Frequency-domain coherent multidimensional spectroscopy when dephasing rivals pulsewidth: Disentangling material and instrument response.
Frequency-domain coherent multidimensional spectroscopy when dephasing rivals pulsewidth: Disentangling material and instrument response.
复制标题
移相与脉冲宽度相媲美时的频域相干多维光谱：解开材料和仪器响应。
DOI：
10.1063/1.4986069
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发表时间：
2017
期刊：
影响因子：
--
通讯作者：
J. C. Wright
中科院分区：
文献类型：
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作者：
Daniel D. Kohler;Blaise J. Thompson;J. C. Wright
超快光谱通常在混合频域/时域中采集，其中脉冲持续时间与系统退相时间相近。在这些实验中，从常见的受驱极限和脉冲极限得出的预期是无效的。这项工作模拟了一个模型系统的混合域四波混频响应，以便为这种更复杂的场 - 物质相互作用建立预期。我们探究了频率轴和延迟轴。我们表明这些线形对激发脉冲宽度和延迟极为敏感。在脉冲接近重叠时，激发脉冲引发的相关性类似于动态不均匀性的特征。我们使用一个与常见的场 - 物质表达式相关的直观图像来描述这些线形。我们制定了区分脉冲引发的相关性和真实系统不均匀性的策略。这些模拟为解释混合域中的超快实验提供了基础。
Ultrafast spectroscopy is often collected in the mixed frequency/time domain, where pulse durations are similar to system dephasing times. In these experiments, expectations derived from the familiar driven and impulsive limits are not valid. This work simulates the mixed-domain four-wave mixing response of a model system to develop expectations for this more complex field-matter interaction. We explore frequency and delay axes. We show that these line shapes are exquisitely sensitive to excitation pulse widths and delays. Near pulse overlap, the excitation pulses induce correlations that resemble signatures of dynamic inhomogeneity. We describe these line shapes using an intuitive picture that connects to familiar field-matter expressions. We develop strategies for distinguishing pulse-induced correlations from true system inhomogeneity. These simulations provide a foundation for interpretation of ultrafast experiments in the mixed domain.