KAg3Ga8S14: 一种高激光损伤阈值的中远红外非线性光学材料※

doi:10.6023/A21120585

化学学报 ›› 2022, Vol. 80 ›› Issue (3): 259-264.DOI: 10.6023/A21120585 上一篇下一篇

所属专题：中国科学院青年创新促进会合辑

研究论文

KAg₃Ga₈S₁₄: 一种高激光损伤阈值的中远红外非线性光学材料^※

赵锦旭^a^,^b, 张铭枢^a, 陈文发^a, 姜小明^a, 刘彬文^a^,^*(), 郭国聪^a^,^*()

a 中国科学院福建物质结构研究所结构化学国家重点实验室福州 350002
b 上海科技大学物质科学与技术学院上海 201210

投稿日期:2021-12-27 发布日期:2022-01-12
通讯作者: 刘彬文, 郭国聪
作者简介:
^※ 庆祝中国科学院青年创新促进会十年华诞.
基金资助:
国家自然科学基金(22075283); 国家自然科学基金(92161125); 中国科学院青年创新促进会(2021300)

KAg₃Ga₈S₁₄: An Mid- and Far-infrared Nonlinear Optical Material Exhibiting High Laser-induced Damage Threshold^※

Jinxu Zhao^a^,^b, Mingshu Zhang^a, Wenfa Chen^a, Xiaoming Jiang^a, Binwen Liu^a(), Guocong Guo^a()

a State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China
b School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China

Received:2021-12-27 Published:2022-01-12
Contact: Binwen Liu, Guocong Guo
About author:
^※ Dedicated to the 10th anniversary of the Youth Innovation Promotion Association, CAS.
Supported by:
National Natural Science Foundation of China(22075283); National Natural Science Foundation of China(92161125); Youth Innovation Promotion Association of CAS(2021300)

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摘要/Abstract

兼具大的非线性光学(NLO)效应和高的激光损伤阈值(LIDT)是中远红外NLO材料领域最具挑战性的问题之一. 这里, 将碱金属离子K⁺引入到以黄铜矿AgGaS₂为基底的材料中, 获得硫属化合物KAg₃Ga₈S₁₄. 它的晶体结构采用与黄铜矿相类似的三维蜂窝状开放框架, 其中畸变四面体GaS₄和AgS₄以高度定向的方式排列, 产生中等的倍频效应 (0.4×AgGaS₂ @1910 nm). 值得注意的是, 通过拓宽带隙(2.95 eV), 该化合物拥有高的激光损伤阈值(4.6×AgGaS₂ @1064 nm). 此外, 通过理论计算表明四面体GaS₄和AgS₄决定硫属化合物KAg₃Ga₈S₁₄的NLO光学性质.

关键词: 硫属化合物, 非线性光学, 倍频效应, 激光损伤阈值, 晶体结构

Nonlinear optical (NLO) crystals can produce tunable lasers due to their second-harmonic generation, sum-frequency generation, difference-frequency generation and optical parametric oscillation. The famous oxide-based NLO materials such as KH₂PO₄ (KDP), β-BaB₂O₄ (BBO) and LiB₃O₅ (LBO) are widely used in ultraviolet-visible (UV-Vis) region. Nevertheless, they are not suitable for the mid- and far-infrared region because of the strong absorption there. Currently, commercially available IR NLO materials are rare, such as chalcogenides AgGaS₂ (AGS), AgGaSe₂ and phosphorus ZnGeP₂, which have the advantages of large NLO coefficient and wide transmission range, but they have drawbacks, like low laser- induced damage threshold (LIDT). Discovering NLO crystals that exhibit simultaneously large NLO and high LIDT is a huge challenge. Here, the introducing electropositive alkali metal ionic K⁺ in chalcopyrite AGS successfully affords a new sulfide KAg₃Ga₈S₁₄by high temperature solid state reaction. Its crystal structure adopts a three-dimensional honeycomb-like open framework, in which all tetrahedral AgS₄ and GaS₄ units are arranged in a highly oriented manner, thereby producing about a medium phase-matching second harmonic generation (SHG) response of 0.4 times that of the benchmark AGS at the incident laser of 1910 nm. Remarkably, the compound possesses a wide band gap (2.95 eV), thus avoiding two-photon absorption of the incident 1064 nm laser, and exhibits a high LIDT of 4.6 times that of the AGS at the laser of 1064 nm. Moreover, KAg₃Ga₈S₁₄ has a wide transmission range (0.25—25.0 μm) that covers the two important atmospheric windows of 3—5 and 8—12 μm. Furthermore, according to theoretical calculations, the conductive band is mostly composed of Ga-4s and S-3p states, mixing with small amounts of Ga-4p state, whereas the valence band near the Fermi level originates predominately from Ag-4p and S-3p states, mixing with small amounts of Ga-4p state, indicating that tetrahedral GaS₄ and AgS₄ units govern the optical and NLO properties of chalcopyrite KAg₃Ga₈S₁₄.

