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Super-resolved snapshot hyperspectral imaging of solid-state quantum emitters for high-throughput integrated quantum technologies

Abstract

Solid-state quantum emitters coupled to integrated photonic nanostructures are quintessential for exploring fundamental phenomena in cavity quantum electrodynamics and are used in a wide range of photonic quantum technologies. One of the most exciting prospects for integrated photonics is the potential for massive production of miniaturized devices on a single chip. However, the efficiency and reproducibility of light–matter coupling are hindered by the spectral and spatial mismatch between the single solid-state quantum emitters and the optical modes supported by the photonic nanostructures. Here we develop a platform and method for hyperspectral imaging of solid-state quantum emitters to address this long-standing issue. Spatially distributed and spectrally broadened InAs quantum dots are embedded in a GaAs/AlGaAs one-dimensional (1D) planar cavity that consists of two distributed Bragg reflectors acting as mirrors. By exploiting the extended mode of the dispersive 1D cavity and the way it shapes the out-of-plane emission from the quantum dots, we extract the spatial position and emission wavelength of each dot from a single wide-field photoluminescence image, with a spatial and spectral accuracy down to 15 nm and 0.4 nm, respectively. We then fabricate quantum light sources by etching the 1D confined planar cavity into 3D confined micropillars. Extension of this technique using an open planar cavity can be exploited for a variety of compact quantum photonic devices with expanded functionalities for large-scale integration. Our technology is particularly appealing for quantum photonic applications that involve the spatial and spectral characterization of a large number of solid-state quantum emitters.

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Fig. 1: Emission characteristics of single solid-state quantum emitters in a 1D nanophotonic planar cavity and a 3D confined microcavity.
Fig. 2: Characterization of the dispersive semiconductor planar cavity.
Fig. 3: Characterization of QDs in a planar cavity.
Fig. 4: Extraction of QD emission wavelengths from their image profiles.
Fig. 5: Experimental verification of HSI by fabricating deterministically coupled QD–micropillar devices.

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Data availability

The data that support the plots within this paper and other findings of this study are available via Figshare at https://doi.org/10.6084/m9.figshare.25594176 (ref. 56). All other data used in this study are available from the corresponding authors upon reasonable request.

Code availability

All codes produced during this research are available from the corresponding authors upon reasonable request.

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Acknowledgements

This research was supported by the National Key Research and Development Program of China (2021YFA1400800); the National Natural Science Foundation of China (62035017, 12334017 and 12304409); the Guangdong Special Support Program (2019JC05X397); the China Postdoctoral Science Foundation (2023M743986) and the National Super-Computer Center in Guangzhou.

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Authors and Affiliations

Authors

Contributions

J.L. and X.W. conceived the project; S.L., J.L. and H.L. designed the epitaxial structure and the devices; H.L. and H.N. grew the QD wafers; S.L. and G.Q. developed the theory model to calculate the image and far-field profile; S.L. and X.L. fabricated the devices; S.L. designed and performed all of the optical measurements with inputs from X.L., J.M. and L.N.; Y.M. and X.H. provided the superconducting nanowire single-photon detector for the lifetime measurements; S.L. and J.L. analysed the data; J.L. and S.L. prepared the paper with inputs from all authors; J.L., Z.N., C.-W.Q. and X.W. supervised the project.

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Correspondence to Xuehua Wang or Jin Liu.

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Nature Photonics thanks Wolfgang Löffler, Rupert Oulton and Glenn Solomon for their contribution to the peer review of this work.

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Extended data

Extended Data Fig. 1 Schematic of the setup for optical characterizations and HSI.

(a) The QDs in a planar cavity are located in a closed-circle cryostat with a base temperature near 3.5 K. To excite the QDs, either a high-power 620 nm LED or a 785 nm continuous wave (CW) laser is coupled to the main optical path with dichroic mirrors (DM). This enables the QDs to be excited either in a wide-field manner or in a single-point confocal configuration. The objective, lens 1 (f = 500 mm), lens 2 (f = 300 mm), and lens 3 (f = 300 mm) are used to map the image or far-field (Fourier) plane to an EMCCD camera or a CCD of a spectrometer for imaging or spectral analysis. The configuration between momentum-space imaging and real-space imaging can be switched by flipping Lens 1. (b) Momentum-space imaging configuration: emission from the sample with wave vector \({{{\rm{k}}}}=\sin (\theta )\) (θ is the emission angle relative to the optical axis) is mapped to a point \(\Delta {{{{\rm{x}}}}}^{{\prime} }\) in the camera. (c) Real-space imaging configuration: a point source in the sample plane at position Δx1 is mapped to a point at a distance \(\Delta {{{{\rm{x}}}}}_{2}^{{\prime\prime} }\) in the camera. DM1: 650 nm longpass dichroic mirror, DM2: 805 nm long-pass dichroic mirror, DM3: 850 nm short-pass dichroic mirror, LPF: 900 nm long-pass filter.

