de gruyter · web viewfigure s5.sem images from left to right show cross section of bulk feps 3...
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Supporting Information
Danyun Xu, Zhe Guo, Yudi Tu, Xinzhe Li, Yu Chen, Zhesheng Chen, Bingbing Tian, Shuqing Chen, Yumeng Shi, Ying Li, Chenliang Su, and Dianyuan Fan
Controllable Nonlinear Optical Properties of
Different-Sized Iron Phosphorus Trichalcogenide
(FePS3) Nanosheets
Corresponding authors: Bingbing Tian and Shuqing Chen, International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen, 518060, China, E-mail:[email protected]; [email protected] Xu, Zhe Guo, Yudi Tu, Xinzhe Li, Yu Chen, Zhesheng Chen, Yumeng Shi, Ying Li, Chenliang Su, and Dianyuan Fan:International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen, 518060, ChinaZhesheng Chen: Laboratoire de Physique des Solides, CNRS, Université Paris Saclay, Orsay 91405, France
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1. Photography of bulk FePS3 crystals
Figure S1. (a) Photograph of bulk FePS3 crystals obtained by CVT method in an
evacuated quartz tube. (b) Bulk FePS3 crystals are shown in opened quartz tube with a
radius of 5.5 mm.
2. XRD spectra of Bulk FePS3 crystals
Figure S2. XRD spectra of bulk FePS3 crystals
3. XRD spectra of exfoliated FePS3 nanosheets
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Figure S3. (a) XRD spectra of exfoliated FePS3 nanosheets. (b) XRD spectra of
exfoliated FePS3 nanosheets and bulk crystals with 2 Theta range from 20 to 80
degree.
4. Illumination of electrochemical exfoliation process
Figure S4. Photograph of the morphology and volume change of the bulk FePS3
crystals with reaction time during electrochemical cathodic exfoliation.
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Figure S5. SEM images from left to right show cross section of bulk FePS3 crystals
and FePS3 crystals after employing a DC bias voltage of -2.5 V for 1 min
(intercalation) and 2 min (expansion) by using tera-n-butylammonium as an
electrolyte salt respectively.
5. The process of gradient centrifugation
Figure S6. Procedure illustration of the gradient centrifugation to obtain the different
sized FePS3 nanosheets.
6. Stability of the FePS3 nanosheets suspensions
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Figure S7. Transmittance spectra of FePS3 nanosheets suspensions from 300 to 1000
nm. Here take the FePS3 nanosheets suspensions obtained at centrifugal speed of 5000
rpm as an example. Here the transmittance of the FePS3 nanosheets at the wavelength
of 532 nm and 633 nm are respectively 13.93% and 18.71%.
7. Determination of lateral size distribution
Methods: an image J software was used to obtain the lateral area (S) of each
nanosheets from the raw AFM, SEM or optical images. The corresponding formula
S=π(D/2)^2 was applied to approximate the lateral size (D) of these nanosheets.
Figure S8. Raw AFM data for lateral size analysis.
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Figure S9. The corresponding profiles of these nanosheets in Figure S5 analyzed by
image J.
8. Determination of thickness distributions
Figure S10. Raw AFM data for thickness analysis.
9. Sizes distribution
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Figure S11. (a) Comprehensive statistics of all nanosheets obtained under the
centrifugal speed of 1000 rpm or above. Lateral dimension distribution diagrams at
different centrifugation speeds of 1000 rpm (b), 3000 rpm (c), 5000 rpm (d), 7000
rpm (e) and 9000 rpm (f), which were measured by particle size description analyser
(PSDA).
10. TEM images
Figure S12. TEM images of FePS3 nanosheets under different centrifugation speeds
of 1000 rpm (a), 3000 rpm (b), 5000 rpm (c), 7000 rpm (d) and 9000 rpm (e) with the
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corresponding scale bar of 1 μm. (f) Mapping analysis of representative FePS3
nanosheet obtained at a centrifugation speed of 5000 rpm with a scale bar of 200 nm.
11. Raman analysis
Figure S13. The Raman spectrum of the silicon substrate at 532 nm laser excitation
wavelength [1].
12. Nonlinear optical properties of different sized FePS3 nanosheets with
different incident intensities
Figure S14. The diffraction rings of the FePS3 dispersion at 5000 rpm obtained by
CCD at λ = 532 nm with different incident intensities.
13. Equations for Power-Dependent Nonlinear Refractive Index
Under the conditions of D ≫ RH or R’H, the relation can be expressed as[2, 3]:
θH =RH
D (1)
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θH' =
RH'
D (2)
θD = θH - θH' =
RD
D (3)
θH = λ2π
(dΔψdr )
max (4)
θH =n2 IC (5)
Here, C= [- 8r Leff
ω02 exp (-2 r2
ω02 )] , r∈[0, +⋈ ) (6) is a constant.
θD =θH - θH' = (n2- n2
' ) IC= ∆ n2 IC (7)
∆ n2
n2 =
θD
θH
(8)
14. n2 and χsingle layer(3) of various two-dimensional materials
Table 1 n2 and χsingle layer(3) of various two-dimensional materials
2D materials Wavelength (nm)
n2 (m2 W–
1)χsingle layer
(3)
(e . s . u .)
Ref.
Graphene 473 10–7 10–7 [4] and [5]532 10–7 10–7
MoS2 488 10–7 10–9
BP 600 10–5 10–8 [6]700 10–5 10–8
1160 10–5 10–8
NbSe2 457 10–5 10–9 [7]532 10–5 10–9
671 10–5 10–9
WSe2 457 10–9 10–6 [8]532 10–10 10–6
671 10–11 10–6
FePS3 532 10–5 10–9 This work
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633 10–5 10–9
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