Abstract
The interaction between ultrashort light pulses and non-absorbing materials is dominated by impulsive stimulated Raman scattering (ISRS). The description of ISRS in the context of pump&probe experiments is based on effective classical models describing the interaction between the phonon and pulsed electromagnetic fields. Here we report a theoretical description of ISRS where we do not make any semi-classical approximation and we treat both photonic and phononic degrees of freedom at the quantum level. The results of the quantum model are compared with semiclassical results and validated by means of spectrally resolved pump&probe measurements on α-quartz.
Highlights
The excitation and measurement of coherent lattice vibrations in time domain experiments rely on the possibility of using ultrashort optical pulses in pairs, one as a pump and a second as a probe
The description of impulsive stimulated Raman scattering (ISRS) in the context of pump&probe experiments is based on effective classical models describing the interaction between the phonon and pulsed electromagnetic fields
Photoexcitation produces coherent vibrational states whose dissipative dynamics can be directly accessed by pump&probe experiments [1,2,3,4,5,6,7,8]
Summary
The excitation and measurement of coherent lattice (or molecular) vibrations in time domain experiments rely on the possibility of using ultrashort optical pulses in pairs, one as a pump and a second as a probe. The situation is simpler in ‘transparent materials’, i.e. in materials where there is no dipole allowed electronic transitions available in the frequency range of the ultrashort pulses In this limit, the interaction between the latter and the vibrational modes is a coherent process, where dissipative electron dynamics can be neglected and the whole process can be described effectively as a direct coupling between the ultrashort pulses and the phonon modes. We conclude with some remarks and new perspectives offered by the fully quantum treatment of timedomain experiments [6, 23,24,25,26]
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