New quasiparticles hystons and coherent photoinduced dynamics of molecules in polar disordered media

Using methods of statistical thermodynamics, it is shown that after pulse excitation the evolution of a “polar luminescent probe—polar disordered medium” system is described by an equation of damping vibrations. This allows the conclusion that in the solvate shell of the probe molecule synchronous rotational vibrations (librations) of the molecules of the medium occur, whose damping is caused by dielectric friction. Such a collective synchronous motion is considered as a motion of a quasiparticle called a hyston. The moment of inertia J_n and mass M_h of a hyston are defined as J_h=2m² ₁a^-3Ω₀ ^-2(ε-1)/(2ε+1), M_h=J_hM_s/J_s, where m₁ is the dipole moment of the probe molecule in the excited S₁-stute; a is the Onsager radius; Ω₀ is the cyclic frequency of harmonic vibrations of the hyston; ε is the dielectric constant; M_s and J_s are the mass and moment of inertia of a molecule of the medium, respectively. The correlation function of the motion of the molecules c(t) is a solution of the equation of hyston motion. The fluorescence response s(t) in measurements with time resolution coincides with the correlation function: s(t)=c(t). The concepts concerning hystons make it possible to describe macroscopic photoinduced coherent motion that is manifested against a background of thermal motion of the medium molecules. Institute of Molecular and Atomic Physics, National Academy of Sciences of Belarus, 70, F. Skorina Ave., Minsk, 220072, Belarus. Translated from Zhurnal Prikladnei Spektroskopii, Vol 65, No. 2, pp. 176–183, March–April, 1998.