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Title: Recording interfacial currents on the subnanometer length and femtosecond time scale by terahertz emission

Abstract

Electron dynamics at interfaces is a subject of great scientific interest and technological importance. Detailed understanding of such dynamics requires access to the angstrom length scale defining interfaces and the femtosecond time scale characterizing interfacial motion of electrons. In this context, the most precise and general way to remotely measure charge dynamics is through the transient current flow and the associated electromagnetic radiation. Here, we present quantitative measurements of interfacial currents on the subnanometer length and femtosecond time scale by recording the emitted terahertz radiation following ultrafast laser excitation. We apply this method to interlayer charge transfer in heterostructures of two transition metal dichalcogenide monolayers less than 0.7 nm apart. We find that charge relaxation and separation occur in less than 100 fs. This approach allows us to unambiguously determine the direction of current flow, to demonstrate a charge transfer efficiency of order unity, and to characterize saturation effects.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [3]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
  3. North Carolina State Univ., Raleigh, NC (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Complex Materials from First Principles (CCM); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1507151
Alternate Identifier(s):
OSTI ID: 1483811
Grant/Contract Number:  
ECCS-1508856; AC02-76SF00515; SC0012575; GBMF4545
Resource Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 5; Journal Issue: 2; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Ma, Eric Yue, Guzelturk, Burak, Li, Guoqing, Cao, Linyou, Shen, Zhi -Xun, Lindenberg, Aaron M., and Heinz, Tony F. Recording interfacial currents on the subnanometer length and femtosecond time scale by terahertz emission. United States: N. p., 2019. Web. doi:10.1126/sciadv.aau0073.
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Ma, Eric Yue, Guzelturk, Burak, Li, Guoqing, Cao, Linyou, Shen, Zhi -Xun, Lindenberg, Aaron M., & Heinz, Tony F. Recording interfacial currents on the subnanometer length and femtosecond time scale by terahertz emission. United States. https://doi.org/10.1126/sciadv.aau0073
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Ma, Eric Yue, Guzelturk, Burak, Li, Guoqing, Cao, Linyou, Shen, Zhi -Xun, Lindenberg, Aaron M., and Heinz, Tony F. Fri . "Recording interfacial currents on the subnanometer length and femtosecond time scale by terahertz emission". United States. https://doi.org/10.1126/sciadv.aau0073. https://www.osti.gov/servlets/purl/1507151.
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@article{osti_1507151,
title = {Recording interfacial currents on the subnanometer length and femtosecond time scale by terahertz emission},
author = {Ma, Eric Yue and Guzelturk, Burak and Li, Guoqing and Cao, Linyou and Shen, Zhi -Xun and Lindenberg, Aaron M. and Heinz, Tony F.},
abstractNote = {Electron dynamics at interfaces is a subject of great scientific interest and technological importance. Detailed understanding of such dynamics requires access to the angstrom length scale defining interfaces and the femtosecond time scale characterizing interfacial motion of electrons. In this context, the most precise and general way to remotely measure charge dynamics is through the transient current flow and the associated electromagnetic radiation. Here, we present quantitative measurements of interfacial currents on the subnanometer length and femtosecond time scale by recording the emitted terahertz radiation following ultrafast laser excitation. We apply this method to interlayer charge transfer in heterostructures of two transition metal dichalcogenide monolayers less than 0.7 nm apart. We find that charge relaxation and separation occur in less than 100 fs. This approach allows us to unambiguously determine the direction of current flow, to demonstrate a charge transfer efficiency of order unity, and to characterize saturation effects.},
doi = {10.1126/sciadv.aau0073},
journal = {Science Advances},
number = 2,
volume = 5,
place = {United States},
year = {Fri Feb 08 00:00:00 EST 2019},
month = {Fri Feb 08 00:00:00 EST 2019}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1126/sciadv.aau0073
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Cited by: 36 works
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Figures / Tables:

Figure 1 Figure 1: Recording subnanometer interfacial currents by THz emission. (A) Schematic of the type II band alignment in a WS2/MoS2 heterostructure. Photogenerated electrons and holes separate into different layers, giving rise to a net current that flows from the MoS2 to WS2 monolayer. (B) An optically triggered interfacial current Jzmore » from the TMDC heterostructure emits a transient EM pulse at THz frequencies. (C) Emitted THz electric field waveforms from WS2/MoS2 and MoS2/WS2 heterostructures upon excitation with 3.1-eV femtosecond pulses as recorded using EO sampling. Inset: Calibration THz waveform from a bulk InSb crystal under identical conditions.« less
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    Infrared Interlayer Exciton Emission in MoS 2 / WSe 2 Heterostructures
    journal, December 2019

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