On-chip quantum interference of indistinguishable single photons from integrated independent molecules
Source abstract
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.
Source: europepmc · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Quantum Information and Cryptography · Mechanical and Optical Resonators · Quantum optics and atomic interactions
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (63)
Show source-provided references
1. Pelucchi, E. et al. The potential and global outlook of integrated photonics for quantum technologies. Nat. Rev. Phys. 4, 194–208 (2022).10.1038/s42254-021-00398-z ↗
2. Lodahl, P., Mahmoodian, S. & Stobbe, S. Interfacing single photons and single quantum dots with photonic nanostructures. Rev. Mod. Phys. 87, 347–400 (2015).10.1103/RevModPhys.87.347 ↗
3. Kok, P. et al. Linear optical quantum computing with photonic qubits. Rev. Mod. Phys. 79, 135–174 (2007).10.1103/RevModPhys.79.135 ↗
4. Qiang, X. G. et al. Large-scale silicon quantum photonics implementing arbitrary two-qubit processing. Nat. Photon. 12, 534–539 (2018).10.1038/s41566-018-0236-y ↗
5. Llewellyn, D. et al. Chip-to-chip quantum teleportation and multi-photon entanglement in silicon. Nat. Phys. 16, 148 (2020).10.1038/s41567-019-0727-x ↗
6. He, Y. M. et al. On-demand semiconductor single-photon source with near-unity indistinguishability. Nat. Nanotechnol. 8, 213–217 (2013).10.1038/nnano.2012.262 ↗
7. Somaschi, N. et al. Near-optimal single-photon sources in the solid state. Nat. Photon. 10, 340–345 (2016).10.1038/nphoton.2016.23 ↗
8. Rezai, M., Wrachtrup, J. & Gerhardt, I. Coherence properties of molecular single photons for quantum networks. Phys. Rev. X 8, 031026 (2018).
9. Liu, F. et al. High Purcell factor generation of indistinguishable on-chip single photons. Nat. Nanotechnol. 13, 835–840 (2018).10.1038/s41565-018-0188-x ↗
10. Evans, R. E. et al. Photon-mediated interactions between quantum emitters in a diamond nanocavity. Science 362, 662 (2018).10.1126/science.aau4691 ↗
11. Wan, N. H. et al. Large-scale integration of artificial atoms in hybrid photonic circuits. Nature 583, 226–231 (2020).10.1038/s41586-020-2441-3 ↗
12. Chen, D. et al. Quantum interference of resonance fluorescence from germanium-vacancy color centers in diamond. Nano Lett. 22, 6306–6312 (2022).10.1021/acs.nanolett.2c01959 ↗
13. Martínez, J. A. et al. Photonic indistinguishability of the tin-vacancy center in nanostructured diamond. Phys. Rev. Lett. 129, 173603 (2022).10.1103/PhysRevLett.129.173603 ↗
14. Türschmann, P. et al. Chip-based all-optical control of single molecules coherently coupled to a nanoguide. Nano Lett. 17, 4941–4945 (2017).10.1021/acs.nanolett.7b02033 ↗
15. Toninelli, C. et al. Single organic molecules for photonic quantum technologies. Nat. Mater. 20, 1615–1628 (2021).10.1038/s41563-021-00987-4 ↗
16. O’Brien, J. L., Furusawa, A. & Vučković, J. Photonic quantum technologies. Nat. Photon. 3, 687–695 (2009).10.1038/nphoton.2009.229 ↗
17. Elshaari, A. W., Pernice, W., Srinivasan, K., Benson, O. & Zwiller, V. Hybrid integrated quantum photonic circuits. Nat. Photon. 14, 285–298 (2020).10.1038/s41566-020-0609-x ↗
18. Kim, J.-H., Aghaeimeibodi, S., Carolan, J., Englund, D. & Waks, E. Hybrid integration methods for on-chip quantum photonics. Optica 7, 291–308 (2020).10.1364/OPTICA.384118 ↗
19. Kimble, H. J. The quantum internet. Nature 453, 1023–1030 (2008).10.1038/nature07127 ↗
20. Davanco, M. et al. Heterogeneous integration for on-chip quantum photonic circuits with single quantum dot devices. Nat. Commun. 8, 889 (2017).10.1038/s41467-017-00987-6 ↗
21. Ren, P. et al. Photonic-circuited resonance fluorescence of single molecules with an ultrastable lifetime-limited transition. Nat. Commun. 13, 3982 (2022).10.1038/s41467-022-31603-x ↗
22. Wang, H. et al. Boson sampling with 20 input photons and a 60-mode interferometer in a 1014-dimensional Hilbert space. Phys. Rev. Lett. 123, 250503 (2019).10.1103/PhysRevLett.123.250503 ↗
