Energy-valley-dependent charge transfer in few-layer transition metal dichalcogenide heterostructures

Valencia-Acuna, Pavel; Amos, Stephanie; Peelaers, Hartwin; Zhao, Hui

doi:10.1103/physrevb.108.085302

Energy-valley-dependent charge transfer in few-layer transition metal dichalcogenide heterostructures

Journal Article · Mon Aug 07 00:00:00 EDT 2023 · Physical Review. B

DOI:https://doi.org/10.1103/physrevb.108.085302· OSTI ID:2242381

Valencia-Acuna, Pavel ^[1]; Amos, Stephanie ^[2]; ^[2]; ^[2]

University of Kansas, Lawrence, KS (United States); The University of Kansas
University of Kansas, Lawrence, KS (United States)

The effect of the energy valley on interlayer charge transfer in transition metal dichalcogenide (TMD) heterostructures is studied by transient absorption spectroscopy and density functional theory. First-principles calculations confirm that the Λ_min valley in the conduction band of few-layer WSe₂ evolves from above its K valley in the monolayer (1L) to below it in 4L. Heterostructure samples of nL–WSe₂/1L–MoS₂, where n = 1,2,3, and 4, are obtained by mechanical exfoliation and dry transfer. Photoluminescence spectroscopy reveals a thickness-dependent WSe₂ band structure and efficient interlayer charge transfer. Transient absorption measurements show that the electron transfer time from the Λ_min valley of 4L WSe₂ to the K valley of MoS₂ is on the order of 30 ps. This process is much slower than the K-K charge transfer in 1L/1L TMD heterostructures. Furthermore, the momentum-indirect interlayer excitons formed after charge transfer have lifetimes >1 ns.

View Accepted Manuscript (DOE)

Research Organization:: University of Kansas, Lawrence, KS (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE): National Science Foundation (NSF)

Grant/Contract Number:: SC0020995

OSTI ID:: 2242381

Journal Information:: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 8 Vol. 108; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (64)

