Microscopic nonlinear optical activities and ultrafast carrier dynamics in layered AgInP<sub>2</sub>S<sub>6</sub>

Zixin Wang; Ningning Dong; Yu Mao; Chenduan Chen; Xin Chen; Chang Xu; Zhouyuan Yan; Jun Wang

doi:10.1364/PRJ.510142

Photonics Research, Volume. 12, Issue 4, 691(2024)

Microscopic nonlinear optical activities and ultrafast carrier dynamics in layered AgInP₂S₆

Zixin Wang^1,2, Ningning Dong^1,2,3,4, Yu Mao^1,2, Chenduan Chen^1,2, Xin Chen^1,2, Chang Xu¹, Zhouyuan Yan^1,2, and Jun Wang^1,2,3、*

Author Affiliations

¹Aerospace Laser Technology and Systems Department, CAS Key Laboratory of Materials for High-Power Laser, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai 201800, China

²Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

³CAS Center for Excellence in Ultra-intense Laser Science (CEULS), State Key Laboratory of High Field Laser Physics, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences, Shanghai 201800, China

⁴e-mail: n.n.dong@siom.ac.cn

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Fig. 1. (a) Typical XRD pattern of AgInP2S6 crystal. (b) XPS survey scan and (c) Ag 3d, (d) In 3d, (e) P 2p, and (f) S 2p region of AgInP2S6. Black dots and red solid lines represent experimental and fitting results, respectively. (g) TEM image of AgInP2S6. The top-right inset is the SAED. (h) SEM image and (i) EDS results of AgInP2S6.

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Fig. 2. (a) Optical image of AgInP2S6 flakes with different thicknesses exfoliated on a quartz substrate. (b) Room temperature Raman spectra obtained under 532 nm CW laser excitation. (c) UV-visible absorption spectra of AgInP2S6 flakes. (d) Tauc plots and the optical bandgap of AgInP2S6 flakes with different thicknesses.

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Fig. 3. Theoretical band structure of (a) monolayer, (b) 10 nm, (c) 100 nm, and (d) 400 nm AgInP2S6. (e) Theoretical bandgap as a function of thickness.

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Fig. 4. (a) Schematic of the μ-Z/I-scan setup used for the nonlinear optical activities experiment. (b) Open-aperture and (d) closed-aperture Z-scan results of the 443.74 nm AgInP2S6 flake at 520 nm femtosecond pulse. (c) Open-aperture and (e) closed-aperture Z-scan results of 443.74 nm AgInP2S6 flake at 1040 nm femtosecond pulse.

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Fig. 5. Relationship graphs between ln(1−T(z)) and ln(I) of 443.74 nm AgInP2S6 flake under the excitation of (a)–(c) 520 nm and (d)–(f) 1040 nm femtosecond pulses.

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Fig. 6. μ-I-scan results of the AgInP2S6 flakes under the excitation of (a) 520 nm and (b) 1040 nm femtosecond pulses, respectively.

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Fig. 7. (a) Schematic of the μ-pump-probe setup used for the ultrafast carrier dynamics experiment. Carrier relaxation process with different pump intensities of the (b) 443.74 nm and (c) 102.95 nm AgInP2S6 flakes. The insets shows ΔR/R versus the pump intensity at zero-time delay. (d) Excitation intensity-dependent PL spectra of 443.74 nm AgInP2S6 obtained under CW laser excitation at 532 nm. (e) Maximum PL intensity as a function of excitation intensity.

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Table 1. Linear and Nonlinear Optical Parameters of the 443.74 nm AgInP₂S₆ Flake

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Table 1. Linear and Nonlinear Optical Parameters of the 443.74 nm AgInP₂S₆ Flake

Thickness (nm)	Laser (nm)	$α_{0}$ ( ${cm}^{- 1}$ )	$β_{0}$ (cm/GW)	$Im χ^{(3)}$ (esu)	${FOM}_{Im}$ (esu cm)	$n_{2}$ ( ${cm}^{2} / W$ )	$Re χ^{(3)}$ (esu)	${FOM}_{Re}$ (esu cm)
443.74	520	8098.79	21.33	$4.34 \times 10^{- 13}$	$5.37 \times 10^{- 17}$	$3.26 \times 10^{- 14}$	$1.02 \times 10^{- 17}$	$1.26 \times 10^{- 21}$
443.74	1040	1753.39	1.21	$6.73 \times 10^{- 14}$	$3.84 \times 10^{- 17}$	$- 3.60 \times 10^{- 15}$	$- 1.54 \times 10^{- 18}$	$- 8.78 \times 10^{- 22}$