Extended Data Fig. 2 Image and Far-field profiles of QDs in bulk GaAs.

(a) Wide-field image of QDs in GaAs bulk, acquired under high-power LED excitation. (b) Schematic of the wafer, the QDs are located at the center of a 200 nm GaAs slab, above 400 nm Al0.75Ga0.25As, grown on GaAs substrate. (c)(d) Far-field patterns and image profiles of six individual QDs, each QD with a different wavelength shares the same far-field pattern and image profile. (e) Fitting of the image profiles by using an Airy function. Typical QD in bulk shows a spot-size with an FWHM of 0.775 μm, which is close to the diffraction limit spot-size (0.761 μm) by using an objective with an NA of 0.6. (f) The extracted spot sizes of the presented six QDs. (g) Representative spectra of QDs in bulk with different emission wavelengths. (h) Corresponding angle-resolved spectra of the QDs in (g), exhibiting no dispersion feature.

Extended Data Fig. 3 Method for extracting the spatial positions of QDs respective to the pre-fabricated alignment markers.

(a) Image of the pre-fabricated alignment markers. The centers of the markers are extracted by fitting the images with Gaussian functions and labeled by the red crosses. The distance between two adjacent markers is 40 μm. (b)(c) Fittings with a Gaussian function to extract the positions of two markers A and B along the X-axis. In this particular image, the centers of A and B are found to be at 105.18 and 544.04 pixels, respectively, with errors of 0.11 and 0.08 pixels. (d) A PL image containing QDs acquired by adjusting the focus to the QD plane. (e)(f) Position of QD1 is extracted to be (399.22,236.50) pixels in the image, by fitting the spot with an airy function, with errors of 0.06 and 0.08 pixels along the x and y direction, respectively. (g) Calculated the distances between QD1 and alignment markers. (h) Histograms of the error of the relative distance between QDs and alignment markers. The mean error for Δx and Δy are 13.7 nm and 14.4 nm, respectively.

Extended Data Fig. 4 Procedure of calculating the image profile of a QD in a planar DBR cavity emitting at a specific wavelength.

(a) Fitting the reflection spectrum (kx = 0) of the planar cavity. (b) Calculating the reflection spectra at different angles using the parameters (thickness of each layer, reflective index of the material) extracted from (a). (c) Reconstructing the dispersion relation of the planar cavity by sweeping the kx of reflection spectra calculated in (b). (d) Extracting the 1D far-field pattern of a QD emitting a specific wavelength from the reconstructed dispersion map. (e) Calculating the full far-field pattern of the targeted QD with a rotation transformation. (f) Obtaining the imaging profile of the QD by performing a Fourier transformation to the far-field pattern in (e).

Extended Data Fig. 5 Comparison of the image profiles with different k-vector distributions.

(a-d) k-vector distributions with gradually reduced low-frequency components and fixed maximal spatial frequency of 0.6. The k-vector distribution in (d) is similar to the far-field distribution of the QD’s emission escaped from the planar cavity. (e-h) Calculated image profiles of (a-d) via a Fourier transformation. (i-l) X-cut of the image profiles in (e-h) The red line is the Airy spot calculated from a full k-distribution with a maximal k-vector of 0.6. The image in (e) shows a standard diffraction-limited spot, which can be perfectly fitted by an Airy function. When reducing the low-frequency component, the profile in the image plane deviates from the standard Airy spot, forming a central spot smaller than the standard diffraction limit set by the NA of the objective, together with brighter and tighter side concentric rings.

Extended Data Fig. 6 Super-resolved imaging enabled by the planar DBR cavity.

(a)(b) Calculated far-field profile of a QD in bulk (without cavity) and a planar DBR cavity collected by an objective with NA = 0.6. The wavelength of QD is selected to guarantee that the emission is escaped from the cavity with kx = ky = 0.6. (c) Crosscuts of calculated far-field distributions without and with a planar cavity. (d)(e) Experimental far-field profile of a QD in the slab (without cavity) and in a planar DBR cavity collected by an objective with NA = 0.6. (f) Crosscuts of experimental far-field distributions without and with a planar cavity. (g)(h) Calculated profile in the image plane of the QD in bulk (without cavity) and in a planar DBR cavity. (i) Crosscuts of the image profiles for QD in bulk and a planar DBR cavity. Emission escaped from GaAs bulk forms a diffraction-limited spot (d = 0.51 λ/NA) with an FWHM of 760.8 nm, while emission escaped from the planar DBR cavity presents a super-resolved spot with an FWHM of 494.2 nm. (j)(k) Experimental profile in the image plane of the QD in bulk (without cavity) and in a planar DBR cavity. (l) Crosscuts of the image profiles for QD in bulk and a planar DBR cavity. Emission escaped from GaAs bulk forms a near-diffraction-limited spot with an FWHM of 775.0 nm, while emission escaped from the planar DBR cavity presents a super-resolved spot with an FWHM of 552.8 nm, which is slightly wider than the calculated one, but is still significantly narrower than the value without the cavity.

