Momentum-Dark Intervalley Exciton in Monolayer Tungsten Diselenide Brightened via Chiral Phonon

Li, Zhipeng; Wang, Tianmeng; Jin, Chenhao; Lu, Zhengguang; Lian, Zhen; Meng, Yuze; Blei, Mark; Gao, Mengnan; Taniguchi, Takashi; Watanabe, Kenji; Ren, Tianhui; Cao, Ting; Tongay, Sefaattin; Smirnov, Dmitry; Zhang, Lifa; Shi, Su-Fei

doi:10.1021/acsnano.9b06682

Title: Momentum-Dark Intervalley Exciton in Monolayer Tungsten Diselenide Brightened via Chiral Phonon

Abstract

Inversion symmetry breaking and 3-fold rotation symmetry grant the valley degree of freedom to the robust exciton in monolayer transition-metal dichalcogenides, which can be exploited for valleytronics applications. However, the short lifetime of the exciton significantly constrains the possible applications. In contrast, the dark exciton could be long-lived but does not necessarily possess the valley degree of freedom. In this work, we report the identification of the momentum-dark, intervalley exciton in monolayer WSe₂ through low-temperature magneto-photoluminescence spectra. Interestingly, the intervalley exciton is brightened through the emission of a chiral phonon at the corners of the Brillouin zone (K point), and the pseudoangular momentum of the phonon is transferred to the emitted photon to preserve the valley information. The chiral phonon energy is determined to be ~23 meV, based on the experimentally extracted exchange interaction (~7 meV), in excellent agreement with the theoretical expectation of 24.6 meV. The long-lived intervalley exciton with valley degree of freedom adds an exciting quasiparticle for valleytronics, and the coupling between the chiral phonon and intervalley exciton furnishes a venue for valley spin manipulation.

Authors:

^[1]; Wang, Tianmeng ^[2]; Jin, Chenhao ^[3]; Lu, Zhengguang ^[4]; Lian, Zhen ^[2]; Meng, Yuze ^[5]; Blei, Mark ^[6]; Gao, Mengnan ^[7]; Taniguchi, Takashi ^[8]; Watanabe, Kenji ^[8];

^[9];

^[10];

^[6];

^[4];

^[7];

^[2]

Rensselaer Polytechnic Inst., Troy, NY (United States); Shanghai Jiao Tong Univ. (China)
Rensselaer Polytechnic Inst., Troy, NY (United States)
Cornell Univ., Ithaca, NY (United States). Kavli Institute for Nanoscale Science
Florida State Univ., Tallahassee, FL (United States). National High Magnetic Field Lab. (MagLab)
Rensselaer Polytechnic Inst., Troy, NY (United States); Nanjing Univ. (China)
Arizona State Univ., Tempe, AZ (United States)
Nanjing Normal University (China)
National Institute for Materials Science, Tsukuba (Japan)
Shanghai Jiao Tong Univ. (China)
Univ. of Washington, Seattle, WA (United States); Stanford Univ., CA (United States)

Publication Date:: Mon Nov 25 00:00:00 EST 2019

Research Org.:: Florida State Univ., Tallahassee, FL (United States)

Sponsoring Org.:: USDOE Office of Science (SC)

OSTI Identifier:: 1800507

Grant/Contract Number:: FG02-07ER46451

Resource Type:: Accepted Manuscript

Journal Name:: ACS Nano

Additional Journal Information:: Journal Volume: 13; Journal Issue: 12; Journal ID: ISSN 1936-0851

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; materials science; intervalley exciton; chiral phonon; magneto-PL; time-resolved PL; tungsten diselenide; monolayers; excitons; phonons; energy; lasers

Citation Formats


                    Li, Zhipeng, Wang, Tianmeng, Jin, Chenhao, Lu, Zhengguang, Lian, Zhen, Meng, Yuze, Blei, Mark, Gao, Mengnan, Taniguchi, Takashi, Watanabe, Kenji, Ren, Tianhui, Cao, Ting, Tongay, Sefaattin, Smirnov, Dmitry, Zhang, Lifa, and Shi, Su-Fei. Momentum-Dark Intervalley Exciton in Monolayer Tungsten Diselenide Brightened via Chiral Phonon.  United States: N. p., 2019. 
Web.  doi:10.1021/acsnano.9b06682.

