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Proximity-induced chiral quantum light generation in strain-engineered WSe2/NiPS3 heterostructures

Nature Materials volume 22, pages 1311–1316 (2023)Cite this article

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Abstract

Quantum light emitters capable of generating single photons with circular polarization and non-classical statistics could enable non-reciprocal single-photon devices and deterministic spin–photon interfaces for quantum networks. To date, the emission of such chiral quantum light relies on the application of intense external magnetic fields, electrical/optical injection of spin-polarized carriers/excitons or coupling with complex photonic metastructures. Here we report the creation of free-space chiral quantum light emitters via the nanoindentation of monolayer WSe2/NiPS3 heterostructures at zero external magnetic field. These quantum light emitters emit with a high degree of circular polarization (0.89) and single-photon purity (95%), independent of pump laser polarization. Scanning diamond nitrogen-vacancy microscopy and temperature-dependent magneto-photoluminescence studies reveal that the chiral quantum light emission arises from magnetic proximity interactions between localized excitons in the WSe2 monolayer and the out-of-plane magnetization of defects in the antiferromagnetic order of NiPS3, both of which are co-localized by strain fields associated with the nanoscale indentations.

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Fig. 1: Strain-engineered WSe2/NiPS3 heterostructures host QEs displaying sharp, localized PL peaks with a strong degree of spontaneous circular polarization.
Fig. 2: Demonstration of quantum light emission from strain-engineered WSe2/NiPS3 heterostructures.
Fig. 3: Correlation of chiral quantum light emission with local magnetization.
Fig. 4: Magneto-PL studies of chiral QEs.

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Source data are provided with this paper. All other data supporting the plots within this paper and other findings of this study are available from the Supplementary Information or from the corresponding author upon reasonable request.

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Acknowledgements

This work was performed at the Center for Integrated Nanotechnologies, an Office of Science User Facility, operated for the US Department of Energy (DOE) Office of Science (OS). Los Alamos National Laboratory (LANL), an affirmative action equal opportunity employer, is managed by Triad National Security LLC for the US DOE’s NNSA, under contract 89233218CNA000001. Laboratory Directed Research and Development (LDRD) program 20200104DR provided primary support for the works of X.L., H.Z., A.P., N.S., S.A.C. and H.H. A.C.J. and V.C. acknowledge support from the DOE Basic Energy Sciences, QIS Infrastructure Development Program, Deterministic Placement and Integration of Quantum Defects. X.L., H.H. and S.A.C. also acknowledge partial support by the Quantum Science Center, a National QIS Research Center supported by the DOE, OS. J.C. and H.Z. also acknowledge partial support from LANL Director’s Postdoctoral Fellow Award. M.T.P. acknowledges support from LDRD awards 20210782ER and 20210640ECR. The National High Magnetic Field Laboratory is supported by the National Science Foundation (NSF) DMR-1644779, the State of Florida, and the US DOE. P.M., D.A.B., M.A.T. and P.R. acknowledge financial support from the National Centre of Competence in Research (NCCR) Quantum Science and Technology (QSIT), a competence centre funded by the Swiss National Science Foundation (SNF), by SNF project no. 188521, and by the ERC consolidator grant project QS2DM. We would like to acknowledge B. Zhou and X. Zhang for the magnetometry experiments using a near-surface ensemble of NV centres, and E. Peterson and C. A. Lane for insightful discussions on the magnetic-exchange proximity interaction.

Author information

Authors and Affiliations

  1. Center for Integrated Nanotechnologies, Materials Physics and Applications Division, Los Alamos National Laboratory, Los Alamos, NM, USA

    Xiangzhi Li, Andrew C. Jones, Huan Zhao, Vigneshwaran Chandrasekaran, Michael T. Pettes & Han Htoon

  2. National High Magnetic Field Laboratory, Materials Physics and Applications Division, Los Alamos National Laboratory, Los Alamos, NM, USA

    Junho Choi & Scott A. Crooker

  3. Theoretical Division, Los Alamos National Laboratory, Los Alamos, NM, USA

    Andrei Piryatinski & Nikolai Sinitsyn

  4. Department of Physics, University of Basel, Basel, Switzerland

    Märta A. Tschudin, Patrick Reiser, David A. Broadway & Patrick Maletinsky

Authors
  1. Xiangzhi Li
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Contributions

