Since the past two decades,ultrafast two-dimensional electronic spectroscopy(2DES)has made remarkable progress,and it plays a pivotal tool in unraveling population and coherent dynamics in photosynthesis,photovoltaic,and low-dimensional materials.This review presents a comprehensive overview of the progress in 2DES,with a focus on its ability to expand spectral windows and dimensions.Furthermore,it examines the current challenges and future directions of this field.From a technical perspective,a key bottleneck preventing the wide application of 2DES is the need to overcome experimental hurdles and develop sophisticated multispectral data analysis methods.In cutting-edge research,a crucial question centers on the development of novel 2DES techniques to effectively probe and disentangle various processes within coherent dynamics and polaritonic systems.
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