Nonradiative Charge Recombination Dynamics in Fully Hydroxylated Hematite Surface: A Time-Domain Ab Initio Study DOI
Yi Liu, Bipeng Wang, Hua Wang

et al.

The Journal of Physical Chemistry C, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 3, 2024

Hematite (α-Fe2O3) is a typical semiconducting transition metal oxide that exhibits attractive properties for photoelectrochemical (PEC) water splitting and other applications. However, it has been widely reported charge recombination in α-Fe2O3 photoanodes serious problem, hindering further improvement the efficiency of PEC splitting. We used ab initio nonadiabatic molecular dynamics (NAMD) to investigate bulk surface phases α-Fe2O3. The NAMD simulations employ decoherence-induced hopping (DISH) method implemented within time-dependent density functional theory. test demonstrate need incorporate both phase-consistency correction all-electron calculation NA coupling, latter needed metals with d-shell electrons. show time scale intrinsic can reach microseconds, accordance existence long-lived photogenerated carriers observed transient absorption measurements on electrodes. hydroxylated iron-termination α-Fe2O3(0001) surface, one most stable surfaces aqueous solution, much faster recombination, about 1 order magnitude compared key factor fast mainly be assigned strong fluctuations NAC energy gap between conduction band minimum (CBM) valence maximum (VBM) quantum anti-Zeno effect. This work extends from phase interfacial α-Fe2O3, approaching reaction conditions, thus assists understanding underlying oxygen evolution (OER) at Fe2O3–water interface design new efficient Fe2O3-based photoanode materials.

Language: Английский

Compression of Organic Molecules Coupled with Hydrogen Bonding Extends the Charge Carrier Lifetime in BA2SnI4 DOI
Xinbo Ma, Wei‐Hai Fang, Run Long

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(23), P. 16314 - 16323

Published: May 30, 2024

Two-dimensional (2D) metal halide perovskites, such as BA2SnI4 (BA═CH3(CH2)3NH3), exhibit an enhanced charge carrier lifetime in experiments under strain. Experiments suggest that significant compression of the BA molecule, rather than inorganic lattice, contributes to this enhancement. To elucidate underlying physical mechanism, we apply a moderate compressive strain entire system and subsequently introduce molecules. We then perform ab initio nonadiabatic molecular dynamics simulations nonradiative electron–hole recombination. observe overall lattice reduces atomic motions decreases coupling, thereby delaying Additionally, molecules enhances hydrogen bonding between iodine atoms, which lengthens Sn–I bonds, distorts [SnI6]4– octahedra, suppresses further, thus reducing coupling. Also, elongated bonds weakened antibonding interactions increase band gap. Altogether, delays recombination by more factor 3. Our provide new valuable insights into how strain, accommodated primarily organic ligands, positively influences optoelectronic properties 2D layered offering promising pathway for further performance improvements.

Language: Английский

Citations

11
Origin of the Improved Photoelectrochemical and Photocatalytic Activity in a ZnO-TiO2 Nanohybrid Revealed by Experimental and Density Functional Theory Studies DOI Creative Commons
Abinash Das, Dongyu Liu, Yifan Wu

et al.

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: 15(29), P. 7524 - 7532

Published: July 18, 2024

Heterojunctions of metal oxides have attracted a great deal attention as photo (electro) catalysts owing to their excellent photoactivity. While multiple fundamental studies been dedicated heteroaggregation, self-assembly oppositely charged particles obtain heterojunctions for energy applications has underexplored. Herein, we report the synthesis ZnO-TiO2 using electrostatic approach. The synthesized were characterized by experimental techniques. Density functional theory calculations conducted establish heterojunction formation mechanism and electronic properties. nanohybrid was tested photodegradation rhodamine B dye water splitting applications. photocatalytic performance is 3.5 times higher than that bare ZnO. In addition, heterostructure exhibited an photocurrent density 2.4 mA cm–2 at low onset potential during photoelectrochemical oxygen evolution. improvements are attributed type II between ZnO TiO2, which suppresses carrier recombination enhances transport, boosting catalytic activity.

