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Hidden multiphoton dynamics in the Heitler regime of resonance fluorescence

Yanfeng Li1,2,3,*, Manman Wang1,2,3,*, Chuanyu Zeng1,2,3, Hanqing Liu4,5, Haiqiao Ni4,5, Zhichuan Niu4,5, and Chengyong Hu1,†

  • *These authors contributed equally to this work.
  • †Contact author: hucy@baqis.ac.cn
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Phys. Rev. Research 8, 013002 – Published 2 January, 2026

DOI: https://doi.org/10.1103/hgzx-twpk

Abstract

Resonance fluorescence from a two-level emitter is a standard route to single-photon generation, where the emitter produces only one photon at a time, and multiphoton emission or scattering is inherently suppressed. In this study, we challenge this paradigm in the weak-excitation limit, where coherent scattering dominates. Using a single quantum dot in a microcavity, we show that the incoherent component exhibits pronounced superbunching, revealing simultaneous multiphoton scattering from a single emitter. In contrast, the total reflected field—comprising the reflected driving field and incoherent scattering—displays perfect antibunching, arising from quantum interference that cancels two-photon probability amplitudes. By spectrally filtering the reflected field, we tune the relative contributions of coherent and incoherent components, observing transitions in photon statistics from antibunching to superbunching, or to Poissonian light. Supported by master-equation simulations and an interference-based model, these results uncover the hidden but fundamental role of multiphoton dynamics in resonance fluorescence, and open avenues for generating nonclassical light in cavity and waveguide quantum electrodynamics.

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References (56)

