Narrow-band high-lying excitons with negative-mass electrons in monolayer WSe2

Lin, Kai-Qiang; Ong, Chin Shen; Bange, Sebastian; Faria Junior, Paulo E.; Peng, Bo; Ziegler, Jonas D.; Zipfel, Jonas; Bäuml, Christian; Paradiso, Nicola; Watanabe, Kenji; Taniguchi, Takashi; Strunk, Christoph; Monserrat, Bartomeu; Fabian, Jaroslav; Chernikov, Alexey; Qiu, Diana Y.; Louie, Steven G.; Lupton, John M.

doi:10.1038/s41467-021-25499-2

Title: Narrow-band high-lying excitons with negative-mass electrons in monolayer WSe2

Journal Article · Fri Sep 17 00:00:00 EDT 2021 · Nature Communications

DOI:https://doi.org/10.1038/s41467-021-25499-2· OSTI ID:1825017

^[1];

^[2];

^[1]; Faria Junior, Paulo E. ^[1];

^[3]; Ziegler, Jonas D. ^[1]; Zipfel, Jonas ^[1]; Bäuml, Christian ^[1]; Paradiso, Nicola ^[1];

^[4];

^[4]; Strunk, Christoph ^[1];

^[3];

^[1];

^[5]; Qiu, Diana Y. ^[6];

^[2];

^[1]

Univ. of Regensburg (Germany)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of Cambridge (United Kingdom). Cavendish Lab.
National Institute for Materials Science (NIMS), Tsukuba (Japan)
Univ. of Regensburg (Germany); Dresden Univ. of Technology (Germany)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Yale Univ., New Haven, CT (United States)

Monolayer transition-metal dichalcogenides (TMDCs) show a wealth of exciton physics. Here, we report the existence of a new excitonic species, the high-lying exciton (HX), in single-layer WSe₂ with an energy of ~3.4 eV, almost twice the band-edge A-exciton energy, with a linewidth as narrow as 5.8 meV. The HX is populated through momentum-selective optical excitation in the K-valleys and is identified in upconverted photoluminescence (UPL) in the UV spectral region. Strong electron-phonon coupling results in a cascaded phonon progression with equidistant peaks in the luminescence spectrum, resolvable to ninth order. Ab initio GW-BSE calculations with full electron-hole correlations explain HX formation and unmask the admixture of upper conduction-band states to this complex many-body excitation. These calculations suggest that the HX is comprised of electrons of negative mass. The coincidence of such high-lying excitonic species at around twice the energy of band-edge excitons rationalizes the excitonic quantum-interference phenomenon recently discovered in optical second-harmonic generation (SHG) and explains the efficient Auger-like annihilation of band-edge excitons.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1825017

Journal Information:: Nature Communications, Vol. 12, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (41)