Semiempirical GGA-type density functional constructed with a long-range dispersion correction Grimme, Stefan Journal of Computational Chemistry, Vol. 27, Issue 15, p. 1787-1799 https://doi.org/10.1002/jcc.20495	journal	January 2006
Ultrafast Electron and Hole Relaxation Pathways in Few-Layer MoS ₂ Nie, Zhaogang; Long, Run; Teguh, Jefri S. The Journal of Physical Chemistry C, Vol. 119, Issue 35 https://doi.org/10.1021/acs.jpcc.5b05048	journal	August 2015
Dielectric Environment-Robust Ultrafast Charge Transfer Between Two Atomic Layers Zhou, Hongzhi; Zhao, Yida; Zhu, Haiming The Journal of Physical Chemistry Letters, Vol. 10, Issue 2 https://doi.org/10.1021/acs.jpclett.8b03596	journal	December 2018
Dissecting Interlayer Hole and Electron Transfer in Transition Metal Dichalcogenide Heterostructures via Two-Dimensional Electronic Spectroscopy Policht, Veronica R.; Russo, Mattia; Liu, Fang Nano Letters, Vol. 21, Issue 11 https://doi.org/10.1021/acs.nanolett.1c01098	journal	May 2021
Probing Interlayer Interactions in Transition Metal Dichalcogenide Heterostructures by Optical Spectroscopy: MoS ₂ /WS ₂ and MoSe ₂ /WSe ₂ Rigosi, Albert F.; Hill, Heather M.; Li, Yilei Nano Letters, Vol. 15, Issue 8 https://doi.org/10.1021/acs.nanolett.5b01055	journal	July 2015
Quantum Coherence Facilitates Efficient Charge Separation at a MoS ₂ /MoSe ₂ van der Waals Junction Long, Run; Prezhdo, Oleg V. Nano Letters, Vol. 16, Issue 3 https://doi.org/10.1021/acs.nanolett.5b05264	journal	February 2016
Evidence for Fast Interlayer Energy Transfer in MoSe ₂ /WS ₂ Heterostructures Kozawa, Daichi; Carvalho, Alexandra; Verzhbitskiy, Ivan Nano Letters, Vol. 16, Issue 7 https://doi.org/10.1021/acs.nanolett.6b00801	journal	June 2016
Interfacial Charge Transfer Circumventing Momentum Mismatch at Two-Dimensional van der Waals Heterojunctions Zhu, Haiming; Wang, Jue; Gong, Zizhou Nano Letters, Vol. 17, Issue 6 https://doi.org/10.1021/acs.nanolett.7b00748	journal	May 2017
Phonon-Assisted Ultrafast Charge Transfer at van der Waals Heterostructure Interface Zheng, Qijing; Saidi, Wissam A.; Xie, Yu Nano Letters, Vol. 17, Issue 10 https://doi.org/10.1021/acs.nanolett.7b03429	journal	September 2017
Effect of Distance on Photoluminescence Quenching and Proximity-Induced Spin–Orbit Coupling in Graphene/WSe₂ Heterostructures Yang, Bowen; Molina, Everardo; Kim, Jeongwoo Nano Letters, Vol. 18, Issue 6 https://doi.org/10.1021/acs.nanolett.8b00691	journal	June 2018
Interlayer Coupling in Twisted WSe ₂ /WS ₂ Bilayer Heterostructures Revealed by Optical Spectroscopy Wang, Kai; Huang, Bing; Tian, Mengkun ACS Nano, Vol. 10, Issue 7 https://doi.org/10.1021/acsnano.6b01486	journal	June 2016
Robust Stacking-Independent Ultrafast Charge Transfer in MoS ₂ /WS ₂ Bilayers Ji, Ziheng; Hong, Hao; Zhang, Jin ACS Nano, Vol. 11, Issue 12 https://doi.org/10.1021/acsnano.7b04541	journal	October 2016
Ultrafast Energy Transfer of Both Bright and Dark Excitons in 2D van der Waals Heterostructures Beyond Dipolar Coupling Wu, Lingling; Chen, Yuzhong; Zhou, Hongzhi ACS Nano https://doi.org/10.1021/acsnano.8b09059	journal	February 2019
Charge Transfer Excitons at van der Waals Interfaces Zhu, Xiaoyang; Monahan, Nicholas R.; Gong, Zizhou Journal of the American Chemical Society, Vol. 137, Issue 26 https://doi.org/10.1021/jacs.5b03141	journal	June 2015
Transient Absorption Microscopy of Monolayer and Bulk WSe ₂ Cui, Qiannan; Ceballos, Frank; Kumar, Nardeep ACS Nano, Vol. 8, Issue 3 https://doi.org/10.1021/nn500277y	journal	February 2014
Ultrafast Charge Separation and Indirect Exciton Formation in a MoS ₂ –MoSe ₂ van der Waals Heterostructure Ceballos, Frank; Bellus, Matthew Z.; Chiu, Hsin-Ying ACS Nano, Vol. 8, Issue 12 https://doi.org/10.1021/nn505736z	journal	November 2014
