- Open Access
Optimally driving multiphoton transitions in the perturbative single-mode regime
Phys. Rev. A 113, 063727 – Published 16 June, 2026
DOI: https://doi.org/10.1103/s5fb-yljk
Abstract
The rate of -photon transitions in matter, induced by an incident light field, depends on the field's -order coherence function. Consequently, the coherence properties of the light field may be shaped to increase the rate of multiphoton transitions. Here, we determine the optimal state of a weak fixed-intensity, narrow-band incident light field, with a restricted maximal photon number, that optimally drives -photon transitions in the case of a short-lived atomic multilevel system. We show that, in this case, no quantum properties of the light field need to be exploited, but that classical mixtures of coherent states are optimal.
Physics Subject Headings (PhySH)
Article Text
References (30)
- M. Shapiro and P. Brumer, Quantum Control of Molecular Processes (Wiley, Weinheim, Germany, 2011).
- S. Mukamel III, M. