Visualizing Nanodomain Superlattices in Halide Perovskites Giving Picosecond Quantum Transients

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Hauptverfasser: Guo, Dengyang, Selby, Thomas A., Kahmann, Simon, Gorgon, Sebastian, Dai, Linjie, Dubajic, Milos, Yang, Terry Chien-Jen, Fairclough, Simon M., Marsh, Thomas, Jacobs, Ian E., Wu, Baohu, Guo, Renjun, Nagane, Satyawan, Doherty, Tiarnan A. S., Ji, Kangyu, Liu, Cheng, Lu, Yang, Kang, Taeheon, Mamak, Capucine, Mao, Jian, Müller-Buschbaum, Peter, Sirringhaus, Henning, Midgley, Paul A., Stranks, Samuel D.
Format: Preprint
Veröffentlicht: 2025
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author Guo, Dengyang
Selby, Thomas A.
Kahmann, Simon
Gorgon, Sebastian
Dai, Linjie
Dubajic, Milos
Yang, Terry Chien-Jen
Fairclough, Simon M.
Marsh, Thomas
Jacobs, Ian E.
Wu, Baohu
Guo, Renjun
Nagane, Satyawan
Doherty, Tiarnan A. S.
Ji, Kangyu
Liu, Cheng
Lu, Yang
Kang, Taeheon
Mamak, Capucine
Mao, Jian
Müller-Buschbaum, Peter
Sirringhaus, Henning
Midgley, Paul A.
Stranks, Samuel D.
author_facet Guo, Dengyang
Selby, Thomas A.
Kahmann, Simon
Gorgon, Sebastian
Dai, Linjie
Dubajic, Milos
Yang, Terry Chien-Jen
Fairclough, Simon M.
Marsh, Thomas
Jacobs, Ian E.
Wu, Baohu
Guo, Renjun
Nagane, Satyawan
Doherty, Tiarnan A. S.
Ji, Kangyu
Liu, Cheng
Lu, Yang
Kang, Taeheon
Mamak, Capucine
Mao, Jian
Müller-Buschbaum, Peter
Sirringhaus, Henning
Midgley, Paul A.
Stranks, Samuel D.
contents 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.
format Preprint
id arxiv_https___arxiv_org_abs_2502_13609
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Visualizing Nanodomain Superlattices in Halide Perovskites Giving Picosecond Quantum Transients
Guo, Dengyang
Selby, Thomas A.
Kahmann, Simon
Gorgon, Sebastian
Dai, Linjie
Dubajic, Milos
Yang, Terry Chien-Jen
Fairclough, Simon M.
Marsh, Thomas
Jacobs, Ian E.
Wu, Baohu
Guo, Renjun
Nagane, Satyawan
Doherty, Tiarnan A. S.
Ji, Kangyu
Liu, Cheng
Lu, Yang
Kang, Taeheon
Mamak, Capucine
Mao, Jian
Müller-Buschbaum, Peter
Sirringhaus, Henning
Midgley, Paul A.
Stranks, Samuel D.
Materials Science
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.
title Visualizing Nanodomain Superlattices in Halide Perovskites Giving Picosecond Quantum Transients
topic Materials Science
url https://arxiv.org/abs/2502.13609