Machine-Learning-Assisted Investigation on Benign Ion Migration in Metal Halide Perovskites

The Journal of Physical Chemistry Letters, Journal Year: 2025, Volume and Issue: unknown, P. 2614 - 2620

Published: March 4, 2025

Defect-assisted ion migration is one of the important issues that results in instability and non-radiative losses hybrid organic-inorganic metal halide perovskite solar cells. In this work, based on deep potential (DP) model, a long-time-scale molecular dynamics (MD) simulation has been employed to capture interstitial-assisted iodine process. The indicate that, when interstitial (Ii) begins migrate, serious structural distortion becomes mild, weakening electron-vibration interaction. trap state induced by trimer undergoes "deep-shallow-deep" dynamic process, which ultimately leads an improvement carrier lifetime during Our work confirms different processes are strongly correlated perovskites demonstrates migration, considered be detrimental, can become benign particular case. reported provide new fundamental insight improve efficiency CH3NH3PbI3

Language: Английский

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Nuclear Quantum Effects Accelerate Hot Carrier Relaxation but Slow Down Recombination in Metal Halide Perovskites

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: March 19, 2025

Inorganic semiconductors are composed of heavy elements whose vibrational motions well described by classical mechanics. Heavy elements, such as Pb and I, support charge carriers in metal halide perovskites. Nevertheless, the soft structure strong coupling between organic inorganic components create conditions which nuclear quantum effects (NQEs) can play important roles. By combining ab initio, ring-polymer, nonadiabatic molecular dynamics approaches with time-domain density functional theory, we demonstrate how NQEs influence structural electronic properties electron-vibrational hybrid organic-inorganic (MAPbI3) all-inorganic (CsPbI3) Quantum zero-point fluctuations enhance disorder, reduce band gap, accelerate elastic scattering responsible for coherence loss. have opposite influences on intraband carrier relaxation interband recombination. These inelastic events governed product overlap-like electron-phonon matrix element atomic velocity. overlap increases The involves many states. Reduction some states is offset other pathways, while an increased velocity makes faster. Electron-hole band-edge plays a key role recombination, its reduction NQEs-enhanced disorder recombination slower. This phenomenon seen both MAPbI3 CsPbI3 much more pronounced when light component present. study offers detailed understanding processes perovskites, offering theoretical insights into hot that govern performance solar cells optoelectronic devices.

Language: Английский

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Peering into interfaces in perovskite solar cells: A first-principles perspective

Journal of Physics Condensed Matter, Journal Year: 2025, Volume and Issue: 37(15), P. 151502 - 151502

Published: Feb. 24, 2025

Over the past decade, perovskite solar cells (PSCs) have experienced a rapid development. The remarkable increase in photoelectric conversion efficiency demonstrates great promise of halide perovskites field photovoltaics. Despite excellent photovoltaic performance, further efforts are needed to enhance and stability. Interfacial engineering plays crucial role enhancing stability PSCs, enabling champion sustain power above 26% for over 1000 h. As powerful theoretical tool characterizing interfaces first-principles calculations contributed understanding interfacial properties guiding materials design. In this Perspective, we highlight recent progress theoretically profiling between other materials, focusing on effects energy band alignment electronic structure carrier transport at interfaces. These help reveal atomic interfaces, provide important guidance experimental research device optimization. We also analyze potential strategies separation discuss challenges accurate modeling which will understand fundamental physics PSCs guide their

Language: Английский

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Self-Passivation at the SnO₂/Perovskite Interface

ACS Energy Letters, Journal Year: 2025, Volume and Issue: unknown, P. 1466 - 1473

Published: Feb. 28, 2025

Language: Английский

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Generalization of Quantum-Trajectory Surface Hopping to Multiple Quantum States

Journal of Chemical Theory and Computation, Journal Year: 2025, Volume and Issue: unknown

Published: March 10, 2025

In this work, we present a generalization of the quantum trajectory surface hopping (QTSH) to multiple states and its implementation in Libra package for nonadiabatic dynamics. lieu ad hoc velocity rescaling used many trajectory-based approaches, QTSH utilizes forces evolve nuclear degrees freedom continuously. It also lifts unphysical constraint enforcing total energy conservation at individual level rather conserves ensemble level. Leveraging our new multistate QTSH, perform comparative analysis method with conventional fewest switches approach. We combine decoherence corrections based on simplified decay mixing (SDM) exact factorization (XF), leading QTSH-SDM QTSH-XF schemes. Using Holstein, superexchange, phenol model Hamiltonians, assess relative accuracy resulting combined schemes reproducing branching ratios, population, coherence dynamics broad range initial conditions. observe that correction is crucial improve as well internal consistency between population from probability active state.

Language: Английский

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Dramatically Prolonged Photoexcited Carrier Lifetimes in Group-III Monochalcogenide Heterostructures through Stacking Modulation

The Journal of Physical Chemistry Letters, Journal Year: 2025, Volume and Issue: unknown, P. 4286 - 4295

Published: April 23, 2025

Modulating the carrier dynamics to achieve effective separation of photoexcited carriers is crucial for enhancing photoelectric conversion efficiency and advancing high-performance optoelectronic devices. A prototype group-III monochalcogenide heterostructure, GaSe/GaTe, has been proposed exhibit a superior light-harvesting capability highly tunable charge characteristics via nonadiabatic molecular (NAMD) simulations. The significant influence stacking patterns on revealed, with electron (hole) transfer occurring within 97 (40) 390 (126) fs, while lifetime dramatically prolonged from 12 213 ns, facilitating electron-hole (e-h) pair separation. Notably, AA' A'A configurations demonstrate remarkably extended lifetimes 161 respectively, exceeding those observed in other 2D heterostructures. weak coupling low-frequency phonon vibrational modes suppress e-h recombination, leading lifetime. These findings offer atomic insights into stacking-dependent dynamics, device design.

Language: Английский

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