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Title: Excitonic effects in two-dimensional semiconductors: Path integral Monte Carlo approach

Abstract

The most striking features of novel two-dimensional semiconductors (e.g., transition metal dichalcogenide monolayers or phosphorene) is a strong Coulomb interaction between charge carriers resulting in large excitonic effects. In particular, this leads to the formation of multicarrier bound states upon photoexcitation (e.g., excitons, trions, and biexcitons), which could remain stable at near-room temperatures and contribute significantly to the optical properties of such materials. In our work we have used the path integral Monte Carlo methodology to numerically study properties of multicarrier bound states in two-dimensional semiconductors. Specifically, we have accurately investigated and tabulated the dependence of single-exciton, trion, and biexciton binding energies on the strength of dielectric screening, including the limiting cases of very strong and very weak screening. Our results of this work are potentially useful in the analysis of experimental data and benchmarking of theoretical and computational models.

Authors:
 [1];  [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Advanced Solar Photophysics (CASP)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1240611
Alternate Identifier(s):
OSTI ID: 1225760
Report Number(s):
LA-UR-15-23355
Journal ID: ISSN 1098-0121; PRBMDO
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review. B, Condensed Matter and Materials Physics
Additional Journal Information:
Journal Volume: 92; Journal Issue: 19; Journal ID: ISSN 1098-0121
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; Material Science; 2D semiconductor, exciton, trion, biexciton, quantum monte carlo

Citation Formats

Velizhanin, Kirill A., and Saxena, Avadh. Excitonic effects in two-dimensional semiconductors: Path integral Monte Carlo approach. United States: N. p., 2015. Web. doi:10.1103/PhysRevB.92.195305.
Velizhanin, Kirill A., & Saxena, Avadh. Excitonic effects in two-dimensional semiconductors: Path integral Monte Carlo approach. United States. doi:https://doi.org/10.1103/PhysRevB.92.195305
Velizhanin, Kirill A., and Saxena, Avadh. Wed . "Excitonic effects in two-dimensional semiconductors: Path integral Monte Carlo approach". United States. doi:https://doi.org/10.1103/PhysRevB.92.195305. https://www.osti.gov/servlets/purl/1240611.
@article{osti_1240611,
title = {Excitonic effects in two-dimensional semiconductors: Path integral Monte Carlo approach},
author = {Velizhanin, Kirill A. and Saxena, Avadh},
abstractNote = {The most striking features of novel two-dimensional semiconductors (e.g., transition metal dichalcogenide monolayers or phosphorene) is a strong Coulomb interaction between charge carriers resulting in large excitonic effects. In particular, this leads to the formation of multicarrier bound states upon photoexcitation (e.g., excitons, trions, and biexcitons), which could remain stable at near-room temperatures and contribute significantly to the optical properties of such materials. In our work we have used the path integral Monte Carlo methodology to numerically study properties of multicarrier bound states in two-dimensional semiconductors. Specifically, we have accurately investigated and tabulated the dependence of single-exciton, trion, and biexciton binding energies on the strength of dielectric screening, including the limiting cases of very strong and very weak screening. Our results of this work are potentially useful in the analysis of experimental data and benchmarking of theoretical and computational models.},
doi = {10.1103/PhysRevB.92.195305},
journal = {Physical Review. B, Condensed Matter and Materials Physics},
number = 19,
volume = 92,
place = {United States},
year = {2015},
month = {11}
}

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Cited by: 19 works
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Works referenced in this record:

Graphene, related two-dimensional crystals, and hybrid systems for energy conversion and storage
journal, January 2015


Progress, Challenges, and Opportunities in Two-Dimensional Materials Beyond Graphene
journal, March 2013

  • Butler, Sheneve Z.; Hollen, Shawna M.; Cao, Linyou
  • ACS Nano, Vol. 7, Issue 4, p. 2898-2926
  • DOI: 10.1021/nn400280c

2D materials: to graphene and beyond
journal, January 2011

  • Mas-Ballesté, Rubén; Gómez-Navarro, Cristina; Gómez-Herrero, Julio
  • Nanoscale, Vol. 3, Issue 1
  • DOI: 10.1039/C0NR00323A

An atlas of two-dimensional materials
journal, January 2014

  • Miró, Pere; Audiffred, Martha; Heine, Thomas
  • Chem. Soc. Rev., Vol. 43, Issue 18
  • DOI: 10.1039/C4CS00102H

Condensed-Matter Simulation of a Three-Dimensional Anomaly
journal, December 1984


