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  • Review Article
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Enhancing spectroscopy and microscopy with emerging methods in photon correlation and quantum illumination

Abstract

Quantum optics has led to important advancements in our ability to prepare and detect correlations between individual photons. Its principles are increasingly translated into nanoscale characterization tools, furthering methods in spectroscopy, microscopy and metrology. In this Review, we discuss the rapid progress in this field driven by advanced technologies of single-photon detectors and quantum-light sources, including time-resolved single-photon counting cameras, superconducting nanowire single-photon detectors and entangled photon sources of increasing brightness. We emphasize emerging applications in super-resolution microscopy, measurements below classical noise limits and photon-number-resolved spectroscopy—a powerful paradigm for the characterization of nanoscale electronic materials. We conclude by discussing key technological challenges and future opportunities in materials science and bionanophotonics alike.

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Fig. 1: Photon correlation for nanomaterials characterization.
Fig. 2: Photon correlation in super-resolution microscopy.
Fig. 3: Nanosystem characterization under quantum-light illumination.
Fig. 4: Quantum-light illumination used in microscopy.

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References

  1. Eisaman, M. D., Fan, J., Migdall, A. & Polyakov, S. V. Invited Review Article: Single-photon sources and detectors. Rev. Sci. Instrum. 82, 071101 (2011).

    Article  CAS  PubMed  Google Scholar 

  2. Cusini, I. et al. Historical perspectives, state of art and research trends of single photon avalanche diodes and their applications (Part 1: single pixels). Front. Phys. 10, 906675 (2022).

    Article  Google Scholar 

  3. Cusini, I. et al. Historical perspectives, state of art and research trends of SPAD arrays and their applications (Part II: SPAD arrays). Front. Phys. 10, 906671 (2022).

    Article  Google Scholar 

  4. Hadfield, R. H. et al. Single-photon detection for long-range imaging and sensing. Optica 10, 1124–1141 (2023).

    Article  CAS  Google Scholar 

  5. You, L. Superconducting nanowire single-photon detectors for quantum information. Nanophotonics 9, 2673–2692 (2020).

    Article  CAS  Google Scholar 

  6. Esmaeil et al. Superconducting nanowire single-photon detectors: a perspective on evolution, state-of-the-art, future developments, and applications. Appl. Phys. Lett. 118, 190502 (2021).

    Article  Google Scholar 

  7. Lau, J. A., Verma, V. B., Schwarzer, D. & Wodtke, A. M. Superconducting single-photon detectors in the mid-infrared for physical chemistry and spectroscopy. Chem. Soc. Rev. 52, 921–941 (2023).

    Article  CAS  PubMed  Google Scholar 

  8. Anwar, A., Perumangatt, C., Steinlechner, F., Jennewein, T. & Ling, A. Entangled photon-pair sources based on three-wave mixing in bulk crystals. Rev. Sci. Instrum. 92, 041101 (2021).

    Article  CAS  PubMed  Google Scholar 

  9. Orieux, A., Versteegh, M. A. M., Jöns, K. D. & Ducci, S. Semiconductor devices for entangled photon pair generation: a review. Rep. Prog. Phys. 80, 076001 (2017).

    Article  PubMed  Google Scholar 

  10. Schimpf, C. et al. Quantum dots as potential sources of strongly entangled photons: perspectives and challenges for applications in quantum networks. Appl. Phys. Lett. 118, 100502 (2021).

    Article  CAS  Google Scholar 

  11. Achar, S., Kundu, A., Chilukoti, A. & Sharma, A. Single and entangled photon pair generation using atomic vapors for quantum communication applications. Front. Quantum Sci. Technol. 3, 1438340 (2024).

    Article  Google Scholar 

  12. Ceccarelli, F. et al. Recent advances and future perspectives of single-photon avalanche diodes for quantum photonics applications. Adv. Quantum Technol. 4, 2000102 (2021).

    Article  CAS  Google Scholar 

  13. Natarajan, C. M., Tanner, M. G. & Hadfield, R. H. Superconducting nanowire single-photon detectors: physics and applications. Supercond. Sci. Technol. 25, 063001 (2012).

    Article  Google Scholar 

  14. Lubin, G. et al. Quantum correlation measurement with single photon avalanche diode arrays. Opt. Express 27, 32863 (2019).

    Article  CAS  PubMed  Google Scholar 

  15. Lubin, G. et al. Heralded spectroscopy reveals exciton–exciton correlations in single colloidal quantum dots. Nano Lett. 21, 6756–6763 (2021).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  16. Szoke, S., He, M., Hickam, B. P. & Cushing, S. K. Designing high-power, octave spanning entangled photon sources for quantum spectroscopy. J. Chem. Phys. 154, 244201 (2021).