The super materials that could trump graphene Gibney, Elizabeth Nature, Vol. 522, Issue 7556 https://doi.org/10.1038/522274a	journal	June 2015
Van der Waals heterostructures and devices Liu, Yuan; Weiss, Nathan O.; Duan, Xidong Nature Reviews Materials, Vol. 1, Issue 9 https://doi.org/10.1038/natrevmats.2016.42	journal	July 2016
Van der Waals heterostructures Geim, A. K.; Grigorieva, I. V. Nature, Vol. 499, Issue 7459, p. 419-425 https://doi.org/10.1038/nature12385	journal	July 2013
The role of collective motion in the ultrafast charge transfer in van der Waals heterostructures Wang, Han; Bang, Junhyeok; Sun, Yiyang Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms11504	journal	May 2016
Directional interlayer spin-valley transfer in two-dimensional heterostructures Schaibley, John R.; Rivera, Pasqual; Yu, Hongyi Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13747	journal	December 2016
Coulomb engineering of the bandgap and excitons in two-dimensional materials Raja, Archana; Chaves, Andrey; Yu, Jaeeun Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms15251	journal	May 2017
Electronics and optoelectronics of two-dimensional transition metal dichalcogenides Wang, Qing Hua; Kalantar-Zadeh, Kourosh; Kis, Andras Nature Nanotechnology, Vol. 7, Issue 11, p. 699-712 https://doi.org/10.1038/nnano.2012.193	journal	November 2012
Ultrafast charge transfer in atomically thin MoS2/WS2 heterostructures Hong, Xiaoping; Kim, Jonghwan; Shi, Su-Fei Nature Nanotechnology, Vol. 9, Issue 9 https://doi.org/10.1038/nnano.2014.167	journal	August 2014
Ultrafast probes of electron–hole transitions between two atomic layers Wen, Xiewen; Chen, Hailong; Wu, Tianmin Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-04291-9	journal	May 2018
Exchange-correlation functionals for band gaps of solids: benchmark, reparametrization and machine learning Borlido, Pedro; Schmidt, Jonathan; Huran, Ahmad W. npj Computational Materials, Vol. 6, Issue 1 https://doi.org/10.1038/s41524-020-00360-0	journal	July 2020
Momentum-space indirect interlayer excitons in transition-metal dichalcogenide van der Waals heterostructures Kunstmann, Jens; Mooshammer, Fabian; Nagler, Philipp Nature Physics, Vol. 14, Issue 8 https://doi.org/10.1038/s41567-018-0123-y	journal	April 2018
Evidence for moiré excitons in van der Waals heterostructures Tran, Kha; Moody, Galan; Wu, Fengcheng Nature, Vol. 567, Issue 7746 https://doi.org/10.1038/s41586-019-0975-z	journal	February 2019
Observation of moiré excitons in WSe2/WS2 heterostructure superlattices Jin, Chenhao; Regan, Emma C.; Yan, Aiming Nature, Vol. 567, Issue 7746 https://doi.org/10.1038/s41586-019-0976-y	journal	February 2019
Resonantly hybridized excitons in moiré superlattices in van der Waals heterostructures Alexeev, Evgeny M.; Ruiz-Tijerina, David A.; Danovich, Mark Nature, Vol. 567, Issue 7746 https://doi.org/10.1038/s41586-019-0986-9	journal	March 2019
Optical signature of symmetry variations and spin-valley coupling in atomically thin tungsten dichalcogenides Zeng, Hualing; Liu, Gui-Bin; Dai, Junfeng Scientific Reports, Vol. 3, Issue 1 https://doi.org/10.1038/srep01608	journal	April 2013
Probing charge transfer excitons in a MoSe ₂ –WS ₂ van der Waals heterostructure Ceballos, Frank; Bellus, Matthew Z.; Chiu, Hsin-Ying Nanoscale, Vol. 7, Issue 41 https://doi.org/10.1039/C5NR04723D	journal	January 2015
Exciton formation in monolayer transition metal dichalcogenides Ceballos, Frank; Cui, Qiannan; Bellus, Matthew Z. Nanoscale, Vol. 8, Issue 22 https://doi.org/10.1039/C6NR02516A	journal	January 2016
