Approaching the intrinsic photoluminescence linewidth in transition metal dichalcogenide monolayers

Ajayi, Obafunso A.; Ardelean, Jenny V.; Shepard, Gabriella D.; Wang, Jue; Antony, Abhinandan; Taniguchi, Takeshi; Watanabe, Kenji; Heinz, Tony F.; Strauf, Stefan; Zhu, X-Y; Hone, James C.

doi:10.1088/2053-1583/aa6aa1

Title: Approaching the intrinsic photoluminescence linewidth in transition metal dichalcogenide monolayers

Abstract

Excitonic states in monolayer transition metal dichalcogenides (TMDCs) have been the subject of extensive recent interest. Their intrinsic properties can, however, be obscured due to the influence of inhomogeneity in the external environment. Here we report methods for fabricating high quality TMDC monolayers with narrow photoluminescence (PL) linewidth approaching the intrinsic limit. We find that encapsulation in hexagonal boron nitride (h-BN) sharply reduces the PL linewidth, and that passivation of the oxide substrate by an alkyl monolayer further decreases the linewidth and also minimizes the charged exciton (trion) peak. The combination of these sample preparation methods results in much reduced spatial variation in the PL emission, with a full-width-at-half-maximum as low as 1.7 meV. Furthermore, analysis of the PL line shape yields a homogeneous width of 1.43 ± 0.08 meV and inhomogeneous broadening of 1.1 ± 0.3 meV.

Authors:

Ajayi, Obafunso A. ^[1]; Ardelean, Jenny V. ^[1]; Shepard, Gabriella D. ^[2]; Wang, Jue ^[1]; Antony, Abhinandan ^[1]; Taniguchi, Takeshi ^[3]; Watanabe, Kenji ^[3]; Heinz, Tony F. ^[4]; Strauf, Stefan ^[2]; Zhu, X-Y ^[1]; Hone, James C. ^[1]

Columbia Univ., New York, NY (United States)
Stevens Institute of Technology, Hoboken, NJ (United States)
National Institute for Materials Science, Tsukuba (Japan)
Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)

Publication Date:: Mon Jul 24 00:00:00 EDT 2017

Research Org.:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1374378

Grant/Contract Number:: AC02-76SF00515; DMR-1420634; ECCS-MRI-1531237; DMR-1608437; DMR-1506711

Resource Type:: Accepted Manuscript

Journal Name:: 2D Materials

Additional Journal Information:: Journal Volume: 4; Journal Issue: 3; Journal ID: ISSN 2053-1583

Publisher:: IOP Publishing

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; transition metal dichalcogenides; photoluminescence; line width

Citation Formats


                    Ajayi, Obafunso A., Ardelean, Jenny V., Shepard, Gabriella D., Wang, Jue, Antony, Abhinandan, Taniguchi, Takeshi, Watanabe, Kenji, Heinz, Tony F., Strauf, Stefan, Zhu, X-Y, and Hone, James C. Approaching the intrinsic photoluminescence linewidth in transition metal dichalcogenide monolayers.  United States: N. p., 2017. 
Web.  doi:10.1088/2053-1583/aa6aa1.

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                    Ajayi, Obafunso A., Ardelean, Jenny V., Shepard, Gabriella D., Wang, Jue, Antony, Abhinandan, Taniguchi, Takeshi, Watanabe, Kenji, Heinz, Tony F., Strauf, Stefan, Zhu, X-Y, & Hone, James C. Approaching the intrinsic photoluminescence linewidth in transition metal dichalcogenide monolayers.  United States.  https://doi.org/10.1088/2053-1583/aa6aa1

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                    Ajayi, Obafunso A., Ardelean, Jenny V., Shepard, Gabriella D., Wang, Jue, Antony, Abhinandan, Taniguchi, Takeshi, Watanabe, Kenji, Heinz, Tony F., Strauf, Stefan, Zhu, X-Y, and Hone, James C. Mon .  
"Approaching the intrinsic photoluminescence linewidth in transition metal dichalcogenide monolayers".  United States.  https://doi.org/10.1088/2053-1583/aa6aa1.  https://www.osti.gov/servlets/purl/1374378.

