Orbital hybridization induces fast photoelectron capture by graphene to promote high gain in transition metal dichalcogenide/graphene heterojunctions DOI
Tingbo Zhang,

Xinying Gao,

Meiling Xu

и другие.

Physical review. B./Physical review. B, Год журнала: 2024, Номер 110(24)

Опубликована: Дек. 2, 2024

Transition metal dichalcogenide/graphene (TMDC/Gr) heterojunction devices exhibit significantly higher photoresponsivity compared to TMDC alone, making them promising for optoelectronic applications. However, experiments demonstrated that graphene cannot prolong the photogenerated carrier lifetime of TMDC/Gr heterojunctions and, further, high density sulfur vacancies in TMDCs complicates dynamics, leaving underlying physical mechanism behind unclear. Herein, we investigate transfer and recombination $\mathrm{Mo}{\mathrm{S}}_{2}$/Gr $\mathrm{W}{\mathrm{S}}_{2}$/Gr through nonadiabatic molecular dynamics simulations. Instead conventional speculation store carriers enhance performance, find hybridization between defect states Dirac points induces fast photoelectron from graphene, promoting gain heterojunctions. Fast derives excitation low-frequency in-plane phonon modes. Meanwhile, does not drastically reduce Therefore, faster electrons long lead gain, resulting superior performance This study provides a comprehensive understanding heterojunctions, laying foundation design high-performance devices.

Язык: Английский

Nuclear Quantum Effects Accelerate Hot Carrier Relaxation but Slow Down Recombination in Metal Halide Perovskites DOI
Yulong Liu, Shiying Shen, Oleg V. Prezhdo

и другие.

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Март 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.

Язык: Английский

Процитировано

1
Nuclear Quantum Effects Accelerate Charge Separation and Recombination in g-C3N4/TiO2 Heterojunctions DOI
Yitong Zhang, Run Long

The Journal of Physical Chemistry Letters, Год журнала: 2024, Номер 15(23), С. 6002 - 6009

Опубликована: Май 30, 2024

We combined ring–polymer molecular dynamics (MD) and ab initio MD with nonadiabatic to study the effects of nuclear quantum (NQEs) on interlayer electron transfer electron–hole recombination at g-C3N4/TiO2 interface. Our simulations indicate that NQEs significantly affect dynamics, accelerating both processes. deform g-C3N4 layer expedite movement carbon nitrogen atoms, thus, enhancing charge delocalization coupling. This improved overlap between electronic state wave functions enhances couplings, facilitating recombination. In addition enhanced couplings transfer, presence narrows energy gap delays decoherence by mitigating overall fluctuations, because restricted TiO2 movements overwhelming thereby making faster. work provides valuable insights into in light-element systems contributes guiding development highly efficient photocatalysts.

Язык: Английский

Процитировано

3
Nonadiabatic Molecular Dynamics in Momentum Space Beyond Harmonic Approximation: Hot Electron Relaxation in Photoexcited Black Phosphorus DOI
Haoran Lu, Wei‐Hai Fang, Run Long

и другие.

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(28), С. 19547 - 19554

Опубликована: Июль 8, 2024

We simulated hot-electron relaxation in black phosphorus using the nonadiabatic molecular dynamics (NA-MD) approach with a non-Condon effect momentum space beyond harmonic approximation. By comparing simulations at Γ point large supercell those few

Язык: Английский

Процитировано

3
Formation and Recombination Dynamics of Polarons in Goethite: A Time-Domain Ab Initio Study DOI
Hongliang Li, Zhaohui Zhou, Andrey S. Vasenko

и другие.

The Journal of Physical Chemistry Letters, Год журнала: 2024, Номер unknown, С. 10018 - 10025

Опубликована: Сен. 25, 2024

The temperature and the coordination environment significantly affect polaron dynamics. Using goethite (FeOOH) as a model, our study examines formation recombination behavior under various conditions, including electron injection, photoexcitation, heterovalent doping. Ab initio nonadiabatic molecular dynamics (NAMD) simulations reveal that in FeOOH is dependent on via an adiabatic mechanism with higher temperatures leading to shorter times. Only polarons form FeOOH, regardless of method. NAMD indicate photoexcited faster than Fe

Язык: Английский

Процитировано

3
Self-Passivation at the SnO2/Perovskite Interface DOI
Kai-Ping Wang,

Dong Xue,

Jinbao Yuan

и другие.