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                    Li, Zhipeng, Wang, Tianmeng, Jin, Chenhao, Lu, Zhengguang, Lian, Zhen, Meng, Yuze, Blei, Mark, Gao, Mengnan, Taniguchi, Takashi, Watanabe, Kenji, Ren, Tianhui, Cao, Ting, Tongay, Sefaattin, Smirnov, Dmitry, Zhang, Lifa, & Shi, Su-Fei. Momentum-Dark Intervalley Exciton in Monolayer Tungsten Diselenide Brightened via Chiral Phonon.  United States.  https://doi.org/10.1021/acsnano.9b06682

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                    Li, Zhipeng, Wang, Tianmeng, Jin, Chenhao, Lu, Zhengguang, Lian, Zhen, Meng, Yuze, Blei, Mark, Gao, Mengnan, Taniguchi, Takashi, Watanabe, Kenji, Ren, Tianhui, Cao, Ting, Tongay, Sefaattin, Smirnov, Dmitry, Zhang, Lifa, and Shi, Su-Fei. Mon .  
"Momentum-Dark Intervalley Exciton in Monolayer Tungsten Diselenide Brightened via Chiral Phonon".  United States.  https://doi.org/10.1021/acsnano.9b06682.  https://www.osti.gov/servlets/purl/1800507.

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@article{osti_1800507,

  title        = {Momentum-Dark Intervalley Exciton in Monolayer Tungsten Diselenide Brightened via Chiral Phonon},

  author       = {Li, Zhipeng and Wang, Tianmeng and Jin, Chenhao and Lu, Zhengguang and Lian, Zhen and Meng, Yuze and Blei, Mark and Gao, Mengnan and Taniguchi, Takashi and Watanabe, Kenji and Ren, Tianhui and Cao, Ting and Tongay, Sefaattin and Smirnov, Dmitry and Zhang, Lifa and Shi, Su-Fei},

  abstractNote = {Inversion symmetry breaking and 3-fold rotation symmetry grant the valley degree of freedom to the robust exciton in monolayer transition-metal dichalcogenides, which can be exploited for valleytronics applications. However, the short lifetime of the exciton significantly constrains the possible applications. In contrast, the dark exciton could be long-lived but does not necessarily possess the valley degree of freedom. In this work, we report the identification of the momentum-dark, intervalley exciton in monolayer WSe2 through low-temperature magneto-photoluminescence spectra. Interestingly, the intervalley exciton is brightened through the emission of a chiral phonon at the corners of the Brillouin zone (K point), and the pseudoangular momentum of the phonon is transferred to the emitted photon to preserve the valley information. The chiral phonon energy is determined to be ~23 meV, based on the experimentally extracted exchange interaction (~7 meV), in excellent agreement with the theoretical expectation of 24.6 meV. The long-lived intervalley exciton with valley degree of freedom adds an exciting quasiparticle for valleytronics, and the coupling between the chiral phonon and intervalley exciton furnishes a venue for valley spin manipulation.},

  doi          = {10.1021/acsnano.9b06682},

  journal      = {ACS Nano},

  number       = 12,

  volume       = 13,

  place        = {United States},

  year         = {Mon Nov 25 00:00:00 EST 2019},

  month        = {Mon Nov 25 00:00:00 EST 2019}

}

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Title: Momentum-Dark Intervalley Exciton in Monolayer Tungsten Diselenide Brightened via Chiral Phonon

Abstract

Citation Formats

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Harnessing chirality for valleytronics journal, October 2014

Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides journal, March 2016

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

Optical manipulation of valley pseudospin journal, September 2016

Long-Lived Valley Polarization of Intravalley Trions in Monolayer WSe 2 journal, December 2016

Biexciton Emission from Edges and Grain Boundaries of Triangular WS 2 Monolayers journal, January 2016

Phonon-driven spin-Floquet magneto-valleytronics in MoS2 journal, February 2018

Magnetoelectric effects and valley-controlled spin quantum gates in transition metal dichalcogenide bilayers journal, June 2013

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

Negative circular polarization emissions from WSe2/MoSe2 commensurate heterobilayers journal, April 2018

Neutral and charged inter-valley biexcitons in monolayer MoSe2 journal, June 2017