Key words: chalcogenide, nonlinear optical, second harmonic generation, laser damage threshold, crystal structure

引用此文

赵锦旭, 张铭枢, 陈文发, 姜小明, 刘彬文, 郭国聪. KAg₃Ga₈S₁₄: 一种高激光损伤阈值的中远红外非线性光学材料^※[J]. 化学学报, 2022, 80(3): 259-264.

Jinxu Zhao, Mingshu Zhang, Wenfa Chen, Xiaoming Jiang, Binwen Liu, Guocong Guo. KAg₃Ga₈S₁₄: An Mid- and Far-infrared Nonlinear Optical Material Exhibiting High Laser-induced Damage Threshold^※[J]. Acta Chimica Sinica, 2022, 80(3): 259-264.

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Empirical formula	KAg₃Ga₈S₁₄
Fw	1369.31
Temperature/K	293(2)
Space group	Cm
a/nm	1.23185(6)
b/nm	1.11823(4)
c/nm	0.92501(4)
α/(°)	90
β/(°)	115.661(4)
γ/(°)	90
Volume/nm³	1.14852(9)
Z	2
D_calc/(g•cm^-3)	3.960
μ/mm^-1	13.161
GOF on F²	1.062
R₁^a [I≥2σ (I)]	0.0172
wR₂^b [I≥2σ (I)]	0.0350
R₁^a [all data]	0.0176
wR₂^b [all data]	0.0351
Flack	0.032(10)
(Δρ_max/Δρ_min)/(e•nm^-3)	820/–500

Empirical formula	KAg₃Ga₈S₁₄
Fw	1369.31
Temperature/K	293(2)
Space group	Cm
a/nm	1.23185(6)
b/nm	1.11823(4)
c/nm	0.92501(4)
α/(°)	90
β/(°)	115.661(4)
γ/(°)	90
Volume/nm³	1.14852(9)
Z	2
D_calc/(g•cm^-3)	3.960
μ/mm^-1	13.161
GOF on F²	1.062
R₁^a [I≥2σ (I)]	0.0172
wR₂^b [I≥2σ (I)]	0.0350
R₁^a [all data]	0.0176
wR₂^b [all data]	0.0351
Flack	0.032(10)
(Δρ_max/Δρ_min)/(e•nm^-3)	820/–500

Bond	Distance/nm	Bond	Distance/nm
K1—S5	0.3496(4)	Ga1—S1	0.2319(1)
K1—S5	0.3496(4)	Ga1—S3	0.2308(2)
K1—S6	0.3436(2)	Ga1—S4	0.2251(9)
K1—S6	0.3436(2)	Ga1—S6	0.2235(9)
K1—S7	0.3445(2)	Ga2—S1	0.2348(4)
K1—S7	0.3445(2)	Ga2—S6	0.2256(2)
K1—S8	0.3297(3)	Ga2—S7	0.2259(2)
K1—S9	0.3312(3)	Ga2—S9	0.2266(2)
Ag1—S2	0.2591(2)	Ga3—S1	0.2318(2)
Ag1—S4	0.2534(2)	Ga3—S2	0.2250(4)
Ag1—S7	0.2490(5)	Ga3—S3	0.2322(2)
Ag1—S7	0.2490(5)	Ga3—S5	0.2250(1)
Ag2—S4	0.2616(2)	Ga4—S3	0.2370(2)
Ag2—S5	0.2573(8)	Ga4—S5	0.2259(2)
Ag2—S5	0.2573(8)	Ga4—S7	0.2262(2)
Ag2—S9	0.2564(5)	Ga4—S8	0.2271(1)
Ag3—S2	0.2602(2)
Ag3—S6	0.2518(6)
Ag3—S6	0.2518(6)
Ag3—S8	0.2492(2)

