Valley phonons and exciton complexes in a monolayer semiconductor

He, Minhao; Rivera, Pasqual; Van Tuan, Dinh; Wilson, Nathan P.; Yang, Min; Taniguchi, Takashi; Watanabe, Kenji; Yan, Jiaqiang; Mandrus, David G.; Yu, Hongyi; Dery, Hanan; Yao, Wang; Xu, Xiaodong

doi:10.1038/s41467-020-14472-0

Title: Valley phonons and exciton complexes in a monolayer semiconductor

Abstract

The coupling between spin, charge, and lattice degrees of freedom plays an important role in a wide range of fundamental phenomena. Monolayer semiconducting transitional metal dichalcogenides have emerged as an outstanding platform for studying these coupling effects. Here, we report the observation of multiple valley phonons – phonons with momentum vectors pointing to the corners of the hexagonal Brillouin zone – and the resulting exciton complexes in the monolayer semiconductor WSe2. We find that these valley phonons lead to efficient intervalley scattering of quasi particles in both exciton formation and relaxation. This leads to a series of photoluminescence peaks as valley phonon replicas of dark trions. Using identified valley phonons, we also uncover an intervalley exciton near charge neutrality. Our work not only identifies a number of previously unknown 2D excitonic species, but also shows that monolayer WSe₂ is a prime candidate for studying interactions between spin, pseudospin, and zone-edge phonons.

Authors:

^[1];

^[1]; Van Tuan, Dinh ^[2]; Wilson, Nathan P. ^[1];

^[2]; Taniguchi, Takashi ^[3];

^[3]; Yan, Jiaqiang ^[4]; Mandrus, David G. ^[4];

^[5]; Dery, Hanan ^[2];

^[5];

^[1]

Univ. of Washington, Seattle, WA (United States)
Univ. of Rochester, NY (United States)
National Inst. for Materials Science, Tsukuba (Japan)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Univ. of Hong Kong (China)

Publication Date:: Thu Jan 30 00:00:00 EST 2020

Research Org.:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES), Materials Sciences & Engineering Division; National Science Foundation (NSF); US Army Research Office (ARO); Research Grants Council of Hong Kong

OSTI Identifier:: 1651248

Grant/Contract Number:: AC05-00OR22725; SC0018171; SC0014349; W911NF-18-1-0431; 1719797; 17312916

Resource Type:: Accepted Manuscript

Journal Name:: Nature Communications

Additional Journal Information:: Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2041-1723

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; Two-dimensional materials

Citation Formats


                    He, Minhao, Rivera, Pasqual, Van Tuan, Dinh, Wilson, Nathan P., Yang, Min, Taniguchi, Takashi, Watanabe, Kenji, Yan, Jiaqiang, Mandrus, David G., Yu, Hongyi, Dery, Hanan, Yao, Wang, and Xu, Xiaodong. Valley phonons and exciton complexes in a monolayer semiconductor.  United States: N. p., 2020. 
Web.  doi:10.1038/s41467-020-14472-0.

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                    He, Minhao, Rivera, Pasqual, Van Tuan, Dinh, Wilson, Nathan P., Yang, Min, Taniguchi, Takashi, Watanabe, Kenji, Yan, Jiaqiang, Mandrus, David G., Yu, Hongyi, Dery, Hanan, Yao, Wang, & Xu, Xiaodong. Valley phonons and exciton complexes in a monolayer semiconductor.  United States.  https://doi.org/10.1038/s41467-020-14472-0

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                    He, Minhao, Rivera, Pasqual, Van Tuan, Dinh, Wilson, Nathan P., Yang, Min, Taniguchi, Takashi, Watanabe, Kenji, Yan, Jiaqiang, Mandrus, David G., Yu, Hongyi, Dery, Hanan, Yao, Wang, and Xu, Xiaodong. Thu .  
"Valley phonons and exciton complexes in a monolayer semiconductor".  United States.  https://doi.org/10.1038/s41467-020-14472-0.  https://www.osti.gov/servlets/purl/1651248.

