DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Atomic-scale diffractive imaging of sub-cycle electron dynamics in condensed matter

Abstract

For interaction of light with condensed-matter systems, we show with simulations that ultrafast electron and X-ray diffraction can provide a time-dependent record of charge-density maps with sub-cycle and atomic-scale resolutions. Using graphene as an example material, we predict that diffraction can reveal localised atomic-scale origins of optical and electronic phenomena. Here, we point out nontrivial relations between microscopic electric current and density in undoped graphene.

Authors:
 [1];  [2];  [3];  [3]
  1. Georgia State Univ., Atlanta, GA (United States); Max-Planck-Institut fur Quantenoptik, Garching (Germany)
  2. Georgia State Univ. Atlanta, GA (United States)
  3. Max-Planck-Institut fur Quantenoptik, Garching (Germany); Ludwig-Maximilians-Univ. Munchen, Garching (Germany)
Publication Date:
Research Org.:
Georgia State Univ., Atlanta, GA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1324962
Grant/Contract Number:  
FG02-01ER15213; FG02-11ER46789
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 5; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; optical properties and devices; ultrafast photonics

Citation Formats

Yakovlev, Vladislav S., Stockman, Mark I., Krausz, Ferenc, and Baum, Peter. Atomic-scale diffractive imaging of sub-cycle electron dynamics in condensed matter. United States: N. p., 2015. Web. doi:10.1038/srep14581.
Yakovlev, Vladislav S., Stockman, Mark I., Krausz, Ferenc, & Baum, Peter. Atomic-scale diffractive imaging of sub-cycle electron dynamics in condensed matter. United States. https://doi.org/10.1038/srep14581
Yakovlev, Vladislav S., Stockman, Mark I., Krausz, Ferenc, and Baum, Peter. Mon . "Atomic-scale diffractive imaging of sub-cycle electron dynamics in condensed matter". United States. https://doi.org/10.1038/srep14581. https://www.osti.gov/servlets/purl/1324962.
@article{osti_1324962,
title = {Atomic-scale diffractive imaging of sub-cycle electron dynamics in condensed matter},
author = {Yakovlev, Vladislav S. and Stockman, Mark I. and Krausz, Ferenc and Baum, Peter},
abstractNote = {For interaction of light with condensed-matter systems, we show with simulations that ultrafast electron and X-ray diffraction can provide a time-dependent record of charge-density maps with sub-cycle and atomic-scale resolutions. Using graphene as an example material, we predict that diffraction can reveal localised atomic-scale origins of optical and electronic phenomena. Here, we point out nontrivial relations between microscopic electric current and density in undoped graphene.},
doi = {10.1038/srep14581},
journal = {Scientific Reports},
number = ,
volume = 5,
place = {United States},
year = {Mon Sep 28 00:00:00 EDT 2015},
month = {Mon Sep 28 00:00:00 EDT 2015}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 34 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Third-generation femtosecond technology
journal, January 2014


Quantum nonlinear optics — photon by photon
journal, August 2014

  • Chang, Darrick E.; Vuletić, Vladan; Lukin, Mikhail D.
  • Nature Photonics, Vol. 8, Issue 9
  • DOI: 10.1038/nphoton.2014.192

Attractive photons in a quantum nonlinear medium
journal, September 2013

  • Firstenberg, Ofer; Peyronel, Thibault; Liang, Qi-Yu
  • Nature, Vol. 502, Issue 7469
  • DOI: 10.1038/nature12512

Ultrafast electron dynamics in phenylalanine initiated by attosecond pulses
journal, October 2014


Microscopy and its focal switch
journal, December 2008


Seeing a single molecule vibrate through time-resolved coherent anti-Stokes Raman scattering
journal, July 2014

  • Yampolsky, Steven; Fishman, Dmitry A.; Dey, Shirshendu
  • Nature Photonics, Vol. 8, Issue 8
  • DOI: 10.1038/nphoton.2014.143

