Twist Angle-Dependent Intervalley Charge Carrier Transfer and Recombination in Bilayer WS2

被引:28
|
作者
Zhu, Yonghao [1 ]
Prezhdo, Oleg V. [2 ]
Long, Run [1 ]
Fang, Wei-Hai [1 ]
机构
[1] Beijing Normal Univ, Coll Chem, Key Lab Theoret & Computat Photochem, Minist Educ, Beijing 100875, Peoples R China
[2] Univ Southern Calif, Dept Chem, Los Angeles, CA 90089 USA
基金
美国国家科学基金会;
关键词
TRANSITION-METAL DICHALCOGENIDES; MOLYBDENUM-DISULFIDE; EXCITON DISSOCIATION; ELECTRONIC-STRUCTURE; MOLECULAR-DYNAMICS; PYXAID PROGRAM; STACKING; MOSE2; SCHEMES; GROWTH;
D O I
10.1021/jacs.3c09170
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
A twist angle at a van der Waals junction provides a handle to tune its optoelectronic properties for a variety of applications, and a comprehensive understanding of how the twist modulates electronic structure, interlayer coupling, and carrier dynamics is needed. We employ time-dependent density functional theory and nonadiabatic molecular dynamics to elucidate angle-dependent intervalley carrier transfer and recombination in bilayer WS2. Repulsion between S atoms in twisted configurations weakens interlayer coupling, increases the interlayer distance, and softens layer breathing modes. Twisting has a minor influence on K valleys while it lowers Gamma valleys and raises Q valleys because their wave functions are delocalized between layers. Consequently, the reduced energy gaps between the K and Gamma valleys accelerate the hole transfer in the twisted structures. Intervalley electron transfer proceeds nearly an order of magnitude faster than hole transfer. The more localized wave functions at K than Q values and larger bandgaps result in smaller nonadiabatic couplings for intervalley recombination, making it 3-4 times slower in twisted than high-symmetry structures. B-2g breathing, E-2g in-plane, and A(1g) out-of-plane modes are most active during intervalley carrier transfer and recombination. The faster intervalley transfer and extended carrier lifetimes in twisted junctions are favorable for optoelectronic device performance.
引用
收藏
页码:22826 / 22835
页数:10
相关论文
共 50 条
  • [1] Twist Angle-Dependent Exciton Mobility in WS2 Bilayers
    Zhong, Yangguang
    Yue, Shuai
    Liang, Jieyuan
    Yuan, Long
    Xia, Yuexing
    Tian, Yubo
    Zheng, Yuanyuan
    Zhang, Yuyang
    Du, Wenna
    Li, Dong
    Chen, Shula
    Pan, Anlian
    Liu, Xinfeng
    NANO LETTERS, 2025, 25 (13) : 5274 - 5282
  • [2] Probing Angle-Dependent Interlayer Coupling in Twisted Bilayer WS2
    Yan, Wei
    Meng, Lan
    Meng, Zhaoshun
    Weng, Yakui
    Kang, Lulu
    Li, Xing-ao
    JOURNAL OF PHYSICAL CHEMISTRY C, 2019, 123 (50): : 30684 - 30688
  • [3] Twist Angle-Dependent Optical Responses in Controllably Grown WS2 Vertical Homojunctions
    Shao, Gonglei
    Xue, Xiong-Xiong
    Liu, Xiao
    Zhang, Danliang
    Jin, Yuanyuan
    Wu, Yangwu
    You, Bingying
    Lin, Yung-Chang
    Li, Shisheng
    Suenaga, Kazu
    Wang, Xiao
    Pan, Anlian
    Li, Huimin
    Hong, Jinhua
    Feng, Yexin
    Liu, Song
    CHEMISTRY OF MATERIALS, 2020, 32 (22) : 9721 - 9729
  • [4] The twist angle has weak influence on charge separation and strong influence on recombination in the MoS2/WS2 bilayer: ab initio quantum dynamics
    Zhu, Yonghao
    Fang, Wei-Hai
    Rubio, Angel
    Long, Run
    Prezhdo, Oleg, V
    JOURNAL OF MATERIALS CHEMISTRY A, 2022, 10 (15) : 8324 - 8333
  • [5] Twist angle-dependent transport properties of twisted bilayer graphene
    Kim, Jin Hong
    Kang, Seoung-Hun
    Yoon, Duhee
    Kim, Hakseong
    Kim, Jin-Soo
    Haidari, Mohd Musaib
    Jang, Dong Jin
    Ko, Jin-Yong
    Son, Young-Woo
    Park, Bae Ho
    Choi, Jin Sik
    NPG ASIA MATERIALS, 2024, 16 (01)
  • [6] Twist Angle-Dependent Molecular Intercalation and Sheet Resistance in Bilayer Graphene
    Araki, Yuji
    Solis-Fernandez, Pablo
    Lin, Yung-Chang
    Motoyama, Amane
    Kawahara, Kenji
    Maruyama, Mina
    Gao, Yanlin
    Matsumoto, Rika
    Suenaga, Kazu
    Okada, Susumu
    Ago, Hiroki
    ACS NANO, 2022, 16 (09) : 14075 - 14085
  • [7] Identification of twist-angle-dependent excitons in WS2/WSe2 heterobilayers
    Ke Wu
    Hongxia Zhong
    Quanbing Guo
    Jibo Tang
    Jing Zhang
    Lihua Qian
    Zhifeng Shi
    Chendong Zhang
    Shengjun Yuan
    Shunping Zhang
    Hongxing Xu
    National Science Review, 2022, 9 (06) : 56 - 63
  • [8] Identification of twist-angle-dependent excitons in WS2/WSe2 heterobilayers
    Wu, Ke
    Zhong, Hongxia
    Guo, Quanbing
    Tang, Jibo
    Zhang, Jing
    Qian, Lihua
    Shi, Zhifeng
    Zhang, Chendong
    Yuan, Shengjun
    Zhang, Shunping
    Xu, Hongxing
    NATIONAL SCIENCE REVIEW, 2022, 9 (06)
  • [9] Ultrafast Interlayer Charge Transfer between Bilayer PtSe2 and Monolayer WS2
    Wang, Pengzhi
    He, Dawei
    Wang, Yongsheng
    Zhang, Xiaoxian
    He, Xiaoyue
    He, Jiaqi
    Zhao, Hui
    ACS APPLIED MATERIALS & INTERFACES, 2021, 13 (48) : 57822 - 57830
  • [10] Twist-angle-dependent interlayer exciton diffusion in WS2–WSe2 heterobilayers
    Long Yuan
    Biyuan Zheng
    Jens Kunstmann
    Thomas Brumme
    Agnieszka Beata Kuc
    Chao Ma
    Shibin Deng
    Daria Blach
    Anlian Pan
    Libai Huang
    Nature Materials, 2020, 19 : 617 - 623