Twist Angle-Dependent Intervalley Charge Carrier Transfer and Recombination in Bilayer WS2 DOI
Y. Zhu, Oleg V. Prezhdo, Run Long

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(41), P. 22826 - 22835

Published: Oct. 5, 2023

A twist angle at a van der Waals junction provides handle to tune its optoelectronic properties for variety of applications, and comprehensive understanding how the modulates electronic structure, interlayer coupling, carrier dynamics is needed. We employ time-dependent density functional theory nonadiabatic molecular elucidate angle-dependent intervalley transfer recombination in bilayer WS2. Repulsion between S atoms twisted configurations weakens increases distance, softens layer breathing modes. Twisting has minor influence on K valleys while it lowers Γ raises Q because their wave functions are delocalized layers. Consequently, reduced energy gaps accelerate hole structures. Intervalley electron proceeds nearly an order magnitude faster than transfer. The more localized values larger bandgaps result smaller couplings recombination, making 3-4 times slower high-symmetry B2g breathing, E2g in-plane, A1g out-of-plane modes most active during recombination. extended lifetimes junctions favorable device performance.

Language: Английский

Ultrafast dynamics in van der Waals heterostructures DOI
Chenhao Jin, Yue Ma, Ouri Karni

et al.

Nature Nanotechnology, Journal Year: 2018, Volume and Issue: 13(11), P. 994 - 1003

Published: Oct. 29, 2018

Language: Английский

Citations

505
Interlayer exciton formation, relaxation, and transport in TMD van der Waals heterostructures DOI Creative Commons
Ying Jiang, Shula Chen, Weihao Zheng

et al.

Light Science & Applications, Journal Year: 2021, Volume and Issue: 10(1)

Published: April 2, 2021

Abstract Van der Waals (vdW) heterostructures based on transition metal dichalcogenides (TMDs) generally possess a type-II band alignment that facilitates the formation of interlayer excitons between constituent monolayers. Manipulation in TMD vdW holds great promise for development excitonic integrated circuits serve as counterpart electronic circuits, which allows photons and to transform into each other thus bridges optical communication signal processing at circuit. As consequence, numerous studies have been carried out obtain deep insight physical properties excitons, including revealing their ultrafast formation, long population recombination lifetimes, intriguing spin-valley dynamics. These outstanding ensure with good transport characteristics, may pave way potential applications efficient devices heterostructures. At present, systematic comprehensive overview exciton relaxation, transport, is still lacking. In this review, we give description discussion these frontier topics provide valuable guidance researchers field.

Language: Английский

Citations

311
Ab initio nonadiabatic molecular dynamics investigations on the excited carriers in condensed matter systems DOI
Qijing Zheng, Weibin Chu, Chuanyu Zhao

et al.

Wiley Interdisciplinary Reviews Computational Molecular Science, Journal Year: 2019, Volume and Issue: 9(6)

Published: March 14, 2019

The ultrafast dynamics of photoexcited charge carriers in condensed matter systems play an important role optoelectronics and solar energy conversion. Yet it is challenging to understand such multidimensional at the atomic scale. Combining real‐time time‐dependent density functional theory with fewest‐switches surface hopping scheme, we develop ab initio nonadiabatic molecular (NAMD) code Hefei‐NAMD simulate excited carrier systems. Using this method, have investigated interfacial transfer dynamics, electron–hole recombination spin‐polarized hole different are studied energy, real momentum spaces. In addition, coupling phonons, defects adsorptions investigated. state‐of‐art NAMD studies provide unique insights This article categorized under: Structure Mechanism > Computational Materials Science Molecular Statistical Mechanics Dynamics Monte‐Carlo Methods Electronic Theory Ab Initio Software Simulation

Language: Английский

Citations

294
Low-frequency lattice phonons in halide perovskites explain high defect tolerance toward electron-hole recombination DOI Creative Commons
Weibin Chu, Qijing Zheng, Oleg V. Prezhdo

et al.

Science Advances, Journal Year: 2020, Volume and Issue: 6(7)

Published: Feb. 14, 2020

Low-cost solution-based synthesis of metal halide perovskites (MHPs) invariably introduces defects in the system, which could form Shockley-Read-Hall (SRH) electron-hole recombination centers detrimental to solar conversion efficiency. Here, we investigate nonradiative processes due native point methylammonium lead (MAPbI3) using ab initio nonadiabatic molecular dynamics within surface-hopping framework. Regardless whether introduce a shallow or deep band state, find that charge MAPbI3 is not enhanced, contrary predictions from SRH theory. We demonstrate this strong tolerance against defects, and hence breakdown SRH, arises because photogenerated carriers are only coupled with low-frequency phonons electron hole states overlap weakly. Both factors appreciably decrease coupling. argue soft nature inorganic lattice small bulk modulus key for defect tolerance, hence, findings general other MHPs.

Language: Английский

Citations

244
Excitons in semiconductor moiré superlattices DOI
Di Huang, Junho Choi, Chih‐Kang Shih

et al.

