Narrow-band High-lying Excitons with Negative-mass Electrons in Monolayer WSe

Overview

Journal Nat Commun

Specialty Biology

Date 2021 Sep 18

PMID 34535654

Citations 9

Authors

Kai-Qiang Lin

Chin Shen Ong

Sebastian Bange

Paulo E Faria Junior

Bo Peng

Jonas D Ziegler

Jonas Zipfel

Christian Bauml

Nicola Paradiso

Kenji Watanabe

Takashi Taniguchi

Christoph Strunk

Bartomeu Monserrat

Jaroslav Fabian

Alexey Chernikov

Diana Y Qiu

Steven G Louie

John M Lupton

Affiliations

Soon will be listed here.

Abstract

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 WSe 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.

Citing Articles

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Excitons stabilize above the band gap in bilayer WSe.

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