and films have lower and higher
3.4. Different Forms of Exciting SSPM nonlinear refractive indices, respectively. In fact, for MoS2 /TiO2
dispersions, the typical rectangular layered structure is broken
3.4.1. SSPM for Regulation of Optical Nonlinearity of 2D Materials and it is difficult to form electronic coherence. For MoS2 /TiO2
composite films, although electronic coherence will not be estab-
The interaction of non-linear light with matter is highly lim- lished, a new absorption mechanism will appear (e.g., interface
ited due to its atomically small thickness of 2D material. For in- charge transfer, excited state absorption) to enhance the nonlin-
stance, the frequency conversion efficiency of 2D material is not ear refraction or other optoelectronic properties of MoS2 . Subse-
high, even with perfect phase matching.[69] Presently, there are quently, Jiang et al. also found enhanced nonlinear refraction and
several methods to enhance the nonlinearity of 2D material, in- absorption at graphene-TiO2 nanostructures (GNP) by SSPM.[198]
cluding plasma enhancement, optical resonators, and photonic It shows the SSPM effect at 1100 nm, but does not show SSPM
metamaterials.[193–196] In fact, SSPM is also an effective method to at 700 nm. One possible explanation is that graphene dominates

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the absorption of GNP at 1100 nm,[199] TiO2 dominates the ab- of composite materials.[208,209] The effective nonlinear optical re-
sorption of GNP at 700 nm,[200] and the thermal effect is also sponse of MDNC is mainly achieved by metal nanoparticles with
excluded. It is expected that the purpose of controlling nonlin- a nonlinear magnetic susceptibility opposite to the main sign.
earity can be achieved by preparing 2D material composites with According to the analysis of the generalized Maxwell–Garnett
different optical properties.[41,158,197] model by Albert et al.,[210] the optical polarization is written as
𝜖 3𝛽f 𝜖 −𝜖
P = 𝜖hL { 𝜖hL [𝜒h + 1−𝛽f ]}E0 = 𝜖hL 𝜒(|E0 |2 )E0 , where 𝛽 = 𝜖 NP+2𝜖h with
h NP h
3.4.2. SSPM of polarized vector field 𝜖h is the dielectric constant of the host, and 𝜖NP is the dielec-
tric constant of the nanoparticles, f is the volume fraction of
In 2012, Gu et al. first studied the SSPM effect of cylindrical vec- nanoparticles, E0 is electric field, 𝜖hL is the linear term of host and
tor beams.[179] They numerically analyzed the SSPM excited by 𝜒h is the host susceptibility. The nonlinear terms of the host and
the cylindrical vector light through the analytical expression of nanoparticles are expressed as
the focal point of the cylindrical vector field of arbitrary integer [ ⟨ ⟩
3 (3) | |2 ( )]
topological charge and the Huygens–Fresnel diffraction integral (NL)
𝜖h
(L)
= 𝜖h 𝜒 h | E 0 | + Υ E0 (18)
method. Moreover, the far-field self-diffraction field of the SSPM 4
excited by the femtosecond vector field also has the characteristic [ ⟨ ⟩ (⟨ ⟩)2
(L) 3 (3) | 5 (5)
𝜒NP |ENP || + 𝜒NP ||ENP ||
(NL) 2 2
of cylindrical vector polarization. Through the vertical polarizer, 𝜖NP = 𝜖h
the radial extinction of the far-field diffraction ring was found to 4 8
have the same number of extinction directions as the topological (⟨ ⟩)3 ]
35 (7)
+ 𝜒NP ||ENP ||
2
charge m and exhibit a radially modulated fan structure. In this (19)
64
study, the SSPM pattern of the focused cylindrical vector field
still maintains its polarization characteristics, and the nonlinear-
where Υ(E0 )corresponds to the higher-order nonlinearity of the
ity has no effect on the distribution of polarization states. Bo et al. (N)
host, and 𝜒NP is the Nth nonlinear magnetic susceptibility of
generated the SSPM effect through the interaction of an ellipti- (3) (5)
cally polarized vector beam (EPVB) with an isotropic nonlinear the nanoparticles. The third-order (𝜒eff ), fifth-order (𝜒eff ), and
(7)
medium (Figure 3a).[201] Figure 3b shows the variation of far-field seventh-order (𝜒eff ) effective nonlinear susceptibility of compos-
diffraction pattern and spin angular momentum (SAM) under ite materials is expressed as [211]
different phase shifts. In addition to the intensity distribution, the
(3) (3) (3)
orientation angle and ellipse angle also exhibit a circular distri- 𝜒eff = f L2 |L|2 𝜒NP + 𝜒h (20)
bution, which is due to the radial nonlinear elliptical polarization [ ( )2 ]
(5) (5) 6 (3) 3 | (3) |2
rotation. Subsequently, Gu et al. studied the SSPM effect of ra- 𝜒eff = f L2 |L|4 𝜒NP − L3 |L|4 𝜒NP − L|L|6 |𝜒NP | (21)
dial deflection vector beams and mixed polarization vector fields 10 10 | |
(Figure 3c).[202,203] Figure 3d shows the intensity pattern of CS2 { ( )3
(7) (7) 12 (3) 3
excited by the mixed polarization vector beam at different phase 𝜒eff = f L2 |L|6 𝜒NP + L4 |L|6 𝜒NP − |L|8
shifts. Anisotropic optical nonlinearity will result in a mixed po- 35 35
larization SSPM with quadruple rotational symmetry, which will [ ( )∗ ]
(3) (3) | (3) |2 4
redistribute the SAM flux in the far-field plane. SSPM can be con- × 4|L|2 𝜒NP + |L|2 𝜒NP |𝜒NP | − L|L|6
| | 7
trolled by an isotropic optically nonlinear mixed polarization vec- [ ( )∗ ] }
tor beam. Figure 3e illustrates the normalized far-field intensity (3) (3) (5)
× 2L2 𝜒NP + |L|2 𝜒NP 𝜒NP (22)
distribution diagram and state of polarization (SoP) schematic di-
agram of the radially polarized beam of anisotropic Kerr medium. (L) (L) (L)
where L = 3𝜀h ∕(𝜀np + 2𝜀h ). By adjusting f, the third-order
Gu et al. also studied anisotropic vector self-diffraction. Figure 3f
nonlinearity can be eliminated to achieve the purpose of non-
simulates the far-field diffraction pattern and light intensity dis-
defective high-order nonlinear magnetic susceptibility. The
tribution with and without vertical polarization.
z-scan is a commonly employed method to determine the effec-
tive nonlinear coefficient. Further, the function of the peak-valley
3.4.3. Higher-Order Nonlinear SSPM difference ΔTp,v in terms of the light intensity is more effective
than that of the normalized transmittance in terms of the
Chen et al. proposed for the first time a method for identifying distance z.[212]
higher-order spatial self-phase modulation.[204] Albertet al. ob-
served high-order SSPM and SXPM effects in metal–dielectric ΔTp,v (1) (2) (3)
≅ 0.406kneff
2
Leff + 0.210kneff
4
ILeff + 0.130kneff
6
I2 Leff + ⋯
nanocomposites (MDNCs) for the first time.[205,206] Local plas- I
mon resonance (LSPR) weakening due to the mismatch of the (23)
dielectric function of the nanoparticles and the host makes
observation of higher-order susceptibility possible.[207] The where neff (N = 2, 4, 6, …) is the n + 1 order nonlinear refractive
N
fifth-order SSPM diffraction pattern of the cases where the (N)
index, andLeff = [1 − exp(−N𝛼0 L)]∕N𝛼0 is the effective length of
wavefront curvature radius R is positive and negative are shown
the sample. The nonlinear phase shift can be expressed as
in Figures 4a and 4b, respectively. Figure 4c,d depicts the cor-
responding intensity distributions. Nonlinear management is ∑ (N)
Δ𝜓 = kneff
2N
IN Leff (24)
an effective control method for the nonlinear optical response N=1