    Article  CAS  PubMed  Google Scholar 

  17. Sultanov, V. et al. Tunable entangled photon-pair generation in a liquid crystal. Nature 631, 294–299 (2024).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  18. Lubin, G., Oron, D., Rossman, U., Tenne, R. & Yallapragada, V. J. Photon correlations in spectroscopy and microscopy. ACS Photonics 9, 2891–2904 (2022).

    Article  CAS  Google Scholar 

  19. Stetefeld, J., McKenna, S. A. & Patel, T. R. Dynamic light scattering: a practical guide and applications in biomedical sciences. Biophys. Rev. 8, 409–427 (2016).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  20. Lloyd, S. Enhanced sensitivity of photodetection via quantum illumination. Science 321, 1463–1465 (2008).

    Article  CAS  PubMed  Google Scholar 

  21. Aspect, A., Dalibard, J. & Roger, G. Experimental test of Bell’s inequalities using time-varying analyzers. Phys. Rev. Lett. 49, 1804–1807 (1982).

    Article  Google Scholar 

  22. Meystre, P. Theoretical developments in cavity quantum optics: a brief review. Phys. Rep. 219, 243–262 (1992).

    Article  Google Scholar 

  23. Srivathsan, B. et al. Narrow band source of transform-limited photon pairs via four-wave mixing in a cold atomic ensemble. Phys. Rev. Lett. 111, 123602 (2013).

    Article  PubMed  Google Scholar 

  24. David, A. & Miller, B. in Quantum Dynamics of Simple Systems (eds Oppo, G.-L. et al.) 239–266 (CRC Press, 2020); https://doi.org/10.1201/9781003072973-9

  25. Bassett, L. C., Alkauskas, A., Exarhos, A. L. & Fu, K.-M. C. Quantum defects by design. Nanophotonics 8, 1867–1888 (2019).

    Article  CAS  Google Scholar 

  26. Hohenester, U. Nano and Quantum Optics: An Introduction to Basic Principles and Theory (Springer, 2019).

  27. Defienne, H. et al. Advances in quantum imaging. Nat. Photon. 18, 1024–1036 (2024).

    Article  CAS  Google Scholar 

  28. Kimble, H. J., Dagenais, M. & Mandel, L. Photon antibunching in resonance fluorescence. Phys. Rev. Lett. 39, 691–695 (1977).

    Article  CAS  Google Scholar 

  29. Hollars, C. W., Lane, S. M. & Huser, T. Controlled non-classical photon emission from single conjugated polymer molecules. Chem. Phys. Lett. 370, 393–398 (2003).

    Article  CAS  Google Scholar 

  30. Kumar, P. et al. Photon antibunching from oriented semiconducting polymer nanostructures. J. Am. Chem. Soc. 126, 3376–3377 (2004).

    Article  CAS  PubMed  Google Scholar 

  31. He, Y.-M. et al. Single quantum emitters in monolayer semiconductors. Nat. Nanotechnol. 10, 497–502 (2015).

    Article  CAS  PubMed  Google Scholar 

  32. Chakraborty, C., Kinnischtzke, L., Goodfellow, K. M., Beams, R. & Vamivakas, A. N. Voltage-controlled quantum light from an atomically thin semiconductor. Nat. Nanotechnol. 10, 507–511 (2015).

    Article  CAS  PubMed  Google Scholar 

  33. Koperski, M. et al. Single photon emitters in exfoliated WSe2 structures. Nat. Nanotechnol. 10, 503–506 (2015).

    Article  CAS  PubMed  Google Scholar 

  34. Srivastava, A. et al. Optically active quantum dots in monolayer WSe2. Nat. Nanotechnol. 10, 491–496 (2015).

    Article  CAS  PubMed  Google Scholar 

  35. Tran, T. T., Bray, K., Ford, M. J., Toth, M. & Aharonovich, I. Quantum emission from hexagonal boron nitride monolayers. Nat. Nanotechnol. 11, 37–41 (2016).

    Article  CAS  PubMed  Google Scholar 

  36. Michler, P. et al. Quantum correlation among photons from a single quantum dot at room temperature. Nature 406, 968–970 (2000).

    Article  CAS  PubMed  Google Scholar 

  37. Somaschi, N. et al. Near-optimal single-photon sources in the solid state. Nat. Photon. 10, 340–345 (2016).

    Article  CAS  Google Scholar 

  38. Nair, G., Zhao, J. & Bawendi, M. G. Biexciton quantum yield of single semiconductor nanocrystals from photon statistics. Nano Lett. 11, 1136–1140 (2011).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  39. Koley, S. et al. Photon correlations in colloidal quantum dot molecules controlled by the neck barrier. Matter 5, 3997–4014 (2022).

    Article  CAS  Google Scholar 

  40. Zhu, H. et al. One-dimensional highly-confined CsPbBr3 nanorods with enhanced stability: synthesis and spectroscopy. Nano Lett. 22, 8355–8362 (2022).

    Article  CAS  PubMed  Google Scholar 

  41. Ma, X. et al. Size-dependent biexciton quantum yields and carrier dynamics of quasi-two-dimensional core/shell nanoplatelets. ACS Nano 11, 9119–9127 (2017).

