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Large-scale optical characterization of solid-state quantum emitters

Nature Materials volume 22, pages 1338–1344 (2023)Cite this article

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Abstract

Solid-state quantum emitters have emerged as a leading quantum memory for quantum networking applications. However, standard optical characterization techniques are neither efficient nor repeatable at scale. Here we introduce and demonstrate spectroscopic techniques that enable large-scale, automated characterization of colour centres. We first demonstrate the ability to track colour centres by registering them to a fabricated machine-readable global coordinate system, enabling a systematic comparison of the same colour centre sites over many experiments. We then implement resonant photoluminescence excitation in a widefield cryogenic microscope to parallelize resonant spectroscopy, achieving two orders of magnitude speed-up over confocal microscopy. Finally, we demonstrate automated chip-scale characterization of colour centres and devices at room temperature, imaging thousands of microscope fields of view. These tools will enable the accelerated identification of useful quantum emitters at chip scale, enabling advances in scaling up colour centre platforms for quantum information applications, materials science and device design and characterization.

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Fig. 1: Techniques for chip-scale characterization.
Fig. 2: Tracking colour centres in a sample with fabricated QR codes.
Fig. 3: Widefield PLE of silicon-vacancy centres.
Fig. 4: Widefield PLE in a FIB-implanted sample.
Fig. 5: Chip-scale verification of fabricated devices at room temperature.

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Data availability

The data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request.

Code availability

The code that supports the plots in this paper is available from the corresponding author upon reasonable request.

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Acknowledgements

M.S. and E.B. acknowledge support from the NASA Space Technology Graduate Research Fellowship Program. I.C. acknowledges support from the National Defense Science and Engineering Graduate Fellowship Program, the National Science Foundation (NSF) EFRI ACQUIRE program EFMA-1641064 and NSF award DMR-1747426. M.S. and M.P.W. acknowledge partial support from the NSF Center for Integrated Quantum Materials (CIQM), DMR-1231319. K.C.C. acknowledges support from the NSF RAISE-TAQS CHE-1839155 and the MITRE Corporation Moonshot program. D.R.E. acknowledges partial support from the NSF Center for Quantum Networks (CQN), EEC-1941583. Construction of the robotic cryogenic microscope was supported in part by the Air Force Office of Scientific Research under award no. FA9550-20-1-0105, supervised by G. Pomrenke. Distribution Statement A. Approved for public release. Distribution is unlimited. Diamond growth is based on work supported by the National Reconnaissance Office (NRO) under Air Force Contract no. FA8702-15-D-0001. Any opinions, findings, conclusions or recommendations expressed in this material are those of the author(s) and do not necessarily reflect the views of the National Reconnaissance Office. The FIB implantation 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. Sandia National Laboratories is a multimission laboratory managed and operated by the National Technology and Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International, Inc., for the US DOE’s National Nuclear Security Administration under contract DE-NA-0003525. The views expressed in the Article do not necessarily represent the views of the US DOE or the United States government. This work made use of the Shared Experimental Facilities supported in part by the MRSEC Program of the NSF under award no. DMR-1419807.

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Authors and Affiliations

  1. Research Laboratory of Electronics, Massachusetts Institute of Technology, Cambridge, MA, USA

    Madison Sutula, Ian Christen, Eric Bersin, Michael P. Walsh, Kevin C. Chen & Dirk R. Englund

  2. Lincoln Laboratory, Massachusetts Institute of Technology, Lexington, MA, USA

    Eric Bersin, Justin Mallek, Alexander Melville, Scott Hamilton, Danielle Braje & P. Benjamin Dixon

  3. Sandia National Laboratories, Albuquerque, NM, USA

    Michael Titze & Edward S. Bielejec

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  1. Madison Sutula
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Contributions

M.S., I.C., E.B. and M.P.W. conceived and performed the experiments, developed the software and built the optical setups. I.C. developed the software and optical setups for widefield data collection and chip-scale sample screening. M.S. analysed the data and wrote the manuscript with assistance from I.C., E.B., M.P.W. and K.C.C. K.C.C. fabricated the QR codes designed by M.P.W. SiV Sample A was produced by J.M., A.M., S.H., D.B. and P.B.D. SiV Sample B was FIB implanted by M.T. and E.S.B. D.R.E. supervised the project. All authors discussed the results and contributed to the manuscript.