Language: Английский

Citations

8
Self-passivation of Halide Interstitial Defects by Organic Cations in Hybrid Lead-Halide Perovskites: Ab Initio Quantum Dynamics DOI
Xinbo Ma, Xue Tian,

Elizabeth Stippell

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(42), P. 29255 - 29265

Published: Oct. 11, 2024

Halide interstitial defects severely hinder the optoelectronic performance of metal halide perovskites, making research on their passivation crucial. We demonstrate, using ab initio nonadiabatic molecular dynamics simulations, that hydrogen vacancies (H

Language: Английский

Citations

7
Detrimental Defect Cooperativity at TiO2/CH3NH3PbI3 Interface: Decreased Stability, Enhanced Ion Diffusion, and Reduced Charge Lifetime and Transport DOI
Kaiping Wang, Zhiwei Wu, K. L. Wang

et al.

ACS Energy Letters, Journal Year: 2024, Volume and Issue: unknown, P. 5888 - 5897

Published: Nov. 18, 2024

Interfaces are essential for solar cell performance since they govern charge separation and transport. Using quantum dynamics simulation, we demonstrate that at interfaces, common defects benign on their own, iodine vacancy in CH3NH3PbI3 (VI) oxygen TiO2 (VO), responsible synergistically poor stability losses. VO promotes VI diffusion accelerates migration. A midgap trap state appears, inhibiting transport accelerating recombination by an order of magnitude. Strong structural distortions strengthen electron-vibrational interactions activate high-frequency phonons. Because the widely reported high defect-tolerance lead-halide perovskites, synergistic detrimental influence perovskite with other materials is often overlooked. The interfacial defect pairing could be a major reason losses cells. results suggest either high-quality or extraction layer may sufficient to achieve performance.

Language: Английский

Citations

6
One Step Synthesis of Carbon Nitride/Carbon Nanotube Composite Nanomaterials Modified Electrode for Sensitive Electrochemical Detection of Bisphenol A DOI Creative Commons
Yanhua Sun, Mang Niu, Yang Bai

et al.

Journal of The Electrochemical Society, Journal Year: 2025, Volume and Issue: 172(2), P. 027503 - 027503

Published: Jan. 29, 2025

In this work, RCN/WCNTs nanocomposites were synthesized using a one-step method and characterized SEM, XPS, FTIR. An electrochemical sensor capable of sensitive rapid detection BPA was developed by modifying on glassy carbon electrode. The exhibited excellent response to in 0.2 M PBS (pH 7.0) under optimal selection conditions. linear range the 0.01–43 μM, limit (S/N = 3) 0.0017 μM. addition, good immunity, stability reproducibility. And it applied real samples.

Language: Английский

Citations

0
Applications of machine learning in surfaces and interfaces DOI Open Access
Shaofeng Xu, Jing‐Yuan Wu, Ying Guo

et al.

Chemical Physics Reviews, Journal Year: 2025, Volume and Issue: 6(1)

Published: March 1, 2025

Surfaces and interfaces play key roles in chemical material science. Understanding physical processes at complex surfaces is a challenging task. Machine learning provides powerful tool to help analyze accelerate simulations. This comprehensive review affords an overview of the applications machine study systems materials. We categorize into following broad categories: solid–solid interface, solid–liquid liquid–liquid surface solid, liquid, three-phase interfaces. High-throughput screening, combined first-principles calculations, force field accelerated molecular dynamics simulations are used rational design such as all-solid-state batteries, solar cells, heterogeneous catalysis. detailed information on for

Language: Английский

Citations

0
Revealing Irradiation-Induced Dynamic Structural Failure in LiCoO2 Cathodes via Electron-Temperature-Dependent Deep Potential Molecular Dynamics DOI
Pengfei Liu, Yuanyuan Liu, Xiaoya Zhang

et al.