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@article{osti_1374378,

  title        = {Approaching the intrinsic photoluminescence linewidth in transition metal dichalcogenide monolayers},

  author       = {Ajayi, Obafunso A. and Ardelean, Jenny V. and Shepard, Gabriella D. and Wang, Jue and Antony, Abhinandan and Taniguchi, Takeshi and Watanabe, Kenji and Heinz, Tony F. and Strauf, Stefan and Zhu, X-Y and Hone, James C.},

  abstractNote = {Excitonic states in monolayer transition metal dichalcogenides (TMDCs) have been the subject of extensive recent interest. Their intrinsic properties can, however, be obscured due to the influence of inhomogeneity in the external environment. Here we report methods for fabricating high quality TMDC monolayers with narrow photoluminescence (PL) linewidth approaching the intrinsic limit. We find that encapsulation in hexagonal boron nitride (h-BN) sharply reduces the PL linewidth, and that passivation of the oxide substrate by an alkyl monolayer further decreases the linewidth and also minimizes the charged exciton (trion) peak. The combination of these sample preparation methods results in much reduced spatial variation in the PL emission, with a full-width-at-half-maximum as low as 1.7 meV. Furthermore, analysis of the PL line shape yields a homogeneous width of 1.43 ± 0.08 meV and inhomogeneous broadening of 1.1 ± 0.3 meV.},

  doi          = {10.1088/2053-1583/aa6aa1},

  journal      = {2D Materials},

  number       = 3,

  volume       = 4,

  place        = {United States},

  year         = {Mon Jul 24 00:00:00 EDT 2017},

  month        = {Mon Jul 24 00:00:00 EDT 2017}

}

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Dutta, Subhojit; Cai, Tao; Buyukkaya, Mustafa Atabey
arXiv
DOI: 10.48550/arxiv.1806.08973

Fundamental exciton linewidth broadening in monolayer transition metal dichalcogenides
text, January 2019

Gupta, Garima; Majumdar, Kausik
arXiv
DOI: 10.48550/arxiv.1901.04391

Controlling excitons in an atomically thin membrane with a mirror
text, January 2019

Zhou, You; Scuri, Giovanni; Sung, Jiho
arXiv
DOI: 10.48550/arxiv.1901.08500

Integration of Single Photon Emitters in 2D Layered Materials with a Silicon Nitride Photonic Chip
text, January 2019

Peyskens, Frédéric; Chakraborty, Chitraleema; Muneeb, Muhammad
arXiv
DOI: 10.48550/arxiv.1904.08841

Excitonic magneto-optics in monolayer transition metal dichalcogenides: From nanoribbons to two-dimensional response
text, January 2019

Have, J.; Peres, N. M. R.; Pedersen, T. G.
arXiv
DOI: 10.48550/arxiv.1905.06651

Exciton-polaritons in multilayer WSe$_2$ in a planar microcavity
text, January 2019

Król, M.; Rechcińska, K.; Nogajewski, K.
arXiv
DOI: 10.48550/arxiv.1908.05300

Magneto-optical Kerr effect in spin split two-dimensional massive Dirac materials
text, January 2019

Catarina, G.; Peres, N. M. R.; Fernández-Rossier, J.
arXiv
DOI: 10.48550/arxiv.1910.13371

Colloquium : Excitons in atomically thin transition metal dichalcogenides
text, January 2018

Wang, Gang; Chernikov, Alexey; Glazov, Mikhail M.
Universität Regensburg
DOI: 10.5283/epub.40518

Environmental Electrometry with Luminescent Carbon Nanotubes
journal, June 2018

Noé, Jonathan C.; Nutz, Manuel; Reschauer, Jonathan
Nano Letters, Vol. 18, Issue 7
DOI: 10.1021/acs.nanolett.8b00871

