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二硒化锗(GeSe2)作为一种层状IV-VI族半导体, 具有面内各向异性结构及宽能带间隙, 表现出了独特的光、电及热学性能. 本文利用偏振拉曼光谱和线性吸收谱分别对GeSe2纳米片的晶轴取向和能带特性进行表征, 并以此为依据采用微区I扫描系统研究了GeSe2在共振能带附近的光学非线性吸收机制. 结果表明, GeSe2中非线性吸收机制为饱和吸收与激发态吸收的叠加, 且对入射光偏振与波长均有强烈的依赖. 近共振激发(450 nm)条件下, 激发态吸收对偏振的依赖程度比较大, 随着入射光偏振的不同, 非线性调制深度可由4.6%变化至9.9%; 而非共振激发(400 nm)时, 该调制深度仅由7.0%变化至9.7%. 同时, 相比于饱和吸收, 激发态吸收的偏振依赖程度受远离共振激发波长的影响而变化更大.Germanium diselenide (GeSe2), a layered IV-VI semiconductor, has an in-plane anisotropic structure and a wide band gap, exhibiting unique optical, electrical, and thermal properties. In this paper, polarization axis Raman spectrum and linear absorption spectrum are used to characterize the crystal axis orientation and energy band characteristics of GeSe2 flake, respectively. Based on the results, a micro-domain I scan system is used to study the optical nonlinear absorption mechanism of GeSe2 near the resonance band. The results show that the nonlinear absorption mechanism in GeSe2 is a superposition of saturation absorption and excited state absorption, and is strongly dependent on the polarization and wavelength of incident light. Under near-resonance excitation (450 nm), the excited state absorption is more greatly dependent on polarization. With different polarizations of incident light, the modulation depth can be changed from 4.6% to 9.9%; for non-resonant excitation (400 nm), the modulation depth only changes from 7.0% to 9.7%. At the same time, compared with saturation absorption, the polarization-dependent excited state absorption is greatly affected by the distance away from the resonance excitation wavelength.
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Keywords:
- anisotropy /
- excited state absorption /
- micro-domain I-scan
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图 1 (a) GeSe2原子结构示意图; (b) 机械剥离GeSe2纳米片的AFM图, 样品的厚度为88 nm; (c) 偏振选择的拉曼光谱, 其中4个拉曼峰位置分别在118, 212, 251, 307 cm–1; (d)—(g) 4个拉曼峰强度分别对应的极坐标示意图
Fig. 1. (a) Schematic diagram of the atomic structure of GeSe2; (b) AFM image of GeSe2 flake by mechanical exfoliation. The thickness of the sample is 88 nm; (c) polarization-dependent Raman spectrum. Four Raman peak positions are at 118, 212, 251, 307 cm–1, respectively; (d)–(g) polar diagrams of the intensity of the four Raman peaks.
图 2 线性吸收谱对层状GeSe2的各向异性能带表征 (a) 0°—180°偏振方向的线性吸收谱, 其中间隔15°; (b) 0°偏振方向的能带确定; 由陶克定理间接得到的能带位置, 其中切线与横坐标交点位置为2.717 eV; (c) 90°偏振方向的能带确定; 由陶克定理间接得到的能带位置, 其中切线与横坐标交点位置为2.7291 eV; (d) 层状GeSe2的各向异性能带; b轴方向上的带隙最大, 而a轴方向的带隙最小; (e) 层状GeSe2在400 nm处的各向异性线性吸收率极坐标图; (f) 层状GeSe2在450 nm处的各向异性线性吸收率极坐标图
Fig. 2. Characterization of anisotropic bands of layered GeSe2 by linear absorption spectrum: (a) Linear absorption spectrum with polarization directions from 0° to 180° with intervals of 15°; (b) the energy band of the 0° polarization direction is determined. The band position obtained indirectly from Tauc’s theorem, where the position of the intersection of the tangent and the abscissa is 2.717 eV; (c) determination of the energy band of the 90° polarization direction. The band position obtained indirectly from Tauc’s theorem, where the position of the intersection of the tangent and the abscissa is 2.7291 eV; (d) anisotropic energy bands of layered GeSe2. The band gap in the b-axis direction is the largest, and the band gap in the a-axis direction is the smallest; (e) polar graph of anisotropic linear absorptivity of layered GeSe2 at 400 nm; (f) polar graph of anisotropic linear absorption of layered GeSe2 at 450 nm.
图 3 400 nm非共振激发下不同偏振方向的叠加态吸收实验结果 (a) I扫描实验结果, 圆圈表示实验数据, 实线表示激发态吸收拟合曲线; (b) 偏振相关的非线性调制深度极坐标图; (c) 偏振相关的线性吸收系数α0变化趋势极坐标图; (d) 偏振相关饱和吸收光强I1,s极坐标图; (e) 偏振相关的激发态吸收系数β0变化趋势极坐标图; (f) 激发态吸收的偏振相关饱和光强I2,s极坐标图
Fig. 3. Experimental results of superposition state absorption of different polarization directions under 400 nm non-resonant excitation: (a) Results of the I-scan experiment. The circles indicate the experimental data, and the solid lines indicate the excited state absorption curve; (b) polarization-dependent non-linear modulation depth polar plot; (c) polar plot of the change in polarization-dependent linear absorption coefficient α0; (d) polarization diagram of polarization-dependent saturated absorption intensity I1,s; (e) polarization diagram of the polarization-dependent excited state absorption coefficient β0; (f) polarized graph of polarization-dependent saturation light intensity I2,s absorbed by the excited state.
