Observation of polaronic state assisted sub-bandgap saturable absorption

TL;DR

This paper reports the first observation of polaronic state assisted saturable absorption in lead halide perovskites, revealing how exciton phonon coupling influences nonlinear optical properties and enabling tunable photonics applications.

Contribution

It introduces the concept of polaron-assisted nonlinear photonics in soft lattice lead halide perovskites, supported by experimental and theoretical evidence, and discusses how to manipulate exciton phonon coupling for tailored optical responses.

Findings

Polaronic states cause sub-bandgap saturable absorption with a redshift over 60 meV.

Transient picosecond polaronic states are responsible for anomalous nonlinear absorption.

Bandgap fluctuation can be tuned via exciton phonon coupling by adjusting Young's modulus.

Abstract

Polaronic effects involving stabilization of localized charge character by structural deformations and polarizations have attracted considerable investigations in soft lattice lead halide perovskites. However, the concept of polaron assisted nonlinear photonics remains largely unexplored, which has a wide range of applications from optoelectronics to telecommunications and quantum technologies. Here, we report the first observation of the polaronic state assisted saturable absorption through subbandgap excitation with a redshift exceeding 60 meV. By combining photoluminescence, transient absorption measurements and density functional theory calculations, we explicate that the anomalous nonlinear saturable absorption is caused by the transient picosecond timescale polaronic state formed by strong carrier exciton phonon coupling effect. The bandgap fluctuation can be further tuned through exciton phonon coupling of perovskites with different Young's modulus. This suggests that we can design targeted soft lattice lead halide perovskite with a specific structure to effectively manipulate exciton phonon coupling and exciton polaron formation. These findings profoundly expand our understanding of exciton polaronic nonlinear optics physics and provide an ideal platform for developing actively tunable nonlinear photonics applications.