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A generalized physical model is introduced to describe the impulsivestimulated scattering (ISS) response of relaxing systems to photothermalexcitation in a periodical grating geometry. The proposed approach starts fromDebye and Havriliak-Negami expressions for both the frequency-dependent heatcapacity, C({\omega}), and thermal expansion coefficient, {\gamma}({\omega}).Simulations are carried out on glycerol to test and compare the developedmodels with the existing semi-empirical model [1]. Debye behavior of thespecific heat capacity is shown to be compatible with a two-temperaturescenario, in which, in addition to the classical, experimentally observabletemperature that characterizes the distribution of the system over vibrationalenergy states, a second temperature characterizes the state of theconfigurational energy landscape. The models here developed have been appliedfor the interpretation of the experimental ISS signals of supercooled glycerol,illustrating simultaneous and separate assessment of C({\omega}) and{\gamma}({\omega}) up to sub-100 MHz from thermoelastic transients.

journal of chemical physics online/the journal of chemical physics/journal of chemical physics

Impulsive stimulated scatttering signal in supercooled liquids with  Debye or Havriliak-Negami relaxation of the specific heat capacity and  thermal expansion coefficient