skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Role of initial magnetic disorder: A time-dependent ab initio study of ultrafast demagnetization mechanisms

Abstract

Despite more than 20 years of development, the underlying physics of the laser-induced demagnetization process is still debated. We present a fast, real-time time-dependent density functional theory (rt-TDDFT) algorithm together with the phenomenological atomic Landau-Lifshitz-Gilbert model to investigate this problem. Our Hamiltonian considers noncollinear magnetic moment, spin-orbit coupling (SOC), electron-electron, electron-phonon, and electron-light interactions. The algorithm for time evolution achieves hundreds of times of speedup enabling calculation of large systems. Our simulations yield a demagnetization rate similar to experiments. We found that (i) the angular momentum flow from light to the system is not essential and the spin Zeeman effect is negligible. (ii) The phonon can play a role but is not essential. (iii) The initial spin disorder and the self-consistent update of the electron-electron interaction play dominant roles and enhance the demagnetization to the experimentally observed rate. Finally, the spin disorder connects the electronic structure theory with the phenomenological three-temperature model.

Authors:
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1565778
Alternate Identifier(s):
OSTI ID: 1603517
Grant/Contract Number:  
[AC02-05CH11231]
Resource Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
[ Journal Volume: 5; Journal Issue: 6]; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; science & technology - other topics

Citation Formats

None, None. Role of initial magnetic disorder: A time-dependent ab initio study of ultrafast demagnetization mechanisms. United States: N. p., 2019. Web. doi:10.1126/sciadv.aau8000.
None, None. Role of initial magnetic disorder: A time-dependent ab initio study of ultrafast demagnetization mechanisms. United States. doi:10.1126/sciadv.aau8000.
None, None. Fri . "Role of initial magnetic disorder: A time-dependent ab initio study of ultrafast demagnetization mechanisms". United States. doi:10.1126/sciadv.aau8000. https://www.osti.gov/servlets/purl/1565778.
@article{osti_1565778,
title = {Role of initial magnetic disorder: A time-dependent ab initio study of ultrafast demagnetization mechanisms},
author = {None, None},
abstractNote = {Despite more than 20 years of development, the underlying physics of the laser-induced demagnetization process is still debated. We present a fast, real-time time-dependent density functional theory (rt-TDDFT) algorithm together with the phenomenological atomic Landau-Lifshitz-Gilbert model to investigate this problem. Our Hamiltonian considers noncollinear magnetic moment, spin-orbit coupling (SOC), electron-electron, electron-phonon, and electron-light interactions. The algorithm for time evolution achieves hundreds of times of speedup enabling calculation of large systems. Our simulations yield a demagnetization rate similar to experiments. We found that (i) the angular momentum flow from light to the system is not essential and the spin Zeeman effect is negligible. (ii) The phonon can play a role but is not essential. (iii) The initial spin disorder and the self-consistent update of the electron-electron interaction play dominant roles and enhance the demagnetization to the experimentally observed rate. Finally, the spin disorder connects the electronic structure theory with the phenomenological three-temperature model.},
doi = {10.1126/sciadv.aau8000},
journal = {Science Advances},
number = [6],
volume = [5],
place = {United States},
year = {2019},
month = {6}
}

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

Citation Metrics:
Cited by: 2 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Ultrafast Magnetism of a Ferrimagnet across the Spin-Flop Transition in High Magnetic Fields
journal, March 2017


Laser-Induced Ultrafast Demagnetization in Ferromagnetic Metals
journal, October 2000


Control of speed and efficiency of ultrafast demagnetization by direct transfer of spin angular momentum
journal, September 2008

  • Malinowski, G.; Dalla Longa, F.; Rietjens, J. H. H.
  • Nature Physics, Vol. 4, Issue 11
  • DOI: 10.1038/nphys1092

Comparing Ultrafast Demagnetization Rates Between Competing Models for Finite Temperature Magnetism
journal, May 2013


Femtosecond Spectrotemporal Magneto-optics
journal, August 2004


Laser-Induced Intersite Spin Transfer
journal, February 2018


Atomistic spin model simulations of magnetic nanomaterials
journal, February 2014


Ultrafast Spin Dynamics of Ferromagnetic Thin Films Observed by fs Spin-Resolved Two-Photon Photoemission
journal, December 1997


Femtosecond control of electric currents in metallic ferromagnetic heterostructures
journal, February 2016

  • Huisman, T. J.; Mikhaylovskiy, R. V.; Costa, J. D.
  • Nature Nanotechnology, Vol. 11, Issue 5
  • DOI: 10.1038/nnano.2015.331

