Abstract
On-chip integration of independent channels of indistinguishable single photons is a prerequisite for scalable optical quantum information processing. This requires separate solid-state single-photon emitters to exhibit identical lifetime-limited transitions. This challenging task is usually further exacerbated by spectral diffusion due to complex charge noise near material surfaces made by nanofabrication processes. Here we develop a molecular quantum photonic chip and demonstrate on-chip Hong–Ou–Mandel quantum interference of indistinguishable single photons from independent molecules. The molecules are embedded in a single-crystalline organic nanosheet and integrated with single-mode waveguides without nanofabrication, thereby ensuring stable, lifetime-limited transitions. With the aid of Stark tuning, we show how 100 waveguide-coupled molecules can be tuned to the same frequency and achieve on-chip Hong–Ou–Mandel interference visibilities exceeding 0.97 for 2 molecules separately coupled to 2 waveguides. For two molecules with a controlled frequency difference, we unveil over 100-µs-long quantum beating in the interference, showing both excellent single-photon purity (particle nature) and long coherence (wave nature) of the emission. Our results showcase a possible strategy towards constructing scalable optical universal quantum processors and a promising platform for studying waveguide quantum electrodynamics with identical single emitters wired via photonic circuits.
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All the data that support the findings of this study are available within the article and its Supplementary Information, and from the corresponding authors upon request. Source data are provided with this paper.
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Acknowledgements
We gratefully acknowledge financial support from the National Natural Science Foundation of China (grant numbers 62235006 and 12525414 to X.-W.C., 12374349 to J.T., 62135011 to Y.S.), the Fundamental Research Funds for the Central Universities (grant numbers 2023BR003 to X.-W.C., 2024BRB002 to J.T.), and the Hubei Provincial Talent Program (J.T.).
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X.-W.C. conceived of the study. X.-W.C. and J.T. designed the experiment. T.H., W.J., M.X., Y.C., P.R., S.W. and Z.B. performed the optical experiments. M.X., S.W. and Y.C. made the DBT-in-anthracene sample and performed hybrid integration of the sample and the photonic circuits. W.L. and Y.S. fabricated and characterized Si3N4-on-silica photonic circuits and microelectrodes. Y.C., J.T., X.-W.C. and Z.B. performed the theoretical analysis. X.-W.C., J.T., T.H., M.X., W.J., Y.C. and Z.B. discussed the results and analysed data. X.-W.C., J.T. and Y.C. wrote the paper with input from all co-authors. X.-W.C., J.T. and Y.S. supervised the project.
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Extended data
Extended Data Fig. 1 Schematic illustration of the full experimental set-up.
AL: aspherical lens; AOFS: acousto-optic frequency shifter; APD: avalanche photodiode single photon detector; BPF: band-pass filter; LPF: long-pass filter; BS: beam splitter; PBS: polarizing beam splitter; SMF: single-mode fibre; PMF: polarization-maintaining single-mode fibre; PH-F: pinhole at Fourier image plane; PH-R: pinhole at real image plane; HWP: half-wave plate; QWP: quarter-wave plate; GM: galvo mirror system; FM: flip mirror; G: grating coupler.
Extended Data Fig. 2 Configurations of acousto-optic frequency shifters for excitation laser frequency control.
a-c, Configurations of AOFS1 and AOFS2 for setting the frequency difference between the excitation laser beams L1 and L2 to be 0 MHz (a), 200 MHz (b), and 3.8 GHz (c). AOFS: acousto-optic frequency shifter; AOM: acousto-optic modulator; BS: beam splitter; PBS: polarizing beam splitter; QWP: quarter-wave plate; PMF: polarization-maintaining single-mode fibre.
Extended Data Fig. 3 Determination of saturation parameter, transition coherence time, and excited-state lifetime for a single molecule.