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Figure 3. SSPM of the vector field. a) Variation of far field intensity pattern (top row), EPVB orientation angles (middle row) and ellipticity angle (bottom
row). b) Variation of far-field diffraction pattern and SAM under different phase shifts. Reproduced with permission.[201] Copyright 2017, Optical Society
of America. c) Normalized far-field intensity map and SoP schematic diagram of the stray vector beam excited by the hybrid polarization vector beam.
d) Experimentally measured and theoretically, the intensity pattern of CS2 excited by the mixed polarization vector beam is at different phase shifts.
Reproduced with permission.[203] Copyright 2016, Optical Society of America. e) Normalized far-field intensity distribution diagram and SoP schematic
diagram of radial polarized beam of anisotropic Kerr medium. Reproduced with permission.[202] Copyright 2016, Optical Society of America. f) simulates
the far-field diffraction pattern and light intensity distribution with and without vertical polarization. Reproduced with permission.[179] Copyright 2012,
Optical Society of America.

Figure 4e–g shows the third-order, fifth-order, and seventh-order 3.4.4. Coherent Rainbows with White Light Laser
nonlinear optical responses of samples at different volume
fractions.[206] Albert et al. also achieved seventh-order SXPM. White light interference has been widely used for the accurate
Figure 4h–j shows that SXPM obtains the seventh-order non- measurement of microstructures due to its non-contact high sen-
linear diffraction pattern in the case of x = 0, 𝜔0 , and 2.2𝜔0 . sitivity and large measurement range.[213–215] The traditional rain-
Figure 4l–n shows the intensity distributions in the case of bow is a non-coherent optical phenomenon, which is mainly
Figure 4h–j. caused by the different refractive index of water with different

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Figure 4. Higher-order spatial self-phase modulation. a,b) The fifth-order spatial self-phase modulated diffraction pattern is for the case where the
wavefront curvature radius R is positive and negative. c,d) The corresponding intensity distributions. e–g) Third-order, fifth-order, and seventh-order
nonlinear optical responses of samples at different volume fractions. h–j) SXPM obtains a seventh-order nonlinear diffraction pattern in the case of x =
0, 𝜔0 , and 2.2𝜔0 . k–m) Intensity distributions in the case of (h)–(j). Reproduced with permission.[206] Copyright 2014, Optical Society of America.

wavelengths of light. Research on diffraction rings generated by to the SSPM effect, and that any transparent liquid is capable of
white laser is currently attracting significant interest. In 2017, producing coherent rainbows. Figure 5a shows the change in the
Sun et al. first used a white-pulse fiber laser to excite diffraction outline of the colored glass after the diffraction ring is excited.
rings in some common liquids, such as water and acetone.[216] Coherence is mainly due to interference caused by reflected light
Notably, this colored ring is different from the sparse middle being reflected to the same angle (Figure 5b).
and dense Newton rings [69] and has similar characteristics to Subsequently, similar coherent rainbows were also observed
the SSPM diffraction ring. At the same time, the horizontally in- in some condensed solids (e.g., ice, colored glass, plastic, and
cident light generates an asymmetric diffraction ring above and colored wax),[217] as shown in Figure 5c–f. For different liquid
below the oval shape, which is essentially a collapse phenomenon samples, the change of the interference ring with the intensity
in the SSPM effect. The authors believe that this is also attributed of white light is reversible, whereas for solid samples (colored

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Figure 5. Coherent rainbow. a) Local changes in colored glass. b) The derivative of the surface profile determines the diffraction pattern. Coherent
rainbow of c) colored glass, d) plastic, e) wax and f) ice. g,h) The changes of the coherent rainbow that increase and decrease the power, respectively.
Reproduced with permission.[216] Copyright 2018, Acta Physica Sinica.

glass), the change of the interference ring with the intensity that electron coherence is unlikely to be behind the coherent
of white light is not. Recently, Sun et al. proposed a qualita- rainbow formation mechanism. White laser heating causes local
tive model to analyze the formation mechanism of coherent deformation of the colored glass with a Gaussian shape. The
rainbows.[218] For liquid samples, coherent rainbows are in- density changes of liquid and solid arise from bubble and phase
consistent with thermal lensing effects that involve only heat changes, respectively, which is essentially attributed to the SSPM
conduction, as they deviate significantly from axial symmetry. effect. Although coherent rainbows have not been reported in
The size and number of rings of the coherent rainbow increase 2D material dispersions, it is boldly speculated that they are
with the increase in laser power until they reach a certain widespread in various 2D materials.
threshold (Figure 5g), after which they do not change, and the
coherent rainbow does not return to the original state when the
power is reduced (Figure 5h). Coherent rainbows appear only 3.4.5. Photonic Band Gap-Dependent SSPM
when the laser is increased to a certain extent, which is incon-
sistent with the thermal lens effect that can rapidly form a local In 2011, Wu et al. observed the SSPM effect in 2D graphene
temperature gradient soon. Therefore, the thermal lens effect for the first time and began to explore the influence of the band
is unlikely to be a mechanism for forming coherent rainbows. structure on the SSPM effect.[22] The electrons in the valence
There are no free-moving electrons inside a solid sample, such band absorb an incident photon and are excited to the conduction

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Figure 6. Band gap dependent SSPM. a) Bandgap-dependent threshold light intensity and 𝜒 (3) under continuous and pulsed light excitation. The
black and red lines represent the theoretically calculated absorption. Reproduced with permission.[322] Copyright 2010, American Physical Society. b)
Several band gaps form SSPM. c) SSPM caused by TPA. Reproduced with permission.[24] Copyright 2015, National Academy of Sciences. d,e) Schematic
diagrams of the band structure allowing SSPM excitation. Reproduced with permission.[52] Copyright 2019, Wiley-VCH. f) and g) are 𝜒 (3) measured by
SSPM as a function of the effective electron mass and carrier mobility of the 2D materials. Reproduced with permission.[44] Copyright 2019, Optical
Society of America.

