Evidence of liquid-liquid transition in triphenyl phosphite from time-resolved light scattering experiments

Here, we study the phase transition kinetics in a supercooled liquid state of triphenyl phosphite by means of time-resolved polarized and depolarized light scattering to address a long-standing controversy on its mechanism, i.e., whether the phenomenon is primarily induced by liquid-liquid transition (LLT) or by nanocrystal formation. We find that the polarized scattering intensity exhibits a peak as a function of time, and its low wave number limit is nonzero for any annealing temperatures, both of which strongly indicate the nonconserved nature of an order parameter governing the transition. We also observe evolution of depolarized scattering. Above the spinodal temperature TSD, the depolarized scattering intensity monotonically increases with time since it is dominated by scattering from nanocrystallites, which are continuously formed during the process. Below TSD, on the other hand, it exhibits a distinct peak as a function of time as the polarized scattering intensity does. This appearance of the peak suggests that dielectric tensor fluctuations responsible for the depolarized scattering mainly come from isotropic density fluctuations and not from nanocrystallites, supporting the occurrence of LLT.