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Title: Ultrafast nonequilibrium evolution of excitonic modes in semiconductors

Abstract

We study the time evolution of excitonic states after photoexcitation in the one-dimensional spinless extended Falicov-Kimball model. Several numerical methods are employed and benchmarked against each other: time-dependent mean-field simulations, the second-Born approximation (2BA) within the Kadanoff-Baym formalism, the generalized Kadanoff-Baym ansatz (GKBA) implemented with the 2BA, and the infinite time-evolving block decimation (iTEBD) method. It is found that the GKBA gives the best agreement with iTEBD and captures the relevant physics. Excitations to the particle-hole continuum and resonant excitations of the equilibrium exciton result in a qualitatively different dynamics. In the former case, the exciton binding energy remains positive and the frequency of the corresponding coherent oscillations is smaller than the band gap. On the other hand, resonant excitations trigger a collective mode whose frequency is larger than the band gap. We discuss the origin of these different behaviors by evaluating the nonequilibrium susceptibility using the nonthermal distribution and a random phase approximation. We note the peculiar mode with frequency larger than the band gap is associated with a partial population inversion with a sharp energy cutoff. We also discuss the effects of the cooling by a phonon bath. We demonstrate the real-time development of coherence in the polarization,more » which indicates excitonic condensation out of equilibrium.« less

Authors:
 [1];  [2];  [3];  [4]
  1. Tokyo Institute of Technology (Japan); Univ. of Fribourg (Switzerland)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
  3. Max Planck Inst. the Physics of Complex Systems, Dresden (Germany)
  4. Univ. of Fribourg (Switzerland)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE; European Research Council (ERC); Swiss National Science Foundation (SNF); Alexander von Humboldt Foundation
OSTI Identifier:
1604932
Report Number(s):
arXiv:1907.06799v2
Journal ID: ISSN 2469-9950; PRBMDO; TRN: US2104353
Grant/Contract Number:  
AC02-76SF00515; 724103
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 101; Journal Issue: 3; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Murakami, Yuta, Schüler, Michael, Takayoshi, Shintaro, and Werner, Philipp. Ultrafast nonequilibrium evolution of excitonic modes in semiconductors. United States: N. p., 2020. Web. doi:10.1103/physrevb.101.035203.
Murakami, Yuta, Schüler, Michael, Takayoshi, Shintaro, & Werner, Philipp. Ultrafast nonequilibrium evolution of excitonic modes in semiconductors. United States. https://doi.org/10.1103/physrevb.101.035203
Murakami, Yuta, Schüler, Michael, Takayoshi, Shintaro, and Werner, Philipp. Tue . "Ultrafast nonequilibrium evolution of excitonic modes in semiconductors". United States. https://doi.org/10.1103/physrevb.101.035203. https://www.osti.gov/servlets/purl/1604932.
@article{osti_1604932,
title = {Ultrafast nonequilibrium evolution of excitonic modes in semiconductors},
author = {Murakami, Yuta and Schüler, Michael and Takayoshi, Shintaro and Werner, Philipp},
abstractNote = {We study the time evolution of excitonic states after photoexcitation in the one-dimensional spinless extended Falicov-Kimball model. Several numerical methods are employed and benchmarked against each other: time-dependent mean-field simulations, the second-Born approximation (2BA) within the Kadanoff-Baym formalism, the generalized Kadanoff-Baym ansatz (GKBA) implemented with the 2BA, and the infinite time-evolving block decimation (iTEBD) method. It is found that the GKBA gives the best agreement with iTEBD and captures the relevant physics. Excitations to the particle-hole continuum and resonant excitations of the equilibrium exciton result in a qualitatively different dynamics. In the former case, the exciton binding energy remains positive and the frequency of the corresponding coherent oscillations is smaller than the band gap. On the other hand, resonant excitations trigger a collective mode whose frequency is larger than the band gap. We discuss the origin of these different behaviors by evaluating the nonequilibrium susceptibility using the nonthermal distribution and a random phase approximation. We note the peculiar mode with frequency larger than the band gap is associated with a partial population inversion with a sharp energy cutoff. We also discuss the effects of the cooling by a phonon bath. We demonstrate the real-time development of coherence in the polarization, which indicates excitonic condensation out of equilibrium.},
doi = {10.1103/physrevb.101.035203},
journal = {Physical Review B},
number = 3,
volume = 101,
place = {United States},
year = {Tue Jan 28 00:00:00 EST 2020},
month = {Tue Jan 28 00:00:00 EST 2020}
}