    Article  CAS  PubMed  Google Scholar 

  42. Mangum, B. D. et al. Influence of the core size on biexciton quantum yield of giant CdSe/CdS nanocrystals. Nanoscale 6, 3712–3720 (2014).

    Article  CAS  PubMed  Google Scholar 

  43. Brouri, R., Beveratos, A., Poizat, J.-P. & Grangier, P. Photon antibunching in the fluorescence of individual color centers in diamond. Opt. Lett. 25, 1294 (2000).

    Article  CAS  PubMed  Google Scholar 

  44. Basché, T., Moerner, W. E., Orrit, M. & Talon, H. Photon antibunching in the fluorescence of a single dye molecule trapped in a solid. Phys. Rev. Lett. 69, 1516–1519 (1992).

    Article  PubMed  Google Scholar 

  45. Tamarat, P. et al. The dark exciton ground state promotes photon-pair emission in individual perovskite nanocrystals. Nat. Commun. 11, 6001 (2020).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  46. Fleury, L., Segura, J.-M., Zumofen, G., Hecht, B. & Wild, U. P. Nonclassical photon statistics in single-molecule fluorescence at room temperature. Phys. Rev. Lett. 84, 1148–1151 (2000).

    Article  CAS  PubMed  Google Scholar 

  47. Dräbenstedt, A. et al. Low-temperature microscopy and spectroscopy on single defect centers in diamond. Phys. Rev. B 60, 11503–11508 (1999).

    Article  Google Scholar 

  48. Dicke, R. H. Coherence in spontaneous radiation processes. Phys. Rev. 93, 99–110 (1954).

    Article  CAS  Google Scholar 

  49. 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).

    Article  CAS  Google Scholar 

  50. Bonifacio, R. & Lugiato, L. A. Cooperative radiation processes in two-level systems: superfluorescence. Phys. Rev. A 11, 1507–1521 (1975).

    Article  Google Scholar 

  51. Bonifacio, R. & Lugiato, L. A. Cooperative radiation processes in two-level systems: superfluorescence. II. Phys. Rev. A 12, 587–598 (1975).

    Article  Google Scholar 

  52. Skribanowitz, N., Herman, I. P., MacGillivray, J. C. & Feld, M. S. Observation of Dicke superradiance in optically pumped HF gas. Phys. Rev. Lett. 30, 309–312 (1973).

    Article  Google Scholar 

  53. Fidder, H., Knoester, J. & Wiersma, D. A. Superradiant emission and optical dephasing in J-aggregates. Chem. Phys. Lett. 171, 529–536 (1990).

    Article  CAS  Google Scholar 

  54. Lim, S.-H., Bjorklund, T. G., Spano, F. C. & Bardeen, C. J. Exciton delocalization and superradiance in tetracene thin films and nanoaggregates. Phys. Rev. Lett. 92, 107402 (2004).

    Article  PubMed  Google Scholar 

  55. Meinardi, F., Cerminara, M., Sassella, A., Bonifacio, R. & Tubino, R. Superradiance in molecular H aggregates. Phys. Rev. Lett. 91, 247401 (2003).

    Article  CAS  PubMed  Google Scholar 

  56. Spano, F. C. The spectral signatures of Frenkel polarons in H- and J-aggregates. Acc. Chem. Res. 43, 429–439 (2010).

    Article  CAS  PubMed  Google Scholar 

  57. Wang, H. Z., Zheng, X. G., Zhao, F. L., Gao, Z. L. & Yu, Z. X. Superradiance of high density frenkel excitons at room temperature. Phys. Rev. Lett. 74, 4079–4082 (1995).

    Article  CAS  PubMed  Google Scholar 

  58. Monshouwer, R., Abrahamsson, M., van Mourik, F. & van Grondelle, R. Superradiance and exciton delocalization in bacterial photosynthetic light-harvesting systems. J. Phys. Chem. B 101, 7241–7248 (1997).

    Article  CAS  Google Scholar 

  59. Scheibner, M. et al. Superradiance of quantum dots. Nat. Phys. 3, 106–110 (2007).

    Article  CAS  Google Scholar 

  60. Kim, J.-H., Aghaeimeibodi, S., Richardson, C. J. K., Leavitt, R. P. & Waks, E. Super-radiant emission from quantum dots in a nanophotonic waveguide. Nano Lett. 18, 4734–4740 (2018).

    Article  CAS  PubMed  Google Scholar 

  61. Grim, J. Q. et al. Scalable in operando strain tuning in nanophotonic waveguides enabling three-quantum-dot superradiance. Nat. Mater. 18, 963–969 (2019).

    Article  CAS  PubMed  Google Scholar 

  62. Zhang, L. et al. New insights into the multiexciton dynamics in phase-pure thick-shell CdSe/CdS quantum dots. J. Phys. Chem. C 122, 25059–25066 (2018).

