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Title: Anisotropic structural dynamics of monolayer crystals revealed by femtosecond surface X-ray scattering

Abstract

Ultrafast X-ray scattering is one of the primary tools to track intrinsic crystallographic evolution with atomic accuracy in real time. However, its application to study nonequilibrium structural properties at the two-dimensional limit remains a long-standing challenge due to a significant reduction of diffraction volume and complexity of data analysis. Here, we report femtosecond surface X-ray diffraction in combination with crystallographic model-refinement calculations to quantify the ultrafast structural dynamics of monolayer WSe2 crystals supported on a substrate. We found the absorbed optical photon energy is preferably coupled to the in-plane lattice vibrations within one picosecond whereas the out-of-plane lattice vibration amplitude remains unchanged during the first ten picoseconds. The model-assisted fitting suggests an asymmetric intralayer spacing change upon excitation. The observed nonequilibrium anisotropic structural dynamics agrees with first-principles modelling in both real and momentum space, marking the distinct structural dynamics of monolayer crystals from their bulk counterparts.

Authors:
 [1]; ORCiD logo [2];  [1];  [1];  [1]; ORCiD logo [3];  [3];  [4];  [4];  [5];  [6];  [6];  [6]; ORCiD logo [6];  [6];  [7];  [7];  [2];  [2];  [1] more »;  [8]; ORCiD logo [2]; ORCiD logo [3];  [8]; ORCiD logo [1] « less
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Univ. of Southern California, Los Angeles, CA (United States)
  3. Univ. of Washington, Seattle, WA (United States)
  4. Stanford Univ., CA (United States)
  5. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  7. Kumamoto Univ., Kumamoto (Japan)
  8. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1532479
Alternate Identifier(s):
OSTI ID: 1532754
Grant/Contract Number:  
AC02-76SF00515; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nature Photonics
Additional Journal Information:
Journal Volume: 13; Journal Issue: 6; Journal ID: ISSN 1749-4885
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Tung, I-Cheng, Krishnamoorthy, Aravind, Sadasivam, Sridhar, Zhou, Hua, Zhang, Qi, Seyler, Kyle L., Clark, Genevieve, Mannebach, Ehren M., Nyby, Clara, Ernst, Friederike, Zhu, Diling, Glownia, James M., Kozina, Michael E., Song, Sanghoon, Nelson, Silke, Kumazoe, Hiroyuki, Shimojo, Fuyuki, Kalia, Rajiv K., Vashishta, Priya, Darancet, Pierre, Heinz, Tony F., Nakano, Aiichiro, Xu, Xiaodong, Lindenberg, Aaron M., and Wen, Haidan. Anisotropic structural dynamics of monolayer crystals revealed by femtosecond surface X-ray scattering. United States: N. p., 2019. Web. doi:10.1038/s41566-019-0387-5.
Tung, I-Cheng, Krishnamoorthy, Aravind, Sadasivam, Sridhar, Zhou, Hua, Zhang, Qi, Seyler, Kyle L., Clark, Genevieve, Mannebach, Ehren M., Nyby, Clara, Ernst, Friederike, Zhu, Diling, Glownia, James M., Kozina, Michael E., Song, Sanghoon, Nelson, Silke, Kumazoe, Hiroyuki, Shimojo, Fuyuki, Kalia, Rajiv K., Vashishta, Priya, Darancet, Pierre, Heinz, Tony F., Nakano, Aiichiro, Xu, Xiaodong, Lindenberg, Aaron M., & Wen, Haidan. Anisotropic structural dynamics of monolayer crystals revealed by femtosecond surface X-ray scattering. United States. doi:10.1038/s41566-019-0387-5.
Tung, I-Cheng, Krishnamoorthy, Aravind, Sadasivam, Sridhar, Zhou, Hua, Zhang, Qi, Seyler, Kyle L., Clark, Genevieve, Mannebach, Ehren M., Nyby, Clara, Ernst, Friederike, Zhu, Diling, Glownia, James M., Kozina, Michael E., Song, Sanghoon, Nelson, Silke, Kumazoe, Hiroyuki, Shimojo, Fuyuki, Kalia, Rajiv K., Vashishta, Priya, Darancet, Pierre, Heinz, Tony F., Nakano, Aiichiro, Xu, Xiaodong, Lindenberg, Aaron M., and Wen, Haidan. Mon . "Anisotropic structural dynamics of monolayer crystals revealed by femtosecond surface X-ray scattering". United States. doi:10.1038/s41566-019-0387-5. https://www.osti.gov/servlets/purl/1532479.
@article{osti_1532479,
title = {Anisotropic structural dynamics of monolayer crystals revealed by femtosecond surface X-ray scattering},
author = {Tung, I-Cheng and Krishnamoorthy, Aravind and Sadasivam, Sridhar and Zhou, Hua and Zhang, Qi and Seyler, Kyle L. and Clark, Genevieve and Mannebach, Ehren M. and Nyby, Clara and Ernst, Friederike and Zhu, Diling and Glownia, James M. and Kozina, Michael E. and Song, Sanghoon and Nelson, Silke and Kumazoe, Hiroyuki and Shimojo, Fuyuki and Kalia, Rajiv K. and Vashishta, Priya and Darancet, Pierre and Heinz, Tony F. and Nakano, Aiichiro and Xu, Xiaodong and Lindenberg, Aaron M. and Wen, Haidan},
abstractNote = {Ultrafast X-ray scattering is one of the primary tools to track intrinsic crystallographic evolution with atomic accuracy in real time. However, its application to study nonequilibrium structural properties at the two-dimensional limit remains a long-standing challenge due to a significant reduction of diffraction volume and complexity of data analysis. Here, we report femtosecond surface X-ray diffraction in combination with crystallographic model-refinement calculations to quantify the ultrafast structural dynamics of monolayer WSe2 crystals supported on a substrate. We found the absorbed optical photon energy is preferably coupled to the in-plane lattice vibrations within one picosecond whereas the out-of-plane lattice vibration amplitude remains unchanged during the first ten picoseconds. The model-assisted fitting suggests an asymmetric intralayer spacing change upon excitation. The observed nonequilibrium anisotropic structural dynamics agrees with first-principles modelling in both real and momentum space, marking the distinct structural dynamics of monolayer crystals from their bulk counterparts.},
doi = {10.1038/s41566-019-0387-5},
journal = {Nature Photonics},
number = 6,
volume = 13,
place = {United States},
year = {2019},
month = {3}
}