  1. R. Loudon, The Quantum Theory of Light (Oxford University Press, Oxford, 2000).
  2. M. O. Scully and M. S. Zubairy, Quantum Optics (Cambridge University Press, Cambridge, 1997).
  3. H. J. Kimble, M. Dagenais, and L. Mandel, Photon antibunching in resonance fluorescence, Phys. Rev. Lett. 39, 691 (1977).
  4. W. Heitler, The Quantum Theory of Radiation (Clarendon Press, Oxford, 1954).
  5. B. R. Mollow, Power spectrum of light scattered by two-level systems, Phys. Rev. 188, 1969 (1969).
  6. C. N. Cohen-Tannoudji, Nobel lecture: Manipulating atoms with photons, Rev. Mod. Phys. 70, 707 (1998).
  7. H. Walther, B. T. H. Varcoe, B.-G. Englert, and T. Becker, Cavity quantum electrodynamics, Rep. Prog. Phys. 69, 1325 (2006).
  8. G. Wrigge, I. Gerhardt, J. Hwang, G. Zumofen, and V. Sandoghdar, Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence, Nat. Phys. 4, 60 (2008).
  9. O. Astafiev, A. M. Zagoskin, A. A. Abdumalikov, Yu A. Pashkin, T. Yamamoto, K. Inomata, Y. Nakamura, and J. S. Tsai, Resonance fluorescence of a single artificial atom, Science 327, 840 (2010).
  10. A. Muller, E. B. Flagg, P. Bianucci, X. Y. Wang, D. G. Deppe, W. Ma, J. Zhang, G. J. Salamo, M. Xiao, and C. K. Shih, Resonance fluorescence from a coherently driven semiconductor quantum dot in a cavity, Phys. Rev. Lett. 99, 187402 (2007).
  11. E. B. Flagg, et al., Resonantly driven coherent oscillations in a solid-state quantum emitter, Nat. Phys. 5, 203 (2009).
  12. A. N. Vamivakas, Y. Zhao, C.-Y. Lu, and M. Atatüre, Spin-resolved quantum-dot resonance fluorescence, Nat. Phys. 5, 198 (2009).
  13. X. Ding, Y. He, Z.-C. Duan, N. Gregersen, M.-C. Chen, S. Unsleber, S. Maier, C. Schneider, M. Kamp, S. Höfling, C.-Y. Lu, and J.-W. Pan, On-demand single photons with high extraction efficiency and near-unity indistinguishability from a resonantly driven quantum dot in a micropillar, Phys. Rev. Lett. 116, 020401 (2016).
  14. H. Wang, Z.-C. Duan, Y.-H. Li, S. Chen, J.-P. Li, Y.-M. He, M.-C. Chen, Yu He, X. Ding, C.-Z. Peng, C. Schneider, M. Kamp, S. Höfling, C.-Y. Lu, and J.-W. Pan, Near-transform-limited single photons from an efficient solid-state quantum emitter, Phys. Rev. Lett. 116, 213601 (2016).
  15. N. Somaschi, V. Giesz, L. De Santis, J. C. Loredo, M. P. Almeida, G. Hornecker, S. L. Portalupi, T. Grange, C. Anton, J. Demory, C. Gomez, I. Sagnes, N. D. Lanzillotti Kimura, A. Lemaitre, A. Auffeves, A. G. White, L. Lanco, and P. Senellart, Near-optimal single-photon sources in the solid state, Nat. Photonics 10, 340 (2016).
  16. H. Wang, et al., Towards optimal single-photon sources from polarized microcavities, Nat. Photonics 13, 770 (2019).
  17. N. Tomm, A. Javadi, N. O. Antoniadis, D. Najer, M. C. Löbl, A. R. Korsch, R. Schott, S. R. Valentin, A. D. Wieck, A. Ludwig, and R. J. Warburton, A bright and fast source of coherent single photons, Nat. Nanotechnol. 16, 399 (2021).
  18. X. Ding, Y.-P. Guo, M.-C. Xu, R.-Z. Liu, G.-Y. Zou, J.-Y. Zhao, Z.-X. Ge, Q.-H. Zhang, H.-L. Liu, L.-J. Wang, M.-C. Chen, H. Wang, Y.-M. He, Y.-H. Huo, C.-Y. Lu, and J.-W. Pan, High-efficiency single-photon source above the loss-tolerant threshold for efficient linear optical quantum computing, Nat. Photonics 19, 387 (2025).
  19. H. S. Nguyen, G. Sallen, C. Voisin, P. Roussignol, C. Diederichs, and G. Cassabois, Ultra-coherent single photon source, Appl. Phys. Lett. 99, 261904 (2011).
  20. C. Matthiesen, A. N. Vamivakas, and M. Atatüre, Subnatural linewidth single photons from a quantum dot, Phys. Rev. Lett. 108, 093602 (2012).
