Observation of positive and negative trions in organic-inorganic hybrid perovskite nanocrystals

Naoki Yarita,Tokuhisa Kawawaki,Ryota Sato,Yoshihiko Kanemitsu,Toshiharu Teranishi,Hirokazu Tahara,Tomoko Aharen,Masaki Saruyama

doi:10.1103/physrevmaterials.2.116003

Naoki Yarita, Tokuhisa Kawawaki + Show 6 more

Open Access

https://doi.org/10.1103/physrevmaterials.2.116003

Copy DOI

Abstract

Lead halide perovskite nanocrystals are promising light emitting materials with high photoluminescence quantum yields and widely tunable emission wavelengths. Their optical responses are significantly influenced by efficient nonradiative Auger recombination of trions (charged excitons) and biexcitons. Here, we report the observation of positive and negative trions in formamidinium lead bromide nanocrystals and discuss their role in the photoluminescence dynamics. It is found that the addition of copper thiocyanate causes an additional intermediate state by photochemical doping. We clarify that as-prepared nanocrystals show a two-state blinking between neutral excitons and positive trions, while the postsynthesis treated nanocrystals exhibit blinking between all three states, including negative trions. We confirmed that the biexciton Auger rate evaluated from femtosecond transient absorption measurements can be expressed as the sum of the Auger rates of positive and negative trions obtained by single-dot spectroscopy.

Highlights

Very recently, there have been extensive studies on optical and transport properties of the lead halide perovskites APbX3 (A = CH3NH3, HC(NH2)2, Cs; X = Cl, Br, I), because they are a class of promising materials for optoelectronic devices such as thin-film solar cells [1,2], light sources [3,4,5], and optical switches [6]
We clarify that as-prepared nanocrystals show a two-state blinking between neutral excitons and positive trions, while the postsynthesis treated nanocrystals exhibit blinking between all three states, including negative trions
We confirmed that the biexciton Auger rate evaluated from femtosecond transient absorption measurements can be expressed as the sum of the Auger rates of positive and negative trions obtained by single-dot spectroscopy

Summary

Introduction

There have been extensive studies on optical and transport properties of the lead halide perovskites APbX3 (A = CH3NH3, HC(NH2), Cs; X = Cl, Br, I), because they are a class of promising materials for optoelectronic devices such as thin-film solar cells [1,2], light sources [3,4,5], and optical switches [6]. The external efficiency of perovskite-based light-emitting diodes (LEDs) has recently increased above 10% [16]. These high efficiencies are originated from the perovskite’s almost ideal electronic structure in which deep trap levels are rarely formed, because of their unique characteristics of chemical bonds and band structures [17,18,19]

Results

Discussion

Conclusion