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@article{osti_1651248,

  title        = {Valley phonons and exciton complexes in a monolayer semiconductor},

  author       = {He, Minhao and Rivera, Pasqual and Van Tuan, Dinh and Wilson, Nathan P. and Yang, Min and Taniguchi, Takashi and Watanabe, Kenji and Yan, Jiaqiang and Mandrus, David G. and Yu, Hongyi and Dery, Hanan and Yao, Wang and Xu, Xiaodong},

  abstractNote = {The coupling between spin, charge, and lattice degrees of freedom plays an important role in a wide range of fundamental phenomena. Monolayer semiconducting transitional metal dichalcogenides have emerged as an outstanding platform for studying these coupling effects. Here, we report the observation of multiple valley phonons – phonons with momentum vectors pointing to the corners of the hexagonal Brillouin zone – and the resulting exciton complexes in the monolayer semiconductor WSe2. We find that these valley phonons lead to efficient intervalley scattering of quasi particles in both exciton formation and relaxation. This leads to a series of photoluminescence peaks as valley phonon replicas of dark trions. Using identified valley phonons, we also uncover an intervalley exciton near charge neutrality. Our work not only identifies a number of previously unknown 2D excitonic species, but also shows that monolayer WSe2 is a prime candidate for studying interactions between spin, pseudospin, and zone-edge phonons.},

  doi          = {10.1038/s41467-020-14472-0},

  journal      = {Nature Communications},

  number       = 1,

  volume       = 11,

  place        = {United States},

  year         = {Thu Jan 30 00:00:00 EST 2020},

  month        = {Thu Jan 30 00:00:00 EST 2020}

}

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text, January 2018

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Title: Valley phonons and exciton complexes in a monolayer semiconductor

Abstract

Citation Formats

Coupled Spin and Valley Physics in Monolayers of MoS 2 and Other Group-VI Dichalcogenides journal, May 2012

Light–valley interactions in 2D semiconductors journal, July 2018

Colloquium : Excitons in atomically thin transition metal dichalcogenides journal, April 2018

Experimental Evidence for Dark Excitons in Monolayer WSe 2 journal, December 2015

Probing dark excitons in atomically thin semiconductors via near-field coupling to surface plasmon polaritons journal, June 2017

Breaking of Valley Degeneracy by Magnetic Field in Monolayer MoSe 2 journal, January 2015

Detecting topological currents in graphene superlattices journal, September 2014

Optical generation of excitonic valley coherence in monolayer WSe2 journal, August 2013

Observation of chiral phonons journal, February 2018

Magnetic brightening and control of dark excitons in monolayer WSe2 journal, June 2017

Tightly Bound Excitons in Monolayer WSe 2 journal, July 2014

Electrically tunable excitonic light-emitting diodes based on monolayer WSe2 p–n junctions journal, March 2014

Emerging Photoluminescence in Monolayer MoS2 journal, April 2010

Gate Tunable Dark Trions in Monolayer WSe 2 journal, July 2019

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

Revealing the biexciton and trion-exciton complexes in BN encapsulated WSe2 journal, September 2018

Emerging photoluminescence from the dark-exciton phonon replica in monolayer WSe2 journal, June 2019

Charge-tuneable biexciton complexes in monolayer WSe2 journal, September 2018

2D transition metal dichalcogenides journal, June 2017

Valley-selective chiral phonon replicas of dark excitons and trions in monolayer WS e 2 journal, October 2019

The valley Zeeman effect in inter- and intra-valley trions in monolayer WSe2 journal, May 2019

Coulomb-bound four- and five-particle intervalley states in an atomically-thin semiconductor journal, September 2018

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

Polarization analysis of excitons in monolayer and bilayer transition-metal dichalcogenides journal, September 2015

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

Valley Splitting and Polarization by the Zeeman Effect in Monolayer MoSe 2 journal, December 2014

Entanglement of single-photons and chiral phonons in atomically thin WSe2 journal, December 2018

Long valley lifetime of dark excitons in single-layer WSe2 journal, September 2019

Valley-Contrasting Physics in Graphene: Magnetic Moment and Topological Transport journal, December 2007

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

Radiative control of dark excitons at room temperature by nano-optical antenna-tip Purcell effect journal, November 2017

The valley Hall effect in MoS2 transistors journal, June 2014

Valley-selective circular dichroism of monolayer molybdenum disulphide journal, January 2012

Observation of biexcitons in monolayer WSe2 journal, May 2015

Valley Zeeman effect in elementary optical excitations of monolayer WSe2 journal, January 2015

Dirac cones and Dirac saddle points of bright excitons in monolayer transition metal dichalcogenides journal, May 2014

Magnetic control of valley pseudospin in monolayer WSe2 journal, January 2015

Fine structure and lifetime of dark excitons in transition metal dichalcogenide monolayers journal, October 2017

Magnetooptics of Exciton Rydberg States in a Monolayer Semiconductor journal, February 2018

Isospin Pomeranchuk effect in twisted bilayer graphene journal, April 2021

Valley contrasting physics in graphene: magnetic moment and topological transport text, January 2007

Optical Generation of Excitonic Valley Coherence in Monolayer WSe2 text, January 2013

