Femtosecond laser-controlled selective excitation of vibrational modes on a multidimensional ground state potential energy surface

Selective spectral filtering of molecular modes of β‐carotene in solution using optimal control in four‐wave‐mixing spectroscopy

“…The relative intensity of these bands changes completely if the phase shape of the laser pulse is varied. 6,14 Silberberg and coworkers have also successfully demonstrated pulse-shaping effects in CARS in a series of experiments. 27 -30 …”

Evolutionary algorithms and their application to optimal control studies

“…In previous experiments [146] it was shown that the distribution of energy in the different modes strongly depends on chirp and delay of the Stokes pulse. Hence it is appropriate to restrict the algorithm mainly to a search for polynomial phase functions, without changing the spectrum of the pulses by an amplitude function.…”

“…The optimum phase function is characterized by a linear chirp which is in accordance with former results. [146]. The same method has been applied for the selective optimization of theν 3 andν 4 modes.…”

“…One technique made use of the Tannor-Rice scheme [6], which is related to the vibrational dynamics in the excitonic states of PDA. The other method included the variation of the chirp of the ultrashort Stokes laser pulse [146], already pointing to the important role of the phase in the selective excitation of vibrational motions.…”

Tailoring pulses for coherent Raman microscopy

“…In coherent control, amplitude and/or phase shaping is used to influence the quantum interferences between multiple pathways, providing control over molecular processes [73,74,75,76,77]. The control of a system by using predetermined pulse shapes is known as open loop control and has been used in CARS for selective excitation of vibrational modes [31,51,78,79,80], non-resonant background suppression [32,81], and improved detection of weak resonances [82]. In this chapter, CARS measurements based on the π and 2π shaping strategies presented in section 2.5 are shown.…”