Broadband high-resolution X-ray frequency combs
journal, June 2014

  • Cavaletto, Stefano M.; Harman, Zoltán; Ott, Christian
  • Nature Photonics, Vol. 8, Issue 7
  • DOI: 10.1038/nphoton.2014.113

Terahertz laser frequency combs
journal, May 2014


Attosecond metrology: from electron capture to future signal processing
journal, February 2014


New CMOS-compatible platforms based on silicon nitride and Hydex for nonlinear optics
journal, July 2013

  • Moss, David J.; Morandotti, Roberto; Gaeta, Alexander L.
  • Nature Photonics, Vol. 7, Issue 8
  • DOI: 10.1038/nphoton.2013.183

Optical-field-induced current in dielectrics
journal, December 2012

  • Schiffrin, Agustin; Paasch-Colberg, Tim; Karpowicz, Nicholas
  • Nature, Vol. 493, Issue 7430
  • DOI: 10.1038/nature11567

Controlling dielectrics with the electric field of light
journal, December 2012

  • Schultze, Martin; Bothschafter, Elisabeth M.; Sommer, Annkatrin
  • Nature, Vol. 493, Issue 7430
  • DOI: 10.1038/nature11720

Ab Initio Simulation of Electrical Currents Induced by Ultrafast Laser Excitation of Dielectric Materials
journal, August 2014


The electronic properties of graphene
journal, January 2009

  • Castro Neto, A. H.; Guinea, F.; Peres, N. M. R.
  • Reviews of Modern Physics, Vol. 81, Issue 1, p. 109-162
  • DOI: 10.1103/RevModPhys.81.109

4D Visualization of Transitional Structures in Phase Transformations by Electron Diffraction
journal, November 2007


Imaging electronic quantum motion with light
journal, July 2012

  • Dixit, G.; Vendrell, O.; Santra, R.
  • Proceedings of the National Academy of Sciences, Vol. 109, Issue 29
  • DOI: 10.1073/pnas.1202226109

Role of electron-electron interference in ultrafast time-resolved imaging of electronic wavepackets
journal, April 2013

  • Dixit, Gopal; Santra, Robin
  • The Journal of Chemical Physics, Vol. 138, Issue 13
  • DOI: 10.1063/1.4798321

Time-resolved ultrafast electron ( e , 2 e ) momentum spectroscopy
journal, May 2013


X-ray imaging of chemically active valence electrons during a pericyclic reaction
journal, November 2014

  • Bredtmann, Timm; Ivanov, Misha; Dixit, Gopal
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms6589

Electron Transfer in a Virtual Quantum State of LiBH 4 Induced by Strong Optical Fields and Mapped by Femtosecond X-Ray Diffraction
journal, October 2012


Perspective: Structural dynamics in condensed matter mapped by femtosecond x-ray diffraction
journal, January 2014

  • Elsaesser, T.; Woerner, M.
  • The Journal of Chemical Physics, Vol. 140, Issue 2
  • DOI: 10.1063/1.4855115

Graphene in ultrafast and superstrong laser fields
journal, January 2015


Response of graphene to femtosecond high-intensity laser irradiation
journal, August 2011

  • Roberts, Adam; Cormode, Daniel; Reynolds, Collin
  • Applied Physics Letters, Vol. 99, Issue 5
  • DOI: 10.1063/1.3623760

High-energy, phase-stable, ultrabroadband kHz OPCPA at 21 μm pumped by a picosecond cryogenic Yb:YAG laser
journal, January 2011

  • Hong, Kyung-Han; Huang, Shu-Wei; Moses, Jeffrey
  • Optics Express, Vol. 19, Issue 16
  • DOI: 10.1364/OE.19.015538

Femtosecond Population Inversion and Stimulated Emission of Dense Dirac Fermions in Graphene
journal, April 2012


Measuring the temporal structure of few-femtosecond free-electron laser X-ray pulses directly in the time domain
journal, November 2014


