Data from: Gate-tunable chiral spin mode in WSe2/WS2 moiré superlattices
Data files
Oct 01, 2026 version files 6.36 MB
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Fig._1D_reflectance_contrast.xlsx
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Fig._2.xlsx
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Fig._3B_D_E_doping_dependence_of_Raman_spectrum.xlsx
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Fig._4A-C_magnetic-field_dependences.xlsx
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Fig._4E-I_temperature_dependences.xlsx
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FIG.S1.xlsx
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FIG.S10.xlsx
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FIG.S11.xlsx
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FIG.S12.xlsx
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FIG.S13.xlsx
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FIG.S14.xlsx
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FIG.S15.xlsx
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FIG.S16.xlsx
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FIG.S17.xlsx
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FIG.S2.xlsx
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FIG.S3.xlsx
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FIG.S4.xlsx
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FIG.S5.xlsx
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FIG.S6.xlsx
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FIG.S7.xlsx
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FIG.S8.xlsx
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FIG.S9.xlsx
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README.md
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Abstract
The interplay between many-body and spin-orbit effects (SOC) can lead to novel phenomena in solids. Chiral spin modes (CSM) are collective spin excitations that arise from such interplay and connect states with opposite chirality, which, however, have been rarely observed. Here, we report a gate-tunable CSM that occurs between conduction SOC-split minibands in near-0-twisted WSe2/WS2 heterobilayers. This mode manifests as a sharp resonance with giant Raman efficiency in the pseudovector-symmetry channel of the Raman spectra. By varying the filling, the CSM transitions from a chiral spin exciton to an excitonic polaron. The spin-flip nature is directly confirmed by the Zeeman effect. Moreover, the filling dependence compellingly evidences a charge-transfer insulator at filling of one. Our results demonstrate transition-metal-dichalcogenides moiré superlattices as a fertile platform for exploring exotic low-lying collective excitations.
https://doi.org/10.5061/dryad.dr7sqvb8n
Description of the data and file structure
This dataset contains optical spectroscopy data from WSe2/WS2 moiré superlattice devices, including doping-dependent reflectance spectra, polarization-resolved, magnetic-field-dependent, and temperature-dependent Raman measurements. The data comprise individual spectra, extracted spectral parameters, and corresponding statistical information, and are organized according to the sequence of figures presented in the article entitled “Gate-tunable chiral spin mode in WSe2/WS2 moiré superlattices.” The dataset also includes measurements from an additional near-0°-twisted device, enabling comparison and reproducibility. For detailed descriptions of device fabrication, experimental procedures, data processing, and instrumentation, please refer to the published article and its Supplementary Materials.
Files and variables
File: Fig._1D_reflectance_contrast.xlsx
Description: This file contains the doping-dependent reflectance-contrast data presented in Figure 1D. The data reveal correlated insulating states in the near-0°-twisted WSe2/WS2 moiré superlattice at representative fillings. The maximum reflectance contrast was extracted within the photon-energy range from 1.65 to 1.72 eV.
Variables:
- Gate voltage,
(V): Applied dual-gate voltage used to tune carrier density. - Filling factor,
: Number of electrons per moiré unit cell. - Photon energy (eV): Energy of the signal in the reflectance-contrast measurement.
- Reflectance contrast R: Defined as the ratio of the reflected light spectrum and
the reference spectrum. - Maximum reflectance contrast: Maximum value of R within the photon energy range from 1.65 to 1.72 eV.
File: Fig._2.xlsx
Description: This file contains the polarization-resolved Raman spectra of the moiré superlattice. The measurements were performed at a filling factor of
2 with an excitation energy of 2.33 eV in four polarization configurations: XX, XY, RR, and RL. The A1, A2, and E symmetry channels were extracted from the polarization-resolved Raman spectra based on the C3v point-group selection rules. A sharp low-energy resonance is observed in the A2 channel and is assigned to the chiral spin mode (CSM).
Variables:
- Raman shift (cm-1): Energy shift between the incident and scattered photons.
