Two-vibron bound states lifetime in a one-dimensional molecular lattice coupled to acoustic phonons

TL;DR

This paper investigates the lifetime of two-vibron bound states in a one-dimensional molecular lattice coupled to acoustic phonons, analyzing how anharmonicity and bath dimensionality influence decay rates.

Contribution

It provides an exact calculation of the two-vibron Green operator and reveals how anharmonicity affects bound state decay in different phonon bath dimensions.

Findings

Decay rate increases with anharmonicity for 1D baths.

Decay rate decreases with anharmonicity for 2D and 3D baths.

Main decay channel varies with bath dimension.

Abstract

The lifetime of two-vibron bound states in the overtone region of a one-dimensional anharmonic molecular lattice is investigated. The anharmonicity, introduced within an attractive Hubbard Hamiltonian for bosons, is responsible for the formation of bound states which belong to a finite linewidth band located below the continuum of two-vibron free states. The decay of these bound states into either bound or free states, is described by considering the coupling between the vibrons and a thermal bath formed by a set of low frequency acoustic phonons. The relaxation rate is expressed in terms of the spectral distribution of the vibron/phonon coupling and of the two-vibron Green operator which is calculated exactly by using the number states method. The behavior of the two-vibron bound states relaxation rate is analyzed with a special emphasis on the influence of the anharmonicity. It is shown that the rate exhibits two distinct regimes depending on the thermal bath dimension. When the bath dimension is equal to unity, the rate increases with the anharmonicity and the decay of the two-vibron bound states into the other bound states appears as the main contribution of the rate. By contrast, when the bath dimension is equal to 2 and 3, the rate decreases as the anharmonicity increases indicating that the two-vibron bound states decay into the two-vibron free states continuum.