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Works referenced in this record:

Exciton Band Structure in Two-Dimensional Materials
journal, February 2016


Analytical approach to excitonic properties of MoS 2
journal, March 2014


Excitons in nanoscale systems
journal, September 2006

  • Scholes, Gregory D.; Rumbles, Garry
  • Nature Materials, Vol. 5, Issue 9
  • DOI: 10.1038/nmat1710

Photoinduced gap closure in an excitonic insulator
journal, July 2016


Excitonic Insulator State in Ta 2 NiSe 5 Probed by Photoemission Spectroscopy
journal, July 2009


Non-stationary excitonic-insulator states in photoexcited semiconductors
journal, June 1993

  • �streich, Th.; Sch�nhammer, K.
  • Zeitschrift f�r Physik B Condensed Matter, Vol. 91, Issue 2
  • DOI: 10.1007/BF01315235

Enhancement of superexchange pairing in the periodically driven Hubbard model
journal, August 2017


Exciton-Photon Strong-Coupling Regime for a Single Quantum Dot Embedded in a Microcavity
journal, August 2005


High-harmonic generation in quantum spin systems
journal, May 2019


Ultrafast Charge Separation and Indirect Exciton Formation in a MoS 2 –MoSe 2 van der Waals Heterostructure
journal, November 2014

  • Ceballos, Frank; Bellus, Matthew Z.; Chiu, Hsin-Ying
  • ACS Nano, Vol. 8, Issue 12
  • DOI: 10.1021/nn505736z

Ab Initio Calculation of Excitonic Effects in the Optical Spectra of Semiconductors
journal, May 1998


Nonequilibrium Quantum Condensation in an Incoherently Pumped Dissipative System
journal, June 2006


Real-time approach to the optical properties of solids and nanostructures: Time-dependent Bethe-Salpeter equation
journal, December 2011


Valley-selective optical Stark effect in monolayer WS2
journal, December 2014

  • Sie, Edbert J.; McIver, James W.; Lee, Yi-Hsien
  • Nature Materials, Vol. 14, Issue 3
  • DOI: 10.1038/nmat4156

Organic Optoelectronic Materials: Mechanisms and Applications
journal, October 2016


Pump-driven normal-to-excitonic insulator transition: Josephson oscillations and signatures of BEC-BCS crossover in time-resolved ARPES
journal, December 2019


Pulse excitation to continuous-wave excitation in a low-dimensional interacting quantum system
journal, September 2016


2D materials and van der Waals heterostructures
journal, July 2016


An ab-initio approach to describe coherent and non-coherent exciton dynamics
journal, August 2018

  • Sangalli, Davide; Perfetto, Enrico; Stefanucci, Gianluca
  • The European Physical Journal B, Vol. 91, Issue 8
  • DOI: 10.1140/epjb/e2018-90126-5

Excitonic Phases
journal, August 1967


Photo-induced semimetallic states realised in electron–hole coupled insulators
journal, October 2018


Relaxation of Antiferromagnetic Order in Spin- 1 / 2 Chains Following a Quantum Quench
journal, April 2009


Multiple amplitude modes in strongly coupled phonon-mediated superconductors
journal, March 2016


Zero-gap semiconductor to excitonic insulator transition in Ta2NiSe5
journal, February 2017

  • Lu, Y. F.; Kono, H.; Larkin, T. I.
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms14408

First-principles approach to excitons in time-resolved and angle-resolved photoemission spectra
journal, December 2016


Dynamic Stark effect in interacting electron-hole systems: Light-enhanced excitons
journal, November 1986


