Experimentally Mapping the Phase Diagrams of Photoexcited Small Polarons

TL;DR

This paper experimentally maps the phase diagrams of photoexcited polarons in various models, revealing how tuning interaction parameters can control polaron formation, with implications for material design.

Contribution

It extends the understanding of excited-state polarons by mapping experimental data onto theoretical models, identifying the t-J-Holstein model as most suitable for iron oxides.

Findings

t-J-Holstein model best describes iron oxides

Tuning electron-phonon coupling controls polaron formation

Experimental data integrated with theoretical models

Abstract

Understanding the fundamental properties that dictate photoexcited polarons in materials is critical to tuning their properties. Theoretical models of polarons have only recently been extended to the excited state. Experimental measurements of polaron formation and transport have been widely undertaken across a range of materials, from photocatalysts and superconductors to soft conducting polymers. Here, we map experimental measurements of quantities such as polaron strength onto phase diagrams of the Holstein, Hubbard-Holstein, and t-J-Holstein models. This work demonstrates that tuning electron-phonon coupling strength, electron localization, and spin exchange can be leveraged to suppress or control polaron formation in transition metal oxides. We find that the t-J-Holstein model best describes the measured iron oxides and could be generally applied to a wide range of systems that exhibit polaron formation in the excited state. This work combines experimental data with ground state models to provide a robust parameter space for informing photoexcited polaron design.