23. Liu, J. et al. Single self-assembled InAs/GaAs quantum dots in photonic nanostructures: the role of nanofabrication. Phys. Rev. Appl. 9, 064019 (2018).10.1103/PhysRevApplied.9.064019 ↗
24. Shkarin, A. et al. Nanoscopic charge fluctuations in a gallium phosphide waveguide measured by single molecules. Phys. Rev. Lett. 126, 133602 (2021).10.1103/PhysRevLett.126.133602 ↗
25. Zhai, L. et al. Quantum interference of identical photons from remote GaAs quantum dots. Nat. Nanotechnol. 17, 829–833 (2022).10.1038/s41565-022-01131-2 ↗
26. You, X. et al. Quantum interference with independent single-photon sources over 300 km fiber. Adv. Photon. 4, 066003 (2022).10.1117/1.AP.4.6.066003 ↗
27. Lettow, R. et al. Quantum interference of tunably indistinguishable photons from remote organic molecules. Phys. Rev. Lett. 104, 123605 (2010).10.1103/PhysRevLett.104.123605 ↗
28. Duquennoy, R. et al. Real-time two-photon interference from distinct molecules on the same chip. Optica 9, 731–737 (2022).10.1364/OPTICA.452317 ↗
29. Papon, C. et al. Independent operation of two waveguide-integrated quantum emitters. Phys. Rev. Appl. 19, L061003 (2023).10.1103/PhysRevApplied.19.L061003 ↗
30. Dusanowski, Ł., Köck, D., Schneider, C. & Höfling, S. On-chip Hong–Ou–Mandel interference from separate quantum dot emitters in an integrated circuit. ACS Photon. 10, 2941–2947 (2023).10.1021/acsphotonics.3c00679 ↗
31. Gao, W. B. et al. Quantum teleportation from a propagating photon to a solid-state spin qubit. Nat. Commun. 4, 2744 (2013).10.1038/ncomms3744 ↗
32. Waltrich, R., Klotz, M., Agafonov, V. N. & Kubanek, A. Two-photon interference from silicon-vacancy centers in remote nanodiamonds. Nanophotonics 12, 3663–3669 (2023).10.1515/nanoph-2023-0379 ↗
33. Hong, C. K., Ou, Z. Y. & Mandel, L. Measurement of subpicosecond time intervals between two photons by interference. Phys. Rev. Lett. 59, 2044–2046 (1987).10.1103/PhysRevLett.59.2044 ↗
34. Nicolet, A. A. et al. Single dibenzoterrylene molecules in an anthracene crystal: main insertion sites. ChemPhysChem 8, 1929–1936 (2007).10.1002/cphc.200700340 ↗
35. Mollow, B. R. Power spectrum of light scattered by two-level systems. Phys. Rev. 188, 1969–1975 (1969).10.1103/PhysRev.188.1969 ↗
36. Wrigge, G., Gerhardt, I., Hwang, J., Zumofen, G. & Sandoghdar, V. Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence. Nat. Phys. 4, 60–66 (2008).10.1038/nphys812 ↗
37. Kimble, H. & Mandel, L. Theory of resonance fluorescence. Phys. Rev. A 13, 2123 (1976).10.1103/PhysRevA.13.2123 ↗
38. Matthiesen, C., Vamivakas, A. N. & Atatüre, M. Subnatural linewidth single photons from a quantum dot. Phys. Rev. Lett. 108, 093602 (2012).10.1103/PhysRevLett.108.093602 ↗
39. Proux, R. et al. Measuring the photon coalescence time window in the continuous-wave regime for resonantly driven semiconductor quantum dots. Phys. Rev. Lett. 114, 067401 (2015).10.1103/PhysRevLett.114.067401 ↗
40. Schofield, R. C. et al. Photon indistinguishability measurements under pulsed and continuous excitation. Phys. Rev. Res. 4, 013037 (2022).10.1103/PhysRevResearch.4.013037 ↗
41. Koong, Z. X. et al. Fundamental limits to coherent photon generation with solid-state atomlike transitions. Phys. Rev. Lett. 123, 167402 (2019).10.1103/PhysRevLett.123.167402 ↗
42. Phillips, C. L. et al. Photon statistics of filtered resonance fluorescence. Phys. Rev. Lett. 125, 043603 (2020).10.1103/PhysRevLett.125.043603 ↗
43. Hanschke, L. et al. Origin of antibunching in resonance fluorescence. Phys. Rev. Lett. 125, 170402 (2020).10.1103/PhysRevLett.125.170402 ↗
44. Wang, D. et al. Turning a molecule into a coherent two-level quantum system. Nat. Phys. 15, 483–489 (2019).10.1038/s41567-019-0436-5 ↗
45. Tiranov, A. et al. Collective super- and subradiant dynamics between distant optical quantum emitters. Science 379, 389–393 (2023).10.1126/science.ade9324 ↗
46. Lange, C. M. et al. Cavity QED with molecular defects coupled to a photonic crystal cavity. Preprint at https://arxiv.org/abs/2506.01917 (2025).