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 Journal of Materials Chemistry A, Vol. 10, Issue 15 https://doi.org/10.1039/D1TA10788G	journal	January 2022
Hybrid functionals based on a screened Coulomb potential Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias The Journal of Chemical Physics, Vol. 118, Issue 18 https://doi.org/10.1063/1.1564060	journal	May 2003
Erratum: “Hybrid functionals based on a screened Coulomb potential” [J. Chem. Phys. 118, 8207 (2003)] Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias The Journal of Chemical Physics, Vol. 124, Issue 21 https://doi.org/10.1063/1.2204597	journal	June 2006
Charge carrier dynamics in bulk MoS ₂ crystal studied by transient absorption microscopy Kumar, Nardeep; He, Jiaqi; He, Dawei Journal of Applied Physics, Vol. 113, Issue 13 https://doi.org/10.1063/1.4799110	journal	April 2013
Intervalley scattering in MoS ₂ imaged by two-photon photoemission with a high-harmonic probe Wallauer, R.; Reimann, J.; Armbrust, N. Applied Physics Letters, Vol. 109, Issue 16 https://doi.org/10.1063/1.4965839	journal	October 2016
Nonlinear optical effect of interlayer charge transfer in a van der Waals heterostructure Yao, Peng; He, Dawei; Zereshki, Peymon Applied Physics Letters, Vol. 115, Issue 26 https://doi.org/10.1063/1.5131165	journal	December 2019
New directions in science and technology: two-dimensional crystals Neto, A. H. Castro; Novoselov, K. Reports on Progress in Physics, Vol. 74, Issue 8 https://doi.org/10.1088/0034-4885/74/8/082501	journal	July 2011
First-principles study of van der Waals interactions in MoS ₂ and MoO ₃ Peelaers, H.; Van de Walle, C. G. Journal of Physics: Condensed Matter, Vol. 26, Issue 30 https://doi.org/10.1088/0953-8984/26/30/305502	journal	July 2014
Ultrafast charge transfer in MoS ₂ /WSe ₂ p–n Heterojunction Peng, Bo; Yu, Guannan; Liu, Xinfeng 2D Materials, Vol. 3, Issue 2 https://doi.org/10.1088/2053-1583/3/2/025020	journal	May 2016
2D materials advances: from large scale synthesis and controlled heterostructures to improved characterization techniques, defects and applications Lin, Zhong; McCreary, Amber; Briggs, Natalie 2D Materials, Vol. 3, Issue 4 https://doi.org/10.1088/2053-1583/3/4/042001	journal	December 2016
Direct determination of momentum-resolved electron transfer in the photoexcited van der Waals heterobilayer W S 2 / Mo S 2 Liu, Fang; Li, Qiuyang; Zhu, X. -Y. Physical Review B, Vol. 101, Issue 20 https://doi.org/10.1103/PhysRevB.101.201405	journal	May 2020
Transient absorption of transition metal dichalcogenide monolayers studied by a photodope-pump-probe technique Valencia-Acuna, Pavel; Zereshki, Peymon; Tavakoli, Mohammad Mahdi Physical Review B, Vol. 102, Issue 3 https://doi.org/10.1103/PhysRevB.102.035414	journal	July 2020
Thickness dependence of work function, ionization energy, and electron affinity of Mo and W dichalcogenides from DFT and GW calculations Kim, Han-gyu; Choi, Hyoung Joon Physical Review B, Vol. 103, Issue 8 https://doi.org/10.1103/PhysRevB.103.085404	journal	February 2021
All-optical control of charge transfer and interlayer excitons in transition metal dichalcogenide heterostructures Zereshki, Peymon; Valencia-Acuna, Pavel; Zhao, Hui Physical Review B, Vol. 103, Issue 16 https://doi.org/10.1103/PhysRevB.103.165416	journal	April 2021
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
Phonon-limited mobility in n -type single-layer MoS 2 from first principles Kaasbjerg, Kristen; Thygesen, Kristian S.; Jacobsen, Karsten W. Physical Review B, Vol. 85, Issue 11 https://doi.org/10.1103/PhysRevB.85.115317	journal	March 2012
Ultrafast and spatially resolved studies of charge carriers in atomically thin molybdenum disulfide Wang, Rui; Ruzicka, Brian A.; Kumar, Nardeep Physical Review B, Vol. 86, Issue 4 https://doi.org/10.1103/PhysRevB.86.045406	journal	July 2012
