Effective temporal resolution in pump-probe spectroscopy with strongly chirped pulses
- IFN-CNR, Dipartimento di Fisica, Politecnico di Milano, Piazza Leonardo da Vinci 32, I-20133 Milano (Italy)
- Chemistry Department, University of California, Irvine, Irvine, California 92697-2025 (United States)
This paper introduces a general theoretical description of femtosecond pump-probe spectroscopy with chirped pulses whose joint spectral and temporal profile is expressed by Wigner spectrograms. We demonstrate that the actual experimental time resolution intimately depends on the pulse-sample interaction and that the commonly used instrumental response function needs to be replaced by a sample-dependent effective response function. We also show that, using the proper configurations in excitation and/or detection, it is possible to overcome the temporal smearing of the measured dynamics due to chirp-induced pulse broadening and recover the temporal resolution that would be afforded by the transform-limited pulses. We verify these predictions with experiments using broadband chirped pump and probe pulses. Our results allow optimization of the temporal resolution in the common case when the chirp of the pump and/or probe pulse is not corrected and may be extended to a broad range of time-resolved experiments.
- OSTI ID:
- 21528725
- Journal Information:
- Physical Review. A, Vol. 82, Issue 5; Other Information: DOI: 10.1103/PhysRevA.82.053809; (c) 2010 The American Physical Society; ISSN 1050-2947
- Country of Publication:
- United States
- Language:
- English
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