Intravalley Spin–Flip Relaxation Dynamics in Single-Layer WS ₂ Wang, Zilong; Molina-Sánchez, Alejandro; Altmann, Patrick Nano Letters, Vol. 18, Issue 11 https://doi.org/10.1021/acs.nanolett.8b02774	journal	September 2018
On the existence of bielectrons in BiI3 Czaja, W.; Harbeke, G.; Krausbauer, L. Solid State Communications, Vol. 13, Issue 9 https://doi.org/10.1016/0038-1098(73)90186-5	journal	November 1973
Colloquium : Excitons in atomically thin transition metal dichalcogenides Wang, Gang; Chernikov, Alexey; Glazov, Mikhail M. Reviews of Modern Physics, Vol. 90, Issue 2 https://doi.org/10.1103/RevModPhys.90.021001	journal	April 2018
Observation of exciton-phonon coupling in ${MoSe}_{2}$ monolayers Shree, S.; Semina, M.; Robert, C. Physical Review B, Vol. 98, Issue 3 https://doi.org/10.1103/PhysRevB.98.035302	journal	July 2018
Multiphonon resonant Raman scattering in MoS ₂ Gołasa, K.; Grzeszczyk, M.; Leszczyński, P. Applied Physics Letters, Vol. 104, Issue 9 https://doi.org/10.1063/1.4867502	journal	March 2014
Auger recombination of dark excitons in WS ₂ and WSe ₂ monolayers Danovich, Mark; Zólyomi, Viktor; Fal’ko, Vladimir I. 2D Materials, Vol. 3, Issue 3 https://doi.org/10.1088/2053-1583/3/3/035011	journal	August 2016
Intrinsic transport properties of electrons and holes in monolayer transition-metal dichalcogenides Jin, Zhenghe; Li, Xiaodong; Mullen, Jeffrey T. Physical Review B, Vol. 90, Issue 4 https://doi.org/10.1103/PhysRevB.90.045422	journal	July 2014
Unifying Optical Selection Rules for Excitons in Two Dimensions: Band Topology and Winding Numbers Cao, Ting; Wu, Meng; Louie, Steven G. Physical Review Letters, Vol. 120, Issue 8 https://doi.org/10.1103/PhysRevLett.120.087402	journal	February 2018
Observation of chiral phonons Zhu, Hanyu; Yi, Jun; Li, Ming-Yang Science, Vol. 359, Issue 6375 https://doi.org/10.1126/science.aar2711	journal	February 2018
Intervalley scattering by acoustic phonons in two-dimensional MoS2 revealed by double-resonance Raman spectroscopy Carvalho, Bruno R.; Wang, Yuanxi; Mignuzzi, Sandro Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms14670	journal	March 2017
Valley polarization and intervalley scattering in monolayer MoS ₂ Kioseoglou, G.; Hanbicki, A. T.; Currie, M. Applied Physics Letters, Vol. 101, Issue 22 https://doi.org/10.1063/1.4768299	journal	November 2012
Tightly Bound Excitons in Monolayer ${WSe}_{2}$ He, Keliang; Kumar, Nardeep; Zhao, Liang Physical Review Letters, Vol. 113, Issue 2 https://doi.org/10.1103/PhysRevLett.113.026803	journal	July 2014
Spin and pseudospins in layered transition metal dichalcogenides Xu, Xiaodong; Yao, Wang; Xiao, Di Nature Physics, Vol. 10, Issue 5 https://doi.org/10.1038/nphys2942	journal	April 2014
BerkeleyGW: A massively parallel computer package for the calculation of the quasiparticle and optical properties of materials and nanostructures Deslippe, Jack; Samsonidze, Georgy; Strubbe, David A. Computer Physics Communications, Vol. 183, Issue 6 https://doi.org/10.1016/j.cpc.2011.12.006	journal	June 2012
Quantum interference in second-harmonic generation from monolayer WSe2 Lin, Kai-Qiang; Bange, Sebastian; Lupton, John M. Nature Physics, Vol. 15, Issue 3 https://doi.org/10.1038/s41567-018-0384-5	journal	January 2019
k · p theory for two-dimensional transition metal dichalcogenide semiconductors Kormányos, Andor; Burkard, Guido; Gmitra, Martin 2D Materials, Vol. 2, Issue 2 https://doi.org/10.1088/2053-1583/2/2/022001	journal	April 2015
Electron correlation in semiconductors and insulators: Band gaps and quasiparticle energies Hybertsen, Mark S.; Louie, Steven G. Physical Review B, Vol. 34, Issue 8, p. 5390-5413 https://doi.org/10.1103/PhysRevB.34.5390	journal	October 1986
Electrical control of second-harmonic generation in a WSe2 monolayer transistor Seyler, Kyle L.; Schaibley, John R.; Gong, Pu Nature Nanotechnology, Vol. 10, Issue 5 https://doi.org/10.1038/nnano.2015.73	journal	April 2015
Continuous Wave Sum Frequency Generation and Imaging of Monolayer and Heterobilayer Two-Dimensional Semiconductors Yao, Kaiyuan; Yanev, Emanuil; Chuang, Hsun-Jen ACS Nano, Vol. 14, Issue 1 https://doi.org/10.1021/acsnano.9b07555	journal	December 2019
Optical Spectrum of ${MoS}_{2}$ : Many-Body Effects and Diversity of Exciton States Qiu, Diana Y.; da Jornada, Felipe H.; Louie, Steven G. Physical Review Letters, Vol. 111, Issue 21 https://doi.org/10.1103/PhysRevLett.111.216805	journal	November 2013
Holstein polaron in a valley-degenerate two-dimensional semiconductor Kang, Mingu; Jung, Sung Won; Shin, Woo Jong Nature Materials, Vol. 17, Issue 8 https://doi.org/10.1038/s41563-018-0092-7	journal	May 2018
Resonant internal quantum transitions and femtosecond radiative decay of excitons in monolayer WSe2 Poellmann, C.; Steinleitner, P.; Leierseder, U. Nature Materials, Vol. 14, Issue 9 https://doi.org/10.1038/nmat4356	journal	July 2015
Intrinsic homogeneous linewidth and broadening mechanisms of excitons in monolayer transition metal dichalcogenides Moody, Galan; Kavir Dass, Chandriker; Hao, Kai Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9315	journal	September 2015