Ultrafast magnetization enhancement in metallic multilayers driven by superdiffusive spin current
journal, January 2012

  • Rudolf, Dennis; La-O-Vorakiat, Chan; Battiato, Marco
  • Nature Communications, Vol. 3, Issue 1
  • DOI: 10.1038/ncomms2029

Laser-induced ultrafast demagnetization time and spin moment in ferromagnets: First-principles calculation
journal, May 2015

  • Zhang, G. P.; Si, M. S.; George, Thomas F.
  • Journal of Applied Physics, Vol. 117, Issue 17
  • DOI: 10.1063/1.4907693

Ultrafast Magneto-Optics in Nickel: Magnetism or Optics?
journal, July 2000


Distinguishing the ultrafast dynamics of spin and orbital moments in solids
journal, May 2010

  • Boeglin, C.; Beaurepaire, E.; Halté, V.
  • Nature, Vol. 465, Issue 7297
  • DOI: 10.1038/nature09070

Reply: "Is the controversy over femtosecond magneto-optics really solved?"
journal, September 2011

  • Zhang, G. P.; Hübner, W.; Lefkidis, Georg
  • Nature Physics, Vol. 7, Issue 9
  • DOI: 10.1038/nphys2069

Ultrafast spin-transfer torque driven by femtosecond pulsed-laser excitation
journal, July 2014

  • Schellekens, A. J.; Kuiper, K. C.; de Wit, R. R. J. C.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5333

Spin current generated by thermally driven ultrafast demagnetization
journal, July 2014

  • Choi, Gyung-Min; Min, Byoung-Chul; Lee, Kyung-Jin
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5334

Ultrafast optical manipulation of magnetic order
journal, September 2010


Is the controversy over femtosecond magneto-optics really solved?
journal, September 2011

  • Carva, Karel; Battiato, Marco; Oppeneer, Peter M.
  • Nature Physics, Vol. 7, Issue 9
  • DOI: 10.1038/nphys2067

XLIX. The magnetization-temperature curves of iron, cobalt, and nickel
journal, February 1931

  • Tyler, F.
  • The London, Edinburgh, and Dublin Philosophical Magazine and Journal of Science, Vol. 11, Issue 70
  • DOI: 10.1080/14786443109461711

Unifying Ultrafast Magnetization Dynamics
journal, December 2005


Nonadiabatic molecular dynamics simulation for carrier transport in a pentathiophene butyric acid monolayer
journal, May 2013


Spin conversion on the nanoscale
journal, July 2017

  • Otani, YoshiChika; Shiraishi, Masashi; Oiwa, Akira
  • Nature Physics, Vol. 13, Issue 9
  • DOI: 10.1038/nphys4192

Probing the timescale of the exchange interaction in a ferromagnetic alloy
journal, March 2012

  • Mathias, S.; La-O-Vorakiat, C.; Grychtol, P.
  • Proceedings of the National Academy of Sciences, Vol. 109, Issue 13
  • DOI: 10.1073/pnas.1201371109

Femtosecond modification of electron localization and transfer of angular momentum in nickel
journal, August 2007

  • Stamm, C.; Kachel, T.; Pontius, N.
  • Nature Materials, Vol. 6, Issue 10
  • DOI: 10.1038/nmat1985

Antiferromagnetic opto-spintronics
journal, March 2018


Ultrafast demagnetization of ferromagnetic transition metals: The role of the Coulomb interaction
journal, November 2009


Dynamics of electron-magnon interaction and ultrafast demagnetization in thin iron films
journal, November 2008


Ultrafast Transport of Laser-Excited Spin-Polarized Carriers in Au / Fe / MgO ( 001 )
journal, August 2011


All-optical control of ferromagnetic thin films and nanostructures
journal, August 2014

  • Lambert, C. -H.; Mangin, S.; Varaprasad, B. S. D. C. S.
  • Science, Vol. 345, Issue 6202
  • DOI: 10.1126/science.1253493

Electron-phonon scattering dynamics in ferromagnetic metals and their influence on ultrafast demagnetization processes
journal, December 2011


Laser-Induced Demagnetization at Ultrashort Time Scales: Predictions of TDDFT
journal, September 2015

  • Krieger, K.; Dewhurst, J. K.; Elliott, P.
  • Journal of Chemical Theory and Computation, Vol. 11, Issue 10
  • DOI: 10.1021/acs.jctc.5b00621

Superdiffusive Spin Transport as a Mechanism of Ultrafast Demagnetization
journal, July 2010


Total angular momentum conservation in laser-induced femtosecond magnetism
journal, August 2008


Coherent ultrafast magnetism induced by femtosecond laser pulses
journal, May 2009

