非简并双光子吸收及其应用研究进展

吴波; 王爵; 王崴; 周国富

doi:10.7498/aps.72.20230911

摘要

非简并双光子吸收是两个能量不同的光子同时被介质吸收, 产生一次电子从基态经过一个中间虚态向激发态跃迁的非线性光学效应. 非简并双光子吸收与简并双光子吸收相比, 由于中间态共振效应, 吸收系数得到了几十倍甚至几百倍的增大, 因此在多个非线性光学应用中具有极大的潜力. 本文首先介绍双光子吸收的基本原理, 解释了非简并双光子吸收的增强机制; 然后详细介绍双光子吸收的基本测量方法; 接着综述三维半导体材料、有机荧光分子、二维材料与量子点的非简并双光子吸收相关研究; 最后重点总结了其在红外探测与成像、双光子荧光显微成像、全光开关与光调制等领域的应用进展, 并对领域领域的未来发展进行了展望.

关键词:

Abstract

Nondegenerate two-photon absorption is a nonlinear optical effect in which two photons with different energy are absorbed by a medium simultaneously, resulting in a single electron transition from ground state to excited state through an intermediate virtual state. Compared with the degenerate two-photon absorption coefficient, the absorption coefficient of nondegenerate two-photon absorption is increased by tens or even hundreds of times due to the intermediate resonance effect, so it has great potentials in many nonlinear optical applications. Firstly, the basic principle of two-photon absorption is introduced and the enhancement mechanism of non-degenerate two-photon absorption is explained in this paper. Secondly, the basic method of measuring two-photon absorption is introduced in detail. Thirdly, the reports on nondegenerate two-photon absorption of three-dimensional semiconductor materials and two-dimensional materials are reviewed. Finally, the application progress of infrared detection and imaging, two-photon fluorescence microscope, all-optical switch and optical modulation is summarized, and the future research in this field is summarized and prospected.

Keywords:

作者及机构信息

1.
华南师范大学, 华南先进光电子研究院, 广东省光信息材料与技术重点实验室, 彩色动态电子纸显示技术研究所, 广州　510006

2.
深圳市国华光电科技有限公司, 深圳　518110

3.
深圳市国华光电研究院, 深圳　518110

通信作者: 吴波, bowu@m.scnu.edu.cn ; 周国富, guofu.zhou@m.scnu.edu.cn

基金项目: 国家自然科学基金(批准号: 62175068)、广东省基础与应用基础研究基金自然科学基金(批准号: 2023B1515020024)、广东省光信息材料与技术重点实验室(批准号: 2017B030301007)和国家绿色光电子国际联合研究中心(批准号: 2016B01018)资助的课题.

Authors and contacts

1.
Institute of Electronic Paper Displays, Guangdong Provincial Key Laboratory of Optical Information Materials and Technology, South China Academy of Advanced Optoelectronics, South China Normal University, Guangzhou 510006, China

2.
Shenzhen Guohua Optoelectronics Tech. Co. Ltd., Shenzhen 518110, China

3.
Academy of Shenzhen Guohua Optoelectronics, Shenzhen 518110, China

Corresponding author: Wu Bo, bowu@m.scnu.edu.cn ; Zhou Guo-Fu, guofu.zhou@m.scnu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 62175068), the Basic and Applied Basic Research Foundation of Guangdong Province, China (Grant No. 2023B1515020024), the Key Laboratory of Optical Information Materials and Technology of Guangdong Province, China (Grant No. 2017B030301007), and the National Green Optoelectronics International Joint Research Center (Grant No. 2016B01018).

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施引文献

图 1 (a) 简并双光子吸收能级示意图; (b) 非简并双光子吸收能级示意图^[23]

Fig. 1. Schematics of (a) D-TPA and (b) ND-TPA processes^[23] .

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图 2 泵浦-探测实验装置

Fig. 2. Schematics of a typical pump-probe setup.

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图 3 典型三维半导体的ND-TPA (a) CdTe和(b) ZnO时间分辨归一化透射率曲线^[34]; (c)—(e) ZnSe, ZnO, CdTe和GaAs的ND-TPA和D-TPA系数与泵浦-探测光子的能量依赖图^[34]; (f) 泵浦-探测偏振方向对闪锌矿型ZnS的ND-TPA的影响, 其中探测光偏振方向平行于z轴, 泵浦偏振平行或者垂直于探测偏振方向^[29]

Fig. 3. The ND-TPA of typical 3D semiconductors: Normalized transmission dynamics of (a) CdTe and (b) ZnO single crystals^[34]; (c)–(e) ND-TPA and D-TPA coefficients of ZnSe, ZnO, CdTe and GaAs^[34]; (f) pump-probe polarization-dependent ND-TPA coefficients for ZnS single crystal. The polarization of the probe beam is along the z axis, while that for the pump beam is either parallel or perpendicular to the probe polarization^[29].