Drawing conclusions from graphene
journal, November 2006


Two-dimensional material nanophotonics
journal, November 2014


Emerging Device Applications for Semiconducting Two-Dimensional Transition Metal Dichalcogenides
journal, January 2014

  • Jariwala, Deep; Sangwan, Vinod K.; Lauhon, Lincoln J.
  • ACS Nano, Vol. 8, Issue 2
  • DOI: 10.1021/nn500064s

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


A roadmap for graphene
journal, October 2012

  • Novoselov, K. S.; Fal′ko, V. I.; Colombo, L.
  • Nature, Vol. 490, Issue 7419
  • DOI: 10.1038/nature11458

Atomically Thin MoS2 A New Direct-Gap Semiconductor
journal, September 2010


Emerging Photoluminescence in Monolayer MoS2
journal, April 2010

  • Splendiani, Andrea; Sun, Liang; Zhang, Yuanbo
  • Nano Letters, Vol. 10, Issue 4, p. 1271-1275
  • DOI: 10.1021/nl903868w

Phosphorene: An Unexplored 2D Semiconductor with a High Hole Mobility
journal, March 2014

  • Liu, Han; Neal, Adam T.; Zhu, Zhen
  • ACS Nano, Vol. 8, Issue 4
  • DOI: 10.1021/nn501226z

Black phosphorus field-effect transistors
journal, March 2014


Effective-mass theory for the anisotropic exciton in two-dimensional crystals: Application to phosphorene
journal, June 2015


Exciton binding energies and luminescence of phosphorene under pressure
journal, March 2015


Large-Gap Quantum Spin Hall Insulators in Tin Films
journal, September 2013


Elemental Analogues of Graphene: Silicene, Germanene, Stanene, and Phosphorene
journal, November 2014


Excitons in ultrathin organic-inorganic perovskite crystals
journal, July 2015


Probing excitonic dark states in single-layer tungsten disulphide
journal, August 2014

  • Ye, Ziliang; Cao, Ting; O’Brien, Kevin
  • Nature, Vol. 513, Issue 7517
  • DOI: 10.1038/nature13734

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


Theory of neutral and charged excitons in monolayer transition metal dichalcogenides
journal, July 2013

  • Berkelbach, Timothy C.; Hybertsen, Mark S.; Reichman, David R.
  • Physical Review B, Vol. 88, Issue 4
  • DOI: 10.1103/PhysRevB.88.045318

Large excitonic effects in monolayers of molybdenum and tungsten dichalcogenides
journal, September 2012


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

Tightly Bound Excitons in Monolayer WSe 2
journal, July 2014


Molecules in flatland
journal, June 2015


Electrical control of neutral and charged excitons in a monolayer semiconductor
journal, February 2013

  • Ross, Jason S.; Wu, Sanfeng; Yu, Hongyi
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms2498

Tightly bound trions in monolayer MoS2
journal, December 2012

  • Mak, Kin Fai; He, Keliang; Lee, Changgu
  • Nature Materials, Vol. 12, Issue 3
  • DOI: 10.1038/nmat3505

Optical manipulation of the exciton charge state in single-layer tungsten disulfide
journal, December 2013


Dielectric Screening of Excitons and Trions in Single-Layer MoS 2
journal, September 2014

  • Lin, Yuxuan; Ling, Xi; Yu, Lili
  • Nano Letters, Vol. 14, Issue 10
  • DOI: 10.1021/nl501988y

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

Observation of Excitonic Fine Structure in a 2D Transition-Metal Dichalcogenide Semiconductor
journal, January 2015

  • Shang, Jingzhi; Shen, Xiaonan; Cong, Chunxiao
  • ACS Nano, Vol. 9, Issue 1
  • DOI: 10.1021/nn5059908

Observation of biexcitons in monolayer WSe2
journal, May 2015

  • You, Yumeng; Zhang, Xiao-Xiao; Berkelbach, Timothy C.
  • Nature Physics, Vol. 11, Issue 6
  • DOI: 10.1038/nphys3324

Quasiparticle band structure calculation of monolayer, bilayer, and bulk MoS 2
journal, May 2012


Optical Spectrum of MoS 2 : Many-Body Effects and Diversity of Exciton States
journal, November 2013


Quasiparticle band structures and optical properties of strained monolayer MoS 2 and WS 2
journal, April 2013


Probing excitonic states in suspended two-dimensional semiconductors by photocurrent spectroscopy
journal, October 2014

  • Klots, A. R.; Newaz, A. K. M.; Wang, Bin
  • Scientific Reports, Vol. 4, Issue 1
  • DOI: 10.1038/srep06608

Linear Scaling of the Exciton Binding Energy versus the Band Gap of Two-Dimensional Materials
journal, August 2015


