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Theory of ultrafast time‐resolved absorption spectroscopy
Author(s) -
Yeh C. Y.,
Chang W. L.,
Ma H.,
Lin S. H.
Publication year - 1991
Publication title -
international journal of quantum chemistry
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.484
H-Index - 105
eISSN - 1097-461X
pISSN - 0020-7608
DOI - 10.1002/qua.560390313
Subject(s) - ultrashort pulse , coherence (philosophical gambling strategy) , adiabatic process , spectroscopy , absorption spectroscopy , density matrix , formalism (music) , spectral line , beat (acoustics) , atomic physics , quantum , physics , time resolved spectroscopy , coherence time , chemistry , molecular physics , optics , quantum mechanics , laser , art , musical , visual arts
Abstract In this paper, the density matrix formalism has been applied to treat ultrafast time‐resolved absorption spectroscopy. We have shown that in the femto‐second (fs) pump‐probe experiments, the observed time‐resolved absorption spectra consist of the contributions from the population (i.e., incoherent contribution) and the coherence (i.e., the phase of the system). The adiabatic approximation has been used to derive the expressions for ultrafast time‐resolved spectra. We have also shown that the dynamics of the coherence will result in quantum beat. Numerical calculations have been performed to demonstrate the theoretical results.