Nature and evolution of the band-edge states in MoS 2 : From monolayer to bulk Padilha, J. E.; Peelaers, H.; Janotti, A. Physical Review B, Vol. 90, Issue 20 https://doi.org/10.1103/PhysRevB.90.205420	journal	November 2014
Measurement of the optical dielectric function of monolayer transition-metal dichalcogenides: MoS 2 , Mo S e 2 , WS 2 , and WS e 2 Li, Yilei; Chernikov, Alexey; Zhang, Xian Physical Review B, Vol. 90, Issue 20 https://doi.org/10.1103/PhysRevB.90.205422	journal	November 2014
Interlayer coupling in commensurate and incommensurate bilayer structures of transition-metal dichalcogenides Wang, Yong; Wang, Zhan; Yao, Wang Physical Review B, Vol. 95, Issue 11 https://doi.org/10.1103/PhysRevB.95.115429	journal	March 2017
Tightly Bound Excitons in Monolayer WSe 2 He, Keliang; Kumar, Nardeep; Zhao, Liang Physical Review Letters, Vol. 113, Issue 2 https://doi.org/10.1103/PhysRevLett.113.026803	journal	July 2014
Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS 2 Chernikov, Alexey; Berkelbach, Timothy C.; Hill, Heather M. Physical Review Letters, Vol. 113, Issue 7 https://doi.org/10.1103/PhysRevLett.113.076802	journal	August 2014
Infrared Interlayer Exciton Emission in MoS 2 / WSe 2 Heterostructures Karni, Ouri; Barré, Elyse; Lau, Sze Cheung Physical Review Letters, Vol. 123, Issue 24 https://doi.org/10.1103/PhysRevLett.123.247402	journal	December 2019
Separating electrons and holes by monolayer increments in van der Waals heterostructures Ceballos, Frank; Zereshki, Peymon; Zhao, Hui Physical Review Materials, Vol. 1, Issue 4 https://doi.org/10.1103/PhysRevMaterials.1.044001	journal	September 2017
Determination of band offsets, hybridization, and exciton binding in 2D semiconductor heterostructures Wilson, Neil R.; Nguyen, Paul V.; Seyler, Kyle Science Advances, Vol. 3, Issue 2 https://doi.org/10.1126/sciadv.1601832	journal	February 2017
Photocarrier generation from interlayer charge-transfer transitions in WS ₂ -graphene heterostructures Yuan, Long; Chung, Ting-Fung; Kuc, Agnieszka Science Advances, Vol. 4, Issue 2 https://doi.org/10.1126/sciadv.1700324	journal	February 2018
Recording interfacial currents on the subnanometer length and femtosecond time scale by terahertz emission Ma, Eric Yue; Guzelturk, Burak; Li, Guoqing Science Advances, Vol. 5, Issue 2 https://doi.org/10.1126/sciadv.aau0073	journal	February 2019
Electric Field Effect in Atomically Thin Carbon Films Novoselov, K. S. Science, Vol. 306, Issue 5696, p. 666-669 https://doi.org/10.1126/science.1102896	journal	October 2004
2D materials and van der Waals heterostructures Novoselov, K. S.; Mishchenko, A.; Carvalho, A. Science, Vol. 353, Issue 6298 https://doi.org/10.1126/science.aac9439	journal	July 2016

Figures / Tables (6)

Similar Records

Layer-engineered interlayer charge transfer in WSe₂/WS₂ heterostructures

Journal Article · Tue Mar 07 19:00:00 EST 2023 · Journal of Physics. D, Applied Physics · OSTI ID:2242507

Charge transfer in transition metal dichalcogenide alloy heterostructures

Journal Article · Mon Feb 17 19:00:00 EST 2025 · Applied Physics Letters · OSTI ID:2551844

Related Subjects

77 NANOSCIENCE AND NANOTECHNOLOGY
Carrier dynamics
Carrier generation & recombination
Density functional theory
Femtosecond laser spectroscopy
Layered semiconductors
Photoexcitation
Photoluminescence
Pump-probe spectroscopy
Transition metal dichalcogenides

Energy-valley-dependent charge transfer in few-layer transition metal dichalcogenide heterostructures

Citation Formats

References (64)

Figures / Tables (6)

Similar Records

Related Subjects