Timmer Daniel, Lünemann Daniel C, Riese Sebastian, Sio Antonietta De, Lienau Christoph
Opt Express. 2024 Jan 1;32(1):835-847. doi: 10.1364/OE.511906.
Two-dimensional electronic spectroscopy (2DES) is a powerful method to study coherent and incoherent interactions and dynamics in complex quantum systems by correlating excitation and detection energies in a nonlinear spectroscopy experiment. Such dynamics can be probed with a time resolution limited only by the duration of the employed laser pulses and in a spectral range defined by the pulse spectrum. In the blue spectral range (<500 nm), the generation of sufficiently broadband ultrashort pulses with pulse durations of 10 fs or less has been challenging so far. Here, we present a 2DES setup based on a hollow-core fiber supercontinuum covering the full visible range (400-700 nm). Pulse compression via custom-made chirped mirrors yields a time resolution of <10 fs. The broad spectral coverage, in particular the extension of the pulse spectra into the blue spectral range, unlocks new possibilities for coherent investigations of blue-light absorbing and multichromophoric compounds, as demonstrated by a 2DES measurement of chlorophyll a.
二维电子光谱学（2DES）是一种强大的方法，通过在非线性光谱实验中关联激发和探测能量，来研究复杂量子系统中的相干和非相干相互作用及动力学。这种动力学可以通过仅受所用激光脉冲持续时间限制的时间分辨率以及由脉冲光谱定义的光谱范围内进行探测。在蓝光光谱范围（<500 nm）内，迄今为止，产生脉宽为10 fs或更短的足够宽带超短脉冲一直具有挑战性。在此，我们展示了一种基于覆盖整个可见光范围（400 - 700 nm）的空心光纤超连续谱的2DES装置。通过定制啁啾镜进行脉冲压缩可实现<10 fs的时间分辨率。如对叶绿素a的二维电子光谱测量所示，宽光谱覆盖，特别是脉冲光谱向蓝光光谱范围的扩展，为蓝光吸收和多发色团化合物的相干研究开启了新的可能性。