图 4 450 nm近共振激发下不同偏振方向的叠加态吸收实验结果 (a) I扫描实验结果, 圆圈表示实验数据, 实线表示激发态吸收拟合曲线; (b) 偏振相关的非线性调制深度极坐标图; (c) 偏振相关的线性吸收系数α0变化趋势极坐标图; (d) 饱和吸收的偏振相关饱和光强I1,s极坐标图; (e) 偏振相关的激发态吸收系数β0变化趋势极坐标图; (f) 激发态吸收的偏振相关饱和光强I2,s极坐标图
Fig. 4. Experimental results of superposition state absorption of different polarization directions under 450 nm non-resonant excitation: (a) Results of the I-scan experiment. The circles indicate the experimental data, and the solid lines indicate the excited state absorption curve: (b) polarization-dependent non-linear modulation depth polar plot: (c) polar plot of the change in polarization-dependent linear absorption coefficient α0; (d) polarization diagram of polarization-dependent saturated absorption intensity I1,s; (e) polarization diagram of the polarization-dependent excited state absorption coefficient β0; (f) polarized graph of polarization-dependent saturation light intensity I2,s absorbed by the excited state.
图 5 GeSe2偏振型全光开关的原理示意图
Fig. 5. Schematic diagram of GeSe2 based polarized-dependent all-optical switching
表 1 400 nm非共振激发偏振相关的I扫描非线性叠加态吸收参数的拟合结果
Table 1. Fitting results of I-scan nonlinear superposition state absorption parameters related to 400 nm non-resonant excitation polarization
Polarization/(°) α0/cm–1 β0/cm·GW–1 I1,s/GW·cm–2 I2,s/GW·cm–2 δT/% 0 31559 508 15947 41 7.0 30 33593 559 7962 38 7.5 60 36579 606 972 35 8.2 90 38790 663 349 34 9.7 120 36972 599 1394 36 8.1 150 34029 543 6629 39 7.3 180 31062 496 17082 41 7.0 
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表 2 450 nm近共振激发偏振相关的I扫描非线性叠加态吸收参数的拟合结果
Table 2. Fitting results of I-scan nonlinear superposition state absorption parameters related to 450 nm non-resonant excitation polarization
Polarization/(°) α0/cm–1 β0/cm·GW–1 I1,s/GW·cm–2 I2,s/GW·cm–2 δT/% 0 43909 175 9390 63 4.6 30 49631 157 1258 69 5.6 60 60289 65 409 75 7.1 90 67501 22 188 79 9.9 120 57266 81 469 76 6.8 150 48345 158 2333 68 5.0 180 43173 176 10483 62 4.6
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[1] Novoselov K S, Geim A K, Morozov S V, Jiang D, Zhang Y, Dubonos S V, Grigorieva I V, Firsov A A 2004 Science 306 666
Google Scholar
[2] Jiang T, Liu H, Huang D, Zhang S, Li Y, Gong X, Shen Y R, Liu W T, Wu S 2014 Nat. Nanotechnol. 9 825
Google Scholar
[3] Zhang J, Ouyang H, Zheng X, You J, Chen R, Zhou T, Sui Y, Liu Y, Cheng X, Jiang T 2018 Opt. Lett. 43 243
Google Scholar
[4] Wang R, Ruzicka B A, Kumar N, Bellus M Z, Chiu H Y, Zhao H 2012 Phys. Rev. B 86 045406
Google Scholar
[5] 令维军, 夏涛, 董忠, 刘勍, 路飞平, 王勇刚 2017 物理学报 66 114207
Google Scholar
Ling W J, Xia T, Dong Z, Liu Q, Lu F P, Wang Y G 2017 Acta Phys. Sin. 66 114207
Google Scholar
[6] Hu Y, Jiang T, Zhou J, Hao H, Sun H, Ouyang H, Tong M, Tang Y, Li H, You J, Zheng X, Xu Z, Cheng X 2019 Nano Energy 68 104280
Google Scholar
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Google Scholar
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Google Scholar
[9] Sobota J A, Yang S L, Kemper A F, Lee J J, Schmitt F T, Li W, Moore R G, Analytis J G, Fisher I R, Kirchmann P S, Devereaux T P, Shen Z X 2013 Phys. Rev. Lett. 111 136802
Google Scholar
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Google Scholar
[11] Jiang T, Miao R, Zhao J, Xu Z, Zhou T, Wei K, You J, Zheng X, Wang Z, Cheng X A 2019 Chin. Opt. Lett. 17 020005
Google Scholar
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Google Scholar
Liu C, Liu X R 2019 Acta Phys. Sin. 68 175
Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
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[18] Guo B, Xiao Q L, Wang S H, Zhang H 2019 Laser Photonics Rev. 13 1800327
Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
[28] Villegas C E P, Rocha A R, Marini A 2016 Phys. Rev. B 94 134306
Google Scholar
[29] Lin Y C, Komsa H P, Yeh C H, Bjorkman T, Liang Z Y, Ho C H, Huang Y S, Chiu P W, Krasheninnikov A V, Suenaga K 2015 ACS Nano 9 11249
Google Scholar
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Google Scholar
[31] 魏钟鸣, 夏建白 2019 物理学报 68 48
Google Scholar
Wei Z M, Xia J B 2019 Acta Phys. Sin. 68 48
Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
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Google Scholar
Liu F, Xing Q R, Hu M L, Li Y F, Wang C L, Chai L, Wang Q Y 2011 Acta Phys. Sin. 60 704
Google Scholar
[41] Meng X, Zhou Y, Chen K, Roberts R H, Wu W, Lin J F, Chen R T, Xu X, Wang Y 2018 Adv. Opt. Mater. 6 1800137
Google Scholar
[42] Chen H, Wang C, Ouyang H, Song Y, Jiang T 2020 Nanophotonics
Google Scholar
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Google Scholar
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Google Scholar
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