band through the transition between bands. Subsequently, they SSPM was also observed in MoSe2 [42] and graphite.[220] Recently,
relax back to the bottom of the cone on two different time scales. numerous studies on the SSPM effect of 2D materials have con-
In the first few hundred femtoseconds, carrier–carrier scattering sidered the photonic band gap.[34,50,164,177] In contrast, the band
represents the main relaxation mechanism. In the subsequent gap of a large number of 2D materials changes with the number
few picoseconds, carrier–phonon relaxation dominates, such of layers. For instance, as the number of layers decreases, the
that the electrons in the energy band structure settle near the band gap of InSe changes from direct to indirect, which is the
bottom.[219] Wu et al. employed 267 nm (4.65 eV) photons with exact opposite of TMDs.[221] Its band gap value also increased
energy comparable to the 𝜋 plasmon mode (4.7 eV) resonance from 1.25 to 2.6 eV.[222] 2D materials synthesized using different
of monolayer graphene films to excite the SSPM of monolayer methods or even the same method often has inconsistent sizes
graphene.[22] Interestingly, the lower threshold was indeed ob- and thicknesses, which consequently have a certain effect on the
tained. Further, a broadband SSPM (267–800 nm) study showed photonic band gap. Therefore, it is important to synthesize 2D
that once a photon falls into the conical region of the energy materials with high quality and uniform thickness. The study
band structure, electrons can be generated, then delocalized of the SSPM effect of 2D materials with different thicknesses is
and moved. Notably, there are also double-layer and few-layer likewise interesting. In 2014, Wang et al. for the first time ob-
graphene sheets in this study. Their band structure has a gap at served the SSPM effect of graphene for different layers; however,
the K (K′) point in the momentum space. In 2015, Zhao et al. they did not analyze the band gap.[48] Recently, Wu et al. observed
discovered the existence of SSPM below the band gap (Eg < h𝜈) the SSPM effect of Te nanosheets with different thicknesses.[162]
by observing the broadband SSPM (473–830 nm) effect of MoS2 A difference in their nonlinear optical response was indeed
nanosheets.[24] More importantly, 𝜒 (3) and threshold power mea- recorded. Further, some studies have shown that for several re-
sured by SSPM are strictly dependent on the photonic band gap. verse saturation absorption materials with large band gaps, such
For instance, at 1.72 eV (722 nm), which is exactly the band gap as h-BN, C3 N4 , and SnS2 ., their diffraction rings are difficult to
value of MoS2 , 𝜒 (3) and the threshold power can change sharply excite.[46,51,223] For instance, the photon energies of 𝜆 = 532, 671,
(Figure 6a). SSPM is an even more powerful method for measur- and 457 nm all fall within the band gap of graphdiyne, such that
ing the bandgap following absorption and photoluminescence. the diffraction rings can be excited (Figure 6d). However, for
In addition, the two-photon SSPM is the most likely mechanism SnS2 , photons with 𝜆 = 532 and 671 nm cannot fall into their
below the band gap (Figure 6b). The excited carriers output two band gaps and thus cannot excite the diffraction ring (Figure 6e).
photons, which is a nonlinear process, nevertheless with a con- In fact, when the band gap is large enough, the corresponding
stant dN/dI (Figure 6c). Subsequently, this band gap-dependent nonlinear optical response becomes very small.

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4. Physical Origin of SSPM Effect Based on 2D stating that the convection velocity at the center of the beam is
Material equal to its maximum value at the center [182]

The exploration of SSPM is an active research topic; however, 𝛽g[ΔT]max 𝜋𝜔0 2

the underlying mechanism remains unclear. The proposition vx = (27)
16𝜇
of numerous mechanisms confuses and misleads whether
SSPM is derived from inherent nonlinear characteristics of where [ΔT]max is the maximum temperature gradient, 𝛽 is the
2D materials. The thermal lens effect is the earliest theory expansion coefficient, g = 9.8 m s−1 is the acceleration of grav-
that has been widely adopted. However, if SSPM is derived ity, and 𝜇 is the viscosity of the liquid. Using the Green function
from the thermal lens effect, it must not be related to the for heat conduction and convection equations, the temperature
nonlinear optical properties of the material; namely, it must distribution is estimated as [232,233]
be independent of 𝜒 (3) , which caused great confusion. Numer-
ous researchers believe that SSPM exhibits a purely electronic { t
𝛼P dt′
coherent behavior due to laser-induced molecular redirection ΔT =
𝜋𝜌c ∫0 8Dt′ + 𝜔0 2
and polymerization. However, SSPM usually requires excitation
[ [( ] ( }
with continuous light to generate sufficiently large average )2 )]
power that reaches the threshold for excitation. At this time, × exp −2 x − vx t′ + y2 ∕ 8Dt′ + 𝜔0 2 (28)
thermally induced nonlinearity is inevitable, which becomes
another competitive mechanism. Some researchers believe that Thus, the phase shift is expressed as
thermally induced nonlinearity and pure electron coexist, and
they proposed a method to distinguish between local and non- [( ) ]
⎧ ⎛ ′ 2 2 ⎞
local nonlinearity. Here we have summarized these methods, t ′ ⎪ ⎜ −2 x − v t + y ⎟
2𝜋 𝛿 dt x
hoping to provide some inspiration for the general mechanism Δ𝜓 = LΔn = ⎨exp ⎜ ( ) ⎟
𝜆 2tc ∫0 1 + 2t′ ⎪ ⎜ 2t′
1 + t 𝜔0 2 ⎟
of SSPM. t c ⎩ ⎝ c ⎠

⎛ ( )2 ⎞⎫
4.1. Thermal Lens Effect ⎜ −2 vx t′ ⎟⎪
− exp ⎜ ( ′
) ⎟⎬ (29)
⎜ 1 + 2t 𝜔0 2 ⎟⎪
The thermal lens effect was first discovered by Gordon et al. by in- ⎝ tc ⎠⎭
serting some absorbing substances into the laser cavity.[224] When
(dn∕dT)𝛼PL
the fundamental mode Gaussian beam passes through an ab- where 𝛿 = 𝜆K
eff
is the on-axis phase shift and Leff =
sorbing medium, the medium absorbs a small part of the en- (1 − e−𝛼L )∕𝛼 is the effective length of the sample. Although the
ergy to generate a radially related temperature distribution, and thermal lens effect is in principle a linear optical phenomenon,
the temperature gradient further leads to a change in the density its dependence on light intensity is similar to photo-induced non-
of the medium, which eventually gives rise to the refractive in- linearity, such that it is difficult to distinguish the two nonlinear
dex gradient.[225–229] Thermal lenses are generally negative lenses effects. Several studies argued that thermal convection has an ef-
and have a parabolic refractive index distribution, and they can be fect on the far-field diffraction pattern of SSPM, which is a favor-
regarded as an ideal thin lens without aberrations.[230,231] The re- able evidence for the thermal lens effect.[234] Time-resolved ther-
fractive index distribution can be described as [60,61] mal lens spectroscopy (TLS) is a common method for measuring
( ) thermo-optic properties of materials.[224,235–237] The thermal
dn diffusion time tc and thermal diffusivity D are easily determined
n = n0 + ΔT (25)
dT by the following equation to obtain the phase shift.[238–240]

