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Title: Exciton diamagnetic shifts and valley Zeeman effects in monolayer WS2 and MoS2 to 65 Tesla

Journal Article · · Nature Communications
DOI:https://doi.org/10.1038/ncomms10643· OSTI ID:1239580
 [1];  [2];  [2];  [3];  [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Naval Research Lab., Washington, DC (United States)
  3. Rice Univ., Houston, TX (United States)

In bulk and quantum-confined semiconductors, magneto-optical studies have historically played an essential role in determining the fundamental parameters of excitons (size, binding energy, spin, dimensionality and so on). Here we report low-temperature polarized reflection spectroscopy of atomically thin WS2 and MoS2 in high magnetic fields to 65 T. Both the A and B excitons exhibit similar Zeeman splittings of approximately –230 μeV T–1 (g-factor ≃–4), thereby quantifying the valley Zeeman effect in monolayer transition-metal disulphides. Crucially, these large fields also allow observation of the small quadratic diamagnetic shifts of both A and B excitons in monolayer WS2, from which radii of ~1.53 and ~1.16 nm are calculated. Further, when analysed within a model of non-local dielectric screening, these diamagnetic shifts also constrain estimates of the A and B exciton binding energies (410 and 470 meV, respectively, using a reduced A exciton mass of 0.16 times the free electron mass). Lastly, these results highlight the utility of high magnetic fields for understanding new two-dimensional materials.

Research Organization:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC52-06NA25396
OSTI ID:
1239580
Report Number(s):
LA-UR-15-28855; ncomms10643
Journal Information:
Nature Communications, Vol. 7; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 218 works
Citation information provided by
Web of Science

