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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 WSe 2 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.
@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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