- Raman intensity (a.u.): Measured Raman-scattering intensity.
- Polarization configuration: XX, XY, RR, and RL denote parallel-linear, cross-linear, co-circular, and cross-circular polarization configurations, respectively.
- Raman symmetry channel: A1, A2, and E channels extracted from the polarization-resolved Raman spectra.
File: Fig._3B_D_E_doping_dependence_of_Raman_spectrum.xlsx
Description: This file contains filling-dependent A2-channel Raman spectra of the moiré superlattice. Sheet “Panel B” provides A2-channel Raman spectra as a function of filling factor over the electron-doping range from 1 to 3
. Sheet “Panel D” provides the filling dependence of the CSM spectral weight. Sheet “Panel E” provides the filling dependence of the CSM frequency.
Variables:
- Filling factor: Number of electrons per moiré unit cell.
- Raman shift (cm-1): Energy shift between the incident and scattered photons.
- Raman intensity (a.u.): Measured Raman-scattering intensity.
- CSM spectral parameters: Spectral weight and mode frequency of the CSM extracted from the Raman spectra.
File: Fig._4A-C_magnetic-field_dependences.xlsx
Description: This file contains magnetic-field-dependent Raman data of the CSM at
. Sheet “Panel A” provides normalized A2-channel Raman spectra measured under varying out-of-plane magnetic fields. Sheets “Panel B” and “Panel C” provide the magnetic-field dependence of the CSM frequency and deconvoluted full width at half maximum (FWHM), respectively.
Variables:
- Magnetic field, B (T): Applied out-of-plane magnetic field.
- Raman shift (cm-1): Energy shift between the incident and scattered photons.
- Normalized A2-channel Raman intensity (a.u.): Normalized Raman response in the A2 symmetry channel.
- CSM spectral parameters: Mode frequency and deconvoluted FWHM of the CSM extracted from the Raman spectra.
File: Fig._4E-I_temperature_dependences.xlsx
Description: This file contains temperature-dependent Raman and reflectance-contrast data of the moiré superlattice. Sheet “Panel E” provides temperature-dependent A2-channel Raman spectra at
filling of 2. Sheet “Panel F” provides filling-dependent maximum reflectance contrast, measured at different temperatures. Sheets “Panel G”, “Panel H”, and “Panel I” provide the temperature dependence of the CSM spectral weight, mode frequency, and deconvoluted FWHM, respectively.
Variables:
- Temperature, T (K): Sample temperature during Raman or reflectance-contrast measurements.
- Filling factor, ν: Number of electrons per moiré unit cell.
- Raman shift (cm-1): Energy shift between the incident and scattered photons.
- Maximum reflectance contrast,
: Maximum value of R within the photon energy range from 1.65 to 1.72 eV. - CSM spectral parameters: Spectral weight, mode frequency, and deconvoluted FWHM of the CSM extracted from the Raman spectra.
File: FIG.S1.xlsx
Description: This file contains reflectance-contrast and photoluminescence (PL) data used to assign the filling factor of the moiré superlattice. Sheet “Panel A” provides doping-dependent reflectance-contrast spectra and the corresponding maximum reflectance contrast,
, around the WSe2 A-exciton resonance. Sheet “Panel B” provides doping-dependent PL spectra and the extracted PL peak energy. The reflectance-contrast and photoluminescence measurements were performed under the same excitation conditions, with a laser energy of 2.33 eV and a power of 1 μW.
Variables:
- Gate voltage,
Vg (V): Applied dual-gate voltage used to tune electron density. - Filling factor, ν: Number of electrons per moiré unit cell.
- Photon energy (eV): Energy of signal in the reflectance-contrast or PL measurements.
- Reflectance contrast, R, and maximum reflectance contrast
: Reflectance contrast and its maximum value around the WSe2 A-exciton resonance. - PL intensity (a.u.) and peak energy (eV): Measured PL signal and extracted peak position.
