Breaking the Condon Approximation for Light Emission from Metal Halide Perovskite Nanocrystals

Strandell, Dallas; Wu, Yifan; Mora-Perez, Carlos; Prezhdo, Oleg; Kambhampati, Patanjali

doi:10.1021/acs.jpclett.3c02826

Cited by 5 publications

(1 citation statement)

References 44 publications

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“…Notably, these time scales exceed the corresponding nonradiative electron–hole recombination times, as illustrated in Table . These findings reveal that the harvested electronic energy by photoexcitation dissipates to phonon modes much faster than the radiative process, − resulting in poor emission in pristine VOHPs. , …”

Section: Resultsmentioning

confidence: 98%

A-Cation-Dependent Excited State Charge Carrier Dynamics in Vacancy-Ordered Halide Perovskites: Insights from Computational and Machine Learning Models

Nayak,

Mora Perez,

Liu

et al. 2024

Chem. Mater.

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Lead-free vacancy-ordered halide perovskites (VOHPs) are emerging as promising materials for environmentally friendly next-generation optoelectronic devices. However, a detailed atomistic understanding of charge carrier dynamics under ambient conditions ( 300 K) is lacking. Thus, attempts to refine the optoelectronic performance of VOHPs through material selection remain challenging. Here, we combine nonadiabatic molecular dynamics, time-domain density functional theory, and an unsupervised machine learning (ML) model for in-depth analyses of prevailing nonradiative carrier recombination and its entropy correlation with real-time structural dynamics. Our key findings illustrate that the thermal fluctuations are intricately linked to the performance-limiting nonradiative recombination in these perovskites. The detailed ML model-based analyses reveal the complex nonlinear correlations between photophysical properties and several structural features that dominantly influence excited state carrier dynamics. The atomistic insights unambiguously demonstrate that the organic methylammonium (MA) cation as the A cation in the lattice significantly impacts thermal fluctuations of the isolated inorganic metal halide octahedral subsystem. The stronger electron−phonon interactions introduce substantially faster nonradiative carrier relaxation over time. The inorganic elements, cesium and rubidium (A cations), largely restrict the lattice dynamics, weakening instantaneous nonradiative electron−phonon coupling in VOHPs. These inorganic VOHPs exhibit longer carrier lifetimes, depicting suppressed nonradiative carrier recombination processes. Our study emphasizes the decisive impacts of complex dynamic structure−excited state property correlations on the charge carrier dynamics in a group of primarily isostructural halide perovskites. This study provides valuable insights into the strategically designed lead-free perovskites for optoelectronic device applications.

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Section: Resultsmentioning

confidence: 98%

A-Cation-Dependent Excited State Charge Carrier Dynamics in Vacancy-Ordered Halide Perovskites: Insights from Computational and Machine Learning Models

Nayak,

Mora Perez,

Liu

et al. 2024

Chem. Mater.

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Extreme Electron‐Photon Interaction in Disordered Perovskites

Kharintsev,

Battalova,

Matchenya

et al. 2024

Advanced Science

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The interaction of light with solids can be dramatically enhanced owing to electron‐photon momentum matching. This mechanism manifests when light scattering from nanometer‐sized clusters including a specific case of self‐assembled nanostructures that form a long‐range translational order but local disorder (crystal‐liquid duality). In this paper, a new strategy based on both cases for the light‐matter‐interaction enhancement in a direct bandgap semiconductor – lead halide perovskite CsPbBr3 – by using electric pulse‐driven structural disorder, is addressed. The disordered state allows the generation of confined photons, and the formation of an electronic continuum of static/dynamic defect states across the forbidden gap (Urbach bridge). Both mechanisms underlie photon‐momentum‐enabled electronic Raman scattering (ERS) and single‐photon anti‐Stokes photoluminescence (PL) under sub‐band pump. PL/ERS blinking is discussed to be associated with thermal fluctuations of cross‐linked [PbBr6]4‐ octahedra. Time‐delayed synchronization of PL/ERS blinking causes enhanced spontaneous emission at room temperature. These findings indicate the role of photon momentum in enhanced light‐matter interactions in disordered and nanostructured solids.

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Unraveling the excitonics of light emission from metal-halide perovskite quantum dots

Kambhampati

2024

Nanoscale

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Breaking the Condon Approximation for Light Emission from Metal Halide Perovskite Nanocrystals

Cited by 5 publications

References 44 publications

A-Cation-Dependent Excited State Charge Carrier Dynamics in Vacancy-Ordered Halide Perovskites: Insights from Computational and Machine Learning Models

A-Cation-Dependent Excited State Charge Carrier Dynamics in Vacancy-Ordered Halide Perovskites: Insights from Computational and Machine Learning Models

Extreme Electron‐Photon Interaction in Disordered Perovskites

Unraveling the excitonics of light emission from metal-halide perovskite quantum dots

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