Nonlinear Optical Response of a WS(2) Monolayer at Room Temperature upon Multicolor Laser Excitation.
Nonlinear Optical Response of a WS(2) Monolayer at Room Temperature upon Multicolor Laser Excitation.
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DOI：
10.1021/acsphotonics.0c01567
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发表时间：
2021-02-17
期刊：
影响因子：
7
通讯作者：
Kuipers L
中科院分区：
文献类型：
--
作者：
Hernandez-Rueda J;Noordam ML;Komen I;Kuipers L
目前，二维材料的非线性光学性质正吸引着越来越多的研究小组的注意，因为它们在广泛的科学学科中具有巨大的应用潜力。在这里，我们研究了室温下WS 2单层的非线性光致发光（PL）和几个简并和非简并非线性光学过程之间的相互作用。我们使用频率为ω1和ω2的两个飞秒激光脉冲照射样品，光子能量低于光学带隙。结果，样品发出的光显示出二次谐波产生、和频产生和四波混频的特征光谱峰。此外，我们发现，共振和非共振非线性激发通过频率混合有助于（非线性）PL发射在A-激子频率。PL与观察到的非线性效应表现出明显的相关性，我们将其归因于通过简并和非简并多光子吸收产生激子。我们的工作说明了进一步了解过渡金属dichalcogenides的参数和非参数非简并光学机制之间的基本关系。反过来，这样的理解有很大的潜力，以扩大在不同的科学和技术领域，其中非线性机制通常限于简并过程的二维材料的非线性光学过程的适用范围。
Currently, the nonlinear optical properties of 2D materials are attracting the attention of an ever-increasing number of research groups due to their large potential for applications in a broad range of scientific disciplines. Here, we investigate the interplay between nonlinear photoluminescence (PL) and several degenerate and nondegenerate nonlinear optical processes of a WS2 monolayer at room temperature. We illuminate the sample using two femtosecond laser pulses at frequencies ω1 and ω2 with photon energies below the optical bandgap. As a result, the sample emits light that shows characteristic spectral peaks of the second-harmonic generation, sum-frequency generation, and four-wave mixing. In addition, we find that both resonant and off-resonant nonlinear excitation via frequency mixing contributes to the (nonlinear) PL emission at the A-exciton frequency. The PL exhibits a clear correlation with the observed nonlinear effects, which we attribute to the generation of excitons via degenerate and nondegenerate multiphoton absorption. Our work illustrates a further step toward understanding the fundamental relation between parametric and nonparametric nondegenerate optical mechanisms in transition-metal dichalcogenides. In turn, such understanding has great potential to expand the range of applicability of nonlinear optical processes of 2D materials in different fields of science and technology, where nonlinear mechanisms are typically limited to degenerate processes.
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