MoS2的多维三重和频光谱及其与吸收光谱和倍频光谱的比较
Multidimensional Triple Sum-Frequency Spectroscopy of MoS2 and Comparisons with Absorption and Second Harmonic Generation Spectroscopies
摘要：
三重和频（TSF）光谱学是近年来发展起来的一种通过共振激发多个振动态和电子态的量子相干性来收集多维光谱的方法。这项工作报告的第一个应用程序的TSF的电子状态的半导体。两个可独立调谐的超快脉冲激发二硫化钼薄膜的A、B和C特征。所测得的TSF光谱与吸收光谱和二次谐波产生光谱有明显不同。这些差异是由于跃迁时刻和联合态密度的相对重要性而产生的。我们开发了一个简单的模型，并全局拟合的吸收光谱和谐波产生光谱提取的联合态密度和跃迁矩从这些光谱。我们的研究结果验证了以前的分配的C功能的一个大的联合密度的状态创建的频带嵌套。
英文摘要：
Triple sum-frequency (TSF) spectroscopy is a recently-developed methodology that enables collection of multidimensional spectra by resonantly exciting multiple quantum coherences of vibrational and electronic states. This work reports the first application of TSF to the electronic states of semiconductors. Two independently tunable ultrafast pulses excite the A, B, and C features of a MoS2 thin film. The measured TSF spectrum differs markedly from absorption and second harmonic generation spectra. The differences arise because of the relative importance of transition moments and the joint density of states. We develop a simple model and globally fit the absorption and harmonic generation spectra to extract the joint density of states and the transition moments from these spectra. Our results validate previous assignments of the C feature to a large joint density of states created by band nesting.
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