Valley Zeeman Effect in Elementary Optical Excitations of a Monolayer WSe2 text, January 2014

Polarization analysis of excitons in monolayer and bilayer transition-metal dichalcogenides text, January 2015

Magnetic brightening and control of dark excitons in monolayer WSe2 text, January 2016

In-plane Propagation of Light in Transition Metal Dichalcogenide Monolayers: Optical Selection Rules text, January 2017

Revealing the Biexciton and Trion-exciton Complexes in BN Encapsulated WSe2 text, January 2018

Entanglement of single-photons and chiral phonons in atomically thin WSe$_2$ text, January 2018

Long valley lifetime of dark excitons in single-layer WSe2 text, January 2019

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

2D transition metal dichalcogenides journal, June 2017

Valley-selective circular dichroism of monolayer molybdenum disulphide journal, January 2012

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

Coulomb-bound four- and five-particle intervalley states in an atomically-thin semiconductor journal, September 2018

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

Emerging photoluminescence from the dark-exciton phonon replica in monolayer WSe2 journal, June 2019

Entanglement of single-photons and chiral phonons in atomically thin WSe2 journal, December 2018

Normal electric field enhanced light-induced polarizations and magnetic detection of valley polarization in silicene journal, October 2020

Transport Theory of Monolayer Transition-Metal Dichalcogenides through Symmetry journal, July 2013

Chiral Phonons at High-Symmetry Points in Monolayer Hexagonal Lattices journal, September 2015

In-Plane Propagation of Light in Transition Metal Dichalcogenide Monolayers: Optical Selection Rules journal, July 2017

Photoluminescence of Isotopically Purified Silicon: How Sharp are Bound Exciton Transitions? journal, June 2001

Observation of chiral phonons journal, February 2018

Electrically Tunable Excitonic Light Emitting Diodes based on Monolayer WSe2 p-n Junctions text, January 2013

Bright excitons in monolayer transition metal dichalcogenides: from Dirac cones to Dirac saddle points text, January 2014

Valley Zeeman Effect in Elementary Optical Excitations of a Monolayer WSe2 text, January 2014

Magnetic Control of Valley Pseudospin in Monolayer WSe2 text, January 2014

Valley Splitting and Polarization by the Zeeman Effect in Monolayer MoSe2 text, January 2014

Probing dark excitons in atomically thin semiconductors via near-field coupling to surface plasmon polaritons text, January 2017

Radiative control of dark excitons at room temperature by nano-optical antenna-tip induced Purcell effect text, January 2017

Charge-tuneable biexciton complexes in monolayer WSe$_{2}$ text, January 2018

Revealing the Biexciton and Trion-exciton Complexes in BN Encapsulated WSe2 text, January 2018

Gate tunable dark trions in monolayer WSe$_2$ text, January 2019

Coupled Spin and Valley Physics in Monolayers of ${MoS}_{2}$ and Other Group-VI Dichalcogenides
journal, May 2012

Light–valley interactions in 2D semiconductors
journal, July 2018

Colloquium : Excitons in atomically thin transition metal dichalcogenides
journal, April 2018

Experimental Evidence for Dark Excitons in Monolayer ${WSe}_{2}$
journal, December 2015

Probing dark excitons in atomically thin semiconductors via near-field coupling to surface plasmon polaritons
journal, June 2017

Breaking of Valley Degeneracy by Magnetic Field in Monolayer ${MoSe}_{2}$
journal, January 2015

Detecting topological currents in graphene superlattices
journal, September 2014

Optical generation of excitonic valley coherence in monolayer WSe2
journal, August 2013

Observation of chiral phonons
journal, February 2018

Magnetic brightening and control of dark excitons in monolayer WSe2
journal, June 2017

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

Electrically tunable excitonic light-emitting diodes based on monolayer WSe2 p–n junctions
journal, March 2014

Emerging Photoluminescence in Monolayer MoS₂
journal, April 2010

Gate Tunable Dark Trions in Monolayer ${WSe}_{2}$
journal, July 2019

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

Revealing the biexciton and trion-exciton complexes in BN encapsulated WSe2
journal, September 2018

Emerging photoluminescence from the dark-exciton phonon replica in monolayer WSe2
journal, June 2019

Charge-tuneable biexciton complexes in monolayer WSe2
journal, September 2018

2D transition metal dichalcogenides
journal, June 2017

Valley-selective chiral phonon replicas of dark excitons and trions in monolayer WS e 2
journal, October 2019

The valley Zeeman effect in inter- and intra-valley trions in monolayer WSe2
journal, May 2019

