Photoproduction of spin and charge carriers in halogen-bridged binuclear platinum chain complexes

TL;DR

This paper theoretically investigates the nonlinear lattice relaxation processes in photoexcited platinum-halide chain compounds, revealing the formation of stable solitonic states and their dynamics, which differ from conventional chains.

Contribution

It introduces a detailed theoretical analysis of relaxation channels and predicts the coexistence of neutral and charged solitons as stable photoproducts in platinum chain complexes.

Findings

High-energy excitations relax into polarons.

Optical gap excitons turn into solitonic states nonradiatively.

Neutral and charged solitons coexist as stable photoproducts.

Abstract

Nonlinear lattice relaxation of photoexcited diplatinum-halide chain compounds is theoretically investigated within a one-dimensional extended Peierls-Hubbard model. We first illuminate the whole relaxation scenario in terms of variational wave functions and then visualize each relaxation channel numerically integrating the Schr\"odinger equation. High-energy excitations above the electron-hole continuum tend to relax into polarons, while excitons pumped within the optical gap, unless luminescent, turn into solitonic states nonradiatively. Neutral and charged solitons coexist as stable photoproducts, which has never been observed in conventional platinum-halide chains, and they are highly resonant on the occasion of their birth and geminate recombination.