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图 4 典型二维材料的ND-TPA　(a)单层WS₂的瞬态透射动力学曲线与功率依赖关系, 激发波长 776 nm, 功率0.23—2.96 mW, 0 fs之前负信号归因为ND-TPA^[45]; (b)单层WS₂的瞬态透射动力学曲线分解为ND-TPA部分和D-TPA部分贡献, 黑点为原始数据, 蓝点源于D-TPA, 红点源于ND-TPA^[45]; (c) 8 nm GaAs/12 nm Al_0.32Ga_0.68As 量子阱的ND-TPA系数及理论预测曲线, 此处泵浦与探测偏振均为TM^[44]; (d) (BA)₂(MA)_n–1Pb_nX_3n+1钙钛矿薄片的超快光透射调控, 泵浦波长760—980 nm, 功率3.5 μW; 探测波长705 nm, 实线为Lorentz拟合的调制宽度为13 fs^[54]

Fig. 4. The ND-TPA of typical 2D semiconductors: (a) Power-dependent transient transmission dynamics of monolayer WS₂, the pump wavelength is 776 nm and power in the range of 0.23–2.96 mW, the dip before time zero is attributed to ND-TPA^[45]; (b) the decoupling of transient transmission dynamics for monolayer WS₂, black squares are original data, blue dots are due to D-TPA and red triangles are attributed to ND-TPA^[45]; (c) ND-TPA coefficients of 8 nm GaAs/12 nm Al_0.32Ga_0.68As quantum well as a function of sum wavelength and its theoretical prediction, and the polarizations of both the pump and probe beams are TM^[44]; (d) ultrafast modulation of light using exfoliated (BA)₂(A)_n–1Pb_nX_3n+1 flakes. Pump beam: 760–980 nm, power: 3.5 μW. Probe beam: 705 nm. Solid line is a fit using Lorentzian function and 13 fs is obtained for the ultrafast modulation^[54].

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图 5 ND-TPA用于红外光子计数与探测　(a) GaAs红外光子计数示意图^[14]; (b) GaAs红外光子计数与信号光功率及泵浦强度的依赖关系^[14]; (c) GaN探测器用于中红外光探测示意图^[27]; (d) GaN探测器输出电压与输入红外信号光能量及泵浦功率依赖关系, 信号波长5.6 μm, 门脉冲390 nm^[27]; (e) Si-APD红外计数速率与输入脉冲能量关系, 泵浦光波长3.07 μm, 能量为0.32 nJ^[13]; (f) MAPbBr₃单晶与Si探头组合对1.7 μm红外光探测^[23]

Fig. 5. ND-TPA for infrared photon counting and detection: (a) Schematics of infrared photon counting using GaAs photodetector^[14]; (b) ND-TPA photon counts as a function of the signal power for different pump intensities using GaAs photodetector; (c) schematics of mid-infrared photodetection using a GaN photodiode^[27]; (d) output voltage of a GaN diode versus 5.6 μm input signal energy in the presence of temporally overlapped 390 nm gating pulses of various energies^[27]; (e) recorded count rates by the SiAPD as a function of input pulse energy, pump pulse wavelength of 3.07 μm, energy of 0.32 nJ^[13]; (f) 1.7 μm infrared photodetection using a combination of MAPbBr₃ single crystal and Si photodiode^[23].

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图 6 ND-TPA用于中红外成像　(a)用于三维红外成像的GaAs半导体孔状结构^[11]; (b)基于GaN的ND-TPA对该结构的三维成像图^[11]; (c)图(b)中A、B两点对应的泵浦探测光互相关信号^[11]; (d)基于硅基CCD相机的ND-TPA中红外振动成像系统示意图^[37]; (e)印有黑色字母的醋酸纤维素薄膜的中红外选择性成像. b, c, d点分别对应的是成像激光远离振动吸收、接近振动吸收峰和与在振动吸收峰上3种波长对应的成像效果图^[37]

Fig. 6. ND-TPA for mid-infrared imaging: (a) GaAs semiconductor structure used for the 3D imaging^[11]; (b) 3D imaging of the GaAs structure using the ND-TPA of a GaN photodiode^[11]; (c) the cross-correlation curves of points A and B in Fig. (b)^[11]; (d) schematics of the vibration imaging method based on the ND-TPA of a Si CCD^[37]; (e) imaging a cellulose acetate film with printed letters at selected wavelengths, wavelength b: far away from the absorption of C-H vibration, c: near the absorption peak; d: at the absorption peak^[37].

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图 7 ND-TPA用于双光子荧光显微生物成像　(a)常用的基于ND-TPA的双光子生物成像的原理示意图^[16]; (b)由脑虹构建的mCerulean (CFP)、mEYFP、tdTomato和/或mCherry编码的荧光蛋白的双光子激发光谱^[16]; (c)小鼠皮层450 μm厚的z堆叠中提取的多色图像(左), 不同深度(z = 50, 250, 400 μm)的成像截面(右)^[16]; (d)基于双色激发(λ₁ = 1055 nm, λ₂ = 1240 nm)的小鼠脑部三维成像图^[17]; (e)小鼠脑部双色双光子激发荧光信号与深度的依赖关系, 1C2P为D-TPA激发(λ₁ = 1055 nm), 2C2P为双色激发(λ₁ = 1055 nm, λ₂ = 1240 nm), τ = –600 fs, 0 fs为两种激发光的时间差^[17]

