P. Hamm | Searcharxiv

arXiv2021

2D Raman-THz spectroscopy of binary CHBr3-MeOH solvent mixture

Hybrid two-dimensional (2D) Raman-terahertz spectroscopy is used to measure the interactions between two solvents pair in the binary CHBr3-MeOH mixture in the frequency range of 1-7 THz. Changes in the cross peak signature are monitored, originating from the coupling of an intramolecular bending mode of CHBr3 to the collective intermolecular degrees of freedom of the mixture. The appearance of a new cross peak in the 2D spectrum measured for solvent mixture with MeOH molar fraction of 0.3 indicates a coupling to a new set of low-frequency modes formed due to the hydrogen bond interactions between the two solvents. This interpretation is supported by the measurement of the CHBr3-CS2 binary solvent mixture as well as by 1D absorption measurements of neat MeOH.

physics.chem-ph↗

arXiv2008

Barrier crossing to the small Holstein polaron regime

We investigate the dimensionality effects of the Holstein polaron from the fully quantum regime, where the crossover between large and small polaron solutions is known to be continuous in all dimensions, into the limit described by the semiclassical Discrete Nonlinear Schrödinger (DNLS) Equation, where the crossover is continuous in 1D but discontinuous in higher dimensions. We use exact numerics on one hand and a two variable parametrization of the Toyozawa ansatz on the other in order to probe the crossover region in all parameter regimes. We find that a barrier appears also in 1D separating the two types of solutions, seemingly in contradiction to the common paradigm for the DNLS according to which the crossover is barrier-free. We quantify the polaron behavior in the crossover region as a function of the exciton overlap and find that the barrier remains small in 1D and tunnelling through it is not rate-limiting.

cond-mat.other↗