Coulomb-bound four- and five-particle intervalley states in an atomically-thin semiconductor
journal, September 2018

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

Polarization analysis of excitons in monolayer and bilayer transition-metal dichalcogenides
journal, September 2015

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

Valley Splitting and Polarization by the Zeeman Effect in Monolayer ${MoSe}_{2}$
journal, December 2014

Entanglement of single-photons and chiral phonons in atomically thin WSe2
journal, December 2018

Long valley lifetime of dark excitons in single-layer WSe2
journal, September 2019

Valley-Contrasting Physics in Graphene: Magnetic Moment and Topological Transport
journal, December 2007

Atomically Thin ${MoS}_{2}$ A New Direct-Gap Semiconductor
journal, September 2010

Radiative control of dark excitons at room temperature by nano-optical antenna-tip Purcell effect
journal, November 2017

The valley Hall effect in MoS2 transistors
journal, June 2014

Valley-selective circular dichroism of monolayer molybdenum disulphide
journal, January 2012

Observation of biexcitons in monolayer WSe2
journal, May 2015

Valley Zeeman effect in elementary optical excitations of monolayer WSe2
journal, January 2015

Dirac cones and Dirac saddle points of bright excitons in monolayer transition metal dichalcogenides
journal, May 2014

Magnetic control of valley pseudospin in monolayer WSe2
journal, January 2015

Fine structure and lifetime of dark excitons in transition metal dichalcogenide monolayers
journal, October 2017

Magnetooptics of Exciton Rydberg States in a Monolayer Semiconductor
journal, February 2018

Isospin Pomeranchuk effect in twisted bilayer graphene
journal, April 2021

Valley contrasting physics in graphene: magnetic moment and topological transport
text, January 2007

Optical Generation of Excitonic Valley Coherence in Monolayer WSe2
text, January 2013

Valley Zeeman Effect in Elementary Optical Excitations of a Monolayer WSe2
text, January 2014

Polarization analysis of excitons in monolayer and bilayer transition-metal dichalcogenides
text, January 2015

Magnetic brightening and control of dark excitons in monolayer WSe2
text, January 2016

In-plane Propagation of Light in Transition Metal Dichalcogenide Monolayers: Optical Selection Rules
text, January 2017

Revealing the Biexciton and Trion-exciton Complexes in BN Encapsulated WSe2
text, January 2018

Entanglement of single-photons and chiral phonons in atomically thin WSe$_2$
text, January 2018

Long valley lifetime of dark excitons in single-layer WSe2
text, January 2019

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

2D transition metal dichalcogenides
journal, June 2017

Valley-selective circular dichroism of monolayer molybdenum disulphide
journal, January 2012

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

Coulomb-bound four- and five-particle intervalley states in an atomically-thin semiconductor
journal, September 2018

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

Emerging photoluminescence from the dark-exciton phonon replica in monolayer WSe2
journal, June 2019

Entanglement of single-photons and chiral phonons in atomically thin WSe2
journal, December 2018

Normal electric field enhanced light-induced polarizations and magnetic detection of valley polarization in silicene
journal, October 2020

Transport Theory of Monolayer Transition-Metal Dichalcogenides through Symmetry
journal, July 2013

Chiral Phonons at High-Symmetry Points in Monolayer Hexagonal Lattices
journal, September 2015

In-Plane Propagation of Light in Transition Metal Dichalcogenide Monolayers: Optical Selection Rules
journal, July 2017

Photoluminescence of Isotopically Purified Silicon: How Sharp are Bound Exciton Transitions?
journal, June 2001

Observation of chiral phonons
journal, February 2018

Electrically Tunable Excitonic Light Emitting Diodes based on Monolayer WSe2 p-n Junctions
text, January 2013

Bright excitons in monolayer transition metal dichalcogenides: from Dirac cones to Dirac saddle points
text, January 2014

Valley Zeeman Effect in Elementary Optical Excitations of a Monolayer WSe2
text, January 2014

Magnetic Control of Valley Pseudospin in Monolayer WSe2
text, January 2014

Valley Splitting and Polarization by the Zeeman Effect in Monolayer MoSe2
text, January 2014

Probing dark excitons in atomically thin semiconductors via near-field coupling to surface plasmon polaritons
text, January 2017

Radiative control of dark excitons at room temperature by nano-optical antenna-tip induced Purcell effect
text, January 2017

Charge-tuneable biexciton complexes in monolayer WSe$_{2}$
text, January 2018

Revealing the Biexciton and Trion-exciton Complexes in BN Encapsulated WSe2
text, January 2018

Gate tunable dark trions in monolayer WSe$_2$
text, January 2019