  • Bigot, Jean-Yves; Vomir, Mircea; Beaurepaire, Eric
  • Nature Physics, Vol. 5, Issue 7
  • DOI: 10.1038/nphys1285

Spatially resolved ultrafast magnetic dynamics initiated at a complex oxide heterointerface
journal, July 2015

  • Först, M.; Caviglia, A. D.; Scherwitzl, R.
  • Nature Materials, Vol. 14, Issue 9
  • DOI: 10.1038/nmat4341

Spin Flips versus Spin Transport in Nonthermal Electrons Excited by Ultrashort Optical Pulses in Transition Metals
journal, September 2017


Accessing the fundamentals of magnetotransport in metals with terahertz probes
journal, July 2015

  • Jin, Zuanming; Tkach, Alexander; Casper, Frederick
  • Nature Physics, Vol. 11, Issue 9
  • DOI: 10.1038/nphys3384

Optical-helicity-driven magnetization dynamics in metallic ferromagnets
journal, April 2017

  • Choi, Gyung-Min; Schleife, André; Cahill, David G.
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms15085

Nonequilibrium Magnetization Dynamics of Nickel
journal, June 1997


Distinguishing attosecond electron–electron scattering and screening in transition metals
journal, June 2017

  • Chen, Cong; Tao, Zhensheng; Carr, Adra
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 27
  • DOI: 10.1073/pnas.1706466114

THz-Driven Ultrafast Spin-Lattice Scattering in Amorphous Metallic Ferromagnets
journal, August 2016


Ultrafast Spin Dynamics in Ferromagnetic Nickel
journal, May 1996


Ab Initio Investigation of the Elliott-Yafet Electron-Phonon Mechanism in Laser-Induced Ultrafast Demagnetization
journal, November 2011


The analysis of a plane wave pseudopotential density functional theory code on a GPU machine
journal, January 2013


Paradigm of the time-resolved magneto-optical Kerr effect for femtosecond magnetism
journal, June 2009

  • Zhang, G. P.; Hübner, W.; Lefkidis, Georgios
  • Nature Physics, Vol. 5, Issue 7
  • DOI: 10.1038/nphys1315

Probing ultrafast photo-induced dynamics of the exchange energy in a Heisenberg antiferromagnet
journal, July 2015


Feedback Effect during Ultrafast Demagnetization Dynamics in Ferromagnets
journal, October 2013


Angular Momentum Conservation for Coherently Manipulated Spin Polarization in Photoexcited NiO: An Ab Initio Calculation
journal, November 2009


Explaining the paradoxical diversity of ultrafast laser-induced demagnetization
journal, December 2009

  • Koopmans, B.; Malinowski, G.; Dalla Longa, F.
  • Nature Materials, Vol. 9, Issue 3
  • DOI: 10.1038/nmat2593

Band-Structure-Dependent Demagnetization in the Heusler Alloy Co 2 Mn 1 x Fe x Si
journal, November 2010


Laser-induced ultrafast spin dynamics in di-, tri- and tetranuclear nickel clusters, and the M process
journal, December 2014


Engineered materials for all-optical helicity-dependent magnetic switching
journal, February 2014

  • Mangin, S.; Gottwald, M.; Lambert, C-H.
  • Nature Materials, Vol. 13, Issue 3
  • DOI: 10.1038/nmat3864

Ultrafast spin transport as key to femtosecond demagnetization
journal, January 2013

  • Eschenlohr, A.; Battiato, M.; Maldonado, P.
  • Nature Materials, Vol. 12, Issue 4
  • DOI: 10.1038/nmat3546

Ultrafast Magnon Generation in an Fe Film on Cu(100)
journal, November 2010


Beyond a phenomenological description of magnetostriction
journal, January 2018


Optical determination of the Néel vector in a CuMnAs thin-film antiferromagnet
journal, January 2017


Ab Initio Theory of Coherent Laser-Induced Magnetization in Metals
journal, September 2016


Band structure evolution during the ultrafast ferromagnetic-paramagnetic phase transition in cobalt
journal, March 2017

  • Eich, Steffen; Plötzing, Moritz; Rollinger, Markus
  • Science Advances, Vol. 3, Issue 3
  • DOI: 10.1126/sciadv.1602094

Magnetic spin moment reduction in photoexcited ferromagnets through exchange interaction quenching: beyond the rigid band approximation
journal, May 2015


Ultrafast heating as a sufficient stimulus for magnetization reversal in a ferrimagnet
journal, January 2012