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Synthesis of Co‐Doped MoS 2 Monolayers with Enhanced Valley Splitting journal February 2020
Spatial variations of valley splitting in monolayer transition metal dichalcogenide journal November 2019
Interlayer Excitons in Transition‐Metal Dichalcogenide Heterobilayers journal November 2019
Recent Advances in Quantum Effects of 2D Materials journal April 2019
Determining the Optimized Interlayer Separation Distance in Vertical Stacked 2D WS 2 :hBN:MoS 2 Heterostructures for Exciton Energy Transfer journal February 2018
Valleytronics in transition metal dichalcogenides materials journal August 2019
Recent Progress in the Fabrication, Properties, and Devices of Heterostructures Based on 2D Materials journal February 2019
Valleytronics in 2D materials journal August 2016
Valley- and spin-polarized Landau levels in monolayer WSe2 journal October 2016
Giant valley splitting in monolayer WS2 by magnetic proximity effect journal September 2019
Enhancing and controlling valley magnetic response in MoS2/WS2 heterostructures by all-optical route journal September 2019
Ambipolar Landau levels and strong band-selective carrier interactions in monolayer WSe2 journal March 2018
Spin-polarized electrons in monolayer MoS2 journal March 2019
Light–valley interactions in 2D semiconductors journal July 2018
Identifying defect-related quantum emitters in monolayer WSe2 journal February 2020
The Effect of Preparation Conditions on Raman and Photoluminescence of Monolayer WS2 journal October 2016
Spin polarization and tunable valley degeneracy in a MoS 2 monolayer via proximity coupling to a Cr 2 O 3 substrate journal January 2019
Physics of excitons and their transport in two dimensional transition metal dichalcogenide semiconductors journal January 2019
Discrete quantum dot like emitters in monolayer MoSe 2 : Spatial mapping, magneto-optics, and charge tuning journal April 2016
Comparative study of the exciton binding energies of thin and ultrathin organic-inorganic perovskites due to dielectric mismatch effects journal July 2017
Valley Zeeman splitting of monolayer MoS 2 probed by low-field magnetic circular dichroism spectroscopy at room temperature journal April 2018
Large g factor in bilayer WS 2 flakes journal March 2019
Valleytronic properties of monolayer WSe 2 in external magnetic field journal April 2019
Valley switch effect based on monolayer WSe 2 modulated by circularly polarized light and valley Zeeman field journal June 2019
Spin–flip processes and radiative decay of dark intravalley excitons in transition metal dichalcogenide monolayers journal August 2016
Orbital, spin and valley contributions to Zeeman splitting of excitonic resonances in MoSe 2 , WSe 2 and WS 2 Monolayers journal October 2018
Zeeman spectroscopy of excitons and hybridization of electronic states in few-layer WSe 2 , MoSe 2 and MoTe 2 journal November 2018
Dielectric impact on exciton binding energy and quasiparticle bandgap in monolayer WS 2 and WSe 2 journal March 2019
Fine structure of K-excitons in multilayers of transition metal dichalcogenides journal February 2019
Excitonic magneto-optics in monolayer transition metal dichalcogenides: From nanoribbons to two-dimensional response journal July 2019
Charged excitons in two-dimensional transition metal dichalcogenides: Semiclassical calculation of Berry curvature effects journal September 2019
Robust circular polarization of indirect Q-K transitions in bilayer 3 R W S 2 journal October 2019
Exciton-phonon relaxation bottleneck and radiative decay of thermal exciton reservoir in two-dimensional materials journal November 2016
Signature of Hanle precession in trilayer MoS 2 : Theory and experiment journal May 2017
Interplay of valley polarization and dynamic nuclear polarization in 2D transition metal dichalcogenides journal September 2017
Band nesting, massive Dirac fermions, and valley Landé and Zeeman effects in transition metal dichalcogenides: A tight-binding model journal February 2018
Tunable topological Nernst effect in two-dimensional transition-metal dichalcogenides journal August 2018
Monolayer transition metal dichalcogenides in strong magnetic fields: Validating the Wannier model using a microscopic calculation journal January 2019
Excitonic Linewidth Approaching the Homogeneous Limit in MoS 2 -Based van der Waals Heterostructures journal May 2017
Optical properties of atomically thin transition metal dichalcogenides: observations and puzzles journal January 2017
Controlling neutral and charged excitons in MoS 2 with defects journal January 2020
Valley-selective directional emission from a transition-metal dichalcogenide monolayer mediated by a plasmonic nanoantenna journal January 2018
Synthesis of Co‐Doped MoS 2 Monolayers with Enhanced Valley Splitting journal July 2020
Toward High-Performance Photodetectors Based on 2D Materials: Strategy on Methods journal March 2018
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Enhanced valley splitting in monolayer WSe2 due to magnetic exchange field journal May 2017
Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields journal September 2019
Optical initialization of a single spin-valley in charged WSe2 quantum dots journal March 2019
Spectrally narrow exciton luminescence from monolayer MoS 2 and MoSe 2 exfoliated onto epitaxially grown hexagonal BN journal July 2018
Long-lived photoluminescence polarization of localized excitons in liquid exfoliated monolayer enriched WS 2 journal June 2018
Controlling valley splitting and polarization of dark- and bi-excitons in monolayer WS 2 by a tilted magnetic field journal July 2019
Exciton states and absorption spectra in freestanding monolayer transition metal dichalcogenides: A variationally optimized diagonalization method journal September 2019
Excitonic magneto-optical Kerr effect in two-dimensional transition metal dichalcogenides induced by spin proximity journal January 2020
Large room-temperature valley polarization by valley-selective switching of exciton ground state journal February 2020
Magnetooptics of Exciton Rydberg States in a Monolayer Semiconductor journal February 2018
Coulomb engineering of the bandgap and excitons in two-dimensional materials text January 2017
Coulomb engineering of the bandgap and excitons in two-dimensional materials text January 2017
Magnetic Proximity Effects in Transition-Metal Dichalcogenides: Converting Excitons text January 2017
Coulomb engineering of the bandgap and excitons in two-dimensional materials journal May 2017
Spin-flip processes and radiative decay of dark intravalley excitons in transition metal dichalcogenide monolayers text January 2016
Exciton-phonon relaxation bottleneck and radiative decay of thermal exciton reservoir in two-dimensional materials text January 2016
The Effect of Preparation Conditions on Raman and Photoluminescence of Monolayer WS2 text January 2016
Magnetic Proximity Effects in Transition-Metal Dichalcogenides: Converting Excitons text January 2017
Interplay of valley polarization and dynamic nuclear polarization in 2D transition metal dichalcogenides text January 2017
Ambipolar Landau levels and strong band-selective carrier interactions in monolayer WSe$_2$ text January 2017
Dynamical screening in monolayer transition-metal dichalcogenides and its manifestations in the exciton spectrum text January 2018
Charged exctions in two-dimensional transition-metal dichalcogenides - semiclassical calculation of Berry-curvature effects text January 2018
Identifying defect-related quantum emitters in monolayer WSe$_2$ text January 2020
Controlling valley splitting and Polarization of dark- and bi-excitons in monolayer WS$_2$ by a tilted magnetic field text January 2020
The valley Zeeman effect in inter- and intra-valley trions in monolayer WSe2 journal May 2019
Optical control of a single spin-valley in charged WSe$_2$ quantum dots text January 2018
Giant Valley Splitting in Monolayer WS2 by Magnetic Proximity Effect text January 2019
Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields text January 2019
Optical control of valley Zeeman effect through many-exciton interactions text January 2020
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Excitons in monolayer semiconductors in complex environments and under external fields text January 2020