    Article  CAS  Google Scholar 

  63. Zhu, C. et al. Single-photon superradiance in individual caesium lead halide quantum dots. Nature 626, 535–541 (2024).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  64. Huang, K. et al. Room-temperature upconverted superfluorescence. Nat. Photon. 16, 737–742 (2022).

    Article  CAS  Google Scholar 

  65. Sipahigil, A. et al. An integrated diamond nanophotonics platform for quantum-optical networks. Science 354, 847–850 (2016).

    Article  CAS  PubMed  Google Scholar 

  66. Rainò, G. et al. Superfluorescence from lead halide perovskite quantum dot superlattices. Nature 563, 671–675 (2018).

    Article  PubMed  Google Scholar 

  67. Findik, G. et al. High-temperature superfluorescence in methyl ammonium lead iodide. Nat. Photon. 15, 676–680 (2021).

    Article  CAS  Google Scholar 

  68. Biliroglu, M. et al. Room-temperature superfluorescence in hybrid perovskites and its origins. Nat. Photon. 16, 324–329 (2022).

    Article  CAS  Google Scholar 

  69. Schedlbauer, J. et al. Tracking exciton diffusion and exciton annihilation in single nanoparticles of conjugated polymers by photon correlation spectroscopy. Adv. Opt. Mater. 10, 2200092 (2022).

    Article  CAS  Google Scholar 

  70. Hofkens, J. et al. Revealing competitive Förster-type resonance energy-transfer pathways in single bichromophoric molecules. Proc. Natl Acad. Sci. USA 100, 13146–13151 (2003).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  71. Bernard, J., Fleury, L., Talon, H. & Orrit, M. Photon bunching in the fluorescence from single molecules: a probe for intersystem crossing. J. Chem. Phys. 98, 850–859 (1993).

    Article  CAS  Google Scholar 

  72. Hedley, G. J. et al. Picosecond time-resolved photon antibunching measures nanoscale exciton motion and the true number of chromophores. Nat. Commun. 12, 1327 (2021).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  73. Stevens, M. J., Glancy, S., Nam, S. W. & Mirin, R. P. Third-order antibunching from an imperfect single-photon source. Opt. Express 22, 3244 (2014).

    Article  PubMed  Google Scholar 

  74. Rundquist, A. et al. Nonclassical higher-order photon correlations with a quantum dot strongly coupled to a photonic-crystal nanocavity. Phys. Rev. A 90, 023846 (2014).

    Article  Google Scholar 

  75. Amgar, D., Yang, G., Tenne, R. & Oron, D. Higher-order photon correlation as a tool to study exciton dynamics in quasi-2D nanoplatelets. Nano Lett. 19, 8741–8748 (2019).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  76. Frenkel, N. et al. Two biexciton types coexisting in coupled quantum dot molecules. ACS Nano 17, 14990–15000 (2023).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  77. Lubin, G. et al. Resolving the controversy in biexciton binding energy of cesium lead halide perovskite nanocrystals through heralded single-particle spectroscopy. ACS Nano 15, 19581–19587 (2021).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  78. Wollman, E. E. et al. Kilopixel array of superconducting nanowire single-photon detectors. Opt. Express 27, 35279 (2019).

    Article  CAS  PubMed  Google Scholar 

  79. Oripov, B. G. et al. A superconducting nanowire single-photon camera with 400,000 pixels. Nature 622, 730–734 (2023).

    Article  CAS  PubMed  Google Scholar 

  80. Zasedatelev, A. V. et al. Single-photon nonlinearity at room temperature. Nature 597, 493–497 (2021).

    Article  CAS  PubMed  Google Scholar 

  81. Pei, J., Yang, J., Yildirim, T., Zhang, H. & Lu, Y. Many-body complexes in 2D semiconductors. Adv. Mater. 31, 1706945 (2019).

    Article  Google Scholar 

  82. Gu, B. & Mukamel, S. Photon correlation signals in coupled-cavity polaritons created by entangled light. ACS Photonics 9, 938–943 (2022).

    Article  CAS  Google Scholar 

  83. Dertinger, T., Colyer, R., Iyer, G., Weiss, S. & Enderlein, J. Fast, background-free, 3D super-resolution optical fluctuation imaging (SOFI). Proc. Natl Acad. Sci. USA 106, 22287–22292 (2009).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  84. Dertinger, T., Colyer, R., Vogel, R., Enderlein, J. & Weiss, S. Achieving increased resolution and more pixels with superresolution optical fluctuation imaging (SOFI). Opt. Express 18, 18875 (2010).

    Article  PubMed  PubMed Central  Google Scholar 

  85. Sroda, A. et al. SOFISM: super-resolution optical fluctuation image scanning microscopy. Optica 7, 1308 (2020).

    Article  Google Scholar 

  86. Zhao, G., Zheng, C., Kuang, C. & Liu, X. Resolution-enhanced SOFI via structured illumination. Opt. Lett. 42, 3956 (2017).