Fig. 7. ND-TPA for two-color two-phonon fluorescence imaging: (a) A typical setup of multicolor two-photon imaging using synchronized pulses^[16]; (b) two-photon excitation spectra of the fluorescent proteins encoded by the Brainbow constructs mCerulean (CFP), mEYFP, tdTomato and/or mCherry, arrows indicate the excitation wavelengths^[16]; (c) multicolor images of a mouse cortex extracted from a 450-μm-thick z stack (left), image slices at different depth (z = 50, 250, 400 μm) (right)^[16]; (d) the 3D image of a mouse brain using the two-color (λ₁ = 1055 nm, λ₂ = 1240 nm) two-phonon fluorescence imaging technique^[17]; (e) two-photon excited fluorescence signal intensity versus tissue depth in a mouse brain. 1C2P: D-TPA excitation (λ₁ = 1055 nm), 2C2P: ND-TPA excitation (λ₁ = 1055 nm, λ₂ = 1240 nm), τ = –600 fs, 0 fs: the time intervals between the excitation pulses^[17].

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图 8 (a) 用于全光开关的实验装置, EDFA: 掺铒光纤放大器, OBF: 光带通滤波器, PD: 光电二极管, DSO: 数字采样示波器^[22]; (b) 1552 nm泵浦脉冲和(c) 1536 nm处的交叉吸收调制连续波信号^[22]; (d) NOR门操作原理和真值表^[20]; (e) P1和P2信号及其逻辑NOR操作的输出信号^[20]

Fig. 8. (a) Experimental setup of a typical all-optical switch, EDFA: erbium-doped fiber amplifier, OBF: optical bandpass filter, PD: photodiode, DSO: digital sampling oscilloscope^[22]; (b) pump pulses at 1552 nm and (c) cross-absorption modulated CW signal at 1536 nm^[22]; (d) operation principle and truth table of NOR gate^[20]; (e) signal P1, P2 and the output cross-modulated CW probe with logic NOR operation^[20].

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表 1 已报道的无机半导体材料的ND-TPA系数

Table 1. Reported ND-TPA coefficients for different inorganic semiconductors.

材料	λ₁/nm	λ₂/nm	β_ND/(cm·GW^–1)	测试条件	β_D/(cm·GW^–1)
CdTe^[34]	870	8840	~1000	10 Hz, 30 ps	~20
ZnS^[34]	~390	~1760	~15	1 kHz, 140 fs	~1
ZnSe^[34]	~480	5600	~270	1 kHz, 140 fs	~2
ZnO^[34]	420	2000	~40	1 kHz, 140 fs	~2.5
GaAs^[34]	870	8840	~800	10 Hz, 30 ps	~10
GaSb^[39]	1720	3550	140	1 kHz, 130 fs	64^[41]
Cu₂O^[42]	800	1494	88	1 kHz, 120 fs	27
MAPbBr₃^[23]	577	1700	53	1 kHz, 100 fs	8^[43]
GaAs/Al_0.32Ga_0.68As QW^[44]	1120	1960	~15	82 MHz, 156 fs	—
WS₂^[45]	620	776	250	80.48 MHz, 250 fs	100
MoSe₂^[45]	790	1500	650	80.48 MHz, 250 fs	80—800
(BA)₂(MA)₃Pb₄X₁₃^[46]	705	760—980	10	100 kHz, 7 fs	—
Si^[40]	1904	1350	0.97	250 kHz, 160 fs	0.5^[47]

下载: 导出CSV

表 2 已报道的有机荧光探针分子的ND-TPA截面

Table 2. Reported ND-TPA cross section for different organic fluorescence probe materials.

材料	λ₁/nm	λ₂/nm	σ_ND/GM	测试条件	σ_D/GM
罗丹明6 G^[57]	800	691	596	溶剂: 甲醇; 浓度: 16.2 mmol/L; 脉宽: 103 fs	38—150^[58,59]
罗丹明 123^[57]	800	660	776	溶剂: 甲醇; 浓度: 4.2 mmol/L; 脉宽: 103 fs	80^[62]
香豆素6^[57]	800	652	1015	溶剂: 甲醇; 浓度: 23.7 mmol/L; 脉宽: 103 fs	—
香豆素343^[57]	800	651	49	溶剂: 氯仿; 浓度: 27.3 mmol/L; 脉宽: 103 fs	—
尼罗红^[57]	800	669	3270	溶剂: 氯仿; 浓度: 0.75 mmol/L; 脉宽: 103 fs	—
尼罗蓝A^[57]	800	626	1407	溶剂: 氯仿; 浓度: 0.68 mmol/L; 脉宽: 103 fs	—
咔唑衍生物BEMC^[60]	800	650	220	溶剂: 甲醇; 浓度: 10 mmol/L; 脉宽: 140 fs	34
氨基七甲噻吩^[63]	925	1020	1860	溶剂: 甲醇; 浓度: 1.3 mmol/L; 脉宽: 75 fs	940

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