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Bidirectional phonon emission in two-dimensional heterostructures triggered by ultrafast charge transfer

Journal Article · · Nature Nanotechnology
 [1];  [2];  [3];  [4];  [1];  [5];  [6];  [6];  [5];  [4];  [6];  [7];  [7];  [2];  [6];  [4];  [1];  [1];  [5];  [3]
  1. SLAC National Accelerator Laboratory, Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES); Stanford University, CA (United States)
  2. University of California, Berkeley, CA (United States)
  3. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  4. University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  5. Stanford University, CA (United States)
  6. SLAC National Accelerator Laboratory, Menlo Park, CA (United States)
  7. National Institute for Materials Science, Tsukuba (Japan)
+ Show Author Affiliations

Photoinduced charge transfer in van der Waals heterostructures occurs on the 100 fs timescale despite weak interlayer coupling and momentum mismatch. However, little is understood about the microscopic mechanism behind this ultrafast process and the role of the lattice in mediating it. Here, using femtosecond electron diffraction, we directly visualize lattice dynamics in photoexcited heterostructures of WSe2/WS2 monolayers. Following the selective excitation of WSe2, we measure the concurrent heating of both WSe2 and WS2 on a picosecond timescale—an observation that is not explained by phonon transport across the interface. Using first-principles calculations, we identify a fast channel involving an electronic state hybridized across the heterostructure, enabling phonon-assisted interlayer transfer of photoexcited electrons. Phonons are emitted in both layers on the femtosecond timescale via this channel, consistent with the simultaneous lattice heating observed experimentally. Taken together, this shows our work indicates strong electron–phonon coupling via layer-hybridized electronic states—a novel route to control energy transport across atomic junctions.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Laboratory Directed Research and Development (LDRD) Program; Natural Science and Engineering Research Council (NSERC); Department of Defense (DoD); Japan Society for the Promotion of Science (JSPS)
Grant/Contract Number:
AC02-76SF00515; AC02-05CH11231
OSTI ID:
1972268
Journal Information:
Nature Nanotechnology, Journal Name: Nature Nanotechnology Journal Issue: 1 Vol. 18; ISSN 1748-3387
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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