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Title: Anisotropic attosecond charge carrier dynamics and layer decoupling in quasi-2D layered SnS 2

Strong quantum confinement effects lead to striking new physics in two-dimensional materials such as graphene or transition metal dichalcogenides. While spectroscopic fingerprints of such quantum confinement have been demonstrated widely, the consequences for carrier dynamics are at present less clear, particularly on ultrafast timescales. This is important for tailoring, probing, and understanding spin and electron dynamics in layered and two-dimensional materials even in cases where the desired bandgap engineering has been achieved. Here in this paper we show by means of core–hole clock spectroscopy that SnS 2 exhibits spindependent attosecond charge delocalization times (τ deloc) for carriers confined within a layer, τ deloc < 400 as, whereas interlayer charge delocalization is dynamically quenched in excess of a factor of 10, τ deloc > 2.7 fs. These layer decoupling dynamics are a direct consequence of strongly anisotropic screening established within attoseconds, and demonstrate that important two-dimensional characteristics are also present in bulk crystals of van der Waalslayered materials, at least on ultrafast timescales.
Authors:
 [1] ;  [1] ;  [2] ; ORCiD logo [3] ;  [4]
  1. Univ. of Arizona, Tucson, AZ (United States). Dept. of Chemistry and Biochemistry
  2. Army Research Lab., Adelphi, MD (United States). Sensors and Electron Devices Directorate
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  4. Univ. of Arizona, Tucson, AZ (United States). Dept. of Chemistry and Biochemistry; Univ. of Arizona, Tucson, AZ (United States). Dept. of Physics
Publication Date:
Grant/Contract Number:
AC02-76SF00515; CHE1213243; CHE1565497
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; Attosecond science; Electronic properties and materials; Two-dimensional materials
OSTI Identifier:
1410520
Alternate Identifier(s):
OSTI ID: 1418215

Eads, Calley N., Bandak, Dmytro, Neupane, Mahesh R., Nordlund, Dennis, and Monti, Oliver L. A.. Anisotropic attosecond charge carrier dynamics and layer decoupling in quasi-2D layered SnS2. United States: N. p., Web. doi:10.1038/s41467-017-01522-3.
Eads, Calley N., Bandak, Dmytro, Neupane, Mahesh R., Nordlund, Dennis, & Monti, Oliver L. A.. Anisotropic attosecond charge carrier dynamics and layer decoupling in quasi-2D layered SnS2. United States. doi:10.1038/s41467-017-01522-3.
Eads, Calley N., Bandak, Dmytro, Neupane, Mahesh R., Nordlund, Dennis, and Monti, Oliver L. A.. 2017. "Anisotropic attosecond charge carrier dynamics and layer decoupling in quasi-2D layered SnS2". United States. doi:10.1038/s41467-017-01522-3. https://www.osti.gov/servlets/purl/1410520.
@article{osti_1410520,
title = {Anisotropic attosecond charge carrier dynamics and layer decoupling in quasi-2D layered SnS2},
author = {Eads, Calley N. and Bandak, Dmytro and Neupane, Mahesh R. and Nordlund, Dennis and Monti, Oliver L. A.},
abstractNote = {Strong quantum confinement effects lead to striking new physics in two-dimensional materials such as graphene or transition metal dichalcogenides. While spectroscopic fingerprints of such quantum confinement have been demonstrated widely, the consequences for carrier dynamics are at present less clear, particularly on ultrafast timescales. This is important for tailoring, probing, and understanding spin and electron dynamics in layered and two-dimensional materials even in cases where the desired bandgap engineering has been achieved. Here in this paper we show by means of core–hole clock spectroscopy that SnS2 exhibits spindependent attosecond charge delocalization times (τdeloc) for carriers confined within a layer, τdeloc < 400 as, whereas interlayer charge delocalization is dynamically quenched in excess of a factor of 10, τdeloc > 2.7 fs. These layer decoupling dynamics are a direct consequence of strongly anisotropic screening established within attoseconds, and demonstrate that important two-dimensional characteristics are also present in bulk crystals of van der Waalslayered materials, at least on ultrafast timescales.},
doi = {10.1038/s41467-017-01522-3},
journal = {Nature Communications},
number = 1,
volume = 8,
place = {United States},
year = {2017},
month = {11}
}

Works referenced in this record:

Projector augmented-wave method
journal, December 1994

Special points for Brillouin-zone integrations
journal, June 1976
  • Monkhorst, Hendrik J.; Pack, James D.
  • Physical Review B, Vol. 13, Issue 12, p. 5188-5192
  • DOI: 10.1103/PhysRevB.13.5188

Extraordinary Sunlight Absorption and One Nanometer Thick Photovoltaics Using Two-Dimensional Monolayer Materials
journal, July 2013
  • Bernardi, Marco; Palummo, Maurizia; Grossman, Jeffrey C.
  • Nano Letters, Vol. 13, Issue 8, p. 3664-3670
  • DOI: 10.1021/nl401544y

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996