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Room-temperature spin injection across a chiral perovskite/III–V interface

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Abstract

Spin accumulation in semiconductor structures at room temperature and without magnetic fields is key to enable a broader range of optoelectronic functionality1. Current efforts are limited owing to inherent inefficiencies associated with spin injection across semiconductor interfaces2. Here we demonstrate spin injection across chiral halide perovskite/III–V interfaces achieving spin accumulation in a standard semiconductor III–V (AlxGa1−x)0.5In0.5P multiple quantum well light-emitting diode. The spin accumulation in the multiple quantum well is detected through emission of circularly polarized light with a degree of polarization of up to 15 ± 4%. The chiral perovskite/III–V interface was characterized with X-ray photoelectron spectroscopy, cross-sectional scanning Kelvin probe force microscopy and cross-sectional transmission electron microscopy imaging, showing a clean semiconductor/semiconductor interface at which the Fermi level can equilibrate. These findings demonstrate that chiral perovskite semiconductors can transform well-developed semiconductor platforms into ones that can also control spin.

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Fig. 1: LED schematic and interface characterization.
Fig. 2: CP-EL emission of (R/S-MBA)2PbI4/(AlxGa1−x)0.5In0.5P spin-LEDs.
Fig. 3: Band alignment and LED operation.

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Data availability

The experimental data used in this paper are freely available at the open science framework https://doi.org/10.17605/OSF.IO/2M35K.

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Acknowledgements

This work was supported as part of the Center for Hybrid Organic-Inorganic Semiconductors for Energy (CHOISE), an Energy Frontier Research Center financed by the Office of Basic Energy Sciences, Office of Science in the US Department of Energy (DOE). This work was authored in part by the National Renewable Energy Laboratory (NREL), operated by Alliance for Sustainable Energy, LLC, for the DOE under contract no. DE-AC36-08GO28308. The views expressed in the article do not necessarily represent the views of the DOE or the US government. Support for structural and microscopy characterization and LED characterization was provided by a Laboratory Directed Research and Development project financed by the NREL. This work was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the DOE Office of Science by Los Alamos National Laboratory (contract 89233218CNA000001) and Sandia National Laboratories (contract DE-NA-0003525). Y.L. acknowledges the support by the French National Research Agency (ANR) SOTspinLED project (no. ANR-22-CE24-0006-01). We thank I. Hinz and C. Velez for their assistance with depositing alumina. The AlGaInP LED device structures were grown by A. Wibowo at MicroLink Devices with funding from the US Department of Energy, Office of Energy Efficiency and Renewable Energy, Buildings Technologies Office.

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Authors and Affiliations

  1. National Renewable Energy Laboratory (NREL), Golden, CO, USA

    Matthew P. Hautzinger, Steven C. Hayden, Jiselle Y. Ye, Qi Jiang, Mickey J. Wilson, Alan J. Phillips, Yifan Dong, Emily K. Raulerson, Ian A. Leahy, Chun-Sheng Jiang, Jeffrey L. Blackburn, Joseph M. Luther, Katherine Jungjohann, Joseph J. Berry, Kirstin Alberi & Matthew C. Beard

  2. Department of Physics & Astronomy, University of Utah, Salt Lake City, UT, USA

    Xin Pan & Z. Valy Vardeny

  3. Department of Physics, Colorado School of Mines, Golden, CO, USA

    Jiselle Y. Ye & Alan J. Phillips

  4. Renewable and Sustainable Energy Institute, University of Colorado Boulder, Boulder, CO, USA

    Joseph M. Luther, Joseph J. Berry, Kirstin Alberi & Matthew C. Beard

  5. Institut Jean Lamour, Université de Lorraine, CNRS, UMR 7198, Nancy, France

    Yuan Lu

  6. Department of Physics, University of Colorado Boulder, Boulder, CO, USA

    Joseph J. Berry

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Contributions

M.P.H., M.C.B., K.A., J.M.L., J.J.B. and Y.L. conceived the research idea and designed the experiments. M.P.H. fabricated the LEDs and measured the CP-EL. M.J.W. deposited the IZO. J.Y.Y. performed XPS. Q.J. and I.A.L. aided in the LED fabrication process and basic LED characterizations. Y.D., A.J.P., J.L.B. and E.K.R. performed spectroscopic characterization. C.-S.J. performed cross-sectional KPFM. X.P. and Z.V.V. performed and interpreted Hanle-effect measurements. M.P.H. and J.M.L. performed the band diagram simulations. All authors discussed the results and contributed to the revisions of the manuscript.

