AI 中文总结
本文提出一种操作中方法，通过干涉自相关测量和反卷积去除泵浦光谱特征，从二维光谱中准确提取分子三阶响应，推动多维光谱走向脉冲极限。
AI 中文摘要
相干多维光谱将极大地受益于近单周期脉冲，这得益于可访问态的谱宽以及可分辨的高频振荡。然而，使用此类脉冲的必要代价是高效自相位调制产生的光谱结构，该结构会引入信号中并使分子响应的解释复杂化。本文开发了一种操作中方法，用于表征并从二维光谱信号中去除泵浦光谱特征。泵浦光谱通过一种与实验同时运行的干涉集成自相关测量获取，从而继承相同的时间和频域特性。随后，一种反卷积程序抑制噪声并从总信号中提取三阶响应。该分析能够校正光谱强度，并将光谱特征明确归属于分子响应。这项工作将多维光谱推向脉冲极限，并使其能够与其他非线性光谱技术（如阿秒光谱）集成——所有这些都不会损害少周期脉冲特性。
英文摘要
Coherent multidimensional spectroscopy will benefit greatly from near single-cycle pulses through the spectral breadth of states that can be accessed and the high frequency oscillations that can be resolved. However, the necessary cost of working with such pulses is the spectral structure arising from efficient self-phase modulation, which imparts into the signal and complicates interpretation of the molecular response. In this paper, we develop an in-operando approach to characterize and remove pump spectral features from two-dimensional spectroscopic signals. The pump spectrum is retrieved via an interferometric integrated autocorrelation measurement that runs concurrently with the experiment and thereby inherits the same time and frequency domain properties. A deconvolution procedure then suppresses noise and extracts the third-order response from the total signal. The analysis enables correction of spectral intensities and unambiguous assignment of spectral features to the molecular response. This work pushes multidimensional spectroscopy toward the impulsive limit and enables integration with other nonlinear spectroscopies such as attosecond spectroscopy - all without compromising few-cycle pulse properties.
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