Potential pitfalls of the early-time dynamics in two-dimensional electronic spectroscopy.
作者： David Paleček , Petra Edlund , Emil Gustavsson , Sebastian Westenhoff , Donatas Zigmantas
DOI: 10.1063/1.5079817
关键词: Energy transfer 、 Physics 、 Spectroscopy 、 Statistical physics 、 Scale (descriptive set theory) 、 Electron spectroscopy 、 Population 、 Time dynamics 、 Pulse (physics) 、 Kinetics
摘要: Two-dimensional electronic spectroscopy, and especially the polarization-controlled version of it, is cutting edge technique for disentangling various types coherences in molecules molecular aggregates. In order to evaluate coherences, which often decay on a 100 fs time scale, early population times have be included analysis. However, signals this region are typically plagued by several artifacts, unavoidable pulse overlap region. paper, we show that, case two-dimensional spectroscopy experiment, early-time dynamics can dominated "incorrect" ordering signals. These affect kinetics at positive well beyond region, when "correct" much weaker. Moreover, contributions oscillatory with spectral signatures energy transfer, may lead misinterpretation fast-decaying coherences.
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