dn [ ( ) ( 2)( ) ]−1
Where is the thermo-optic coefficient of the material, and tc −1 tc −2
dT 𝛿
𝛼P 2r 2 2r 2 I(t) = I0 1−𝛿 1+ + 1+ (30)
ΔT = 4𝜋K
{E i (− 𝜔 2 ) − Ei (− 𝜔 2 𝜏)} is the temperature gradient, 2t 2 2t
0 0
where 𝜏 = (1 + 2t∕tc )−1 , t being the absorption time; tc = 𝜔2 ∕4D,
where D = K∕𝜌c is the thermal diffusivity; K is the thermal con- Certain studies claim that SSPM is caused by thermal lensing
ductivity; c is the specific heat capacity; 𝜌 is the density; P is the and call it thermal blooming.[241–244] Further, TLS technology
laser power, and Ei is the exponential integral. The asymmetry of was also used to measure thermo-optic properties. Recently,
the temperature distribution caused by convection must be con- Sadrolhosseini et al. observed the SSPM effect of graphene oxide
sidered. The convection caused by laser heating is given by the with different diameters.[245] By adding platinum nanoparticles
following heat conduction equation with different volume fractions, the SSPM effect was enhanced
( ) along with the thermal diffusion coefficient. In fact, thus far,
dΔT most research objects that believe that the physical origin of
𝜌c + v∇ΔT − ∇(KΔT) = Q (26)
dt SSPM is the thermal lens effect are absorbing liquids, such as
various organic solvents (ethanol, propanol, butanol, formic
where Q = 𝛼I is the heat absorbed by the laser, and v is the con- acid, acetic acid, acetone, etc.), dye molecules, C60 , and carbon
vection velocity. According to the assumption by Whinnery et al., nanotubes.[246–249]

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In 2017, Wang et al. believed that SSPM in 2D materials was the disc, and R is its radius. When the pulse traverses the disc,
entirely a pure thermal lens effect, and 2D materials only played the initial angular velocity obtained is
a role in absorbing the heat generated by the laser.[58] The au-
thors claimed that the SSPM of graphene has a significant de- 1 (𝜀r −1) √
∫ Mdt 4
sin 2𝜃 𝜀r
𝜀0 E02 𝜋R2 h (𝜋∕2)𝜏
pendence on the type of solvent, temperature, and power of the Ω0 = = (31)
laser, whereas it is independent of the electronic and optical prop- J2DM + JSolution J2DM + JSolution
erties of the material, as similar diffraction rings are also found
in insulating Co3 O 4 . For Newtonian fluids, the rotating and non-rotating interface has
a constant speed-limiting linear velocity vand viscosity coefficient
𝜂, such that the rotational torque generated by the viscosity force
4.2. 𝝌 (3) of 2D Material Itself can be expressed as
𝜋
4.2.1. Nonlocal Electronic Coherence dv
 =𝜂 (R sin 𝜑)(𝜉 ⋅ 2𝜋R sin 𝜑)(Rd𝜑) = 𝜋𝜂Ω𝜉R3 (32)
∫0 dr
As early as 2011, Zhao’s research team has maintained that the
physical origin of SSPM is caused by non-local coherence of where 𝜉 is the part of the fluid rotating with the disc (close to 0),
3
electrons, as the SSPM effect was discovered in graphene.[22] The and Ω = Ω0 e−(𝜋𝜂𝜉R ∕(J2DM +JSolutan ))t is the rotation speed. The cumu-
main reasons are as follows. First, the laser causes polarization lative rotation angle of a single pulse is expressed as
of graphene flakes, and the graphene is oriented and reoriented T ∞
under the action of the electric field, which is the case of liquid Ω0 e−(𝜋𝜂𝜉R ∕(J2DM +JSolutan ))t dt
3
𝛿𝜃 = Ωdt ≈
crystal.[23] Subsequently, the authors proposed the wind chime ∫0 ∫0
model to perfectly prove this interpretation.[24] Second, under ( )
𝜀r − 1 2TIh
the condition that the total average power is equal, they observe = sin 2𝜃 (33)
that the ultrafast and continuous SSPM have the same effect. 𝜀r 4𝜂𝜉Rc
Furthermore, the threshold power to generate SSPM and the
calculated 𝜒 3 are strictly dependent on the photonic band gap The formation time of SSPM is
of 2D materials. Subsequently, they continued investigations to ( )
∑
N
𝜀r − 1 2TIh
confirm their views.[42,220] Wu et al. found that the mobility of 𝛿𝜃i = ⋅ N ⋅ sin 2𝜃i (34)
carriers (C60 and graphene) has a significant influence on 𝜒 3 , i=1
𝜀r 4𝜂𝜉Rc
which seems to prove the origin of electrons. Recently, Zhao’s
team found that the effective mass of electrons and the carrier Zhao et al. found that the formation time of SSPM in the MoS2
mobility depend on 𝜒 3 strictly by summarizing some of SSPM’s dispersion is consistent with the prediction of the wind chime
work (Figure 6f,g).[44] The SSPM relation to electrons is crucial model, which indicates strong support for the latter. The SSPM
evidence for the pure coherence theory. formation time does not depend on the repetition frequency and
pulse width of the laser, and the results obtained by continuous
and pulsed light excitations are consistent. Further, in the earli-
4.2.2. Wind Chime Model and Electronic Coherence of est SSPM study, continuous and pulsed light yielded the same
Communication result, with the same excitation power.[22] AC electronic coher-
ence, which is different from steady-state electronic coherence,
√ The electron wave function at rA can be expressed
The wind chime model was first used by Zhao et al. to explain the likewise exists.
physical origin of SSPM in the MoS2 nanosheet dispersion.[24] as 𝜓A (rA ) = 𝜌A (rA )ei𝜙(rA ) , where 𝜓A∗ (rA ) ⋅ 𝜓A (rA ) = 𝜌A (rA ) is the
There is an arbitrary orientation angle 𝜃 between 2D material local electron density. The phase 𝜙(rA ) = k ⋅ rA − 𝜔t + 𝜙0 (rA ) of
nanosheets and the electric field. Once energy relaxation occurs, the electronic wave function is determined by the external light
the force of the electric field reorients the nanosheets such that field. Here, 𝜙0 (rA ) represents the phase lag after responding to
each domain contains an axis parallel to the polarization of the the external field, and 𝜔(1014 Hz) is the frequency of the light
external field, just like every domain hanging by a vertical “line.” wave. The wave function of the electron at rB can be expressed in
The laser pulse generates angular momentum on each nanosheet the same manner and is coherent with the electron wave func-
of 2D material, rotating them until they form an axis parallel to tion at rA , which arises from both wave functions being coherent
the polarization of the external electric field. Then, the viscous with the light wave. The electrons are not far from their equilib-
force at the edge of the nanosheet continuously decreases the an- rium position. Once the wind chimes are formed, more electron
gular velocity until it becomes static. When the following pulse coherence is generated, and there are less collisions due to the
arrives, the same process is repeated, and the integration result orientation of the 2D material nanosheets. The electric field at
is the formation of wind chimes. Assume that 2𝜋∕𝜔0 is less than rC is corrected to
the width of the pulse 𝜏. The electric field polarization in the
( ) ( ) ( )
nanosheet domain can be expressed as P = (𝜀r −1)𝜀0 E(z, t) cos 𝜃, E rC = 𝜁 𝜒 (3) 𝜓 rC (35)
2 2 2
where E(z, t) = E0 e−((ct−z) ∕c 𝜏 ) sin(kz − 𝜔0 t) is the electric field.
Assuming that the domain shape of the nanosheet is a disc, √ √
where 𝜓(rC ) = ei(k⋅rC −𝜔t+𝜙0 ) [ 𝜌A (rA )e−ik⊥ ⋅rA + 𝜌B (rB )e−ik⊥ ⋅rB ] de-
the rotational torque generated by the laser can be expressed as notes the optical phase, and 𝜁 (𝜒 (3) ) is the exact coefficient deter-
(𝜀 −1) 2 2 2
M = 14 sin 2𝜃 r𝜀 𝜀0 E02 𝜋R2 he−(2(ct−z) ∕c 𝜏 ) , where h is the height of mined by the third-order nonlinear susceptibility. The nonlinear
r