H.H. conceived and led the experiment. X.L., under the supervision of H.H., initiated the idea of using the nanoindentation method for enhancing the magnetic proximity effect along with the deterministic creation of localized QEs, prepared the samples and conducted the experiments. A.C.J. guided X.L. in creating nanoindentations in the WSe2/NiPS3 heterostructure and scanning probe microscopy studies. S.A.C. contributed the key idea of the temperature-dependent magneto-PL experiment and X.L. and J.C. conducted the experiment. H.Z., M.T.P. and V.C. assisted X.L. in a variety of optical spectroscopy experiments. N.S. and A.P. provided the theoretical model. D.A.B., M.A.T. and P.R. performed the NV magnetometry measurements under the supervision of P.M. H.H. and X.L. wrote the manuscript with the assistance of all the authors.

Corresponding author

Correspondence to Han Htoon.

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Extended data

Extended Data Fig. 1 Experimental setup for low-temperature polarization resolved PL spectroscopy.

a. OBJ: Objective, DM: Dichroic mirror, QWP: quarter-wave plate, WP: Wollaston prism. For the linear polarization measurements, QWP is removed and two half-wave plates (HWP1 and HWP2) are inserted in excitation and collection channels. b. Schematic of the HBT experiment. BS: 50/50 beam splitter, APD1, APD2: Avalanche photo diodes, Counter: Hydra400 TCSPC module.

Extended Data Fig. 2 Control experiments.

a-d. Low temperature, σ+/- polarized PL spectra of WSe2 monolayer, region R1 of Fig. 1b(a, b) and un-indented WSe2/NiPS3 heterostructure, region R2 of Fig. 1b(c, d) excited by σ+ (a, c) and σ- (b, d) 514 nm laser. The data show no detectable DCP in the emission of both monolayer and un-indented WSe2/NiPS3 hetrostructure indicating that spin-polarized excitons injected at 514 nm were depolarized completely upon relaxation to the band-edge. e, f. Low temperature, linearly (S, P) polarized PL spectra (left panel) and plot of DLP as the function of polarization detection angle (right panel) for the sharp emission peak at 1.47 eV (e) and WSe2 exciton emission (f). (g) Upper Panel. Strong DLP (0.76) observed for 1.47 eV sharp emission peak is consistent with prior studies that attributed the emission to highly anisotropic excitons reflecting the emergence of AFM order in NiPS3. Lower Panel. PL of unstrained WSe2/NiPS3 heterostructure shows a weak degree of linear polarization consistent with the behavior of WSe2 monolayer.

Source data

Extended Data Fig. 3 Control experiment and invariance of circularly polarized PL emission under laser excitation of different polarization.

a. σ+/σ- polarization resolved PL spectra from WSe2/hBN/PMMA structures with similar nano-indents of Fig. 1, acquired under σ+(left) and σ- (right) polarized laser excitation, respectively. While localized exciton emission peaks of similar line shapes were created, no circularly polarized emission were detected. b. σ+/σ- polarization resolved PL spectra from 3 nano-indents of Fig. 1a, b acquired under σ+(left) and σ- (right) polarized laser excitation, respectively. While most nano-indents show circularly polarized localized exciton emission (bottom two panels), some show no circular polarization (top panels). When the excitation laser polarization is switched from σ+ to σ-, the polarities of the circularly polarized emission peak remain the same (peak marked a and b) but some quantitative change in DCPs as well as relative intensities of the localized PL peaks occur. c. Circularly polarized PL emission also remain qualitatively the same when the orientation of linearly polarized PL excitation is changed from 0 – 60 degree.

Source data

Extended Data Fig. 4 Spectral image and analysis of the spatial distribution of PL intensity.

a. PL spectral image of a nanoindentation in Fig. 1 a,b. σ+ and σ- PL emissions are simultaneously recorded on two different regions of the CCD array (upper). Degree of circular polarization (DoCP) spectrum calculated from integrated σ+ and σ- PL spectra (lower). b. Magnified spectra image of the region marked in (a). c. Blue data points: Intensity distribution of the localized emission peaks marked 1-5 in (b). By fitting the PL intensity distribution with Gaussian function (black fitted curves), we can determine the centroid of the emission peak with ± 0.1 pixel precision. The position of each peak and fitting error is listed next to the peak. Based on the magnification factor of the microscope objective (50X) and pixel dimensions of the CCD (20 μm), we can estimate that all peaks, marked 1- 5 originated from slightly different locations around the nano-indents. The separation between Peak 2 and 3 is ~ 50 nm.

