4.8 Article

Charge Transfer Dynamics in MoSe2/hBN/WSe2 Heterostructures

Journal

NANO LETTERS
Volume 22, Issue 24, Pages 10140-10146

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.2c04030

Keywords

Ultrafast dynamics; transient absorption spectroscopy; interlayer charge transfer; exciton-exciton annihilation; van der Waals heterostructures

Funding

  1. Center for Computational Study of Excited-State Phenomena in Energy Materials (C2SEPEM) at LBNL - U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division [DE-AC02-05CH11231]
  2. U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division within the van der Waals heterostructure program [DE-AC0205CH11231, KCWF16]
  3. NSF [CMMI 1825594, DMR-1955889, CMMI-1933214, 1904716, 1935994, ECCS 2052527, DMR 2111812, CMMI 2129412]
  4. JSPS KAKENHI [19H05790, 20H00354]
  5. [DOE-SC0020653]
  6. Direct For Biological Sciences
  7. Div Of Biological Infrastructure [1935994] Funding Source: National Science Foundation

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Ultrafast charge transfer processes provide a simple way to create interlayer excitons in directly contacted transition metal dichalcogenide (TMD) layers. More sophisticated TMD/hBN/TMD heterostructures enable control over interlayer exciton properties and the emergence of novel exciton phenomena. The study investigates the charge transfer dynamics in a heterostructure composed of MoSe2 and WSe2 monolayers with a 1 nm thick hBN spacer, observing slower hole transfer compared to TMD layers without a spacer, as well as strong competition between interlayer charge transfer and intralayer exciton-exciton annihilation processes at high excitation densities.
Ultrafast charge transfer processes provide a facile way to create interlayer excitons in directly contacted transition metal dichalcogenide (TMD) layers. More sophisticated heterostructures composed of TMD/hBN/TMD enable new ways to control interlayer exciton properties and achieve novel exciton phenomena, such as exciton insulators and condensates, where longer lifetimes are desired. In this work, we experimentally study the charge transfer dynamics in a heterostructure composed of a 1 nm thick hBN spacer between MoSe2 and WSe2 monolayers. We observe the hole transfer from MoSe2 to WSe2 through the hBN barrier with a time constant of 500 ps, which is over 3 orders of magnitude slower than that between TMD layers without a spacer. Furthermore, we observe strong competition between the interlayer charge transfer and intralayer exciton-exciton annihilation processes at high excitation densities. Our work opens possibilities to understand charge transfer pathways in TMD/hBN/TMD heterostructures for the efficient generation and control of interlayer excitons.

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