Nature Nanotechnology, Journal Year: 2022, Volume and Issue: 17(3), P. 227 - 238

Published: March 1, 2022

Language: Английский

Citations

185
Interface Characterization and Control of 2D Materials and Heterostructures DOI
Xiaolong Liu, Mark C. Hersam

Advanced Materials, Journal Year: 2018, Volume and Issue: 30(39)

Published: July 23, 2018

Abstract 2D materials and heterostructures have attracted significant attention for a variety of nanoelectronic optoelectronic applications. At the atomically thin limit, material characteristics functionalities are dominated by surface chemistry interface coupling. Therefore, methods comprehensively characterizing precisely controlling surfaces interfaces required to realize full technological potential materials. Here, properties that govern performance introduced. Then experimental approaches resolve phenomena down atomic scale, as well strategies allow tuning optimization interfacial interactions in van der Waals heterostructures, systematically reviewed. Finally, future outlook delineates remaining challenges opportunities characterization control is presented.

Language: Английский

Citations

170
Material platforms for defect qubits and single-photon emitters DOI Creative Commons
Gang Zhang, Yuan Cheng, Jyh‐Pin Chou

et al.

Applied Physics Reviews, Journal Year: 2020, Volume and Issue: 7(3)

Published: Sept. 1, 2020

Quantum technology has grown out of quantum information theory and now provides a valuable tool that researchers from numerous fields can add to their toolbox research methods. To date, various systems have been exploited promote the application processing. The be used for include superconducting circuits, ultracold atoms, trapped ions, semiconductor dots, solid-state spins emitters. In this review, we will discuss state-of-the-art material platforms spin-based technology, with focus on progress in emitters several leading host materials, including diamond, silicon carbide, boron nitride, silicon, two-dimensional semiconductors, other materials. We highlight how first-principles calculations serve as an exceptionally robust finding novel defect qubits single-photon solids, through detailed predictions electronic, magnetic, optical properties.

Language: Английский

Citations

157
Rational Design and Characterization of Direct Z-Scheme Photocatalyst for Overall Water Splitting from Excited State Dynamics Simulations DOI
Xianghong Niu, Xiaowan Bai, Zhaobo Zhou

et al.

ACS Catalysis, Journal Year: 2020, Volume and Issue: 10(3), P. 1976 - 1983

Published: Jan. 8, 2020

Direct Z-scheme heterostructure photocatalysts possess tremendous potential to solar-driven overall water splitting, but how rationally design and comprehensively characterize high-efficient direct heterostructures remains a great challenge. Herein, we report the of metal-free C3B/C3N through constructing p-n heterojunction as photocatalyst for splitting by combining first-principles excited state dynamics simulations. Our calculations show that strong interlayer interaction in provides large built-in electric field with about 0.4 V/Å interface nonadiabatic coupling which significantly accelerates recombination carriers weak redox capacity (∼0.5 ps) retards lifetime (∼4 ps). Meanwhile, B atoms, serving Lewis acid sites, are good catalytic centers trap molecules. The hydrogen reduction reaction complex four-electronic oxidation can happen smoothly on C3B C3N surface, respectively, without additional overpotential cocatalyst. This work not only also paves way rational high-performance photocatalysts.

Language: Английский

Citations

153
Structure modulation of two-dimensional transition metal chalcogenides: recent advances in methodology, mechanism and applications DOI
Yao Xiao, Chengyi Xiong, Miaomiao Chen

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(4), P. 1215 - 1272

Published: Jan. 1, 2023

Together with the development of two-dimensional (2D) materials, transition metal dichalcogenides (TMDs) have become one most popular series model materials for fundamental sciences and practical applications. Due to ever-growing requirements customization multi-function, dozens modulated structures been introduced in TMDs. In this review, we present a systematic comprehensive overview structure modulation TMDs, including point, linear out-of-plane structures, following updating conventional classification silicon related bulk semiconductors. particular, focus on structural characteristics TMD analyse corresponding root causes. We also summarize recent progress modulating methods, mechanisms, properties applications based structures. Finally, demonstrate challenges prospects TMDs forecast potential directions about what how breakthroughs can be achieved.

Language: Английский

Citations

69
Photoelectron “Bridge” in Van Der Waals Heterojunction for Enhanced Photocatalytic CO2 Conversion Under Visible Light DOI
Pir Muhammad Ismail, Sajjad Ali, Sharafat Ali

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(38)

Published: June 26, 2023

Constructing Van der Waals heterojunction is a crucial strategy to achieve excellent photocatalytic activity. However, in most heterojunctions synthesized by ex situ assembly, electron transfer encounters huge hindrances at the interface between two components due large spacing and potential barrier. Herein, phosphate-bridged of cobalt phthalocyanine (CoPc)/tungsten disulfide (WS2 ) bridged phosphate (xCoPc-nPO4- -WS2 designed prepared traditional wet chemistry method. By introducing small molecule into CoPc WS2 , creates an "bridge", resulting compact combination eliminating space Therefore, (PO4- bridge can serve as efficient channel efficiently transmit photoelectrons from under excited states. These are captured catalytic central Co2+ subsequently convert CO2 molecules CO CH4 products, achieving 17-fold enhancement on 3CoPc-0.6PO4- sample compared that pure . Introducing "bridge" create provides new perspective designing photocatalysts for reduction valuable products.

Language: Английский

Citations

54