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With the help of a two-dimensional model system comprising a slow conformational degree of freedom and a higher-frequency vibration, we investigate the molecular-level origin and dynamical information content of femtosecond stimulated Raman spectroscopy (fissors) signals. Our treatment avails itself of the time scale separation between conformational and(More)
Mobile robots are an increasingly important part of search and rescue efforts as well as military combat. In order for users to accept these robots and use them effectively , the user must be able to communicate clearly with the robots and obtain explanations of the robots' behavior that will allow the user to understand its actions. This paper describes(More)
In this work, we demonstrate the use of broad-band pump-probe spectroscopy to measure femtosecond solvation dynamics. We report studies of a rhodamine dye in methanol and cryptophyte algae light-harvesting proteins in aqueous suspension. Broad-band impulsive excitation generates a vibrational wavepacket that oscillates on the excited-state potential energy(More)
We rebuild the theory of ultrafast transient-absorption/transmission spectroscopy starting from the optical response of an individual molecule to incident femtosecond pump and probe pulses. The resulting description makes use of pulse propagators and free molecular evolution operators to arrive at compact expressions for the several contributions to a(More)
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