  21. C. Matthiesen, M. Geller, C. H. H. Schulte, C. Le Gall, J. Hansom, Z. Li, M. Hugues, E. Clarke, and M. Atatüre, Phase-locked indistinguishable photons with synthesized waveforms from a solid-state source, Nat. Commun. 4, 1600 (2013).
  22. L. Hanschke, L. Schweickert, J. C. L. Carreño, E. Schöll, K. D. Zeuner, T. Lettner, E. Z. Casalengua, M. Reindl, S. F. C. da Silva, R. Trotta, J. J. Finley, A. Rastelli, E. del Valle, F. P. Laussy, V. Zwiller, K. Müller, and K. D. Jöns, Origin of antibunching in resonance fluorescence, Phys. Rev. Lett. 125, 170402 (2020).
  23. C. L. Phillips, A. J. Brash, D. P. S. McCutcheon, J. Iles-Smith, E. Clarke, B. Royall, M. S. Skolnick, A. M. Fox, and A. Nazir, Photon statistics of filtered resonance fluorescence, Phys. Rev. Lett. 125, 043603 (2020).
  24. J. C. Lopez Carrero, E. Z. Casalengua, F. P. Laussy, and E. del Valle, Joint subnatural-linewidth and single-photon emission from resonance fluorescence, Quantum Sci. Technol. 3, 045001 (2018).
  25. A. Gonzalez-Tudela, F. P. Laussy, C. Tejedor, M. J. Hartmann, and E. del Valle, Two-photon spectra of quantum emitters, New J. Phys. 15, 033036 (2013).
  26. J. Dalibard and S. Reynaud, Correlation signals in resonance fluorescence: Interpretation via photon scattering amplitudes, J. Phys. France 44, 1337 (1983).
  27. L. Masters, X.-X. Hu, M. Cordier, G. Maron, L. Pache, A. Rauschenbeutel, M. Schemmer, and J. Volz, On the simultaneous scattering of two photons by a single two-level atom, Nat. Photonics 17, 972 (2023).
  28. A. Aspect, G. Roger, S. Reynaud, J. Dalibard, and C. Cohen-Tannoudji, Time correlations between the two sidebands of the resonance fluorescence triplet, Phys. Rev. Lett. 45, 617 (1980).
  29. A. Ulhaq, S. Weiler, S. M. Ulrich, R. Roßbach, M. Jetter, and P. Michler, Cascaded single-photon emission from the Mollow triplet sidebands of a quantum dot, Nat. Photonics 6, 238 (2012).
  30. C. W. Gardiner and M. J. Collett, Input and output in damped quantum systems: Quantum stochastic differential equations and the master equation, Phys. Rev. A 31, 3761 (1985).
  31. D. F. Walls and G. J. Milburn, Quantum Optics (Springer-Verlag, Berlin, 1994).
  32. M. M. Wang, Y. F. Li, C. Y. Zeng, G. Q. Huang, L. Liu, W. Y. Wang, W. J. Ji, H. Q. Liu, H. Q. Ni, Z. C. Niu, and C. Y. Hu, Converting laser light into single photons with ultralong coherence time, Optica 12, 1838 (2025).
  33. A. Faraon, I. Fushman, D. Englund, N. Stoltz, P. Petroff, and J. Vučković, Coherent generation of non-classical light on a chip via photon-induced and blockade, Nat. Phys. 4, 859 (2008).
  34. A. Majumdar, M. Bajcsy, A. Rundquist, and J. Vučković, Loss-enabled sub-Poissonian light generation in a bimodal nanocavity, Phys. Rev. Lett. 108, 183601 (2012).
  35. J.-T. Shen and S. H. Fan, Strongly correlated two-photon transport in a one-dimensional waveguide coupled to a two-level system, Phys. Rev. Lett. 98, 153003 (2007).
  36. T. Shi, S. H. Fan, and C. P. Sun, Two-photon transport in a waveguide coupled to a cavity in a two-level system, Phys. Rev. A 84, 063803 (2011).
  37. D. E. Chang, A. S. Søensen, E. A. Demler, and M. D. Lukin, A single-photon transistor using nanoscale surface plasmons, Nat. Phys. 3, 807 (2007).
  38. A. Javadi, et al., Single-photon non-linear optics with a quantum dot in a waveguide, Nat. Commun. 6, 8655 (2015).
  39. D. Wang, H. Kelkar, D. Martín-Cano, D. Rattenbacher, A. Shkarin, T. Utikal, S. Götzinger, and V. Sandoghdar, Turning a molecule into a coherent two-level quantum system, Nat. Phys. 15, 483 (2019).
  40. N. O. Antoniadis, N. Tomm, T. Jakubczyk, R. Schott, S. R. Valentin, A. D. Wieck, A. Ludwig, R. J. Warburton, and A. Javadi, A chiral one-dimensional atom using a quantum dot in an open microcavity, npj Quantum Inf. 8, 27 (2022).