    Article  PubMed  Google Scholar 

  87. Schwartz, O. & Oron, D. Improved resolution in fluorescence microscopy using quantum correlations. Phys. Rev. A 85, 033812 (2012).

    Article  Google Scholar 

  88. Schwartz, O. et al. Superresolution microscopy with quantum emitters. Nano Lett. 13, 5832–5836 (2013).

    Article  CAS  PubMed  Google Scholar 

  89. Tenne, R. et al. Super-resolution enhancement by quantum image scanning microscopy. Nat. Photon. 13, 116–122 (2019).

    Article  CAS  Google Scholar 

  90. Chen, Y., Tsao, C., Cobb-Bruno, C. & Utzat, H. Stochastic frequency fluctuation super-resolution imaging. Opt. Express 33, 6514–6525 (2025).

    Article  PubMed  Google Scholar 

  91. Meuret, S. et al. Nanoscale relative emission efficiency mapping using cathodoluminescence g(2) imaging. Nano Lett. 18, 2288–2293 (2018).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  92. Tizei, L. H. G. & Kociak, M. Spatially resolved quantum nano-optics of single photons using an electron microscope. Phys. Rev. Lett. 110, 153604 (2013).

    Article  CAS  PubMed  Google Scholar 

  93. Meuret, S. et al. Lifetime measurements well below the optical diffraction limit. ACS Photonics 3, 1157–1163 (2016).

    Article  CAS  Google Scholar 

  94. Yanagimoto, S. et al. Time-correlated electron and photon counting microscopy. Commun. Phys. 6, 260 (2023).

    Article  Google Scholar 

  95. Rosławska, A. et al. Atomic-scale dynamics probed by photon correlations. ACS Nano 14, 6366–6375 (2020).

    Article  PubMed  PubMed Central  Google Scholar 

  96. Yanagimoto, S., Yamamoto, N., Yuge, T., Sannomiya, T. & Akiba, K. Unveiling the nature of cathodoluminescence from photon statistics. Commun. Phys. 8, 56 (2025).

    Article  Google Scholar 

  97. Meuret, S. et al. Photon bunching in cathodoluminescence. Phys. Rev. Lett. 114, 197401 (2015).

    Article  CAS  PubMed  Google Scholar 

  98. Kazakevich, E., Aharon, H. & Kfir, O. Spatial electron-photon entanglement. Phys. Rev. Res. 6, 043033 (2024).

    Article  CAS  Google Scholar 

  99. Harper, N., Hickam, B. P., He, M. & Cushing, S. K. Entangled photon correlations allow a continuous-wave laser diode to measure single-photon, time-resolved fluorescence. J. Phys. Chem. Lett. 14, 5805–5811 (2023).

    Article  CAS  PubMed  Google Scholar 

  100. Eshun, A. et al. Fluorescence lifetime measurements using photon pair correlations generated via spontaneous parametric down conversion (SPDC). Opt. Express 31, 26935 (2023).

    Article  PubMed  Google Scholar 

  101. Li, Q. et al. Single-photon absorption and emission from a natural photosynthetic complex. Nature 619, 300–304 (2023).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  102. Eshun, A., Varnavski, O., Villabona-Monsalve, J. P., Burdick, R. K. & Goodson, T. I. Entangled photon spectroscopy. Acc. Chem. Res. 55, 991–1003 (2022).

    Article  CAS  PubMed  Google Scholar 

  103. Hickam, B. P., He, M., Harper, N., Szoke, S. & Cushing, S. K. Single-photon scattering can account for the discrepancies among entangled two-photon measurement techniques. J. Phys. Chem. Lett. 13, 4934–4940 (2022).

    Article  CAS  PubMed  Google Scholar 

  104. Varnavski, O. & Goodson, T. I. Two-photon fluorescence microscopy at extremely low excitation intensity: the power of quantum correlations. J. Am. Chem. Soc. 142, 12966–12975 (2020).

    Article  CAS  PubMed  Google Scholar 

  105. Steinberg, A. M., Kwiat, P. G. & Chiao, R. Y. Dispersion cancellation in a measurement of the single-photon propagation velocity in glass. Phys. Rev. Lett. 68, 2421–2424 (1992).

    Article  CAS  PubMed  Google Scholar 

  106. Ou, Z.-Y. J. Multi-Photon Quantum Interference (Springer, 2007); https://doi.org/10.1007/978-0-387-25554-5

  107. Ryu, J., Cho, K., Oh, C.-H. & Kang, H. All-order dispersion cancellation and energy-time entangled state. Opt. Express 25, 1360 (2017).

    Article  CAS  PubMed  Google Scholar 

  108. Okano, M. et al. Dispersion cancellation in high-resolution two-photon interference. Phys. Rev. A 88, 043845 (2013).