Source data

Extended Data Fig. 5 Analyzing linear polarization of strain-engineered WSe2/NiPS3 heterostructure and distribution of linewidth of chiral quantum emitters and pump-dependent measurements.

a, top panel. σ+/σ- polarized PL spectra acquired under σ+ excitation. Inset. Zoom-in view of the NiPS3 anisotropic exciton peak displaying peak DCP of 0.4. lower panels. S and P linearly polarized PL spectra acquired at different polarization detection angles indicated in the panels. All three spectra are excited by σ+ polarized laser in the same way as the top panel. b. DLP of NiPS3 anisotropic exciton (red data points and trace of top panel) and PL peak 1-3 (lower panels) as the function of polarization detection angle. Black data points and trace plot DLP of NiPS3 anisotropic excitons in unstrained NiPS3. c. Histogram of the linewidths of chiral quantum light emitters yielding 3.6 ± 1.3 meV average and standard deviation, respectively. ~40% of the QEs display linewidth narrower than 3 meV. We believe the linewidth can be further minimized via encapsulation in hBN. Both linewidth and chirality show no notable dependence on laser excitation power. d. Pump-dependent study of a nanoindentation with two circularly polarized PL peaks. e, f. The plot of DCP and linewidth as the function of the pump displays a little change over 3 orders of magnitude change in pump power. The DCP of peaks a & b is calculated by taking the rise of the un-polarized PL background into account.

Source data

Extended Data Fig. 6 Another Chiral Quantum Light Emitter showing -0.7 DCP and 96% single photon purity.

a. Chiral PL spectra (σ+ (blue) and σ- (red)) of another indentation spot under linearly polarized laser excitation showing >70% of DCP. b. PL intensity time trace, c. PL decay curve, d. 2nd order photon correlation trace collected at 10 K showing a g(2)(0) = 0.04.

Source data

Extended Data Fig. 7 Room temperature (RT) scanning diamond NV microscopy study of indented NiPS3.

a. Topographical image of the indentation shown in Fig. 3c. The RT scanning NV system utilized a slightly sharper NV probe yielding a higher resolution topographical image. b. Magnetic field image of the same area showing only the noise.

Source data

Extended Data Fig. 8 Complete data set for Fig. 4a.

Center panel. Low-temperature σ+ and σ- polarized PL spectra acquired under -6.0 T to +6.0 T external magnetic field applied perpendicular to the sample plane. Left and right panels. Zoom-in view of the gray and red spectra ranges of the center panels. Because magneto-PL spectra were acquired under 633 nm σ+ laser excitation, a weak DCP is observed at zero B field. A weak magnetic field-dependent change in DCP likely resulting from field-induced polarization of localized excitons is also observed in the 1.65 to 1.70 eV spectral range.

Source data

Extended Data Fig. 9 Complete data set for Figs. 4c and 4d.

a-b, c-d. Complete B field dependent σ+/- polarized PL spectra shown in the bottom 3 panels of Fig. 4c and Fig. 4d. e-f. After chiral emission is fully restored at 0 T in b, PL spectra of the same location were collected by sweeping the field from 0 T to 6 T and then 6 T to -6 T.

Source data

Extended Data Fig. 10 Observation of Chiral Localized Exciton Emission from WSe2/FePS3 and WSe2/MnPS3 heterostructures with nano-indents.

a-b. Optical images of the WSe2/FePS3 (a) and WSe2/MnPS3 (b) heterostructures with nano-indents. c-d. σ+ and σ- polarized PL spectra acquired under linearly polarized laser excitation at 4 K from two different nano-indents of WSe2/FePS3 (c) and WSe2/MnPS3 (d), respectively.

Source data

Supplementary information

Supplementary Information

Discussion on competition between anisotropic exchange and Zeeman splitting.

Source data

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Li, X., Jones, A.C., Choi, J. et al. Proximity-induced chiral quantum light generation in strain-engineered WSe2/NiPS3 heterostructures. Nat. Mater. 22, 1311–1316 (2023). https://doi.org/10.1038/s41563-023-01645-7

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