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Raman Chirped Adiabatic Passage: a New Method for Selective Excitation of High Vibrational States
Author(s) -
Chelkowski S.,
Bandrauk A. D.
Publication year - 1997
Publication title -
journal of raman spectroscopy
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.748
H-Index - 110
eISSN - 1097-4555
pISSN - 0377-0486
DOI - 10.1002/(sici)1097-4555(199706)28:6<459::aid-jrs124>3.0.co;2-y
Subject(s) - stimulated raman adiabatic passage , raman spectroscopy , excitation , adiabatic process , polarizability , excited state , laser , atomic physics , population , raman scattering , coherent anti stokes raman spectroscopy , materials science , molecular physics , chemistry , physics , optics , molecule , quantum mechanics , sociology , demography
It is demonstrated that efficient and high vibrational excitation can be achieved using non‐resonant stimulated Raman transitions for subsequent step by step climbing of vibrational levels. The pump laser (or both the pump and Stokes laser) frequency are to be swept in such a way that the frequency difference sweeping allows molecular anharmonicities of the final states to be matched. It is shown that amplitudes of successive Raman transitions can be quantitatively described with the help of the effective Raman two‐level systems. This selective scheme of vibrational excitation, called Raman chirped adiabatic passage (RCAP), should be useful in controlling excited‐state populations and chemical reactions. The limitations of another well known adiabatic scheme of population transfer, stimulated Raman adiabatic passage (STIRAP), are outlined and it is shown that RCAP is a complementary method to STIRAP. RCAP should be useful for selective excitation of highly polarizable symmetric bonds such as metal–metal bonds. © 1997 John Wiley & Sons, Ltd.