    Article  Google Scholar 

  109. Lyons, A. et al. Attosecond-resolution Hong–Ou–Mandel interferometry. Sci. Adv. 4, eaap9416 (2018).

    Article  PubMed  PubMed Central  Google Scholar 

  110. Ndagano, B. et al. Quantum microscopy based on Hong–Ou–Mandel interference. Nat. Photon. 16, 384–389 (2022).

    Article  CAS  Google Scholar 

  111. Dorfman, K. E., Asban, S., Gu, B. & Mukamel, S. Hong–Ou–Mandel interferometry and spectroscopy using entangled photons. Commun. Phys. 4, 49 (2021).

    Article  Google Scholar 

  112. Kalashnikov, D. A. et al. Quantum interference in the presence of a resonant medium. Sci. Rep. 7, 11444 (2017).

    Article  PubMed  PubMed Central  Google Scholar 

  113. Eshun, A. et al. Investigations of molecular optical properties using quantum light and Hong–Ou–Mandel interferometry. J. Am. Chem. Soc. 143, 9070–9081 (2021).

    Article  CAS  PubMed  Google Scholar 

  114. Gregory, T., Moreau, P.-A., Toninelli, E. & Padgett, M. J. Imaging through noise with quantum illumination. Sci. Adv. 6, eaay2652 (2020).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  115. Defienne, H., Reichert, M., Fleischer, J. W. & Faccio, D. Quantum image distillation. Sci. Adv. 5, eaax0307 (2019).

    Article  PubMed  PubMed Central  Google Scholar 

  116. Morris, P. A., Aspden, R. S., Bell, J. E. C., Boyd, R. W. & Padgett, M. J. Imaging with a small number of photons. Nat. Commun. 6, 5913 (2015).

    Article  CAS  PubMed  Google Scholar 

  117. Brida, G., Genovese, M. & Ruo Berchera, I. Experimental realization of sub-shot-noise quantum imaging. Nat. Photon. 4, 227–230 (2010).

    Article  CAS  Google Scholar 

  118. Aspden, R. S. et al. Photon-sparse microscopy: visible light imaging using infrared illumination. Optica 2, 1049 (2015).

    Article  CAS  Google Scholar 

  119. Padgett, M. J. & Boyd, R. W. An introduction to ghost imaging: quantum and classical. Philos. Trans. R. Soc. A 375, 20160233 (2017).

    Article  Google Scholar 

  120. Bennink, R. S., Bentley, S. J. & Boyd, R. W. “Two-photon” coincidence imaging with a classical source. Phys. Rev. Lett. 89, 113601 (2002).

    Article  PubMed  Google Scholar 

  121. Gatti, A., Brambilla, E., Bache, M. & Lugiato, L. A. Correlated imaging, quantum and classical. Phys. Rev. A 70, 013802 (2004).

    Article  Google Scholar 

  122. Karmakar, S. & Shih, Y. Two-color ghost imaging with enhanced angular resolving power. Phys. Rev. A 81, 033845 (2010).

    Article  Google Scholar 

  123. Valencia, A., Scarcelli, G., D’Angelo, M. & Shih, Y. Two-photon imaging with thermal light. Phys. Rev. Lett. 94, 063601 (2005).

    Article  PubMed  Google Scholar 

  124. Lopaeva, E. D. et al. Experimental realization of quantum illumination. Phys. Rev. Lett. 110, 153603 (2013).

    Article  CAS  PubMed  Google Scholar 

  125. Lemos, G. B. et al. Quantum imaging with undetected photons. Nature 512, 409–412 (2014).

    Article  CAS  PubMed  Google Scholar 

  126. Kviatkovsky, I., Chrzanowski, H. M., Avery, E. G., Bartolomaeus, H. & Ramelow, S. Microscopy with undetected photons in the mid-infrared. Sci. Adv. 6, eabd0264 (2020).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  127. Walther, P. et al. De Broglie wavelength of a non-local four-photon state. Nature 429, 158–161 (2004).

    Article  CAS  PubMed  Google Scholar 

  128. Nagata, T., Okamoto, R., O’Brien, J. L., Sasaki, K. & Takeuchi, S. Beating the standard quantum limit with four-entangled photons. Science 316, 726–729 (2007).

    Article  CAS  PubMed  Google Scholar 

  129. Dowling, J. P. Quantum optical metrology—the lowdown on high-N00N states. Contemp. Phys. 49, 125–143 (2008).

    Article  CAS  Google Scholar 

  130. Ono, T., Okamoto, R. & Takeuchi, S. An entanglement-enhanced microscope. Nat. Commun. 4, 2426 (2013).

    Article  PubMed  Google Scholar 

  131. Israel, Y., Rosen, S. & Silberberg, Y. Supersensitive polarization microscopy using NOON states of light. Phys. Rev. Lett. 112, 103604 (2014).

    Article  PubMed  Google Scholar 

  132. Boto, A. N. et al. Quantum interferometric optical lithography: exploiting entanglement to beat the diffraction limit. Phys. Rev. Lett. 85, 2733–2736 (2000).