File: FIG.S2.xlsx
Description: This file contains power-dependent polarization-resolved Raman data of the moiré superlattice. Sheets “Panel A”, “Panel C”, and “Panel E” provide Raman spectra in the XX, RL, and XY polarization configurations, respectively, at excitation powers ranging from 0.5 to 8 uW
. Sheets “Panel B” and “Panel D” provide the integrated Raman intensities in the XX and RL configurations. Sheets “Panel F”, “Panel G”, and “Panel H” provide the power dependence of the CSM integrated intensity, mode frequency, and deconvoluted FWHM, respectively.
Variables:
- Excitation power (μW): Incident laser power.
- Raman shift (cm-1): Energy shift between the incident and scattered photons.
- Raman intensity (a.u.): Measured Raman-scattering intensity.
- CSM spectral parameters: Integrated intensity, mode frequency, and deconvoluted FWHM.
File: FIG.S3.xlsx
Description: This file contains polarization-angle-dependent Raman data at
. Sheets “Panel A” to “Panel D” present parallel-polarized (XX) and cross-polarized (XY) Raman spectra measured at orientation angles of 0
, 50
, 90
, and 140
degrees, respectively. Sheets “Panel E” to “Panel G” provide the angular dependence of the integrated intensities of the A1-channel modes and the CSM.
Variables:
- Polarization angle
(degree): Orientation of the incident linear polarization relative to the device axis. - Raman shift (cm-1): Energy shift between the incident and scattered photons.
- Raman intensity (a.u.): Measured Raman-scattering intensity.
- Integrated mode intensity (a.u.): Integrated intensities of the A1-channel modes and CSM.
File: FIG.S4.xlsx
Description: This file contains doping-dependent polarized Raman spectra over an extended filling range. Sheets “Panel A” to “Panel D” provide spectra measured in the XX, XY, RR, and RL polarization configurations, respectively. Sheets “Panel E” to “Panel G” provide the corresponding Raman spectra extracted in the A1, A2, and E symmetry channels.
Variables:
- Filling factor, ν: Number of electrons per moiré unit cell.
- Raman shift (cm-1): Energy shift between the incident and scattered photons.
- Raman intensity (a.u.): Measured Raman-scattering intensity.
- Polarization configuration or symmetry channel: XX, XY, RR, and RL denote polarization configurations; A1, A2, and E denote symmetry-resolved channels.
File: FIG.S5.xlsx
Description: This file contains reproducibility measurements from an additional near-0
-twisted WSe2/WS2 moiré-superlattice device. Sheet “Panel A” presents doping-dependent reflectance-contrast spectra. Sheet “Panel B” provides filling-dependent Raman spectra in the A2 channel. Sheets “Panel C” and “Panel D” show the filling dependence of the CSM frequency and spectral weight, respectively.
Variables:
- Filling factor, ν: Number of electrons per moiré unit cell.
- Photon energy or Raman shift (eV or cm-1): Spectral energy scale for reflectance-contrast or Raman measurements.
- CSM spectral parameters: Mode frequency and spectral weight.
File: FIG.S6.xlsx
Description: This file contains control measurements on near-60
-twisted and 20
-twisted WSe2/WS2 bilayers, in which no CSM is observed. Sheets “Panel A” to “Panel C” present reflectance-contrast and polarization-resolved Raman data from the near-60
-twisted bilayer using an excitation energy of 2.33 eV. Sheets “Panel D” to “Panel F” provide similar measurements using an excitation energy of 1.959 eV. Sheets “Panel G” to “Panel I” provide corresponding measurements from the 20°-twisted bilayer.
Variables:
- Gate voltage
(V): Applied dual-gate voltage used to tune electron density. - Photon energy or Raman shift (eV or cm-1): Spectral energy scale for the optical measurements.
- Reflectance contrast, R: Defined as
the ratio of the reflected light spectrum and
the reference spectrum. - Polarized Raman intensity (a.u.): Raman intensity measured in the specified polarization configuration.