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dΔ𝜓 all-optical modulation, which was first discovered by Zhao et al.

refractive index n2 determines k⊥ = dr
, and the carriers in 2D
materials determine 𝜒 (3) . (Figure 7a).[24] Generally, it has the following characteristics. One
is that the ring number of the diffraction pattern or phase of the
probe light is determined by both its own light intensity and the
4.3. Other Theories pump light intensity (Figure 7b). Photons of one wavelength can
diffract photons of another wavelength. Figure 7d shows the de-
A large number of research groups believe that the thermal pendence of the ring number of the probe light on the total in-
lens effect and electron coherence coexist. Recently, Xiao et al. put light intensity, which conforms to the linear superposition of
claimed to observe two mechanisms simultaneously in SSPM individual light intensity cases. In the 2D materials-based SSPM
with Bi2 TeSe2 nanosheets.[250] Han et al. used fullerene as a car- all-light modulation system, two beams affect each other, which is
rier to explore the physical origin of SSPM and also observed different from the situation where two beams meet with a small
local and non-local nonlinearity.[251] Moreover, [ΔT]max increases angle in free space. When the light intensity of probe beam is
linearly with increasing radiant power, and tends to saturate at fixed (even below the threshold), and the light intensity of pump
relatively high radiant power. The refractive index change caused beam is increased, the number of rings and the diameter of each
by temperature is corrected as [251] beam will increase at the same time (Figure 7c). Hence, the in-
tensity of the pump light can change not only its own phase, but
[ ]
dn 𝛼P exp −ur 2 ∕𝜔2 (z) also the phase of the probe light. Small changes in the intensity
Δn = ( ) (36) of the pump light will cause the diffraction pattern of the probe
dT 2𝜋K 1 + P∕PS (1 + z2 )u∕2
light to shift in space, achieving the effect of an on or off function,
where PS is the saturation power, and u is the order of that is, an all-optical switch function.
nonlocality.[181] The nonlinear phase shift at this time can be ex- All-optical switches based on the SSPM effect of 2D materi-
pressed as als have some unique features, including weak control, cascade,
high contrast, and broadband. In 2017, Li et al. adopted the same
2𝜋
Leff configuration and realized a three-phase (focusing, diffraction,
Δ𝜓 = n (n2 I + Δn)dz (37) constant) all-optical switch uniquely by adjusting the angles of
𝜆 0 ∫0
the pump light and the detection light. However, the self-focusing
The formula for calculating the number of diffraction rings can is instantaneous, and it is quickly replaced by self-diffraction. In
be modified as [251] addition, for transmitted light, the phase distribution of the illu-
[ ] minated area was obtained according to the Gerchberg–Saxton
2n L P n2 dn 𝛼 algorithm. Subsequently, Lu et al. implemented an SSPM-based
N = 0 eff + ( ) (38) all-optical switch in few layer bismuthene.[34] More importantly,
𝜆 𝜋𝜔20 dT 4𝜋K 1 + P∕PS
the principle of superposition, that is, the total number of diffrac-
Subsequently, the authors used z-scan to identify local and non- tion rings formed after all-light modulation, has a linear depen-
local nonlinearity and verified the correctness of the model.[59,252] dence on the total intensity of the two beams. Further, the inves-
∑
Overall, the current research on the physical origin of SSPM is tigation also proved that the light modulation depth Δn2 ∕ n2 is
not mature enough, and it is necessary to propose a universal the- related to the incident energy, and the maximum modulation
ory to explain all the laws and phenomena of SSPM. Jiang et al. depth is reached when the intensity of the probe light is below
used hybrid graphene-TiO2 nanostructures to excite SSPM and the threshold of the diffraction ring. In fact, this all-light modula-
found that the structure had an SSPM effect at 1100 nm and no tion does not necessarily require two beams of light to form a cer-
signal at 700 nm.[198] TiO2 exhibits a large reverse saturation ab- tain angle. In 2018, Wu et al. achieved full-light modulation based
sorption (RSA) at 700 nm, which indicates that the nonlinear op- on the SPPM effect in few-layer SnS by completely coupling the
tical properties of graphene at 1100 nm play a large role, such that two beams with a beam splitter.[175] Wu et al. proposed to apply
SSPM is unlikely to be a simple thermal effect. Further, there is a the all-optical modulation of SSPM to information conversion.
large number of studies indicating that SSPM is pure electronic By controlling the light to reconstruct the diffraction ring of the
coherence. signal light, information transmission from one optical band to
another optical band is achieved. Unfortunately, there is always a
large delay time for signal light compared to control light, which
5. Perspectives and Applications of 2D is mainly due to the time required for the establishment of non-
Material-Based SSPM local electronic coherence.[24]
The SSPM light modulation system based on 2D materials
5.1. All-Optical Modulation and All-Optical Switching can also be applied to all-light modulators based on single wave-
lengths. Single-wavelength light is divided into signal light and
Numerous studies have shown that applying 2D materials to detection light by the beam splitter, whereby similar modula-
all-optical modulation and switching has numerous unique tion effects can be obtained.[50] Recently, Wang et al. realized a
advantages.[24,80,253–255] Thus far, most all-light modulation us- thermally induced broadband all-optical switch in InP quantum
ing 2D materials is based on the material’s third-order nonlin- dots (Figure 7h) [258] with adjustable bandgap.[259] This configura-
ear response (e.g., saturation absorption [83] or Kerr effect [256] ) tion differs from SSPM-based all-optical modulation in that only
and thermo-optic effect.[257] All-optical modulation based on the pump light participates in focusing to generate a change in the re-
SSPM effect of 2D materials is a novel mechanism for free-space fractive index. Figure 7i shows the diffraction pattern of the probe