    Article  CAS  PubMed  Google Scholar 

  133. Kok, P. et al. Quantum-interferometric optical lithography: towards arbitrary two-dimensional patterns. Phys. Rev. A 63, 063407 (2001).

    Article  Google Scholar 

  134. Barreiro, J. T., Langford, N. K., Peters, N. A. & Kwiat, P. G. Generation of hyperentangled photon pairs. Phys. Rev. Lett. 95, 260501 (2005).

    Article  PubMed  Google Scholar 

  135. Kwiat, P. G. Hyper-entangled states. J. Mod. Opt. 44, 2173–2184 (1997).

    Article  Google Scholar 

  136. Zhang, Y. et al. Quantum imaging of biological organisms through spatial and polarization entanglement. Sci. Adv. 10, eadk1495 (2024).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  137. Camphausen, R. et al. A quantum-enhanced wide-field phase imager. Sci. Adv. 7, eabj2155 (2021).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  138. Defienne, H., Ndagano, B., Lyons, A. & Faccio, D. Polarization entanglement-enabled quantum holography. Nat. Phys. 17, 591–597 (2021).

    Article  CAS  Google Scholar 

  139. Aasi, J. et al. Enhanced sensitivity of the LIGO gravitational wave detector by using squeezed states of light. Nat. Photon. 7, 613–619 (2013).

    Article  CAS  Google Scholar 

  140. Casacio, C. A. et al. Quantum-enhanced nonlinear microscopy. Nature 594, 201–206 (2021).

    Article  CAS  PubMed  Google Scholar 

  141. Chu, X.-L., Götzinger, S. & Sandoghdar, V. A single molecule as a high-fidelity photon gun for producing intensity-squeezed light. Nat. Photon. 11, 58–62 (2017).

    Article  CAS  Google Scholar 

  142. Lounis, B. & Orrit, M. Single-photon sources. Rep. Prog. Phys. 68, 1129–1179 (2005).

    Article  CAS  Google Scholar 

  143. Loredo, J. C. et al. Scalable performance in solid-state single-photon sources. Optica 3, 433–440 (2016).

    Article  Google Scholar 

  144. Mandel, L. & Wolf, E. Optical Coherence and Quantum Optics (Cambridge Univ. Press, 1995); https://doi.org/10.1017/CBO9781139644105

  145. Steinhauer, S., Gyger, S. & Zwiller, V. Progress on large-scale superconducting nanowire single-photon detectors. Appl. Phys. Lett. 118, 100501 (2021).

    Article  CAS  Google Scholar 

  146. Mueller, A. S. et al. Free-space coupled superconducting nanowire single-photon detector with low dark counts. Optica 8, 1586–1587 (2021).

    Article  Google Scholar 

  147. Harper, N. A. et al. Highly efficient visible and near-IR photon pair generation with thin-film lithium niobate. Opt. Quantum 2, 103–109 (2024).

    Article  Google Scholar 

  148. Cortes, C. L., Adhikari, S., Ma, X. & Gray, S. K. Accelerating quantum optics experiments with statistical learning. Appl. Phys. Lett. 116, 184003 (2020).

    Article  CAS  Google Scholar 

  149. Kudyshev, Z. A. et al. Machine learning assisted quantum super-resolution microscopy. Nat. Commun. 14, 4828 (2023).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  150. Proppe, A. H. et al. Time-resolved line shapes of single quantum emitters via machine learned photon correlations. Phys. Rev. Lett. 131, 053603 (2023).

    Article  CAS  PubMed  Google Scholar 

  151. Lavoie, J. et al. Phase-modulated interferometry, spectroscopy, and refractometry using entangled photon pairs. Adv. Quantum Technol. 3, 1900114 (2020).

    Article  CAS  Google Scholar 

  152. Yin, L. et al. Analysis of the spatial properties of correlated photon in collinear phase-matching. Photonics 8, 12 (2021).

    Article  CAS  Google Scholar 

  153. Sansa Perna, A., Ortega, E., Gräfe, M. & Steinlechner, F. Visible-wavelength polarization-entangled photon source for quantum communication and imaging. Appl. Phys. Lett. 120, 074001 (2022).

    Article  CAS  Google Scholar 

  154. Lu, X. et al. Chip-integrated visible–telecom entangled photon pair source for quantum communication. Nat. Phys. 15, 373–381 (2019).

    Article  CAS  Google Scholar 

  155. Wang, H. et al. On-demand semiconductor source of entangled photons which simultaneously has high fidelity, efficiency, and indistinguishability. Phys. Rev. Lett. 122, 113602 (2019).

    Article  CAS  PubMed  Google Scholar 

  156. Huber, D., Reindl, M., Aberl, J., Rastelli, A. & Trotta, R. Semiconductor quantum dots as an ideal source of polarization-entangled photon pairs on-demand: a review. J. Opt. 20, 073002 (2018).