File: FIG.S7.xlsx
Description: This file contains density-functional-theory (DFT) calculation data for the near-0
-twisted WSe2/WS2 moiré superlattice. Sheet “Panel B” provides the conduction miniband structure.
Variables:
- Wave vector: Momentum along the calculated miniband path.
- Energy (eV): Calculated conduction-miniband energy.
- Miniband index: C1, C1', C2, and C2' denote the four lowest-energy conduction minibands.
File: FIG.S8.xlsx
Description: This file contains reflectance-contrast and polarization-resolved Raman data measured with an excitation energy of 2.33 eV, close to the WS2 B-exciton resonance. Sheets “Panel A” to “Panel D” provide doping-dependent reflectance-contrast spectra, representative line cuts, reflectance contrast at 2.33 eV, and the B-exciton resonance magnitude. Sheets “Panel F” and “Panel G” provide filling-dependent Raman spectra in the XX and XY polarization configurations. Sheets “Panel H”, “Panel I”, and “Panel J” show the filling dependence of A1-channel spectral weight, CSM frequency, and CSM spectral weight, respectively.
Variables:
- Filling factor, ν: Number of electrons per moiré unit cell.
- Photon energy or Raman shift (eV or cm-1): Spectral energy scale for reflectance-contrast or Raman measurements.
- Reflectance contrast or Raman intensity (a.u.): Measured optical response.
- CSM spectral parameters: Mode frequency and spectral weight.
File: FIG.S9.xlsx
Description: This file contains reflectance-contrast and polarization-resolved Raman data measured with an excitation energy of 1.959 eV, close to the WS2 A-exciton resonance. Sheets “Panel A” to “Panel D” provide doping-dependent reflectance-contrast spectra, representative line cuts, reflectance contrast at 1.959 eV, and the A-exciton resonance magnitude. Sheets “Panel F” and “Panel G” provide filling-dependent Raman spectra in the XX and XY polarization configurations. Sheets “Panel H”, “Panel I”, and “Panel J” show the filling dependence of A1-channel spectral weight, CSM frequency, and CSM spectral weight, respectively.
Variables:
- Filling factor, ν: Number of electrons per moiré unit cell.
- Photon energy or Raman shift (eV or cm-1): Spectral energy scale for reflectance-contrast or Raman measurements.
- Reflectance contrast or Raman intensity (a.u.): Measured optical response.
- CSM spectral parameters: Mode frequency and spectral weight.
File: FIG.S10.xlsx
Description: This file contains control measurements performed with an excitation energy of 1.58 eV, for which no CSM is observed. Sheet “Panel A” provides doping-dependent reflectance-contrast spectra. Sheets “Panel B”, and “Panel C” provide doping-dependent Raman spectra in the XX and XY polarization configurations, respectively.
Variables:
- Filling factor, ν: Number of electrons per moiré unit cell.
- Photon energy or Raman shift (eV or cm-1): Spectral energy scale for reflectance-contrast or Raman measurements.
- Reflectance contrast or Raman intensity (a.u.): Measured optical response.
File: FIG.S11.xlsx
Description: This file contains polarization-dependent Raman data of the CSM at filling of 2
under an out-of-plane magnetic field of 9 T. Sheet “Panel A” provides Raman spectra measured in the XX, XY, RR, RL, LL, and LR polarization configurations. Sheet “Panel B” provides the A2-channel Raman spectra extracted from the XY, RR, and LL configurations.
Variables:
- Raman shift (cm-1): Energy shift between the incident and scattered photons.
- Raman intensity (a.u.): Measured Raman-scattering intensity.
- Polarization configuration: XX, XY, RR, RL, LL, and LR polarization configurations.
- A2-channel Raman intensity (a.u.): Raman response extracted in the A₂ symmetry channel.
File: FIG.S12.xlsx
Description: This file contains Raman-efficiency calibration data for the CSM. Sheet “Panel A” provides the CSM Raman spectrum at
, while Sheet “Panel B” provides the Raman spectrum of the G phonon of single-layer graphene. Both measurements were performed in the XY configuration under the same incident power and exposure time.
