Visualizing Nanodomain Superlattices in Halide Perovskites Giving Picosecond Quantum Transients

TL;DR

This study uncovers ultrafast quantum transients in halide perovskite nanodomain superlattices, revealing potential for advanced quantum optoelectronic applications through multimodal analysis.

Contribution

It demonstrates the existence of ~2 picosecond quantum transients in bulk perovskite films and links them to nanodomain superlattices formed by specific octahedral arrangements.

Findings

Ultrafast quantum transients of ~2 ps observed at low temperature.

Nanodomain superlattices consist of alternating ordered octahedral layers.

Transient photoluminescence matches photoabsorption with ultra-narrow linewidth.

Abstract

The high optoelectronic quality of halide perovskites lends them to be utilized in optoelectronic devices and recently in emerging quantum emission applications. Advancements in perovskite nanomaterials have led to the discovery of processes in which luminescence decay times are sub-100 picoseconds, stimulating the exploration of even faster radiative rates for advanced quantum applications, which have only been prominently realised in III-V materials grown through costly epitaxial growth methods. Here, we discovered ultrafast quantum transients of time scales ~2 picoseconds at low temperature in bulk formamidinium lead iodide films grown through scalable solution or vapour approaches. Using a multimodal strategy, combining ultrafast spectroscopy, optical and electron microscopy, we show that these transients originate from quantum tunnelling in nanodomain superlattices. The outcome of the transient decays, photoluminescence, mirrors the photoabsorption of the states, with an ultra-narrow linewidth at low temperature as low as <2 nm (~4 meV). Localized correlation of the emission and structure reveals that the nanodomain superlattices are formed by alternating ordered layers of corner sharing and face sharing octahedra. This discovery opens new applications leveraging intrinsic quantum properties and demonstrates powerful multimodal approaches for quantum investigations.