    Article  Google Scholar 

  157. Kim, H., Park, H. S. & Choi, S.-K. Three-photon N00N states generated by photon subtraction from double photon pairs. Opt. Express 17, 19720 (2009).

    Article  CAS  PubMed  Google Scholar 

  158. Mitchell, M. W., Lundeen, J. S. & Steinberg, A. M. Super-resolving phase measurements with a multiphoton entangled state. Nature 429, 161–164 (2004).

    Article  CAS  PubMed  Google Scholar 

  159. Sun, F. W., Ou, Z. Y. & Guo, G. C. Projection measurement of the maximally entangled N-photon state for a demonstration of the N-photon de Broglie wavelength. Phys. Rev. A 73, 023808 (2006).

    Article  Google Scholar 

  160. Sun, F. W., Liu, B. H., Huang, Y. F., Ou, Z. Y. & Guo, G. C. Observation of the four-photon de Broglie wavelength by state-projection measurement. Phys. Rev. A 74, 033812 (2006).

    Article  Google Scholar 

  161. Liu, B. H. et al. Demonstration of the three-photon de Broglie wavelength by projection measurement. Phys. Rev. A 77, 023815 (2008).

    Article  Google Scholar 

  162. Resch, K. J. et al. Time-reversal and super-resolving phase measurements. Phys. Rev. Lett. 98, 223601 (2007).

    Article  CAS  PubMed  Google Scholar 

  163. Afek, I., Ambar, O. & Silberberg, Y. High-NOON states by mixing quantum and classical light. Science 328, 879–881 (2010).

    Article  CAS  PubMed  Google Scholar 

  164. Fuenzalida, J. et al. Resolution of quantum imaging with undetected photons. Quantum 6, 646 (2022).

    Article  Google Scholar 

  165. Viswanathan, B., Barreto Lemos, G. & Lahiri, M. Resolution limit in quantum imaging with undetected photons using position correlations. Opt. Express 29, 38185 (2021).

    Article  PubMed  Google Scholar 

  166. Dorfman, K. E., Schlawin, F. & Mukamel, S. Nonlinear optical signals and spectroscopy with quantum light. Rev. Mod. Phys. 88, 045008 (2016).

    Article  Google Scholar 

  167. Ko, L., Cook, R. L. & Whaley, K. B. Dynamics of photosynthetic light harvesting systems interacting with N-photon Fock states. J. Chem. Phys. 156, 244108 (2022).

    Article  CAS  PubMed  Google Scholar 

  168. Roslyak, O., Marx, C. A. & Mukamel, S. Nonlinear spectroscopy with entangled photons: manipulating quantum pathways of matter. Phys. Rev. A 79, 033832 (2009).

    Article  Google Scholar 

  169. Rodriguez-Camargo, C. D., Gestsson, H. O., Nation, C., Jones, A. R. & Olaya-Castro, A. Perturbation-theory approach for predicting vibronic selectivity by entangled-photon-pair absorption. Phys. Rev. A 111, 063101 (2025).

    Article  CAS  Google Scholar 

  170. Loudon, R. The Quantum Theory of Light (Oxford Univ. Press, 2000).

  171. Fox, M. Quantum Optics: An Introduction (Oxford Univ. Press, 2006).

  172. Feynman, R. P. & Hibbs, A. R. Quantum Mechanics and Path Integrals: Emended Edition (Dover Publications, 2010).

  173. Feynman, R. P., Leighton, R. B. & Sands, M. The Feynman Lectures on Physics Vol. 3 (Addison Wesley, 1971).

  174. 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).

    Article  CAS  PubMed  Google Scholar 

  175. Berchera, I. R. & Degiovanni, I. P. Quantum imaging with sub-Poissonian light: challenges and perspectives in optical metrology. Metrologia 56, 024001 (2019).

    Article  CAS  Google Scholar 

  176. Hadfield, R. H. Single-photon detectors for optical quantum information applications. Nat. Photon. 3, 696–705 (2009).

    Article  CAS  Google Scholar 

  177. McCaughan, A. N. Readout architectures for superconducting nanowire single photon detectors. Supercond. Sci. Technol. 31, 040501 (2018).

    Article  Google Scholar 

  178. McCaughan, A. N. et al. The thermally-coupled imager: a scalable readout architecture for superconducting nanowire single photon detectors. Appl. Phys. Lett. 121, 102602 (2022).

    Article  CAS  Google Scholar 

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Acknowledgements

This work was financially supported by the College of Chemistry at the University of California, Berkeley and the US Department of Energy (DE-AC02-05CH11231).

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Tsao, C., Ling, H., Hinkle, A. et al. Enhancing spectroscopy and microscopy with emerging methods in photon correlation and quantum illumination. Nat. Nanotechnol. 20, 1001–1016 (2025). https://doi.org/10.1038/s41565-025-01992-3

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