Femtosecond Raman-induced polarisation spectroscopy of coherent rotational wave packets: D2, N2 and NO2

Experimental Coherent Laser Control of Physicochemical Processes

“…When the incident field is resonant, it is possible to manipulate the phase of the light that excites a particular rovibronic transition. This degree of finesse has been demonstrated by Leone's research group. ,,,,,− The effect of different phase modulation, for example, chirp, on the rotation of diatomics has been explored by Sarkisov and Lozovoy …”

“…The measured introduction of positive or negative chirp can be accomplished by the use of prism or grating pairs. , More sophisticated phase modulation required the introduction of pulse shapers. Experimental demonstrations of wave packet manipulation, using phase-modulated pulses, are listed in Table . ,,,− ,− For example, Bucksbaum's group has demonstrated Rydberg-state wave packet sculpting based on phase shaping. − Leone has taken this method one step further with relative control over the phase of rotational and vibrational levels in a diatomic molecule. − In Leone's experiment, they used a narrow bandwidth laser to excite a single rovibrational state from which they could launch the wave packets. This initial step served to circumvent the initial thermal distribution.…”

COHERENTNONLINEARSPECTROSCOPY: From Femtosecond Dynamics to Control

“…Experimental (40) and theoretical (41,42) studies on the effect of chirped pulses on the multiphoton excitation of molecules showed that the traditional saturation limits can be exceeded, thereby facilitating population inversion. The groups of Shank, Wilson, Leone, and others have shown experimental evidence that tailored femtosecond pulses can be used to modify the initial wave packet formed by the excitation laser (43)(44)(45)(46)(47)(48)(49)(50)(51)(52)(53). In some cases, tailored pulses (chirp) can be used to enhance single and multiphoton transitions (54)(55)(56)(57) as well as excitation of high vibrational states (58,59).…”

Ultrafast Probing and Control of Molecular Dynamics: Beyond the Pump‐Probe Method

“…Time resolved rotational coherence has been pursued for the determination of complex molecular systems in the gas phase [34]. Femtosecond time resolution allows work on lighter molecules such as D 2 [35] and work at high temperatures.…”