Ultra-fast and ultra-intense x-ray sciences: first results from the Linac Coherent Light Source free-electron laser
journal, August 2013

  • Bostedt, C.; Bozek, J. D.; Bucksbaum, P. H.
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 46, Issue 16
  • DOI: 10.1088/0953-4075/46/16/164003

Femtosecond X-ray Pulses at 0.4 A Generated by 90  Thomson Scattering: A Tool for Probing the Structural Dynamics of Materials
journal, October 1996


Single-molecule electron diffraction imaging with charge replacement
journal, September 2008


4D electron imaging: principles and perspectives
journal, January 2008

  • Shorokhov, Dmitry; Zewail, Ahmed H.
  • Physical Chemistry Chemical Physics, Vol. 10, Issue 20
  • DOI: 10.1039/b801626g

Femtosecond electron diffraction: heralding the era of atomically resolved dynamics
journal, August 2011


Compression of Subrelativistic Space-Charge-Dominated Electron Bunches for Single-Shot Femtosecond Electron Diffraction
journal, December 2010


Mapping molecular motions leading to charge delocalization with ultrabright electrons
journal, April 2013

  • Gao, Meng; Lu, Cheng; Jean-Ruel, Hubert
  • Nature, Vol. 496, Issue 7445
  • DOI: 10.1038/nature12044

Hybrid dc–ac electron gun for fs-electron pulse generation
journal, December 2007


Towards ultimate temporal and spatial resolutions with ultrafast single-electron diffraction
journal, June 2014


Quantum coherent optical phase modulation in an ultrafast transmission electron microscope
journal, May 2015

  • Feist, Armin; Echternkamp, Katharina E.; Schauss, Jakob
  • Nature, Vol. 521, Issue 7551
  • DOI: 10.1038/nature14463

Femtosecond single-electron diffraction
journal, May 2014

  • Lahme, S.; Kealhofer, C.; Krausz, F.
  • Structural Dynamics, Vol. 1, Issue 3
  • DOI: 10.1063/1.4884937

Structural dynamics of nanoscale gold by ultrafast electron crystallography
journal, October 2011


Coherent and Incoherent Electron-Phonon Coupling in Graphite Observed with Radio-Frequency Compressed Ultrafast Electron Diffraction
journal, December 2014


Direct observation of d-orbital holes and Cu–Cu bonding in Cu2O
journal, September 1999

  • Zuo, J. M.; Kim, M.; O'Keeffe, M.
  • Nature, Vol. 401, Issue 6748
  • DOI: 10.1038/43403

The interplay between structure and orbitals in the chemical bonding of graphite
journal, August 2010


Snapshots of cooperative atomic motions in the optical suppression of charge density waves
journal, November 2010

  • Eichberger, Maximilian; Schäfer, Hanjo; Krumova, Marina
  • Nature, Vol. 468, Issue 7325
  • DOI: 10.1038/nature09539

Snapshots of the retarded interaction of charge carriers with ultrafast fluctuations in cuprates
journal, March 2015

  • Dal Conte, S.; Vidmar, L.; Golež, D.
  • Nature Physics, Vol. 11, Issue 5
  • DOI: 10.1038/nphys3265

Ab Initio G W Many-Body Effects in Graphene
journal, November 2008


First Direct Observation of a Nearly Ideal Graphene Band Structure
journal, November 2009


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

On the exponential solution of differential equations for a linear operator
journal, November 1954


A pedagogical approach to the Magnus expansion
journal, June 2010


Expokit: a software package for computing matrix exponentials
journal, March 1998


Relativistic separable dual-space Gaussian pseudopotentials from H to Rn
journal, August 1998


Dark-field transmission electron microscopy and the Debye-Waller factor of graphene
journal, January 2013


Imaging electronic motions in atoms by energy-resolved ultrafast electron diffraction
journal, September 2014


Concerted electron and proton transfer in ionic crystals mapped by femtosecond x-ray powder diffraction
journal, August 2010