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Figure 7. All-optical switching. a) Schematic diagram of all-optical modulation. b,d) The relationship between the ring number of signal light and the light
intensity. c) Increase the intensity of the pump light to increase the number of signal lights. Reproduced with permission.[24] Copyright 2015, National
Academy of Sciences. e) Schematic diagram of cross modulation. f) Variation of far-field diffraction pattern with power at a fixed detection position. g)
The result of light modulation. Reproduced with permission.[162] Copyright 2019, Wiley-VCH. h) Schematic diagram of all-optical switching. i) When the
pump light is turned on and off, the diffraction pattern of the signal light. j) Oscilloscope signals of pump light and signal light at different switching
frequencies. Reproduced with permission.[258] Copyright 2017, American Chemical Society. k) Schematic diagram of a two-color all-optical switching.
l) Control the light diffraction pattern and radial light intensity distribution under different powers. Reproduced with permission.[263] Copyright 2017,
Multidisciplinary Digital Publishing Institute. m) Schematic diagram of polarization-dependent all-optical switching. n) Transmittance of signal light
with or without switching light. Reproduced with permission.[321] Copyright 2019, Wiley-VCH.

light when the pump light is turned on and off. In this scheme, power of the pump light (60–80 mW) changes the received sig-
the substantially nonlinear medium InP quantum dots are re- nal from 1 to 0 and then to 1, respectively (Figure 7f). Figure 7g
garded as a thermal lens. Although there is only a diffraction shows the corresponding on and off data of the probe light as the
pattern and no diffraction ring throughout the experiment, it re- power of the pump light increases. More recently, Wu et al. suc-
mains possible that it is an all-light modulation based on SSPM. cessfully applied SSPM-based all-optical modulation to all-optical
In 2006, Ji et al. showed that the unfocused laser can also give rise logic gates in the Te@Bi QD NTs hybrid heterojunction.[51]
to the SSPM effect.[65] Further, the on/off ratio will decrease as the Te@Bi QD NTs heterojunctions exhibit an enhanced nonlin-
modulation frequency increases (Figure 7j). Wu et al. proposed ear optical response, because the built-in electric field gener-
another novel concept of all-optical switching based on SXPM ated by them can effectively promote the separation of photo-
(Figure 7e).[260] The change in intensity causes a change in the generated carriers.[261,262] Moreover, the response sensitivity
phase shift, which eventually induces movement of the diffrac- of the logic gate is related to the photon energy. For instance,
tion ring. Fixing the position of the detector and increasing the when lasers with 𝜆 = 671 nm and 𝜆 = 532 nm are used as pump

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Figure 8. Optical limiting. a) Diagram of the experimental setup for optical limiting. b) Optical limiting at different locations. c) Theoretical simulation
of the diffraction pattern and normalized intensity distribution at different locations. Reproduced with permission.[274] Copyright 2017, Elsevier.

light, the response sensitivities are 13.46 and 23.93 s−1 , respec- ring.[271] Subsequent investigations have shown that the center
tively. Wu et al. designed the two-color all-optical switching, as of the diffraction ring is dark when the wavefront curvature ra-
shown in Figure 7k,[263] which shortened the diffraction pattern dius R(z) and phase shift (Δ𝜓) have opposite signs.[272] In fact,
formation time, indicating that the all-optical switching time is if the nonlinear absorption and thermal effects are considered,
shorter. Figure 7l shows the intensity pattern and radial intensity the above conclusions may not be true.[181] Earlier, Leite et al. ap-
distribution of signal light with respect to the optical power of plied the SSPM effect to the optical limiter.[273] Recently, Zhang
light excitation. Figure 7m shows a schematic of the all-optical et al. studied the optical limiting of Rb atoms through the SSPM
switching related to polarization. Figure 7n depicts the switching effect (Figure 8a).[274] Both thermal and Kerr effects are consid-
signal under the armchair polarization direction and the perpen- ered, and the center of the diffraction ring appears dark. On the
dicular polarization. basis of the SSPM device, an aperture is added to achieve the pur-
pose of optical limiting. The sample can be moved back and forth
5.2. Optical Limiting near the focal point to achieve the lowest clamping output and
limit threshold. The center of the diffraction ring is designed to
Optical limiting devices are used to protect human eyes or be bright, and the diffraction pattern and intensity distribution at
sensors in optical systems.[223] At present, two main mecha- different positions are shown in Figure 8b. More recently, our re-
nisms are believed to enable optical limiting, one is nonlinear search team based on the SSPM effect proposed a photonic diode
scattering,[264] and the other is nonlinear absorption (such as, re- that is also essentially optical limiting for its reverse.[46]
verse saturation absorption, excited state absorption).[265–267] In
addition, the output threshold and clamp output are two impor- 5.3. All-Optical Diode
tant parameters. Evidently, based on the characteristics of SSPM,
optical limiting is easy to implement.[268,269] Notably, the center Similar to electronic diodes with p-n junctions, all-optical diodes
of the diffraction ring is bright in some investigations [270] and (AODs) are designed to achieve irreversible unidirectional trans-
dark in others,[23] which is directly related to the performance mission of light in space.[275,276] To date, various mechanisms
of the light confinement device. At the same time, some stud- have been proposed to achieve the unidirectional transmis-
ies have shown that a second fine ring exists in the diffraction sion of light in space, including magneto-optical effects,[277]

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Figure 9. All-optical diode. a,b) Schematic diagram of an all-optical diode based on asymmetric nonlinear absorption. c) Normalized transmittance for
forward detection and reverse detection. d) z-Scan results of BLG, FLG, and C60 . Reproduced with permission.[284] Copyright 2013, American Chemical
Society. e,f) Forward and reverse measurement results nonlinear measurement results for CsPbI3 QDs/Bi2 Se3 NSs structure and CsPbI3 QDs/Bi NSs
structure. e,g) Schematic diagrams of photonic diodes. Reproduced with permission.[177] Copyright 2018, Wiley-VCH. i) Schematic diagram of the
preparation of solid-state diodes. j,k) The far-field diffraction patterns of the diode. l,m) The number of diffraction rings in forward detection and reverse
detection as a function of light intensity. Reproduced with permission.[52] Copyright 2019, Wiley-VCH.

photonic crystals,[278] heterojunctions,[279] optical non- of graphene (TLG) and few-layers of graphene (FLG) is expressed
linearities,[280] and metamaterials.[281] Low power consump- as
tion, large operating bandwidth, and high transmission contrast
are three important performance indicators.[282] There are nu- dI 𝛼I
= − o −1 − 𝛽I2 (39)
merous studies on the non-reciprocal light propagation due to dz 1 + Is
the non-linear discontinuity caused by the two materials being
close together.[139,283–285] Taking the research of Anand et al. as dI
= −𝛼o I − 𝛽I2 (40)
an example, Figure 9a,b illustrates the schematic diagram of the dz
diode based on asymmetric nonlinearity. Figure 9c shows the
change of the forward and reverse transmittance of graphene where Is is the saturated light intensity, and 𝛽 is the two-photon
with the light intensity. The propagation equation for two layers absorption coefficient.