Two-dimensional semiconductors in the regime of strong light-matter coupling
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Schneider, Christian; Glazov, Mikhail M.; Korn, Tobias
arXiv
DOI: 10.48550/arxiv.1804.06771

Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields
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Goryca, M.; Li, J.; Stier, A. V.
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DOI: 10.48550/arxiv.1904.03238

Cavity-control of interlayer excitons in van der Waals heterostructures
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Förg, Michael; Colombier, Léo; Patel, Robin K.
Karlsruhe
DOI: 10.5445/ir/1000097945

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Title: Approaching the intrinsic photoluminescence linewidth in transition metal dichalcogenide monolayers

Abstract

Citation Formats

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

Tightly Bound Excitons in Monolayer WSe 2 journal, July 2014

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

Tightly bound trions in monolayer MoS2 journal, December 2012

Control of valley polarization in monolayer MoS2 by optical helicity journal, June 2012

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

Strong light–matter coupling in two-dimensional atomic crystals journal, December 2014

Enhanced radiative recombination of free excitons in GaAs quantum wells journal, October 1991

Exciton dynamics in GaAs quantum wells under resonant excitation journal, October 1994

Prolonged spontaneous emission and dephasing of localized excitons in air-bridged carbon nanotubes journal, July 2013

Engineering Bandgaps of Monolayer MoS 2 and WS 2 on Fluoropolymer Substrates by Electrostatically Tuned Many-Body Effects journal, May 2016

Radiatively Limited Dephasing and Exciton Dynamics in MoSe 2 Monolayers Revealed with Four-Wave Mixing Microscopy journal, August 2016

Optical Coherence in Atomic-Monolayer Transition-Metal Dichalcogenides Limited by Electron-Phonon Interactions journal, March 2016

Homogeneous linewidth broadening and exciton dephasing mechanism in MoT e 2 journal, February 2016

Intrinsic homogeneous linewidth and broadening mechanisms of excitons in monolayer transition metal dichalcogenides journal, September 2015

Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides journal, November 2016

Exciton Radiative Lifetimes in Two-Dimensional Transition Metal Dichalcogenides journal, March 2015

Exciton radiative lifetime in transition metal dichalcogenide monolayers journal, May 2016

Radiative lifetimes of excitons and trions in monolayers of the metal dichalcogenide MoS 2 journal, January 2016

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

Boron nitride substrates for high-quality graphene electronics journal, August 2010

One-Dimensional Electrical Contact to a Two-Dimensional Material journal, October 2013

Highly Stable, Dual-Gated MoS 2 Transistors Encapsulated by Hexagonal Boron Nitride with Gate-Controllable Contact, Resistance, and Threshold Voltage journal, June 2015

General observation of n-type field-effect behaviour in organic semiconductors journal, March 2005

Reliable Exfoliation of Large-Area High-Quality Flakes of Graphene and Other Two-Dimensional Materials journal, September 2015

Strain tuning of optical emission energy and polarization in monolayer and bilayer MoS 2 journal, September 2013

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

Precise and reversible band gap tuning in single-layer MoSe 2 by uniaxial strain journal, January 2016

Phonon softening and direct to indirect band gap crossover in strained single-layer MoSe 2 journal, March 2013

Charge Transfer Excitons at van der Waals Interfaces journal, June 2015

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

Valley-polarized exciton dynamics in a 2D semiconductor heterostructure journal, February 2016

Isospin Pomeranchuk effect in twisted bilayer graphene journal, April 2021

Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides conference, February 2017

Prolonged spontaneous emission and dephasing of localized excitons in air-bridged carbon nanotubes text, January 2013

Probing Excitonic Dark States in Single-layer Tungsten Disulfide text, January 2014

Exciton Radiative Lifetime in Transition Metal Dichalcogenide Monolayers text, January 2016