  • Woerner, Michael; Zamponi, Flavio; Ansari, Zunaira
  • The Journal of Chemical Physics, Vol. 133, Issue 6
  • DOI: 10.1063/1.3469779

Coherence of femtosecond single electrons exceeds biomolecular dimensions
journal, June 2013


Ultrafast relaxation dynamics of hot optical phonons in graphene
journal, February 2010

  • Wang, Haining; Strait, Jared H.; George, Paul A.
  • Applied Physics Letters, Vol. 96, Issue 8
  • DOI: 10.1063/1.3291615

Optical-field-induced current in dielectrics
journal, December 2012

  • Schiffrin, Agustin; Paasch-Colberg, Tim; Karpowicz, Nicholas
  • Nature, Vol. 493, Issue 7430
  • DOI: 10.1038/nature11567

Controlling dielectrics with the electric field of light
journal, December 2012

  • Schultze, Martin; Bothschafter, Elisabeth M.; Sommer, Annkatrin
  • Nature, Vol. 493, Issue 7430
  • DOI: 10.1038/nature11720

New CMOS-compatible platforms based on silicon nitride and Hydex for nonlinear optics
journal, July 2013

  • Moss, David J.; Morandotti, Roberto; Gaeta, Alexander L.
  • Nature Photonics, Vol. 7, Issue 8
  • DOI: 10.1038/nphoton.2013.183

Broadband high-resolution X-ray frequency combs
journal, June 2014

  • Cavaletto, Stefano M.; Harman, Zoltán; Ott, Christian
  • Nature Photonics, Vol. 8, Issue 7
  • DOI: 10.1038/nphoton.2014.113

Quantum nonlinear optics — photon by photon
journal, August 2014

  • Chang, Darrick E.; Vuletić, Vladan; Lukin, Mikhail D.
  • Nature Photonics, Vol. 8, Issue 9
  • DOI: 10.1038/nphoton.2014.192

4D electron imaging: principles and perspectives
journal, January 2008

  • Shorokhov, Dmitry; Zewail, Ahmed H.
  • Physical Chemistry Chemical Physics, Vol. 10, Issue 20
  • DOI: 10.1039/b801626g

Femtosecond X-ray diffraction maps field-driven charge dynamics in ionic crystals
journal, January 2014

  • Woerner, Michael; Holtz, Marcel; Juvé, Vincent
  • Faraday Discuss., Vol. 171
  • DOI: 10.1039/c4fd00026a

Perspective: Structural dynamics in condensed matter mapped by femtosecond x-ray diffraction
journal, January 2014

  • Elsaesser, T.; Woerner, M.
  • The Journal of Chemical Physics, Vol. 140, Issue 2
  • DOI: 10.1063/1.4855115

Femtosecond single-electron diffraction
journal, May 2014

  • Lahme, S.; Kealhofer, C.; Krausz, F.
  • Structural Dynamics, Vol. 1, Issue 3
  • DOI: 10.1063/1.4884937

Femtosecond electron diffraction: heralding the era of atomically resolved dynamics
journal, August 2011


Detecting Electron Motion in Atoms and Molecules
journal, December 2010


Beam by design: Laser manipulation of electrons in modern accelerators
journal, July 2014


Ultrafast electron dynamics in phenylalanine initiated by attosecond pulses
journal, October 2014


Single-molecule electron diffraction imaging with charge replacement
text, January 2008


First direct observation of a nearly ideal graphene band structure
text, January 2009


Compression of sub-relativistic space-charge-dominated electron bunches for single-shot femtosecond electron diffraction
text, January 2010


Imaging electronic quantum motion with light
text, January 2012


Ab Initio Simulation of Electrical Currents Induced by Ultrafast Laser Excitation of Dielectric Materials
text, January 2014


Works referencing / citing this record:

High-temporal-resolution electron microscopy for imaging ultrafast electron dynamics
journal, May 2017


Diffraction and microscopy with attosecond electron pulse trains
journal, November 2017