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The nonlinear parameters of graphene/C60 are obtained by fit- tonic crystal.[294] The advent of 2D materials such as graphene
ting the z-scan data from the above two equations (Figure 9d). has led to the production of OB devices of smaller dimensions,
Precise control of the non-reciprocity factor is achieved by chang- lower operation power, shorter switching times, and lower
ing the nonlinear control methods, such as the number and con- thresholds.[295–299] Recently, the OB phenomenon has also
centration of graphene or C60 . In 2018, Wu et al. discovered the been observed through the SSPM effect of 2D materials (Fig-
reciprocity of the forward and reverse of the SSPM pattern by ure 10a).[300] When the laser is incident on a 2D material/PMMA
combining CsPbI3 QDs and Bi2 Se3 NSs for the first time (Fig- (PMMA has no nonlinear optical response), the SSPM effect is
ure 9e).[177] However, for this combination of CsPbI3 QDs and generated and the diffraction ring is excited. When the incident
Bi NSs, the non-reciprocity is relatively small (Figure 9f). The re- laser power increases from 0 to 116.54 W, the diffraction rings
ciprocal shape of the nonlinear photonic diode is not the same increase from 0 to 7, and the first diffraction ring appears at
as the widely studied nonlinear photon diode of transmittance 38 W. However, as the laser power decreases, the tendency of
reciprocity. Although these two methods of achieving light reci- the diffraction ring to decrease becomes weaker, and even at
procity employ the same configuration, in the experiments of lower powers (0.25 W), the diffraction ring can still be observed.
transmittance reciprocity, few researchers have pointed out the There is currently no reasonable explanation for this OB, and
existence of the SSPM effect. its physical mechanism is worthy of further investigation. When
Recently, Wu et al. used the SSPM effect to design an AOD the wavelengths of the excitation light are 532 (Figure 10b)
based on a 2D Te/SnS2 Ns dispersions mixed structure to achieve and 671 nm (Figure 1c), the change in the ring number si-
irreversible light propagation.[162] In this mixed structure, the 2D multaneously exhibits OB characteristics. Subsequently, Arpita
Te exhibits strong Kerr nonlinearity (n2 ≈ 105 cmW−1 ) and can et al. achieved three different cycles of OB based on the SSPM
be easily excited into a diffraction ring, SnS2 has a large band effect.[57] They paid more attention to the transmission OB
gap (2.6 eV),[286] and its diffraction ring is difficult to excite. Fur- characteristic than the diffraction ring, and bubble mediation
ther, SnS2 has been shown to exhibit the behavior of RSA.[287] is considered as its physical mechanism. As the input power
For the reverse direction of this AOD, when the incident light increases, the transmission signal increases almost linearly.
first passes through SnS2 , the light intensity is reduced due to When the power increases to a certain value, the transmission
its RSA property, and the light intensity incident to 2D Te is not signal suddenly drops to a very low value, and then decreases the
sufficient to excite the diffraction ring. For the forward direction power. The transmission signal continues to decrease on this
of this AOD, the diffraction ring has the same size and shape as basis, exhibiting OB characteristics.
the laser alone passing through 2D Te, except that the absorption
intensity of SnS2 is slightly weakened. Subsequently, Wu et al.
designed an AOD in 2D graphdiyne/SnS2 based on the same 5.5. Dark Hollow Beams Generation
method (Figure 9g,h).[52] The dry 2D SnS2 and graphdiyne were
mixed with polymethyl methacrylate (PMMA) to achieve an all- Dark hollow beams (DHB) are circular beams with a light
solid-state AOD (Figure 9i). Notably, when light passes through intensity of zero in the propagation direction, including
this AOD, due to the lack of non-axisymmetric thermal convec- hollow Gaussian beams (HGB), Laguerre–Gaussian beams
tion, the diffraction ring is not distorted in the vertical direction, (LGB), Bessel–Gaussian beam (BGB), and local hollow beams
which is advantageous for practical applications (Figure 9j,k). (LHB).[301] These have been applied in numerous fields, such as
Further, it has the characteristics of broadband response, and its laser processing,[302] optical tweezers,[303,304] optical imaging,[305]
reciprocity does not change with power (Figures 9l,m). More re- optical communication, and nonlinear optics,[306] owing to their
cently, Shan et al. demonstrated that the energy of incident pho- non-diffraction and self-healing characteristics. At present, the
tons determines whether AOD is effective.[169] For instance, in main methods for generating DHB are spatial light modulators
the case of 𝜆 = 532 and 671 nm, the AOD functions effectively, (SLMs) [307] and axicon lenses.[308] In 2014, Du et al. generated
whereas in the case of 𝜆 = 457 nm, the laser can excite the diffrac- DHB in the nonlinear crystal ZnSe.[309] In 2015, Zhang et al.
tion ring in both forward (Bi2 S3 /SnS2 ) and reverse directions found that the SSPM effect of Rb atoms is affected by the incident
(SnS2 /Bi2 S3 ), which means that the AOD fails to function nor- frequency and the atomic coefficient density.[310] In 2017, Swaim
mally. Once the conditions of use are met, this method of AOD re- et al. used the SSPM effect for the first time to generate a Bessel–
alization seems to be universally applicable for 2D materials (i.e., Gauss-like beam.[53] The output mode was controlled by chang-
AOD based on InSe/g-C3 N4 has also been realized).[52] Further, ing the optical power, temperature of atomic vapor, and laser
we have specifically studied the reciprocity of its transmittance. frequency. Figure 11a illustrates the diagram of the experimental
device for generating Bessel-like Gaussian beams, where A is the
typical output mode of SSPM; B and C are the patterns that have
5.4. Optical Bistability just been blocked and reconstructed after blocking. The local in-
tensity of the input mode will induce the soft hole effect of spatial
Optical bistability (OB) is a nonlinear optical phenomenon that variation, and the far-field interference is the basis of the far-field
corresponds to two states of stable output for a given input pattern conversion. Subsequently, Cheng et al. proposed a SXPM
state. OB has application prospects in numerous aspects, in- method to generate Bessel beams [54] (Figure 11b). The size of the
cluding optical transistors,[288] all-optical switching,[289] optical Bessel beam is adjusted by changing the power of the incident
memories,[290] and limiters.[291] The current methodologies for pump light and the concentration of the sample. Furthermore,
achieving OB are mainly the Fabry–Perot cavity,[292] surface compared with the method of generating a Bessel beam based on
plasmon,[293] guided mode resonance,[294] and nonlinear pho- SSPM, the method of generating Bessel beam based on SXPM

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Figure 10. OB in SSPM process. Reproduced with permission.[300] Copyright 2020, Wiley-VCH. a) The change of the diffraction ring pattern, as the
incident power increases and decreases. b) The number of diffraction rings changes as the incident power increases or decreases with𝜆 = 671nm. c)
The number of diffraction rings changes as the incident power increases or decreases with𝜆 = 532nm.