Effect of Dielectric Environment on Excitonic Dynamics in Monolayer WS 2 journal, September 2019

Refractive Index Dispersion of Hexagonal Boron Nitride in the Visible and Near‐Infrared journal, October 2018

Two-dimensional semiconductors in the regime of strong light-matter coupling journal, July 2018

Efficient generation of neutral and charged biexcitons in encapsulated WSe2 monolayers journal, September 2018

Site-selectively generated photon emitters in monolayer MoS2 via local helium ion irradiation journal, June 2019

Cavity-control of interlayer excitons in van der Waals heterostructures journal, August 2019

Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields journal, September 2019

Integration of single photon emitters in 2D layered materials with a silicon nitride photonic chip journal, September 2019

Disorder in van der Waals heterostructures of 2D materials journal, May 2019

Nano-imaging of intersubband transitions in van der Waals quantum wells journal, August 2018

Deterministic coupling of site-controlled quantum emitters in monolayer WSe2 to plasmonic nanocavities journal, October 2018

Spin-polarized electrons in monolayer MoS2 journal, March 2019

Dielectric disorder in two-dimensional materials journal, August 2019

Direct exciton emission from atomically thin transition metal dichalcogenide heterostructures near the lifetime limit journal, September 2017

Exciton physics and device application of two-dimensional transition metal dichalcogenide semiconductors journal, September 2018

Chemical synthesis of two-dimensional atomic crystals, heterostructures and superlattices journal, January 2018

Negative effective excitonic diffusion in monolayer transition metal dichalcogenides journal, January 2020

Substrate-induced strain and charge doping in CVD-grown monolayer MoS 2 journal, October 2017

Impact of photodoping on inter- and intralayer exciton emission in a MoS 2 /MoSe 2 /MoS 2 heterostructure journal, August 2018

Coupling quantum emitters in WSe 2 monolayers to a metal-insulator-metal waveguide journal, November 2018

Band evolution of two-dimensional transition metal dichalcogenides under electric fields journal, August 2019

Atomic-scale defects and electronic properties of a transferred synthesized MoS 2 monolayer journal, May 2018

Impact of environment on dynamics of exciton complexes in a WS 2 monolayer journal, April 2018

Zeeman spectroscopy of excitons and hybridization of electronic states in few-layer WSe 2 , MoSe 2 and MoTe 2 journal, November 2018

Chemical and structural stability of 2D layered materials journal, July 2019

Dynamics of cleaning, passivating and doping monolayer MoS 2 by controlled laser irradiation journal, August 2019

Exciton-polaritons in multilayer WSe 2 in a planar microcavity journal, October 2019

High optical quality of MoS 2 monolayers grown by chemical vapor deposition journal, November 2019

Magnetic field mixing and splitting of bright and dark excitons in monolayer MoSe 2 journal, November 2019

Magneto-optical Kerr effect in spin split two-dimensional massive Dirac materials journal, January 2020

Excitonic magneto-optics in monolayer transition metal dichalcogenides: From nanoribbons to two-dimensional response journal, July 2019

Exciton broadening in WS 2 /graphene heterostructures journal, November 2017

Fundamental exciton linewidth broadening in monolayer transition metal dichalcogenides journal, February 2019

Bright Luminescence from Indirect and Strongly Bound Excitons in h-BN journal, February 2019

Engineering of optical and electronic band gaps in transition metal dichalcogenide monolayers through external dielectric screening journal, October 2017

Exciton States in Monolayer MoSe 2 and MoTe 2 Probed by Upconversion Spectroscopy journal, September 2018

Heterogeneous Integration of 2D Materials: Recent Advances in Fabrication and Functional Device Applications journal, December 2019

Enhanced two-photon absorption and two-photon luminescence in monolayer MoS 2 and WS 2 by defect repairing journal, January 2019

Exciton broadening in WS2 /graphene heterostructures text, January 2017

Cavity-control of interlayer excitons in van der Waals heterostructures text, January 2019

Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer ${WS}_{2}$
journal, August 2014

Tightly Bound Excitons in Monolayer ${WSe}_{2}$
journal, July 2014

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

Tightly bound trions in monolayer MoS2
journal, December 2012

Control of valley polarization in monolayer MoS2 by optical helicity
journal, June 2012

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

Strong light–matter coupling in two-dimensional atomic crystals
journal, December 2014

Enhanced radiative recombination of free excitons in GaAs quantum wells
journal, October 1991

Exciton dynamics in GaAs quantum wells under resonant excitation
journal, October 1994

Prolonged spontaneous emission and dephasing of localized excitons in air-bridged carbon nanotubes
journal, July 2013

Engineering Bandgaps of Monolayer MoS ₂ and WS ₂ on Fluoropolymer Substrates by Electrostatically Tuned Many-Body Effects
journal, May 2016

Radiatively Limited Dephasing and Exciton Dynamics in MoSe ₂ Monolayers Revealed with Four-Wave Mixing Microscopy
journal, August 2016

Optical Coherence in Atomic-Monolayer Transition-Metal Dichalcogenides Limited by Electron-Phonon Interactions
journal, March 2016

Homogeneous linewidth broadening and exciton dephasing mechanism in $MoT e_{2}$
journal, February 2016

Intrinsic homogeneous linewidth and broadening mechanisms of excitons in monolayer transition metal dichalcogenides
journal, September 2015

Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides
journal, November 2016

Exciton Radiative Lifetimes in Two-Dimensional Transition Metal Dichalcogenides
journal, March 2015

Exciton radiative lifetime in transition metal dichalcogenide monolayers
journal, May 2016

Radiative lifetimes of excitons and trions in monolayers of the metal dichalcogenide ${MoS}_{2}$
journal, January 2016

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

Boron nitride substrates for high-quality graphene electronics
journal, August 2010

One-Dimensional Electrical Contact to a Two-Dimensional Material
journal, October 2013

Highly Stable, Dual-Gated MoS ₂ Transistors Encapsulated by Hexagonal Boron Nitride with Gate-Controllable Contact, Resistance, and Threshold Voltage
journal, June 2015

General observation of n-type field-effect behaviour in organic semiconductors
journal, March 2005

Reliable Exfoliation of Large-Area High-Quality Flakes of Graphene and Other Two-Dimensional Materials
journal, September 2015

Strain tuning of optical emission energy and polarization in monolayer and bilayer MoS $_{2}$
journal, September 2013

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

Precise and reversible band gap tuning in single-layer MoSe ₂ by uniaxial strain
journal, January 2016

Phonon softening and direct to indirect band gap crossover in strained single-layer MoSe $_{2}$
journal, March 2013

Charge Transfer Excitons at van der Waals Interfaces
journal, June 2015

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

Valley-polarized exciton dynamics in a 2D semiconductor heterostructure
journal, February 2016

Isospin Pomeranchuk effect in twisted bilayer graphene
journal, April 2021

Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides
conference, February 2017

Prolonged spontaneous emission and dephasing of localized excitons in air-bridged carbon nanotubes
text, January 2013

Probing Excitonic Dark States in Single-layer Tungsten Disulfide
text, January 2014

Exciton Radiative Lifetime in Transition Metal Dichalcogenide Monolayers
text, January 2016

Effect of Dielectric Environment on Excitonic Dynamics in Monolayer WS ₂
journal, September 2019

Refractive Index Dispersion of Hexagonal Boron Nitride in the Visible and Near‐Infrared
journal, October 2018

Two-dimensional semiconductors in the regime of strong light-matter coupling
journal, July 2018

Efficient generation of neutral and charged biexcitons in encapsulated WSe2 monolayers
journal, September 2018

Site-selectively generated photon emitters in monolayer MoS2 via local helium ion irradiation
journal, June 2019

Cavity-control of interlayer excitons in van der Waals heterostructures
journal, August 2019

Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields
journal, September 2019

Integration of single photon emitters in 2D layered materials with a silicon nitride photonic chip
journal, September 2019

Disorder in van der Waals heterostructures of 2D materials
journal, May 2019

Nano-imaging of intersubband transitions in van der Waals quantum wells
journal, August 2018

Deterministic coupling of site-controlled quantum emitters in monolayer WSe2 to plasmonic nanocavities
journal, October 2018

Spin-polarized electrons in monolayer MoS2
journal, March 2019

Dielectric disorder in two-dimensional materials
journal, August 2019

Direct exciton emission from atomically thin transition metal dichalcogenide heterostructures near the lifetime limit
journal, September 2017

Exciton physics and device application of two-dimensional transition metal dichalcogenide semiconductors
journal, September 2018

Chemical synthesis of two-dimensional atomic crystals, heterostructures and superlattices
journal, January 2018

Negative effective excitonic diffusion in monolayer transition metal dichalcogenides
journal, January 2020

Substrate-induced strain and charge doping in CVD-grown monolayer MoS ₂
journal, October 2017

Impact of photodoping on inter- and intralayer exciton emission in a MoS ₂ /MoSe ₂ /MoS ₂ heterostructure
journal, August 2018

Coupling quantum emitters in WSe ₂ monolayers to a metal-insulator-metal waveguide
journal, November 2018

Band evolution of two-dimensional transition metal dichalcogenides under electric fields
journal, August 2019

Atomic-scale defects and electronic properties of a transferred synthesized MoS ₂ monolayer
journal, May 2018

Impact of environment on dynamics of exciton complexes in a WS ₂ monolayer
journal, April 2018

Zeeman spectroscopy of excitons and hybridization of electronic states in few-layer WSe ₂ , MoSe ₂ and MoTe ₂
journal, November 2018

Chemical and structural stability of 2D layered materials
journal, July 2019

Dynamics of cleaning, passivating and doping monolayer MoS ₂ by controlled laser irradiation
journal, August 2019

Exciton-polaritons in multilayer WSe ₂ in a planar microcavity
journal, October 2019

High optical quality of MoS ₂ monolayers grown by chemical vapor deposition
journal, November 2019

Magnetic field mixing and splitting of bright and dark excitons in monolayer MoSe ₂
journal, November 2019

Magneto-optical Kerr effect in spin split two-dimensional massive Dirac materials
journal, January 2020

Excitonic magneto-optics in monolayer transition metal dichalcogenides: From nanoribbons to two-dimensional response
journal, July 2019

Exciton broadening in ${WS}_{2}$ /graphene heterostructures
journal, November 2017

Fundamental exciton linewidth broadening in monolayer transition metal dichalcogenides
journal, February 2019

Bright Luminescence from Indirect and Strongly Bound Excitons in h-BN
journal, February 2019

Engineering of optical and electronic band gaps in transition metal dichalcogenide monolayers through external dielectric screening
journal, October 2017

Exciton States in Monolayer ${MoSe}_{2}$ and ${MoTe}_{2}$ Probed by Upconversion Spectroscopy
journal, September 2018

Heterogeneous Integration of 2D Materials: Recent Advances in Fabrication and Functional Device Applications
journal, December 2019

Enhanced two-photon absorption and two-photon luminescence in monolayer MoS ₂ and WS ₂ by defect repairing
journal, January 2019

Exciton broadening in WS2 /graphene heterostructures
text, January 2017

Cavity-control of interlayer excitons in van der Waals heterostructures
text, January 2019

Realization of an Electrically Tunable Narrow-Bandwidth Atomically Thin Mirror Using Monolayer MoSe2
text, January 2018

Zeeman Splitting and Inverted Polarization of Biexciton Emission in Monolayer WS2
text, January 2018

Direct exciton emission from atomically thin transition metal dichalcogenide heterostructures near the lifetime limit
text, January 2017