  • Ostler, T. A.; Barker, J.; Evans, R. F. L.
  • Nature Communications, Vol. 3, Issue 1
  • DOI: 10.1038/ncomms1666

The Magnetization of Pure Iron and Nickel
journal, March 1971

  • Crangle, J.; Goodman, G. M.
  • Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 321, Issue 1547
  • DOI: 10.1098/rspa.1971.0044

Femtosecond Spin Current Pulses Generated by the Nonthermal Spin-Dependent Seebeck Effect and Interacting with Ferromagnets in Spin Valves
journal, July 2017


Controlling the Competition between Optically Induced Ultrafast Spin-Flip Scattering and Spin Transport in Magnetic Multilayers
journal, May 2013


    Works referencing / citing this record:

    The analysis of a plane wave pseudopotential density functional theory code on a GPU machine
    journal, January 2013


    Laser-Induced Demagnetization at Ultrashort Time Scales: Predictions of TDDFT
    journal, September 2015

    • Krieger, K.; Dewhurst, J. K.; Elliott, P.
    • Journal of Chemical Theory and Computation, Vol. 11, Issue 10
    • DOI: 10.1021/acs.jctc.5b00621

    Laser-Induced Intersite Spin Transfer
    journal, February 2018


    Distinguishing the ultrafast dynamics of spin and orbital moments in solids
    journal, May 2010

    • Boeglin, C.; Beaurepaire, E.; Halté, V.
    • Nature, Vol. 465, Issue 7297
    • DOI: 10.1038/nature09070

    Optical-helicity-driven magnetization dynamics in metallic ferromagnets
    journal, April 2017

    • Choi, Gyung-Min; Schleife, André; Cahill, David G.
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/ncomms15085

    Ultrafast heating as a sufficient stimulus for magnetization reversal in a ferrimagnet
    journal, January 2012

    • Ostler, T. A.; Barker, J.; Evans, R. F. L.
    • Nature Communications, Vol. 3, Issue 1
    • DOI: 10.1038/ncomms1666

    Ultrafast magnetization enhancement in metallic multilayers driven by superdiffusive spin current
    journal, January 2012

    • Rudolf, Dennis; La-O-Vorakiat, Chan; Battiato, Marco
    • Nature Communications, Vol. 3, Issue 1
    • DOI: 10.1038/ncomms2029

    Ultrafast spin-transfer torque driven by femtosecond pulsed-laser excitation
    journal, July 2014

    • Schellekens, A. J.; Kuiper, K. C.; de Wit, R. R. J. C.
    • Nature Communications, Vol. 5, Issue 1
    • DOI: 10.1038/ncomms5333

    Spin current generated by thermally driven ultrafast demagnetization
    journal, July 2014

    • Choi, Gyung-Min; Min, Byoung-Chul; Lee, Kyung-Jin
    • Nature Communications, Vol. 5, Issue 1
    • DOI: 10.1038/ncomms5334

    Femtosecond modification of electron localization and transfer of angular momentum in nickel
    journal, August 2007

    • Stamm, C.; Kachel, T.; Pontius, N.
    • Nature Materials, Vol. 6, Issue 10
    • DOI: 10.1038/nmat1985

    Explaining the paradoxical diversity of ultrafast laser-induced demagnetization
    journal, December 2009

    • Koopmans, B.; Malinowski, G.; Dalla Longa, F.
    • Nature Materials, Vol. 9, Issue 3
    • DOI: 10.1038/nmat2593

    Ultrafast spin transport as key to femtosecond demagnetization
    journal, January 2013

    • Eschenlohr, A.; Battiato, M.; Maldonado, P.
    • Nature Materials, Vol. 12, Issue 4
    • DOI: 10.1038/nmat3546

    Engineered materials for all-optical helicity-dependent magnetic switching
    journal, February 2014

    • Mangin, S.; Gottwald, M.; Lambert, C-H.
    • Nature Materials, Vol. 13, Issue 3
    • DOI: 10.1038/nmat3864

    Spatially resolved ultrafast magnetic dynamics initiated at a complex oxide heterointerface
    journal, July 2015

    • Först, M.; Caviglia, A. D.; Scherwitzl, R.
    • Nature Materials, Vol. 14, Issue 9
    • DOI: 10.1038/nmat4341

    Femtosecond control of electric currents in metallic ferromagnetic heterostructures
    journal, February 2016

    • Huisman, T. J.; Mikhaylovskiy, R. V.; Costa, J. D.
    • Nature Nanotechnology, Vol. 11, Issue 5
    • DOI: 10.1038/nnano.2015.331

    Probing ultrafast photo-induced dynamics of the exchange energy in a Heisenberg antiferromagnet
    journal, July 2015