ACS Energy Letters, Год журнала: 2025, Номер unknown, С. 1466 - 1473

Опубликована: Фев. 28, 2025

Язык: Английский

Процитировано

0
Interplay of Ultrafast Electron–Phonon and Electron–Electron Scattering in Ti3C2Tx MXenes: Ab Initio Quantum Dynamics DOI
Shiying Shen, Haoran Lu, Shriya Gumber

и другие.

Nano Letters, Год журнала: 2025, Номер unknown

Опубликована: Апрель 24, 2025

Nonthermal electrons are vital in solar energy and optoelectronics, yet their relaxation pathways not fully understood. Ab initio quantum dynamics reveal that Ti3C2O2 electron-phonon (e-ph) is faster than electron-electron (e-e) scattering due to strong coupling with the A1g phonon at 190 cm-1 presence of light C O atoms. Nuclear effects minimal; vibrations influence e-e only indirectly, mode' zero-point much lower thermal ambient conditions. Substituting heavier S Ti3C2OS slows e-ph enhances scattering, making it a process. However, both channels proceed concurrently, challenging time scale separation often used for metals. These results underscore need atomistic-level understanding nonthermal electron dynamics, especially light-element systems such as MXenes, provide guidance optimizing electronic advanced optoelectronic materials devices.

Язык: Английский

Процитировано

0
Nuclear Quantum Effects Enhance Structural Stability but Accelerate Charge Carrier Recombination in MHyPbBr3 Perovskite DOI

X.G. Zhen,

Run Long

The Journal of Physical Chemistry Letters, Год журнала: 2024, Номер unknown, С. 12076 - 12082

Опубликована: Ноя. 26, 2024

Hybrid organic–inorganic perovskites exhibit significant nuclear quantum effects (NQEs) due to their light hydrogen atoms. By performing ring polymer molecular dynamics, ab initio and nonadiabatic dynamics simulations on the MHyPbBr3 (MHy+ = CH3NH2NH2+) perovskites, we demonstrate that NQEs stabilize lattice by suppressing atomic motions accelerate nonradiative charge recombination. This stabilization arises from synergistic of Pb–N coordination bonds N–H···Br bonds, which enhance interactions. As a result, Pb–Br octahedra, particularly [Pb(1)Br6]4– octahedra supporting electron hole, are well-preserved, promoting electronic wavefunction delocalization increasing electron–hole overlap. These coupling overcoming reduced motions. Overall, this prolonged decoherence time recombination NQEs. Our study highlights unique influence geometrical stability carrier in MHyPbBr3, offering fundamental insights for future material design.

Язык: Английский

Процитировано

1
Orbital hybridization induces fast photoelectron capture by graphene to promote high gain in transition metal dichalcogenide/graphene heterojunctions DOI
Tingbo Zhang,

Xinying Gao,

Meiling Xu

и другие.

Physical review. B./Physical review. B, Год журнала: 2024, Номер 110(24)

Опубликована: Дек. 2, 2024

Transition metal dichalcogenide/graphene (TMDC/Gr) heterojunction devices exhibit significantly higher photoresponsivity compared to TMDC alone, making them promising for optoelectronic applications. However, experiments demonstrated that graphene cannot prolong the photogenerated carrier lifetime of TMDC/Gr heterojunctions and, further, high density sulfur vacancies in TMDCs complicates dynamics, leaving underlying physical mechanism behind unclear. Herein, we investigate transfer and recombination $\mathrm{Mo}{\mathrm{S}}_{2}$/Gr $\mathrm{W}{\mathrm{S}}_{2}$/Gr through nonadiabatic molecular dynamics simulations. Instead conventional speculation store carriers enhance performance, find hybridization between defect states Dirac points induces fast photoelectron from graphene, promoting gain heterojunctions. Fast derives excitation low-frequency in-plane phonon modes. Meanwhile, does not drastically reduce Therefore, faster electrons long lead gain, resulting superior performance This study provides a comprehensive understanding heterojunctions, laying foundation design high-performance devices.

Язык: Английский

Процитировано

1