Figure 11. The generation of dark hollow beams. a) Schematic diagram of an experimental device for generating self-reconstructed Bessel-like beams
through SSPM. Reproduced with permission.[53] Copyright 2017, Springer Natere. b) Schematic diagram of the experimental setup for generating variable
parameter Bessel-like beams through SXPM. Reproduced with permission.[54] Copyright 2017, Optical Society of America. c) Schematic diagram of the
experimental setup for the hollow beam generated by the SXPM method for particle trapping and manipulation. Reproduced with permission.[311]
Copyright 2018, Institute of Physics. d) Schematic diagram of the experimental setup of the Bessel beam generated by the SXPM method for enhancing
conjugate degenerate four-wave mixing. Reproduced with permission.[312] Copyright 2018, Chinese Laser Press.

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www.advancedsciencenews.com www.ann-phys.org

Figure 12. Identify the vortex beam OAM pattern. a) Schematic diagram of the experiment to identify the OAM mode of vortex beam by SSPM. b)
Theory: SSPM diffraction pattern under uniform phase shift (Δ𝜓 = 12𝜋). c) Experiment: SSPM diffraction pattern at fixed excitation power (150 mW).
Reproduced with permission.[35] Copyright 2020, Institute of Physics.

has a lower threshold and can achieve the effective modulation have several disadvantages. Namely, the interference method
of weak light. In the same year, Zhang et al. proposed a method usually requires complicated equipment. Although the diffrac-
for simultaneously generating Bessel beam hollow beam based tion method is simple, the efficiency is very low, and it is difficult
on the SXPM effect.[55] Interestingly, the intensity distribution to detect high-order VB. Further, most previous studies on
of the Bessel beam obtained by this configuration is more stable, SSPM have used fundamental mode Gaussian beams to excite
and there are no specific requirements on the wavelength. diffraction rings. Recently, Su et al. employed VB light to stim-
He et al. captured the micron-level particles through the ulate SSPM for the first time [56] (Figure 12a). Interestingly, VB
hollow beam of ethanol generated by SXPM with an accuracy on interacts with 2D WS2 to excite a diffraction ring with a tail. More
the order of microns [311] (Figure 11c). The low intensity of the importantly, the magnitude of the OAM mode is the same as
hollow beam generated by SXPM will not damage the particles, the tail of the diffraction ring, and the sign is determined by the
indicating its potential for the in situ exploration of individual direction of the tail (Figure 12b). It has also been experimentally
particles. In 2018, Zhang et al. generated a Bessel beam through verified that the OAM pattern is easily identifiable (Figure 12c).
a thermo-optically nonlinear SXPM and realized twofold en- Furthermore, the phase shift is determined by the power,
hancement of the four-wave mixing signal [312] (Figure 11d). whereas the shape of the diffraction ring is basically unaffected
This method can generate non-diffractive length, adjustable size by it, as only the size and number of rings change. The OAM
Bessel beam, and optimize the generation of FWM. Recently, identification mode based on the SSPM method has a simple
Lin et al. generated a double-ring far-field diffraction pattern in device and is capable of measuring high-order modes, indicating
the Rb atomic vapor based on the SSPM and SXPM effects.[313] its great application potential in optical communication.
By controlling experimental parameters such as power, polar-
ization state of the incident beam, frequency detuning, and
atom density, a ring beam can be generated with very low input
6. Conclusions and Outlook
light intensity (0.5 W cm−2 ). Yao et al. generated ring beams SSPM distinguishes itself from other nonlinear optical effects
in various solvents through the SXPM effect, which indicates as a ubiquitous novel nonlinear optical effect. At present, it is
that the generation of ring beams may be universally realized attracting increasing attention, as it can realize a large number of
in 2D materials.[246] More recently, Lu et al. generated a hollow optical applications and possibly generate some novel nonlinear
Gaussian beam through SSPM and realized the transformation optical effects. However, the exploration of SSPM is still in its
with a quasi-hollow beam. The theoretical model constructed initial stages, as its physical mechanism is controversial. Appli-
shows that the quasi-hollow beam can be expressed as the super- cations based on SSPM are to date not sufficiently mature, which
position of different orders of the single hollow beam, and the implies both an opportunity and a challenge. Prospects and a
application of optical limiting was realized experimentally.[314] brief summary are provided here as some important directions in
Zhang et al. generated a dark hollow beam through SXPM and this area:
realized its conversion from the Bessel beam.[315]
– Establishing a consensus of understanding of SSPM and solv-
ing its physical origin or identifying its physical origin are
5.6. Recognition of Vortex Light Orbit Angular Momentum highly important tasks.
Patterns by SSPM – Novel nonlinear optical phenomena are expected to be discov-
ered in different SSPM excitation modes.
Optical vortex beams (VBs) are structured lights that carry – Measuring the nonlinear optical response of 2D materials
orbital angular momentum (OAM).[316] Based on the OAM op- through SSPM is a rapid process; however, the accuracy is not
tical communication, it is highly important to obtain the mode sufficiently high, and thus it is necessary to find ways to im-
of OAM.[317] The current methods for detecting OAM modes prove the measurement accuracy.
include interferometry and diffraction methods, such as the – The bandgap of 2D materials using SSPM is an interesting re-
Mach–Zehnder interferometer,[318] Sagnac interferometer,[319] search topic. Therefore, 2D materials with excellent properties
and diffraction grating.[320] However, these methods generally such as a controllable layer number and uniform surface are

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1900631.

Yunlong Liao is currently working toward a graduate degree in the Physics and Optoelectronic En-
gineering College, Shenzhen University, Shenzhen, China. His main research interest is nonlinear
optics.

Chunmei Song received her B.S. degree in Optoelectronic Information Science and Engineering from
Changchun University of Science and Technology, China, in 2018. At present, she is a graduate student
of the Physics and Optoelectronic Engineering College of Shenzhen University. Her main research is
nonlinear optics of 2D layered materials.

Yuanjiang Xiang received his Ph.D. degree in electronic circuits and systems from Hunan University,
Changsha, China, in 2011. He is currently a Professor at Hunan University, Changsha, China. His main
research interests include theory and simulation of nonlinear metamaterials and photonic crystals,
theory of optical solitons, and characterization of high performance optical switcher and optical filter
for optical communications.

Xiaoyu Dai received her Ph.D. degree in technology of computer application from Hunan University,
Changsha, China, in 2009. She is currently an Associate Professor at Hunan University, Changsha,
China. Her main research interests include theory of nonlinear metamaterials and optical solitons and
interaction of electromagnetic waves with matter.

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