Extended Data Fig. 7 Procedure for high throughput fabrication of deterministically coupled QD-micropillar devices by employing snapshot HSI.

(a) Epitaxial growth of the DBR and QDs. (b) Fabrication of alignment marks. (c) HSI for acquiring the positions and spectral information of the QDs. (d) Wafer with patterned E-beam resist after aligned EBL. (e) Formation of deterministically coupled micropillars after dry etch.

Extended Data Fig. 8 Snapshot HSI of QDs in a planar open cavity for building thin-film QD devices with expanded functionalities and reduced footprints.

(a) Schematics of the proposed planar open cavity for snapshot HSI. A 180 nm GaAs layer containing InAs QDs and a 450-nm-thick Al0.7Ga0.3As sacrificial layer are grown on a bottom DBR consisting of 20 pairs of 1/4λ GaAs/Al0.9Ga0.1As layer. A movable DBR mirror made of 20 pairs of 1/4λ GaAs/Al0.9Ga0.1As layer is placed on the top of the QD wafer with an air gap of 1000 nm, which could be precisely controlled by a piezo-nanopositioner. (b) Reflection spectrum in the normal direction for the planar open cavity, exhibiting two cavity resonances in the stop band. We intentionally designed the fundamental cavity resonance to the proximity of the InAs QD emission wavelength range (895 nm – 920 nm) for HSI. The blue area denotes the spectral range of the targeted QD emission. (c) Dispersion relation of the fundamental cavity mode used for HSI. There is a one-to-one correspondence between the emission angle (k-vector) and the emission wavelength. Top insets: far-field radiation patterns for QDs with different wavelengths. (d) Relation between the emission wavelength and image profile for the QDs in the planar open cavity. Top insets: image profiles for QDs with different wavelengths. (e) Suspended circular Bragg resonators and photonic crystal cavities fabricated from the QDs in the planar open cavity by removing the AlGaAs sacrificial layer. (f) Large-scale integrated quantum photonic circuit consisting of quantum light sources, frequency converters, phase shifters, interferometers, and grating couplers fabricated from a planar open cavity by transferring thin-film GaAs layer with QDs on a low-index insulator substrate.

Extended Data Fig. 9 Procedure for fabricating suspended membrane cavities deterministically coupled with QD by employing snapshot HSI.

(a) QD wafer with a sacrificial layer and a bottom DBR mirror. A 180 nm GaAs layer containing InAs QDs and a 450-nm-thick Al0.7Ga0.3As sacrificial layer is grown on a bottom DBR consisting of 20 pairs of 1/4λ GaAs/Al0.9Ga0.1As layer. A movable DBR mirror made of 20 pairs of 1/4λ GaAs/Al0.9Ga0.1As layer is placed on the top of the QD wafer with an air gap of 1000 nm, which could be precisely controlled by a piezo-nanopositioner (b) Fabrication of alignment marks. (c) HSI of QDs by employing an external DBR mirror to form a planar cavity. (d) Patterning the circular Bragg gratings and photonic crystals at the QD positions with an E-beam lithography process. (e) Fabrications of the suspended cavities by using dry etch and selective wet etch.

Extended Data Fig. 10 Procedure for fabricating large-scale quantum photonic circuits based on QD by employing snapshot HSI.

(a) QD wafer with a sacrificial layer and a bottom DBR mirror. (b) Fabrication of alignment marks. (c) HSI of QDs by employing an external DBR mirror to form a planar cavity. (d) Flip-chip bonding of the QD wafer to a transparent substrate. (e) Removal of the substrate, DBR, and sacrificial layers of the QD wafer to form a GaAs-on-insulator chip. (f) Fabrications of large-scale quantum photonic circuits at the QD positions.

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Liu, S., Li, X., Liu, H. et al. Super-resolved snapshot hyperspectral imaging of solid-state quantum emitters for high-throughput integrated quantum technologies. Nat. Photon. (2024). https://doi.org/10.1038/s41566-024-01449-4

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