Abstract
‘‘Impulsive’’ stimulated scattering (ISS) of femtosecond laser pulses was used to coherently excite and probe a low‐lying (61‐cm‐1) electronic excitation in the cooperative Jahn‐Teller crystal, terbium vanadate. Coherent terahertz oscillations and their dephasing were observed in the time domain. ISS is a general aspect of ultrashort‐pulse interactions with matter, through which coherent excitations are produced whenever a sufficiently short laser pulse enters a Raman‐active medium. Its use for measurement of vibrational and electronic dephasing and lifetimes, and for time‐resolved spectroscopy of vibrationally distorted crystals and molecules, is discussed.
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