47. Reithmaier, G. et al. On-chip generation, routing, and detection of resonance fluorescence. Nano Lett. 15, 5208–5213 (2015).10.1021/acs.nanolett.5b01444 ↗
48. Gimeno-Segovia, M., Rudolph, T. & Economou, S. E. Deterministic generation of large-scale entangled photonic cluster state from interacting solid state emitters. Phys. Rev. Lett. 123, 070501 (2019).10.1103/PhysRevLett.123.070501 ↗
49. Brod, D. J. et al. Photonic implementation of boson sampling: a review. Adv. Photon. 1, 034001 (2019).
50. Briegel, H. J., Dür, W., Cirac, J. I. & Zoller, P. Quantum repeaters: the role of imperfect local operations in quantum communication. Phys. Rev. Lett. 81, 5932–5935 (1998).10.1103/PhysRevLett.81.5932 ↗
51. Trebbia, J. B., Deplano, Q., Tamarat, P. & Lounis, B. Tailoring the superradiant and subradiant nature of two coherently coupled quantum emitters. Nat. Commun. 13, 2962 (2022).10.1038/s41467-022-30672-2 ↗
52. Lukin, D. M. et al. Two-emitter multimode cavity quantum electrodynamics in thin-film silicon carbide photonics. Phys. Rev. X 13, 011005 (2023).
53. Rattenbacher, D. et al. On-chip interference of scattering from two individual molecules. Optica 10, 1595–1601 (2023).10.1364/OPTICA.502221 ↗
54. Lange, C. M., Daggett, E., Walther, V., Huang, L. & Hood, J. D. Superradiant and subradiant states in lifetime-limited organic molecules through laser-induced tuning. Nat. Phys. 20, 836–842 (2024).10.1038/s41567-024-02404-4 ↗
55. Carusotto, I. & Ciuti, C. Quantum fluids of light. Rev. Mod. Phys. 85, 299–366 (2013).10.1103/RevModPhys.85.299 ↗
56. Sheremet, A. S., Petrov, M. I., Iorsh, I. V., Poshakinskiy, A. V. & Poddubny, A. N. Waveguide quantum electrodynamics: collective radiance and photon-photon correlations. Rev. Mod. Phys. 95, 015002 (2023).10.1103/RevModPhys.95.015002 ↗
57. Loudon, R. The Quantum Theory of Light 3rd edn (Oxford Univ. Press, 2000).10.1093/oso/9780198501770.003.0002 ↗
58. Grandi, S. et al. Quantum dynamics of a driven two-level molecule with variable dephasing. Phys. Rev. A 94, 063839 (2016).10.1103/PhysRevA.94.063839 ↗
59. Cohen-Tannoudji, C., Dupont-Roc, J. & Grynberg, G. Atom–Photon Interactions: Basic Process and Applications (Wiley, 1998).10.1002/9783527617197 ↗
60. Manzano, D. A short introduction to the Lindblad master equation. AIP Adv. 10, 025106 (2020).10.1063/1.5115323 ↗
61. Henry, C. Theory of the linewidth of semiconductor lasers. IEEE J. Quantum Electron. 18, 259–264 (1982).10.1109/JQE.1982.1071522 ↗
62. Eberly, J. H. & Wódkiewicz, K. The time-dependent physical spectrum of light. J. Opt. Soc. Am. 67, 1252–1261 (1977).10.1364/JOSA.67.001252 ↗
63. del Valle, E., Gonzalez-Tudela, A., Laussy, F. P., Tejedor, C. & Hartmann, M. J. Theory of frequency-filtered and time-resolved N-photon correlations. Phys. Rev. Lett. 109, 183601 (2012).10.1103/PhysRevLett.109.183601 ↗