a, Fluorescence excitation spectra at a series of excitation powers. The corresponding saturation parameters S are marked on the colour bar along with the power values. Solid lines represent fits to Lorentzian functions. The background, determined via Lorentzian fitting, has been subtracted from each spectrum. b, Extracted fluorescence intensity at a series of excitation powers (S parameters). The fluorescence intensity for each excitation power (S parameter) is extracted by fitting the excitation spectrum in a to a Lorentzian function, with the error bar representing the fitting uncertainty (1σ). The red curve is a fitting of the experimental data to the saturation curve \(I={I}_{{\rm{sat}}}/\left(1+{P}_{{\rm{sat}}}/P\right)\). c, Extracted linewidth Δν at a series of excitation powers (saturation parameters). The linewidth\(\Delta {\rm{\nu }}\) for each S is extracted by fitting the excitation spectrum to a Lorentzian function, with the error bar representing the fitting uncertainty (1σ). The red curve is a fitting of the experimental data to the theoretical expression \(\Delta {\rm{\nu }}=\sqrt{1+S}/\left(\pi {\tau }_{2}\right)\). From the fitting, the transition coherence time \({\tau }_{2}\) is determined to be 9.37 ± 0.43 ns, where the uncertainty is the fitting uncertainty (1σ). d, Photoluminescence decay curve. The red curve is a fitting of the experimental curve to an exponential decay function. From the fitting, the excited-state lifetime \({\tau }_{1}\) is determined to be 4.69 ± 0.03 ns, where the uncertainty is the fitting uncertainty (1σ).
Extended Data Fig. 4 Emission spectra of single molecules resonantly driven by a CW laser at varied excitation rates.
a, b, Emission spectra of molecules M1 (a) and M2 (b) at a series of excitation levels (S = 0.2, 0.5, 1, 2, and 9).
Extended Data Fig. 5 Results of the additional rounds of TPQI experiments.
a-c, Second-order cross-correlation functions and time-delay dependent visibilities for additional round #1 (a), round #2 (b), and round #3 (c). Upper panels represent \({g}_{{\rm{HOM}}}^{(2)}\left(\tau \right)\) (as in Fig. 4d), middle panels represent \({g}_{{\rm{HOM}},{\rm{d}}}^{(2)}\left(\tau \right)\) (as in Fig. 4g), and lower panels represent \(V\left(\tau \right)=[{g}_{{\rm{HOM}},{\rm{d}}}^{(2)}\left(\tau \right)-{g}_{{\rm{HOM}}}^{\left(2\right)}(\tau )]/{g}_{{\rm{HOM}},{\rm{d}}}^{(2)}\left(\tau \right)\) (as in Fig. 4h). For each round of experiment, we re-assemble a new DBT-doped anthracene nanosheet with the photonic circuit. For a summary of the interference visibility / photon indistinguishability values evaluated from these rounds of experiments, see Extended Data Table 1. The error bars represent uncertainty derived via error propagation from counting statistics of the raw detection events (Methods).
Extended Data Fig. 6 On-chip quantum beating experiment for another pair of molecules with a frequency difference of 200 MHz.
a, Second-order cross-correlation of the RF photons detected from output G3 and G4 when M1 and M2 are resonantly driven at the excitation level of S = 1.3. The red trace is the theoretical curve for the ideal situation where the emitters have no pure dephasing and the detection is perfect (without background and dark counts). b, Same as a but for long time delays around 100 µs.
Extended Data Fig. 7 On-chip quantum beating experiment with two molecules having a frequency difference of 400 MHz.
a, Second-order cross-correlation of the RF photons detected from output G3 and G4 when M1 and M2 are resonantly driven at the excitation level of S = 0.5. The red trace is the theoretical curve for the ideal situation where the emitters have no pure dephasing and the detection is perfect (without background and dark counts). The cross-correlation curve exhibits a pronounced beating feature with a period of 2.5 ns, in accordance with the 400 MHz frequency detuning between the molecules. b, Same as a but for long time delays around 100 µs.
Extended Data Fig. 8 Theoretically calculated effect of spectral filtering on quantum beating.
a, b, Calculated second-order correlation function for a series of filter bandwidth \(\varGamma\) at excitation levels S = 0.2 (a) and 1 (b), respectively. We assume that the filters are applied to each molecule before the interference. When \(\varGamma \gg {\varGamma }_{1}\), quantum beating behaviour mirrors that of the case without filtering. As \(\varGamma\) decreases, the suppression of correlation at zero time delay diminishes, and the beating amplitude increases. This trend reflects a weakening of particle nature and an enhancement of wave nature. For \(\varGamma \ll {\varGamma }_{1}\), the correlation function converges to pure coherent laser interference: zero-time-delay suppression vanishes, and the beating amplitude saturates at 0.5.
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Huang, T., Xu, M., Jin, W. et al. On-chip quantum interference of indistinguishable single photons from integrated independent molecules. Nat. Nanotechnol. 20, 1748–1756 (2025). https://doi.org/10.1038/s41565-025-02043-7
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DOI: https://doi.org/10.1038/s41565-025-02043-7
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