Classical Simulation of Infinite-Size Quantum Lattice Systems in One Spatial Dimension
journal, February 2007


Charge-separation energy in films of π-conjugated organic molecules
journal, September 2000


Transition Metal Chalcogenides: Ultrathin Inorganic Materials with Tunable Electronic Properties
journal, December 2014

  • Heine, Thomas
  • Accounts of Chemical Research, Vol. 48, Issue 1
  • DOI: 10.1021/ar500277z

Nonequilibrium Many-Body Theory of Quantum Systems
book, March 2013


Orthorhombic-to-monoclinic phase transition of Ta 2 NiSe 5 induced by the Bose-Einstein condensation of excitons
journal, January 2013


Two-photon absorption in two-dimensional materials: The case of hexagonal boron nitride
journal, October 2018


Photoinduced Enhancement of Excitonic Order
journal, December 2017


Optical suppression of electron motion in low-dimensional correlated electron system
journal, February 2017


Excitonic Insulator
journal, June 1967


Generalized Kadanoff-Baym ansatz for deriving quantum transport equations
journal, November 1986


Cavity Control of Excitons in Two-Dimensional Materials
journal, May 2019


Semiconductor excitons in new light
journal, July 2006

  • Koch, S. W.; Kira, M.; Khitrova, G.
  • Nature Materials, Vol. 5, Issue 7
  • DOI: 10.1038/nmat1658

Charge Separation in Donor–C 60 Complexes with Real-Time Green Functions: The Importance of Nonlocal Correlations
journal, January 2018


Tightly Bound Excitons in Monolayer WSe 2
journal, July 2014


Quench dynamics and Hall response of interacting Chern insulators
journal, July 2019


Strong Light-Matter Interactions in Heterostructures of Atomically Thin Films
journal, May 2013


Nonequilibrium dynamical mean-field theory and its applications
journal, June 2014


Collective Strong Light-Matter Coupling in Hierarchical Microcavity-Plasmon-Exciton Systems
journal, November 2018


Evidence for an Excitonic Insulator Phase in 1 T TiSe 2
journal, October 2007


Two-dimensional atomic crystals
journal, July 2005

  • Novoselov, K. S.; Jiang, D.; Schedin, F.
  • Proceedings of the National Academy of Sciences, Vol. 102, Issue 30, p. 10451-10453
  • DOI: 10.1073/pnas.0502848102

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

Light-Driven Electron-Hole Bardeen-Cooper-Schrieffer-Like State in Bulk GaAs
journal, November 2019


Temporal decay of Néel order in the one-dimensional Fermi-Hubbard model
journal, May 2015


Ultrafast Electronic Band Gap Control in an Excitonic Insulator
journal, August 2017


Electron-Hole Excitations in Semiconductors and Insulators
journal, September 1998


Quantum kinetics regime during and immediately after laser excitation of semiconductors
journal, August 1997


Magnetization and phase transition induced by circularly polarized laser in quantum magnets
journal, August 2014


Nonequilibrium dynamics in the pump-probe spectroscopy of excitonic insulators
journal, December 2018


Single-layer MoS2 transistors
journal, January 2011

  • Radisavljevic, B.; Radenovic, A.; Brivio, J.
  • Nature Nanotechnology, Vol. 6, Issue 3, p. 147-150
  • DOI: 10.1038/nnano.2010.279

Beyond the quasiparticle approximation: Fully self-consistent G W calculations
journal, October 2018


Coherent ultrafast charge transfer in an organic photovoltaic blend
journal, May 2014


Time-domain classification of charge-density-wave insulators
journal, January 2012

  • Hellmann, S.; Rohwer, T.; Kalläne, M.
  • Nature Communications, Vol. 3, Issue 1
  • DOI: 10.1038/ncomms2078

Photoinduced enhancement of excitonic order in the two-orbital Hubbard model
journal, March 2018


Exciton–LO-Phonon Quantum Kinetics: Evidence of Memory Effects in Bulk GaAs
journal, September 1995


Damping of the collective amplitude mode in superconductors with strong electron-phonon coupling
journal, September 2016