Table 2. Fitting Parameters of the AgInP₂S₆ Flakes

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Table 2. Fitting Parameters of the AgInP₂S₆ Flakes

	520 nm				1040 nm
Thickness (nm)	$β_{0}$ (cm/GW)	$I_{s}$ ( $GW / {cm}^{2}$ )	$Im χ^{(3)}$ (esu)	${FOM}_{Im}$ (esu cm)	$β_{0}$ (cm/GW)	$I_{s}$ ( $GW / {cm}^{2}$ )	$Im χ^{(3)}$ (esu)	${FOM}_{Im}$ (esu cm)
11.14	$6.06 \times 10^{2}$	$3.48 \times 10^{1}$	$1.23 \times 10^{- 11}$	$1.23 \times 10^{- 16}$	$9.79 \times 10^{1}$	$0.60 \times 10^{2}$	$5.44 \times 10^{- 12}$	$9.72 \times 10^{- 17}$
21.15	$5.17 \times 10^{2}$	$6.18 \times 10^{1}$	$1.05 \times 10^{- 11}$	$7.14 \times 10^{- 17}$	$9.10 \times 10^{1}$	$2.49 \times 10^{2}$	$5.06 \times 10^{- 12}$	$9.45 \times 10^{- 17}$
23.76	$5.01 \times 10^{2}$	$7.49 \times 10^{1}$	$1.02 \times 10^{- 11}$	$5.96 \times 10^{- 17}$	$8.07 \times 10^{1}$	$3.80 \times 10^{2}$	$4.49 \times 10^{- 12}$	$6.48 \times 10^{- 17}$
29.29	$4.16 \times 10^{2}$	$8.79 \times 10^{1}$	$8.47 \times 10^{- 12}$	$4.80 \times 10^{- 17}$	$7.61 \times 10^{1}$	$5.53 \times 10^{2}$	$4.23 \times 10^{- 12}$	$6.12 \times 10^{- 17}$
102.95	$1.11 \times 10^{2}$	$7.33 \times 10^{1}$	$2.26 \times 10^{- 12}$	$7.56 \times 10^{- 17}$	$6.35 \times 10^{1}$	$6.12 \times 10^{2}$	$3.53 \times 10^{- 12}$	$7.14 \times 10^{- 17}$
443.74	$0.22 \times 10^{2}$	$8.08 \times 10^{1}$	$4.48 \times 10^{- 13}$	$5.53 \times 10^{- 17}$	$0.25 \times 10^{1}$	$6.18 \times 10^{2}$	$1.39 \times 10^{- 13}$	$7.93 \times 10^{- 17}$

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Zixin Wang, Ningning Dong, Yu Mao, Chenduan Chen, Xin Chen, Chang Xu, Zhouyuan Yan, Jun Wang. Microscopic nonlinear optical activities and ultrafast carrier dynamics in layered AgInP₂S₆[J]. Photonics Research, 2024, 12(4): 691

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Paper Information

Category: Nonlinear Optics

Received: Oct. 27, 2023

Accepted: Jan. 23, 2024

Published Online: Mar. 20, 2024

The Author Email: Jun Wang (jwang@siom.ac.cn)

DOI:10.1364/PRJ.510142

Topics

laser devices and laser physics

Lasers and Laser Optics

Laser physics

laser manufacturing

Instrumentation, Measurement and Metrology

Table 1. Linear and Nonlinear Optical Parameters of the 443.74 nm AgInP2S6 Flake

Table 1. Linear and Nonlinear Optical Parameters of the 443.74 nm AgInP2S6 Flake

Table 2. Fitting Parameters of the AgInP2S6 Flakes

Table 2. Fitting Parameters of the AgInP2S6 Flakes

Table 1. Linear and Nonlinear Optical Parameters of the 443.74 nm AgInP₂S₆ Flake

Table 1. Linear and Nonlinear Optical Parameters of the 443.74 nm AgInP₂S₆ Flake

Table 2. Fitting Parameters of the AgInP₂S₆ Flakes

Table 2. Fitting Parameters of the AgInP₂S₆ Flakes