The Journal of Physical Chemistry Letters, Journal Year: 2025, Volume and Issue: unknown, P. 4155 - 4161

Published: April 18, 2025

In lithium-ion batteries (LIBs) used for deep-space exploration, LiCoO2 cathode materials face significant challenges in high-radiation environments, including structural degradation and ion migration. This study investigates the dynamic evolution of under irradiation using electron-temperature-dependent deep potential (ETD-DP) model. Compared with traditional ab initio molecular dynamics (AIMD) simulations, ETD-DP method extends both spatial temporal scales by several orders magnitude. The results reveal that LiCoO2's response to occurs on nanosecond time scale, divided into three stages: traversal, intense local adjustment, structure relaxation. During adjustment stage, induces migration transition metal ions toward lithium layers. relaxation cobalt displaced from their equilibrium positions form a dumbbell adjacent Co ions. simulation were validated through high-energy electron beam experiments aberration-corrected microscopy. provides valuable insights improving tolerance LIB offers new perspectives application particle-beam-based fine characterization techniques advanced battery applications.

Language: Английский

Citations

0
Reactive Site Transformation in Non-Metal Doped Polymeric Carbon Nitride Improving CO2 Photoreduction Efficiency DOI
Yuehua Kong, Jinhua Ye, Kaining Ding

et al.

The Journal of Physical Chemistry Letters, Journal Year: 2025, Volume and Issue: unknown, P. 4869 - 4874

Published: May 9, 2025

Polymeric carbon nitride (PCN, also called melon) was a potential photocatalyst for the CO2 reduction reaction (CO2RR), but conjugation of system inhibited efficiency. By modifying melon with non-metal elements such as boron (B), phosphorus (P), oxygen (O), and sulfur (S), we found that S (or O) doped (S/melon, O/melon) transformed reactive site pyridine nitrogen (N) to (C), which promoted COOH* hydrogenation CO* and, thus, improved reactivity CO selectivity significantly. In addition, nonadiabatic molecular dynamics simulations showed trap states O/melon S/melon can rapidly capture excited electrons participate in CO2RR improve photocatalytic This work provided theoretical insight design efficient photocatalysts based on metal-free materials.

Language: Английский

Citations

0
Enhancement of hole capture and water dissociation on rutile TiO2(110) by intermolecular hydrogen bonding: time-domain ab initio study DOI
Yitong Zhang, Cheng Cheng, Yifan Wu

et al.

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(38), P. 26178 - 26187

Published: Jan. 1, 2024

Enhanced intermolecular hydrogen bonds accelerate photogenerated hole capture and water dissociation.

Language: Английский

Citations

3
Nonradiative Charge Recombination Dynamics in Fully Hydroxylated Hematite Surface: A Time-Domain Ab Initio Study DOI
Yi Liu, Bipeng Wang, Hua Wang

et al.

The Journal of Physical Chemistry C, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 3, 2024

Hematite (α-Fe2O3) is a typical semiconducting transition metal oxide that exhibits attractive properties for photoelectrochemical (PEC) water splitting and other applications. However, it has been widely reported charge recombination in α-Fe2O3 photoanodes serious problem, hindering further improvement the efficiency of PEC splitting. We used ab initio nonadiabatic molecular dynamics (NAMD) to investigate bulk surface phases α-Fe2O3. The NAMD simulations employ decoherence-induced hopping (DISH) method implemented within time-dependent density functional theory. test demonstrate need incorporate both phase-consistency correction all-electron calculation NA coupling, latter needed metals with d-shell electrons. show time scale intrinsic can reach microseconds, accordance existence long-lived photogenerated carriers observed transient absorption measurements on electrodes. hydroxylated iron-termination α-Fe2O3(0001) surface, one most stable surfaces aqueous solution, much faster recombination, about 1 order magnitude compared key factor fast mainly be assigned strong fluctuations NAC energy gap between conduction band minimum (CBM) valence maximum (VBM) quantum anti-Zeno effect. This work extends from phase interfacial α-Fe2O3, approaching reaction conditions, thus assists understanding underlying oxygen evolution (OER) at Fe2O3–water interface design new efficient Fe2O3-based photoanode materials.

Language: Английский

Citations

2