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Works referenced in this record:

2D materials and van der Waals heterostructures
journal, July 2016


Two-dimensional van der Waals materials
journal, September 2016

  • Ajayan, Pulickel; Kim, Philip; Banerjee, Kaustav
  • Physics Today, Vol. 69, Issue 9
  • DOI: 10.1063/PT.3.3297

Population inversion and giant bandgap renormalization in atomically thin WS2 layers
journal, June 2015


Lightwave-driven quasiparticle collisions on a subcycle timescale
journal, May 2016

  • Langer, F.; Hohenleutner, M.; Schmid, C. P.
  • Nature, Vol. 533, Issue 7602
  • DOI: 10.1038/nature17958

Valley-polarized exciton dynamics in a 2D semiconductor heterostructure
journal, February 2016


Substrate induced changes in atomically thin 2-dimensional semiconductors: Fundamentals, engineering, and applications
journal, March 2017

  • Sun, Yinghui; Wang, Rongming; Liu, Kai
  • Applied Physics Reviews, Vol. 4, Issue 1
  • DOI: 10.1063/1.4974072

Two-dimensional phonon transport in graphene
journal, May 2012


Optically excited structural transition in atomic wires on surfaces at the quantum limit
journal, March 2017


Superior Thermal Conductivity of Single-Layer Graphene
journal, March 2008

  • Balandin, Alexander A.; Ghosh, Suchismita; Bao, Wenzhong
  • Nano Letters, Vol. 8, Issue 3, p. 902-907
  • DOI: 10.1021/nl0731872

Dimensional crossover of thermal transport in few-layer graphene
journal, May 2010

  • Ghosh, Suchismita; Bao, Wenzhong; Nika, Denis L.
  • Nature Materials, Vol. 9, Issue 7
  • DOI: 10.1038/nmat2753

Interfacial mode coupling as the origin of the enhancement of Tc in FeSe films on SrTiO3
journal, November 2014

  • Lee, J. J.; Schmitt, F. T.; Moore, R. G.
  • Nature, Vol. 515, Issue 7526
  • DOI: 10.1038/nature13894

Unusual Exciton–Phonon Interactions at van der Waals Engineered Interfaces
journal, January 2017


Interlayer electron–phonon coupling in WSe2/hBN heterostructures
journal, October 2016

  • Jin, Chenhao; Kim, Jonghwan; Suh, Joonki
  • Nature Physics, Vol. 13, Issue 2
  • DOI: 10.1038/nphys3928

Femtosecond electron-phonon lock-in by photoemission and x-ray free-electron laser
journal, July 2017


Direct Observation of Optically Induced Transient Structures in Graphite Using Ultrafast Electron Crystallography
journal, August 2008


Ultrafast non-radiative dynamics of atomically thin MoSe2
journal, November 2017


Momentum-Resolved View of Electron-Phonon Coupling in Multilayer WSe 2
journal, July 2017


Femtosecond electron imaging of defect-modulated phonon dynamics
journal, April 2016

