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Title: Intervalley biexcitons and many-body effects in monolayer MoS 2

Abstract

Interactions amidst two excitons can result in the formation of bound quasiparticles, known as biexcitons. Their properties are determined by the constituent excitons, with orbital and spin states resembling those of atoms. Monolayer transition metal dichalcogenides (TMDs) present a unique system where excitons acquire a new degree of freedom, the valley pseudospin, from which a novel intervalley biexciton can be created. These biexcitons comprise two excitons from different valleys, which are distinct from biexcitons in conventional semiconductors and have no direct analog in atomic and molecular systems. However, their valley properties are not accessible to traditional transport and optical measurements. Here, we report the observation of intervalley biexcitons in the monolayer TMDMoS 2 using ultrafast pump-probe spectroscopy. By applying broadband probe pulses with different helicities, we identify two species of intervalley biexcitons with large binding energies of 60 and 40 meV. Furthermore, we also reveal effects beyond biexcitonic pairwise interactions in which the exciton energy redshifts at increasing exciton densities, indicating the presence of many-body interactions among them.

Authors:
 [1];  [2];  [3];  [1];  [1]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Harvard Univ., Cambridge, MA (United States)
  3. National Tsing Hua Univ., Hsinchu (Taiwan)
Publication Date:
Research Org.:
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1505594
Alternate Identifier(s):
OSTI ID: 1215748
Grant/Contract Number:  
FG02-08ER46521; SC0006423
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review. B, Condensed Matter and Materials Physics
Additional Journal Information:
Journal Volume: 92; Journal Issue: 12; Journal ID: ISSN 1098-0121
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Sie, Edbert J., Frenzel, Alex J., Lee, Yi-Hsien, Kong, Jing, and Gedik, Nuh. Intervalley biexcitons and many-body effects in monolayer MoS2. United States: N. p., 2015. Web. doi:10.1103/physrevb.92.125417.
Sie, Edbert J., Frenzel, Alex J., Lee, Yi-Hsien, Kong, Jing, & Gedik, Nuh. Intervalley biexcitons and many-body effects in monolayer MoS2. United States. doi:10.1103/physrevb.92.125417.
Sie, Edbert J., Frenzel, Alex J., Lee, Yi-Hsien, Kong, Jing, and Gedik, Nuh. Fri . "Intervalley biexcitons and many-body effects in monolayer MoS2". United States. doi:10.1103/physrevb.92.125417. https://www.osti.gov/servlets/purl/1505594.
@article{osti_1505594,
title = {Intervalley biexcitons and many-body effects in monolayer MoS2},
author = {Sie, Edbert J. and Frenzel, Alex J. and Lee, Yi-Hsien and Kong, Jing and Gedik, Nuh},
abstractNote = {Interactions amidst two excitons can result in the formation of bound quasiparticles, known as biexcitons. Their properties are determined by the constituent excitons, with orbital and spin states resembling those of atoms. Monolayer transition metal dichalcogenides (TMDs) present a unique system where excitons acquire a new degree of freedom, the valley pseudospin, from which a novel intervalley biexciton can be created. These biexcitons comprise two excitons from different valleys, which are distinct from biexcitons in conventional semiconductors and have no direct analog in atomic and molecular systems. However, their valley properties are not accessible to traditional transport and optical measurements. Here, we report the observation of intervalley biexcitons in the monolayer TMDMoS2 using ultrafast pump-probe spectroscopy. By applying broadband probe pulses with different helicities, we identify two species of intervalley biexcitons with large binding energies of 60 and 40 meV. Furthermore, we also reveal effects beyond biexcitonic pairwise interactions in which the exciton energy redshifts at increasing exciton densities, indicating the presence of many-body interactions among them.},
doi = {10.1103/physrevb.92.125417},
journal = {Physical Review. B, Condensed Matter and Materials Physics},
number = 12,
volume = 92,
place = {United States},
year = {2015},
month = {9}
}

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Cited by: 45 works
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Figures / Tables:

FIG. 1 FIG. 1: (a) Schematic band structure of the two valleys. (b) Optical transitions to intervalley biexciton state. (c) Measured equilibrium absorbance of monolayer MoS2. (d) Pump-induced absorption of the probe pulses at Δt = 0.3 ps using different helicities. (e) The difference between the two Δα spectra shown in (d),more » where the biexciton binding energies are obtained. (f) Δα spectra at Δt = 4 ps.« less

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.