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Correspondence to Matthew C. Beard.

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Extended data figures and tables

Extended Data Fig. 1 SEM micrographs for LED characterization.

a–c, (R-MBA)2PbI4 deposited on (AlxGa1−x)0.5In0.5P surface. d, TFB/(R-MBA)2PbI4/(AlxGa1−x)0.5In0.5P. e, IZO/Al2O3/TFB/(R-MBA)2PbI4/(AlxGa1−x)0.5In0.5P. The (R-MBA)2PbI4 exhibits impinged spherulites with no gaps observed. The spherulitic structure is maintained through the deposition of TFB and IZO. f, Cross-sectional imaging of the LED with visible layer from top down: gold/IZO/(R-MBA)2PbI4/p-cladding/MQW/n-cladding.

Extended Data Fig. 2 XPS of the (Al0.53Ga0.47)0.5In0.5P cladding layer before (R/S-MBA)2PbI4 deposition.

Spectra of Al 2p (a), Ga 3d (b), In 3d (c) and P 2p (d). Core levels are shown at the top of each plot. The low broadening of the In 3d peak (c) shows low surface oxidation.

Extended Data Fig. 3 Basic characterization of the spin-LED.

a, EL spectra (not polarized) with increasing applied current. b, EL intensity versus applied current showing linear increase. I–V curves of the LEDs in dark and under illumination: the LED with no (R/S-MBA)2PbI4 present (c,d) and the full LED stack including (R/S-MBA)2PbI4 (e,f).

Extended Data Fig. 4 Continued examples of independently fabricated LEDs’ CP-EL with (R-MBA)2PbI4.

Circularly polarized emission data from (R-MBA)2PbI4 spin injection into AlGaInP (a,c; same LED architecture as the main text; device 1 and device 2 labelled) and the corresponding polarization versus current plots (b,d). Error bars are one standard deviation of five consecutive measurements (n = 5). The source of the variation in the devices can be attributed to the Joule heating, as described in Extended Data Fig. 6.

Extended Data Fig. 5 Continued examples of independently fabricated LEDs’ CP-EL with (S-MBA)2PbI4.

Circularly polarized emission data from (S-MBA)2PbI4 spin injection into AlGaInP (a,c; same LED architecture as the main text; device 3 and device 4 labelled) and the corresponding polarization versus current plots (b,d). Error bars are one standard deviation of five consecutive measurements (n = 5). The source of the variation in the devices can be attributed to the Joule heating, as described in Extended Data Fig. 6.

Extended Data Fig. 6 Further CP-EL characterization.

In situ measurement in which a quarter-wave plate is rotated during device operation, showing the increase and decrease with selectivity for right-handed (RH) and left-handed (LH) circular polarization. Scan number corresponds to increasing time. Decrease in overall luminescence is presumed to be because of Joule heating.

Extended Data Fig. 7 Absorbance, photoluminescence and circular dichroism of (R/S-MBA)2PbI4.

Absorbance and photoluminescence (a) and circular dichroism (b) of (R/S-MBA)2PbI4.

Extended Data Fig. 8 Hanle-effect measurement.

Hanle-effect measurement for out-of-plane applied magnetic field (that is, parallel to the inorganic planes of the (R/S-MBA)2PbI4 or long axis of the device) (a) and in-plane applied magnetic field (orthogonal to the inorganic planes of the (R/S-MBA)2PbI4; along the short axis of the device) (b). Both orientations seem to decrease the DOCP with magnetic field, albeit to different extents. This suggests that the spin-orientation direction is non-trivial (that is, neither along the a–b direction (parallel, out-of-plane) nor in the c direction (orthogonal, in-plane) of the (R/S-MBA)2PbI4)59.

Extended Data Fig. 9 Spin and carrier lifetime measurements.

a, Circularly polarized transient absorbance measurement to determine the spin lifetime of carriers in the AlGaInP MQWs. b, Time-resolved photoluminescence of the AlGaInP MQWs to determine the carrier lifetime.

Extended Data Table 1 Collection of previous organic–inorganic-based CISS spin-LEDs
Full size table

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Hautzinger, M.P., Pan, X., Hayden, S.C. et al. Room-temperature spin injection across a chiral perovskite/III–V interface. Nature (2024). https://doi.org/10.1038/s41586-024-07560-4

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