    Optical determination of the Néel vector in a CuMnAs thin-film antiferromagnet
    journal, January 2017


    Control of speed and efficiency of ultrafast demagnetization by direct transfer of spin angular momentum
    journal, September 2008

    • Malinowski, G.; Dalla Longa, F.; Rietjens, J. H. H.
    • Nature Physics, Vol. 4, Issue 11
    • DOI: 10.1038/nphys1092

    Coherent ultrafast magnetism induced by femtosecond laser pulses
    journal, May 2009

    • Bigot, Jean-Yves; Vomir, Mircea; Beaurepaire, Eric
    • Nature Physics, Vol. 5, Issue 7
    • DOI: 10.1038/nphys1285

    Paradigm of the time-resolved magneto-optical Kerr effect for femtosecond magnetism
    journal, June 2009

    • Zhang, G. P.; Hübner, W.; Lefkidis, Georgios
    • Nature Physics, Vol. 5, Issue 7
    • DOI: 10.1038/nphys1315

    Is the controversy over femtosecond magneto-optics really solved?
    journal, September 2011

    • Carva, Karel; Battiato, Marco; Oppeneer, Peter M.
    • Nature Physics, Vol. 7, Issue 9
    • DOI: 10.1038/nphys2067

    Reply: "Is the controversy over femtosecond magneto-optics really solved?"
    journal, September 2011

    • Zhang, G. P.; Hübner, W.; Lefkidis, Georg
    • Nature Physics, Vol. 7, Issue 9
    • DOI: 10.1038/nphys2069

    Accessing the fundamentals of magnetotransport in metals with terahertz probes
    journal, July 2015

    • Jin, Zuanming; Tkach, Alexander; Casper, Frederick
    • Nature Physics, Vol. 11, Issue 9
    • DOI: 10.1038/nphys3384

    Spin conversion on the nanoscale
    journal, July 2017

    • Otani, YoshiChika; Shiraishi, Masashi; Oiwa, Akira
    • Nature Physics, Vol. 13, Issue 9
    • DOI: 10.1038/nphys4192

    Beyond a phenomenological description of magnetostriction
    journal, January 2018


    Antiferromagnetic opto-spintronics
    journal, March 2018


    Laser-induced ultrafast demagnetization time and spin moment in ferromagnets: First-principles calculation
    journal, May 2015

    • Zhang, G. P.; Si, M. S.; George, Thomas F.
    • Journal of Applied Physics, Vol. 117, Issue 17
    • DOI: 10.1063/1.4907693

    Probing the timescale of the exchange interaction in a ferromagnetic alloy
    journal, March 2012

    • Mathias, S.; La-O-Vorakiat, C.; Grychtol, P.
    • Proceedings of the National Academy of Sciences, Vol. 109, Issue 13
    • DOI: 10.1073/pnas.1201371109

    Distinguishing attosecond electron–electron scattering and screening in transition metals
    journal, June 2017

    • Chen, Cong; Tao, Zhensheng; Carr, Adra
    • Proceedings of the National Academy of Sciences, Vol. 114, Issue 27
    • DOI: 10.1073/pnas.1706466114

    XLIX. The magnetization-temperature curves of iron, cobalt, and nickel
    journal, February 1931

    • Tyler, F.
    • The London, Edinburgh, and Dublin Philosophical Magazine and Journal of Science, Vol. 11, Issue 70
    • DOI: 10.1080/14786443109461711

    Atomistic spin model simulations of magnetic nanomaterials
    journal, February 2014


    Magnetic spin moment reduction in photoexcited ferromagnets through exchange interaction quenching: beyond the rigid band approximation
    journal, May 2015


    The Magnetization of Pure Iron and Nickel
    journal, March 1971

    • Crangle, J.; Goodman, G. M.
    • Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 321, Issue 1547
    • DOI: 10.1098/rspa.1971.0044

    Efficient Real-Time Time-Dependent Density Functional Theory Method and its Application to a Collision of an Ion with a 2D Material
    journal, February 2015


    Band structure evolution during the ultrafast ferromagnetic-paramagnetic phase transition in cobalt
    journal, March 2017

    • Eich, Steffen; Plötzing, Moritz; Rollinger, Markus
    • Science Advances, Vol. 3, Issue 3
    • DOI: 10.1126/sciadv.1602094

    All-optical control of ferromagnetic thin films and nanostructures
    journal, August 2014

    • Lambert, C. -H.; Mangin, S.; Varaprasad, B. S. D. C. S.
    • Science, Vol. 345, Issue 6202
    • DOI: 10.1126/science.1253493