  41. S. K. Liu, O. A. D. Sandberg, M. L. Chan, B. Schrinski, Y. Anyfantaki, R. B. Nielsen, R. G. Larsen, A. Skalkin, Y. Wang, L. Midolo, S. Scholz, A. D. Wieck, A. Ludwig, A. S. Sørensen, A. Tiranov, and P. Lodahl, Violation of Bell inequality by photon scattering on a two-level emitter, Nat. Phys. 20, 1429 (2024).
  42. N. Tomm, N. O. Antoniadis, M. Janovitch, M. Brunelli, R. Schott, S. R. Valentin, A. D. Wieck, A. Ludwig, P. Potts, A. Javadi, and R. J. Warburton, Realization of a coherent and efficient one-dimensional atom, Phys. Rev. Lett. 133, 083602 (2024).
  43. J. Wang, X.-L. Zhou, Z.-M. Shen, D.-Y. Huang, S.-J. He, Q.-Y. Huang, Y.-J. Liu, C.-F. Li, and G.-C. Guo, Purcell-enhanced generation of photonic Bell states via the inelastic scattering off single atoms, Phys. Rev. Lett. 134, 053401 (2025).
  44. Y. J. Lu and Z. Y. Ou, Observation of nonclassical photon statistics due to quantum interference, Phys. Rev. Lett. 88, 023601 (2001).
  45. A. Kuhlmann, J. Houel, A. Ludwig, L. Greuter, D. Reuter, A. D. Wieck, M. Poggio, and R. J. Warburton, Charge noise and spin noise in a semiconductor quantum device, Nat. Phys. 9, 570 (2013).
  46. M. M. Wang, Y. F. Li, H. Q. Liu, H. Q. Ni, Z. C. Niu, X. G. Wei, R. F. Yang, and C. Y. Hu, Interference of single photons with ultralong coherence time, Appl. Phys. Lett. 125, 154002 (2024).
  47. Y. F. Li, M. M. Wang, C. Y. Zeng, H. Q. Liu, H. Q. Ni, Z. C. Niu, and C. Y. Hu, Two-photon interference between an independent laser and single photons with ultralong coherence time, Phys. Rev. Res. 7, 043128 (2025).
  48. P. Zeng, H. Zhou, W. Wu, and X. F. Ma, Mode-pairing quantum key distribution, Nat. Commun. 13, 3903 (2022).
  49. Y.-M. Xie, Y.-S. Lu, C.-X. Wen, X.-Y. Cao, Z.-Y. Jia, Y. Bao, Y. Wang, Y. Fu, H.-L. Yin, and Z.-B. Chen, Breaking the rate-loss bound of quantum key distribution with asynchronous two-photon interference, PRX Quantum 3, 020315 (2022).
  50. H.-T. Zhu, et al., Experimental mode-pairing measurement-device-independent quantum key distribution without global phase locking, Phys. Rev. Lett. 130, 030801 (2023).
  51. L. Zhou, J. Lin, Y.-M. Xie, Y.-S. Lu, Y. Jing, H.-L. Yin, and Z. Yuan, Experimental quantum communication overcomes the rate-loss limit without global phase tracking, Phys. Rev. Lett. 130, 250801 (2023).
  52. L. Zhang, W. Li, J. Pan, Y. Lu, W. Li, Z.-P. Li, Y. Huang, X. Ma, F. Xu, and J.-W. Pan, Experimental mode-pairing quantum key distribution surpassing the repeaterless bound, Phys. Rev. X 15, 021037 (2025).
  53. S.-F. Shao, L. Zhou, J. Lin, M. Minder, C. Ge, Y.-M. Xie, A. Shen, Z. Yan, H.-L. Yin, and Z. Yuan, High-rate measurement-device-independent quantum communication without optical reference light, Phys. Rev. X 15, 021066 (2025).
  54. M. Zou, et al., Realization of an untrusted intermediate relay architecture using a quantum dot single-photon source, Nat. Phys. 21, 1670 (2025).
  55. J. R. Johansson, P. D. Nation, and F. Nori, QuTiP 2: A Python framework for the dynamics of open quantum systems, Comput. Phys. Commun. 184, 1234 (2013).
  56. C. Y. Hu and J. G. Rarity, Extended linear regime of cavity-QED enhanced optical circular birefringence induced by a charged quantum dot, Phys. Rev. B 91, 075304 (2015).

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Phys. Rev. Research 8, 013002– Published 2 January, 2026
  • Received 10 September 2025
  • Accepted 12 December 2025
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

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