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


Absorption of light by excitons and trions in monolayers of metal dichalcogenide Mo S 2 : Experiments and theory
journal, May 2014


Exciton complexes in low dimensional transition metal dichalcogenides
journal, August 2014


Time-dependent density-matrix functional theory for trion excitations: Application to monolayer MoS 2 and other transition-metal dichalcogenides
journal, August 2014

  • Ramirez-Torres, Alfredo; Turkowski, Volodymyr; Rahman, Talat S.
  • Physical Review B, Vol. 90, Issue 8
  • DOI: 10.1103/PhysRevB.90.085419

Three-Particle Complexes in Two-Dimensional Semiconductors
journal, March 2015


Path integrals in the theory of condensed helium
journal, April 1995


Introduction to the diffusion Monte Carlo method
journal, May 1996

  • Kosztin, Ioan; Faber, Byron; Schulten, Klaus
  • American Journal of Physics, Vol. 64, Issue 5
  • DOI: 10.1119/1.18168

Variational quantum Monte Carlo study of charged excitons in fractional dimensional space
journal, July 2011


Order-Disorder Transition in Nanoscopic Semiconductor Quantum Rings
journal, April 2001


First principles approach to binding energies of excitons, trions and biexcitons in quantum wells
journal, August 2003

  • Filinov, A. V.; Bonitz, M.; Lozovik, Yu. E.
  • physica status solidi (c), Vol. 0, Issue 5
  • DOI: 10.1002/pssc.200303197

Monte Carlo simulations of dense quantum plasmas
journal, April 2006

  • Filinov, V. S.; Bonitz, M.; Fortov, V. E.
  • Journal of Physics A: Mathematical and General, Vol. 39, Issue 17
  • DOI: 10.1088/0305-4470/39/17/S17

Tuning biexciton binding and antibinding in core/shell quantum dots
journal, September 2012


Dielectric screening in two-dimensional insulators: Implications for excitonic and impurity states in graphane
journal, August 2011


Stability of four-body systems in three and two dimensions: A theoretical and quantum Monte Carlo study of biexciton molecules
journal, June 1998


Binding Energy of Biexcitons in Two-Dimensional Semiconductors
journal, August 1998


Singlet and triplet states of X + and X - trions in two-dimensional quantum wells
journal, November 2001


Universal estimation of X- trion binding energy in semiconductor quantum wells
journal, October 2005


Trion ground state, excited states, and absorption spectrum using electron-exciton basis
journal, September 2012


Electronic structure and absorption spectrum of biexciton obtained by using exciton basis
journal, September 2013


Binding energy of two-dimensional biexcitons
journal, June 1996


Ground state energy and optical absorption of excitonic trions in two dimensional semiconductors
journal, January 1989


Two-dimensional charged-exciton complexes
journal, March 1997


Stability of two- and three-dimensional excitonic complexes
journal, February 1999


Exciton energy levels in thin semiconductor films
journal, February 1982


Equation of State Calculations by Fast Computing Machines
journal, June 1953

  • Metropolis, Nicholas; Rosenbluth, Arianna W.; Rosenbluth, Marshall N.
  • The Journal of Chemical Physics, Vol. 21, Issue 6
  • DOI: 10.1063/1.1699114

Circumventing the pathological behavior of path-integral Monte Carlo for systems with Coulomb potentials
journal, July 1997

  • Müser, M. H.; Berne, B. J.
  • The Journal of Chemical Physics, Vol. 107, Issue 2
  • DOI: 10.1063/1.474442

Energy-consistent pseudopotentials for quantum Monte Carlo calculations
journal, June 2007

  • Burkatzki, M.; Filippi, C.; Dolg, M.
  • The Journal of Chemical Physics, Vol. 126, Issue 23
  • DOI: 10.1063/1.2741534

Computational Complexity and Fundamental Limitations to Fermionic Quantum Monte Carlo Simulations
journal, May 2005


Solving the fermion sign problem in quantum Monte Carlo simulations by Majorana representation
journal, June 2015


Spin and pseudospins in layered transition metal dichalcogenides
journal, April 2014

  • Xu, Xiaodong; Yao, Wang; Xiao, Di
  • Nature Physics, Vol. 10, Issue 5
  • DOI: 10.1038/nphys2942

Band Edge Structure of PbS, PbSe, and PbTe
journal, August 1964


Theoretical Energy-Band Parameters for the Lead Salts
journal, November 1966


Electronic structure and optical properties of PbS and PbSe quantum dots
journal, January 1997