  • Cremons, Daniel R.; Plemmons, Dayne A.; Flannigan, David J.
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms11230

Defect-mediated phonon dynamics in TaS 2 and WSe 2
journal, July 2017

  • Cremons, Daniel R.; Plemmons, Dayne A.; Flannigan, David J.
  • Structural Dynamics, Vol. 4, Issue 4
  • DOI: 10.1063/1.4982817

Ultrafast electron crystallography: Transient structures of molecules, surfaces, and phase transitions
journal, January 2004

  • Ruan, C. -Y.; Vigliotti, F.; Lobastov, V. A.
  • Proceedings of the National Academy of Sciences, Vol. 101, Issue 5
  • DOI: 10.1073/pnas.0307302101

Ultrafast Electron Crystallography of Interfacial Water
journal, April 2004


Dynamic Structural Response and Deformations of Monolayer MoS 2 Visualized by Femtosecond Electron Diffraction
journal, September 2015


Rippling ultrafast dynamics of suspended 2D monolayers, graphene
journal, October 2016

  • Hu, Jianbo; Vanacore, Giovanni M.; Cepellotti, Andrea
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 43
  • DOI: 10.1073/pnas.1613818113

Dynamic Optical Tuning of Interlayer Interactions in the Transition Metal Dichalcogenides
journal, November 2017


Phase-Sensitive Sum-Frequency Spectroscopy
journal, April 2013


Excitonic luminescence upconversion in a two-dimensional semiconductor
journal, December 2015

  • Jones, Aaron M.; Yu, Hongyi; Schaibley, John R.
  • Nature Physics, Vol. 12, Issue 4
  • DOI: 10.1038/nphys3604

Exciton-phonon coupling and band-gap renormalization in monolayer WSe 2
journal, July 2018


Resonant internal quantum transitions and femtosecond radiative decay of excitons in monolayer WSe2
journal, July 2015

  • Poellmann, C.; Steinleitner, P.; Leierseder, U.
  • Nature Materials, Vol. 14, Issue 9
  • DOI: 10.1038/nmat4356

Observation of chiral phonons
journal, February 2018


Surface X-ray diffraction
journal, May 1992


Ripples and Layers in Ultrathin MoS 2 Membranes
journal, December 2011

  • Brivio, Jacopo; Alexander, Duncan T. L.; Kis, Andras
  • Nano Letters, Vol. 11, Issue 12
  • DOI: 10.1021/nl2022288

The structure of suspended graphene sheets
journal, March 2007

  • Meyer, Jannik C.; Geim, A. K.; Katsnelson, M. I.
  • Nature, Vol. 446, Issue 7131, p. 60-63
  • DOI: 10.1038/nature05545

Large nonadiabatic quantum molecular dynamics simulations on parallel computers
journal, January 2013

  • Shimojo, Fuyuki; Ohmura, Satoshi; Mou, Weiwei
  • Computer Physics Communications, Vol. 184, Issue 1
  • DOI: 10.1016/j.cpc.2012.08.001

Theory of Thermal Relaxation of Electrons in Semiconductors
journal, September 2017


Vapor-transport growth of high optical quality WSe 2 monolayers
journal, October 2014

  • Clark, Genevieve; Wu, Sanfeng; Rivera, Pasqual
  • APL Materials, Vol. 2, Issue 10
  • DOI: 10.1063/1.4896591

Oxide surfaces and metal/oxide interfaces studied by grazing incidence X-ray scattering
journal, January 1998


Precise Structure of Pentacene Monolayers on Amorphous Silicon Oxide and Relation to Charge Transport
journal, June 2009

  • Mannsfeld, Stefan C. B.; Virkar, Ajay; Reese, Colin
  • Advanced Materials, Vol. 21, Issue 22
  • DOI: 10.1002/adma.200803328

Measurement of the optical dielectric function of monolayer transition-metal dichalcogenides: MoS 2 , Mo S e 2 , WS 2 , and WS e 2
journal, November 2014


A divide-conquer-recombine algorithmic paradigm for large spatiotemporal quantum molecular dynamics simulations
journal, May 2014

  • Shimojo, Fuyuki; Hattori, Shinnosuke; Kalia, Rajiv K.
  • The Journal of Chemical Physics, Vol. 140, Issue 18
  • DOI: 10.1063/1.4869342

Inhomogeneous Electron Gas
journal, November 1964


Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965


Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Projector augmented-wave method
journal, December 1994


Semiempirical GGA-type density functional constructed with a long-range dispersion correction
journal, January 2006

  • Grimme, Stefan
  • Journal of Computational Chemistry, Vol. 27, Issue 15, p. 1787-1799
  • DOI: 10.1002/jcc.20495