Excitonic luminescence upconversion in a two-dimensional semiconductor journal, December 2015

Observation of biexcitons in monolayer WSe2 journal, May 2015

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

Valleytronics in 2D materials journal, August 2016

Electronic structures and theoretical modelling of two-dimensional group-VIB transition metal dichalcogenides journal, January 2015

Observation of ultralong valley lifetime in WSe 2 /MoS 2 heterostructures journal, July 2017

Giant magnetic splitting inducing near-unity valley polarization in van der Waals heterostructures journal, November 2017

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

Evidence of indirect gap in monolayer WSe2 journal, October 2017

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

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

Zeeman Splitting and Inverted Polarization of Biexciton Emission in Monolayer WS 2 journal, August 2018

Microsecond Valley Lifetime of Defect-Bound Excitons in Monolayer WSe 2 journal, August 2018

Harnessing chirality for valleytronics journal, October 2014

Atomically inspired $k \cdot p$ approach and valley Zeeman effect in transition metal dichalcogenide monolayers text, January 2016

Fine Structure and Lifetime of Dark Excitons in Transition Metal Dichalcogenide Monolayers text, January 2017

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

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

Carrier and Polarization Dynamics in Monolayer ${MoS}_{2}$
journal, January 2014

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

Observation of chiral phonons
journal, February 2018

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

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

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

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

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

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

Trion fine structure and coupled spin–valley dynamics in monolayer tungsten disulfide
journal, September 2016

Biexciton fine structure in monolayer transition metal dichalcogenides
journal, October 2018

Ultrafast dynamics in van der Waals heterostructures
journal, November 2018

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

Zeeman splitting via spin-valley-layer coupling in bilayer MoTe2
journal, October 2017

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

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

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

Van der Waals engineering of ferromagnetic semiconductor heterostructures for spin and valleytronics
journal, May 2017

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

Zeeman-type spin splitting controlled by an electric field
journal, July 2013

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

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

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

Valley Zeeman Splitting and Valley Polarization of Neutral and Charged Excitons in Monolayer MoTe ₂ at High Magnetic Fields
journal, May 2016

Valley Polarization of Trions and Magnetoresistance in Heterostructures of MoS ₂ and Yttrium Iron Garnet
journal, October 2016

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

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

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

Harnessing chirality for valleytronics
journal, October 2014

Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides
journal, March 2016

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

Optical manipulation of valley pseudospin
journal, September 2016

Long-Lived Valley Polarization of Intravalley Trions in Monolayer ${WSe}_{2}$
journal, December 2016

Biexciton Emission from Edges and Grain Boundaries of Triangular WS ₂ Monolayers
journal, January 2016

Phonon-driven spin-Floquet magneto-valleytronics in MoS2
journal, February 2018

Magnetoelectric effects and valley-controlled spin quantum gates in transition metal dichalcogenide bilayers
journal, June 2013

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

Negative circular polarization emissions from WSe2/MoSe2 commensurate heterobilayers
journal, April 2018

Neutral and charged inter-valley biexcitons in monolayer MoSe2
journal, June 2017

Excitonic luminescence upconversion in a two-dimensional semiconductor
journal, December 2015

Observation of biexcitons in monolayer WSe2
journal, May 2015

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

Valleytronics in 2D materials
journal, August 2016

Electronic structures and theoretical modelling of two-dimensional group-VIB transition metal dichalcogenides
journal, January 2015

Observation of ultralong valley lifetime in WSe ₂ /MoS ₂ heterostructures
journal, July 2017

Giant magnetic splitting inducing near-unity valley polarization in van der Waals heterostructures
journal, November 2017

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

Evidence of indirect gap in monolayer WSe2
journal, October 2017

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

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

Zeeman Splitting and Inverted Polarization of Biexciton Emission in Monolayer ${WS}_{2}$
journal, August 2018

Microsecond Valley Lifetime of Defect-Bound Excitons in Monolayer WSe 2
journal, August 2018

Harnessing chirality for valleytronics
journal, October 2014

Atomically inspired $k \cdot p$ approach and valley Zeeman effect in transition metal dichalcogenide monolayers
text, January 2016

Fine Structure and Lifetime of Dark Excitons in Transition Metal Dichalcogenide Monolayers
text, January 2017

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