Bond	Distance/nm	Bond	Distance/nm
K1—S5	0.3496(4)	Ga1—S1	0.2319(1)
K1—S5	0.3496(4)	Ga1—S3	0.2308(2)
K1—S6	0.3436(2)	Ga1—S4	0.2251(9)
K1—S6	0.3436(2)	Ga1—S6	0.2235(9)
K1—S7	0.3445(2)	Ga2—S1	0.2348(4)
K1—S7	0.3445(2)	Ga2—S6	0.2256(2)
K1—S8	0.3297(3)	Ga2—S7	0.2259(2)
K1—S9	0.3312(3)	Ga2—S9	0.2266(2)
Ag1—S2	0.2591(2)	Ga3—S1	0.2318(2)
Ag1—S4	0.2534(2)	Ga3—S2	0.2250(4)
Ag1—S7	0.2490(5)	Ga3—S3	0.2322(2)
Ag1—S7	0.2490(5)	Ga3—S5	0.2250(1)
Ag2—S4	0.2616(2)	Ga4—S3	0.2370(2)
Ag2—S5	0.2573(8)	Ga4—S5	0.2259(2)
Ag2—S5	0.2573(8)	Ga4—S7	0.2262(2)
Ag2—S9	0.2564(5)	Ga4—S8	0.2271(1)
Ag3—S2	0.2602(2)
Ag3—S6	0.2518(6)
Ag3—S6	0.2518(6)
Ag3—S8	0.2492(2)

Bond	Angle/(°)	Bond	Angle/(°)
S6—K1—S6	70.64(7)	S4—Ga1—S1	104.51(6)
S6—K1—S7	101.95(8)	S4—Ga1—S3	110.72(6)
S6—K1—S7	61.16(4)	S6—Ga1—S1	111.14(6)
S7—K1—S5	61.36(3)	S6—Ga1—S3	116.20(6)
S7—K1—S5	133.90(7)	S6—Ga1—S4	107.34(6)
S7—K1—S5	133.89(7)	S6—Ga2—S1	108.19(6)
S7—K1—S7	73.19(6)	S6—Ga2—S7	115.76(6)
S8—K1—S5	88.42(4)	S6—Ga2—S9	104.80(7)
S8—K1—S6	124.55(6)	S7—Ga2—S1	110.09(6)
S8—K1—S7	63.44(5)	S7—Ga2—S9	104.53(6)
S8—K1—S9	168.34(10)	S9—Ga2—S1	113.49(7)
S9—K1—S5	89.48(4)	S1—Ga3—S3	109.81(6)
S9—K1—S6	64.10(5)	S2—Ga3—S1	108.62(6)
S9—K1—S7	124.94(7)	S2—Ga3—S3	109.34(7)
S4—Ag1—S2	96.10(7)	S5—Ga3—S1	106.19(6)
S7—Ag1—S2	107.33(5)	S5—Ga3—S2	116.45(7)
S7—Ag1—S7	111.08(7)	S5—Ga3—S3	106.28(6)
S5—Ag2—S4	106.49(5)	S5—Ga4—S3	103.62(6)
S5—Ag2—S5	113.54(7)	S5—Ga4—S7	112.28(6)
S9—Ag2—S4	97.06(7)	S5—Ga4—S8	123.47(6)
S9—Ag2—S5	115.49(4)	S7—Ga4—S3	105.67(6)
S6—Ag3—S2	101.87(5)	S7—Ga4—S8	103.00(6)
S6—Ag3—S2	101.88(5)	S8—Ga4—S3	107.60(6)
S6—Ag3—S6	104.13(8)

KAg₃Ga₈S₁₄: 一种高激光损伤阈值的中远红外非线性光学材料^※

KAg₃Ga₈S₁₄: An Mid- and Far-infrared Nonlinear Optical Material Exhibiting High Laser-induced Damage Threshold^※

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样品	能量/ mJ	光斑面积/ mm²	脉冲宽度/ns	LIDT/ (MW•cm^-2)
AGS	3.2	4.1	10	2.4
KAg₃Ga₈S₁₄	14.6	4.1	10	11.1

样品	能量/ mJ	光斑面积/ mm²	脉冲宽度/ns	LIDT/ (MW•cm^-2)
AGS	3.2	4.1	10	2.4
KAg₃Ga₈S₁₄	14.6	4.1	10	11.1