Probing excitonic dark states in single-layer tungsten disulphide Ye, Ziliang; Cao, Ting; O’Brien, Kevin Nature, Vol. 513, Issue 7517 https://doi.org/10.1038/nature13734	journal	August 2014
Deterministic transfer of two-dimensional materials by all-dry viscoelastic stamping Castellanos-Gomez, Andres; Buscema, Michele; Molenaar, Rianda 2D Materials, Vol. 1, Issue 1 https://doi.org/10.1088/2053-1583/1/1/011002	journal	April 2014
Controlling photons using electromagnetically induced transparency Lukin, M. D.; Imamoğlu, A. Nature, Vol. 413, Issue 6853 https://doi.org/10.1038/35095000	journal	September 2001
Efficient phonon cascades in WSe2 monolayers Paradisanos, Ioannis; Wang, Gang; Alexeev, Evgeny M. Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-020-20244-7	journal	January 2021
Polymer Coatings Tune Electromagnetically Induced Transparency in Two-Dimensional Semiconductors Lin, Kai-Qiang; Martin, Robert; Bange, Sebastian ACS Photonics, Vol. 6, Issue 12 https://doi.org/10.1021/acsphotonics.9b01141	journal	November 2019
Electronic structures and theoretical modelling of two-dimensional group-VIB transition metal dichalcogenides Liu, Gui-Bin; Xiao, Di; Yao, Yugui Chemical Society Reviews, Vol. 44, Issue 9 https://doi.org/10.1039/C4CS00301B	journal	January 2015
Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides Selig, Malte; Berghäuser, Gunnar; Raja, Archana Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13279	journal	November 2016
Defect Structure of Localized Excitons in a ${WSe}_{2}$ Monolayer Zhang, Shuai; Wang, Chen-Guang; Li, Ming-Yang Physical Review Letters, Vol. 119, Issue 4 https://doi.org/10.1103/PhysRevLett.119.046101	journal	July 2017
Absorption, Photoluminescence, and Resonant Raman Scattering in Bil3 Petroff, Y.; Yu, P. Y.; Shen, Y. R. physica status solidi (b), Vol. 61, Issue 2 https://doi.org/10.1002/pssb.2220610206	journal	February 1974
Twist-angle engineering of excitonic quantum interference and optical nonlinearities in stacked 2D semiconductors Lin, Kai-Qiang; Faria Junior, Paulo E.; Bauer, Jonas M. Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-21547-z	journal	March 2021
Electron-hole excitations and optical spectra from first principles Rohlfing, Michael; Louie, Steven G. Physical Review B, Vol. 62, Issue 8 https://doi.org/10.1103/PhysRevB.62.4927	journal	August 2000
Nonlinear photoluminescence in atomically thin layered ${WSe}_{2}$ arising from diffusion-assisted exciton-exciton annihilation Mouri, Shinichiro; Miyauchi, Yuhei; Toh, Minglin Physical Review B, Vol. 90, Issue 15 https://doi.org/10.1103/PhysRevB.90.155449	journal	October 2014
Generation and Evolution of Spin-, Valley-, and Layer-Polarized Excited Carriers in Inversion-Symmetric ${WSe}_{2}$ Bertoni, R.; Nicholson, C. W.; Waldecker, L. Physical Review Letters, Vol. 117, Issue 27 https://doi.org/10.1103/PhysRevLett.117.277201	journal	December 2016
Valley depolarization due to intervalley and intravalley electron-hole exchange interactions in monolayer ${MoS}_{2}$ Yu, T.; Wu, M. W. Physical Review B, Vol. 89, Issue 20 https://doi.org/10.1103/PhysRevB.89.205303	journal	May 2014
Camel's back excitons in GaP Altarelli, M.; Sabatini, R. A.; Lipari, N. O. Solid State Communications, Vol. 25, Issue 12 https://doi.org/10.1016/0038-1098(78)90917-1	journal	March 1978
Optically active quantum dots in monolayer WSe2 Srivastava, Ajit; Sidler, Meinrad; Allain, Adrien V. Nature Nanotechnology, Vol. 10, Issue 6 https://doi.org/10.1038/nnano.2015.60	journal	May 2015
Enabling valley selective exciton scattering in monolayer WSe2 through upconversion Manca, M.; Glazov, M. M.; Robert, C. Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms14927	journal	April 2017
Phonon-assisted oscillatory exciton dynamics in monolayer MoSe2 Chow, Colin M.; Yu, Hongyi; Jones, Aaron M. npj 2D Materials and Applications, Vol. 1, Issue 1 https://doi.org/10.1038/s41699-017-0035-1	journal	October 2017

Similar Records

Dynamics and Spin-Valley Locking Effects in Monolayer Transition Metal Dichalcogenides

Journal Article · Wed Aug 01 00:00:00 EDT 2018 · Nano Letters · OSTI ID:1825017

Ciccarino, Christopher J.; Christensen, Thomas; Sundararaman, Ravishankar; +1 more

Strong interaction between interlayer excitons and correlated electrons in WSe2/WS2 moiré superlattice

Journal Article · Mon Jun 14 00:00:00 EDT 2021 · Nature Communications · OSTI ID:1825017

Miao, Shengnan; Wang, Tianmeng; Huang, Xiong; +11 more

Magnetic brightening and control of dark excitons in monolayer WSe₂

Journal Article · Mon Jun 26 00:00:00 EDT 2017 · Nature Nanotechnology · OSTI ID:1825017

Zhang, Xiao -Xiao; Cao, Ting; Lu, Zhengguang; +9 more

Related Subjects

75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY

Title: Narrow-band high-lying excitons with negative-mass electrons in monolayer WSe2

Citation Formats

References (41)

Similar Records

Related Subjects