Ultrafast electron crystallography of the cooperative reaction path in vanadium dioxide
journal, May 2016

  • Yang, Ding-Shyue; Baum, Peter; Zewail, Ahmed H.
  • Structural Dynamics, Vol. 3, Issue 3
  • DOI: 10.1063/1.4953370

Design and implementation of an optimal laser pulse front tilting scheme for ultrafast electron diffraction in reflection geometry with high temporal resolution
journal, July 2017

  • Pennacchio, Francesco; Vanacore, Giovanni M.; Mancini, Giulia F.
  • Structural Dynamics, Vol. 4, Issue 4
  • DOI: 10.1063/1.4991483

Attomicroscopy: from femtosecond to attosecond electron microscopy
journal, January 2018

  • Hassan, Mohammed Th
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 51, Issue 3
  • DOI: 10.1088/1361-6455/aaa183

Attosecond physics at the nanoscale
journal, March 2017

  • Ciappina, M. F.; Pérez-Hernández, J. A.; Landsman, A. S.
  • Reports on Progress in Physics, Vol. 80, Issue 5
  • DOI: 10.1088/1361-6633/aa574e

Terahertz Compression of Electron Pulses at a Planar Mirror Membrane
journal, February 2019


Tilted Electron Pulses
journal, August 2018


All-optical control and metrology of electron pulses
journal, April 2016


Compression of picosecond pulses from a thin-disk laser to 30fs at 4W average power
journal, January 2018

  • Chen, Bo-Han; Kretschmar, Martin; Ehberger, Dominik
  • Optics Express, Vol. 26, Issue 4
  • DOI: 10.1364/oe.26.003861

Octave-spanning single-cycle middle-infrared generation through optical parametric amplification in LiGaS 2
journal, January 2019

  • Chen, Bo-Han; Wittmann, Emanuel; Morimoto, Yuya
  • Optics Express, Vol. 27, Issue 15
  • DOI: 10.1364/oe.27.021306

Second-harmonic generation and self-phase modulation of few-cycle mid-infrared pulses
journal, January 2019

  • Chen, Bo-Han; Hofer, Christina; Pupeza, Ioachim
  • Optics Letters, Vol. 44, Issue 16
  • DOI: 10.1364/ol.44.004079

Ultrashort Free-Electron Laser X-ray Pulses
journal, September 2017

  • Helml, Wolfram; Grguraš, Ivanka; Juranić, Pavle
  • Applied Sciences, Vol. 7, Issue 9
  • DOI: 10.3390/app7090915

Ultrashort Free-Electron Laser X-ray Pulses
text, January 2017

  • Helml, Wolfram; Grguraš, Ivanka; Juranic, Pavle
  • Deutsches Elektronen-Synchrotron, DESY, Hamburg
  • DOI: 10.3204/pubdb-2018-00272

Attosecond physics at the nanoscale
text, January 2016


Ultrafast electron crystallography of the cooperative reaction path in vanadium dioxide
journal, May 2016

  • Yang, Ding-Shyue; Baum, Peter; Zewail, Ahmed H.
  • Structural Dynamics, Vol. 3, Issue 3
  • DOI: 10.1063/1.4953370

Design and implementation of an optimal laser pulse front tilting scheme for ultrafast electron diffraction in reflection geometry with high temporal resolution
journal, July 2017

  • Pennacchio, Francesco; Vanacore, Giovanni M.; Mancini, Giulia F.
  • Structural Dynamics, Vol. 4, Issue 4
  • DOI: 10.1063/1.4991483

Ultrashort Free-Electron Laser X-ray Pulses
text, January 2017

  • Helml, Wolfram; Grguraš, Ivanka; Juranic, Pavle
  • Deutsches Elektronen-Synchrotron, DESY, Hamburg
  • DOI: 10.3204/pubdb-2018-00272

Attosecond physics at the nanoscale
text, January 2016


Theoretical Atto-nano Physics
text, January 2019