  • Kang, Inuk; Wise, Frank W.
  • Journal of the Optical Society of America B, Vol. 14, Issue 7
  • DOI: 10.1364/JOSAB.14.001632

Experimental Proof of the Existence of a New Electronic Complex in Silicon
journal, April 1960


Trions in semiconducting single-walled carbon nanotubes
journal, January 2012


Biexciton, single carrier, and trion generation dynamics in single-walled carbon nanotubes
journal, May 2013


Relative stability of excitonic complexes in quasi-one-dimensional semiconductors
journal, December 2014


Monolayer MoS 2 : Trigonal warping, the Γ valley, and spin-orbit coupling effects
journal, July 2013


k · p theory for two-dimensional transition metal dichalcogenide semiconductors
journal, April 2015


Mobility engineering and a metal–insulator transition in monolayer MoS2
journal, June 2013

  • Radisavljevic, Branimir; Kis, Andras
  • Nature Materials, Vol. 12, Issue 9
  • DOI: 10.1038/nmat3687

Optical properties of cubic hafnia stabilized with yttria
journal, January 1990

  • Wood, D. L.; Nassau, Kurt; Kometani, T. Y.
  • Applied Optics, Vol. 29, Issue 4, p. 604-607
  • DOI: 10.1364/AO.29.000604

Simulation of excited states and the sign problem in the path integral Monte Carlo method
journal, July 2005


Highly efficient carrier multiplication in PbS nanosheets
journal, April 2014

  • Aerts, Michiel; Bielewicz, Thomas; Klinke, Christian
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4789

Tailoring the Height of Ultrathin PbS Nanosheets and Their Application as Field-Effect Transistors
journal, October 2014


Relativistic quasiparticle self-consistent electronic structure of hybrid halide perovskite photovoltaic absorbers
journal, April 2014


Halide perovskite materials for solar cells: a theoretical review
journal, January 2015

  • Yin, Wan-Jian; Yang, Ji-Hui; Kang, Joongoo
  • Journal of Materials Chemistry A, Vol. 3, Issue 17
  • DOI: 10.1039/C4TA05033A

    Works referencing / citing this record:

    Many-Body Complexes in 2D Semiconductors
    journal, August 2018


    Theory and Ab Initio Calculation of Optically Excited States—Recent Advances in 2D Materials
    journal, December 2019


    Trion and Biexciton in Monolayer Transition Metal Dichalcogenides
    journal, December 2016


    Few-Body Systems in Condensed Matter Physics
    journal, July 2019


    Exciton diamagnetic shifts and valley Zeeman effects in monolayer WS2 and MoS2 to 65 Tesla
    journal, February 2016

    • Stier, Andreas V.; McCreary, Kathleen M.; Jonker, Berend T.
    • Nature Communications, Vol. 7, Issue 1
    • DOI: 10.1038/ncomms10643

    Room temperature observation of biexcitons in exfoliated WS 2 monolayers
    journal, May 2017

    • Paradisanos, I.; Germanis, S.; Pelekanos, N. T.
    • Applied Physics Letters, Vol. 110, Issue 19
    • DOI: 10.1063/1.4983285

    Optical absorption by indirect excitons in a transition metal dichalcogenide/hexagonal boron nitride heterostructure
    journal, May 2018

    • Brunetti, Matthew N.; Berman, Oleg L.; Kezerashvili, Roman Ya
    • Journal of Physics: Condensed Matter, Vol. 30, Issue 22
    • DOI: 10.1088/1361-648x/aabe53

    Dynamical screening in monolayer transition-metal dichalcogenides and its manifestations in the exciton spectrum
    journal, March 2019

    • Scharf, Benedikt; Van Tuan, Dinh; Žutić, Igor
    • Journal of Physics: Condensed Matter, Vol. 31, Issue 20
    • DOI: 10.1088/1361-648x/ab071f

    Trions in bulk and monolayer materials: Faddeev equations and hyperspherical harmonics
    journal, February 2018


    Binding energies and structures of two-dimensional excitonic complexes in transition metal dichalcogenides
    journal, March 2016


    Excitons and optical spectra of phosphorene nanoribbons
    journal, July 2016


    Many-body theory of trion absorption features in two-dimensional semiconductors
    journal, January 2017


    Superfluidity of dipolar excitons in a transition metal dichalcogenide double layer
    journal, September 2017


    Complexes of dipolar excitons in layered quasi-two-dimensional nanostructures
    journal, April 2018


    Coulomb interaction in monolayer transition-metal dichalcogenides
    journal, September 2018


    Marrying Excitons and Plasmons in Monolayer Transition-Metal Dichalcogenides
    journal, November 2017