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Correspondence to Madison Sutula.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–9, Sections 1–10 and Table 1.

Supplementary Video 1

Widefield PLE of silicon-vacancy centres in chemical-vapour-deposited diamond. a–d, Scanning over the A, B, C and D optical transitions of the SiV, in a field of view. As expected, the C transition is the brightest of the four. The frequency of the resonant laser for a given frame is noted in the lower-left part of the panel. Scale bar, 10 μm. Every frame represents approximately half a second of measurement (video displayed at ×10 speed). All the panels are linearly scaled to the same fixed colour limit.

Supplementary Video 2

Chip-scale measurement of a sample with nanofabricated pillars. a, Bright-field images of each field of view, with boxes marking features that are detected as checksum-satisfying QR codes. The green boxes satisfy the majority-vote conditions for the field of view, and are considered correct. The yellow boxes usually result from noise that happens to satisfy the checksum, or from a bit error event that fails in the majority-vote condition. b, Fluorescence measurements with a 737 nm bandpass filter targeting the SiV colour centres. c, Fluorescence measurements with a 640 nm longpass filter, with a lower signal-to-noise ratio. This is probably due to fluorescence from the NV centres or other emitters in the sample, especially in the bulk. Scale bars, 10 μm. Every frame represents approximately 40 s of alignment and 20 s of measurement (video displayed at ×600 speed). Each panel is linearly scaled to the maximum and minimum of each frame, except for b, which is scaled to a fixed colour limit.

Supplementary Video 3

Chip-scale measurement of a sample with deleterious noise. a, Bright-field images with the same box colour coding as Supplementary Video 2. This video demonstrates the robustness of our convolutional QR detection algorithm: we are able to detect QRs even through regions coated with stochastic particulates that pose a challenge for non-convolutional approaches. Every frame represents approximately 20 s of alignment and 20 s of measurement (video displayed at ×400 speed). This panel is linearly scaled to the maximum and minimum of each frame.

Supplementary Video 4

Chip-scale measurement of a sample with complex fabricated structures. a, Bright-field images with the same box colour coding as Supplementary Video 2. Despite the bright and varying nature of these fabricated structures, we are still able to conduct full-chip measurements. b, Fluorescence measurements at each field of view. The bright spots on the waveguides are attributed to either colour centres, largely tin vacancy in this case, or points where waveguide-coupled fluorescence is scattered upwards. Scale bars, 10 μm. Every frame represents approximately 20 s of alignment and 10 s of measurement (video displayed at ×300 speed). Here a is linearly scaled to the maximum and minimum of each frame and b is scaled to a fixed colour limit.

Supplementary Video 5

Chip-scale measurement of sample B—a sample co-implanted with silicon, germanium and tin. a, Bright-field images with the same box colour coding as Supplementary Video 2. b, Fluorescence images with a 640 nm longpass filter. c, False-colour images composited from three fluorescent measurements using 737, 620 and 600 nm bandpass filters with ~10 nm bandwidth on the red-, green- and blue-coloured channels. These filters target the ZPLs of silicon-, tin- and germanium-vacancy colour centres, respectively, although germanium appears as cyan due to its phonon sideband overlapping with the filter targeting the ZPL of tin. Scale bars, 10 μm. Every frame represents approximately 30 s of alignment and 25 s of measurement (video displayed at ×550 speed). Here a and b are linearly scaled to the maximum and minimum of each frame and c is shown with a fixed colour range in the log scale to increase the visibility of regions implanted with low dose.

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Sutula, M., Christen, I., Bersin, E. et al. Large-scale optical characterization of solid-state quantum emitters. Nat. Mater. 22, 1338–1344 (2023). https://doi.org/10.1038/s41563-023-01644-8

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