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

Abstract

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:
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)
OSTI Identifier:
1410520
Alternate Identifier(s):
OSTI ID: 1418215
Grant/Contract Number:  
AC02-76SF00515; CHE1213243; CHE1565497
Resource 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
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

Citation Formats

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., 2017. 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. Wed . "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}
}

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Works referenced in this record:

Many-Body Effects in Valleytronics: Direct Measurement of Valley Lifetimes in Single-Layer MoS 2
journal, December 2013

  • Mai, Cong; Barrette, Andrew; Yu, Yifei
  • Nano Letters, Vol. 14, Issue 1
  • DOI: 10.1021/nl403742j

Vertical field-effect transistor based on graphene–WS2 heterostructures for flexible and transparent electronics
journal, December 2012

  • Georgiou, Thanasis; Jalil, Rashid; Belle, Branson D.
  • Nature Nanotechnology, Vol. 8, Issue 2
  • DOI: 10.1038/nnano.2012.224

Projector augmented-wave method
journal, December 1994


Negative electronic compressibility and tunable spin splitting in WSe2
journal, September 2015

  • Riley, J. M.; Meevasana, W.; Bawden, L.
  • Nature Nanotechnology, Vol. 10, Issue 12
  • DOI: 10.1038/nnano.2015.217

Hybrid functionals based on a screened Coulomb potential
journal, May 2003

  • Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias
  • The Journal of Chemical Physics, Vol. 118, Issue 18
  • DOI: 10.1063/1.1564060

Robust optical emission polarization in MoS 2 monolayers through selective valley excitation
journal, August 2012


MoS2 transistors with 1-nanometer gate lengths
journal, October 2016


Direct observation of the transition from indirect to direct bandgap in atomically thin epitaxial MoSe2
journal, December 2013


Valence and conduction band structure of the quasi-two-dimensional semiconductor Sn S 2
journal, February 2016


Ultrafast electron dynamics in two dimensional layered systems: two-photon photoemission studies of SnS2
journal, June 1997


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

Exciton diffusion in monolayer and bulk MoSe 2
journal, January 2014

  • Kumar, Nardeep; Cui, Qiannan; Ceballos, Frank
  • Nanoscale, Vol. 6, Issue 9
  • DOI: 10.1039/C3NR06863C

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

Spin-dependent trapping of electrons at spinterfaces
journal, February 2013

  • Steil, Sabine; Großmann, Nicolas; Laux, Martin
  • Nature Physics, Vol. 9, Issue 4
  • DOI: 10.1038/nphys2548

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


Quasi 2D electronic states with high spin-polarization in centrosymmetric MoS2 bulk crystals
journal, June 2016

  • Gehlmann, Mathias; Aguilera, Irene; Bihlmayer, Gustav
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep26197

Magnetoelectric effects and valley-controlled spin quantum gates in transition metal dichalcogenide bilayers
journal, June 2013

  • Gong, Zhirui; Liu, Gui-Bin; Yu, Hongyi
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms3053

Electron spectroscopic determinations of M and N core-hole lifetimes for the elements Nb—Te ( Z = 41 52 )
journal, December 1981


Ultrafast charge transfer in atomically thin MoS2/WS2 heterostructures
journal, August 2014

  • Hong, Xiaoping; Kim, Jonghwan; Shi, Su-Fei
  • Nature Nanotechnology, Vol. 9, Issue 9
  • DOI: 10.1038/nnano.2014.167

Charge-transfer dynamics studied using resonant core spectroscopies
journal, July 2002


Electric control of the spin Hall effect by intervalley transitions
journal, August 2014

  • Okamoto, N.; Kurebayashi, H.; Trypiniotis, T.
  • Nature Materials, Vol. 13, Issue 10
  • DOI: 10.1038/nmat4059

Direct observation of electron dynamics in the attosecond domain
journal, July 2005

  • Föhlisch, A.; Feulner, P.; Hennies, F.
  • Nature, Vol. 436, Issue 7049
  • DOI: 10.1038/nature03833

Atomic level widths for x-ray spectrometry
journal, November 1995


Atomic M -Shell Coster-Kronig, Auger, and Radiative Rates, and Fluorescence Yields for Ca-Th
journal, March 1972


Evolution of the Valley Position in Bulk Transition-Metal Chalcogenides and Their Monolayer Limit
journal, July 2016


Direct Measurement of the Tunable Electronic Structure of Bilayer MoS 2 by Interlayer Twist
journal, January 2016


The importance of gap states for energy level alignment at hybrid interfaces
journal, October 2015

  • Racke, D. A.; Kelly, L. L.; Monti, O. L. A.
  • Journal of Electron Spectroscopy and Related Phenomena, Vol. 204
  • DOI: 10.1016/j.elspec.2015.04.003

Growth and Characterization of Tin Disulfide Single Crystals
journal, June 2006

  • Sharp, Laura; Soltz, David; Parkinson, B. A.
  • Crystal Growth & Design, Vol. 6, Issue 6
  • DOI: 10.1021/cg050335y

Intervalley scattering in MoS 2 imaged by two-photon photoemission with a high-harmonic probe
journal, October 2016

  • Wallauer, R.; Reimann, J.; Armbrust, N.
  • Applied Physics Letters, Vol. 109, Issue 16
  • DOI: 10.1063/1.4965839

Ultrafast charge transfer at surfaces accessed by core electron spectroscopies
journal, January 2008

  • Menzel, Dietrich
  • Chemical Society Reviews, Vol. 37, Issue 10
  • DOI: 10.1039/b719546j

Direct observation of spin-polarized bulk bands in an inversion-symmetric semiconductor
journal, October 2014

  • Riley, J. M.; Mazzola, F.; Dendzik, M.
  • Nature Physics, Vol. 10, Issue 11
  • DOI: 10.1038/nphys3105

Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS 2
journal, August 2014


A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu
journal, April 2010

  • Grimme, Stefan; Antony, Jens; Ehrlich, Stephan
  • The Journal of Chemical Physics, Vol. 132, Issue 15
  • DOI: 10.1063/1.3382344

Generation and Evolution of Spin-, Valley-, and Layer-Polarized Excited Carriers in Inversion-Symmetric WSe 2
journal, December 2016


Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor
journal, August 2014

  • Ugeda, Miguel M.; Bradley, Aaron J.; Shi, Su-Fei
  • Nature Materials, Vol. 13, Issue 12
  • DOI: 10.1038/nmat4061

Monolayer behaviour in bulk ReS2 due to electronic and vibrational decoupling
journal, February 2014

  • Tongay, Sefaattin; Sahin, Hasan; Ko, Changhyun
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4252

The Effective Fine-Structure Constant of Freestanding Graphene Measured in Graphite
journal, November 2010


Tin Disulfide—An Emerging Layered Metal Dichalcogenide Semiconductor: Materials Properties and Device Characteristics
journal, September 2014

  • Huang, Yuan; Sutter, Eli; Sadowski, Jerzy T.
  • ACS Nano, Vol. 8, Issue 10
  • DOI: 10.1021/nn504481r

Observation of long-lived interlayer excitons in monolayer MoSe2–WSe2 heterostructures
journal, February 2015

  • Rivera, Pasqual; Schaibley, John R.; Jones, Aaron M.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms7242