Variables:
- Raman shift (cm-1): Energy shift between the incident and scattered photons.
- Raman intensity (a.u.): Measured Raman-scattering intensity.
- Sample: WSe2/WS2 moiré superlattice or single-layer graphene.
- Raman efficiency cm-1 sr-1): Raman scattering efficiency determined by sample substitution method.
File: FIG.S13.xlsx
Description: This file contains polarization-angle-dependent second-harmonic-generation (SHG) data used to characterize the twist angle of the moiré superlattice. Sheet “Panel C” provides SHG intensity as a function of polarization angle for the monolayer WSe2 and bilayer regions.
Variables:
- Polarization angle (degrees): Orientation of the excitation polarization.
- SHG intensity (a.u.): Measured second-harmonic-generation intensity.
- Measurement region: Monolayer WSe2 or WSe2/WS2 bilayer region.
File: FIG.S14.xlsx
Description: This file contains doping-dependent reflectance-contrast spectra measured without and with laser excitation. Sheets “Panel A” and “Panel B” provide the reflectance-contrast spectra without and with laser excitation, respectively, demonstrating laser-induced gate voltage shifts at representative fillings. Measurements were performed with a laser energy of 2.33 eV and a power of 1 μW.
Variables:
- Gate voltage Vg
(V): Applied dual-gate voltage used to tune carrier density.
- Photon energy (eV): Energy of signal in the reflectance-contrast measurement.
- Reflectance contrast, R: Defined as
the ratio between the reflected light spectrum and
the reference spectrum. - Laser condition: Measurements performed with or without laser excitation.
File: FIG.S15.xlsx
Description: This file contains a comparison of CSM spectral parameters obtained from Voigt analyses with and without a baseline. Sheets “Panel A” and “Panel B” provide A2-channel Raman spectra at selected filling factors analyzed with and without a baseline, respectively. Sheets “Panel C”, “Panel D”, and “Panel E” provide the resulting filling dependence of CSM frequency, spectral weight, and deconvoluted FWHM.
Variables:
- Filling factor,
: Number of electrons per moiré unit cell. - Raman shift (cm-1): Energy shift between the incident and scattered photons.
- Baseline condition: Spectral analysis performed with or without a baseline.
- CSM spectral parameters: Mode frequency, spectral weight, and deconvoluted FWHM of the CSM extracted from the Raman spectra.
File: FIG.S16.xlsx
Description: This file contains a comparison between Voigt and Fano analyses of the CSM at excitation energies of 2.33 eV and 1.959 eV. Sheets “Panel A” to “Panel E” provide spectra and extracted CSM parameters obtained at 2.33 eV. Sheets “Panel F” to “Panel J” provide the corresponding data obtained at 1.959 eV. The extracted parameters include mode frequency, deconvoluted FWHM, and Fano factor q.
Variables:
- Filling factor,
: Number of electrons per moiré unit cell. - Raman shift (cm-1): Energy shift between the incident and scattered photons.
- Excitation energy (eV): Energy of the incident laser.
- CSM spectral parameters: Mode frequency, deconvoluted FWHM, and Fano factor q of the CSM extracted from the Raman spectra.
File: FIG.S17.xlsx
Description: This file contains Stokes and anti-Stokes Raman spectra of the CSM at
under out-of-plane magnetic fields of 0 T, +4 T, and −4 T. Sheets “Panel A,” “Panel B”, and “Panel C” provide polarized Raman spectra measured at 0 T, +4 T, and −4 T, respectively. Spectra containing the CSM were normalized to the Stokes-peak intensity.
Variables:
- Magnetic field, B (T): Applied out-of-plane magnetic field.
- Raman shift (cm-1): Energy shift between the incident and scattered photons.
- Raman intensity (a.u.): Measured Raman-scattering intensity.
- Polarization configuration: XX, XY, RR, RL, LL, and LR polarization configurations.
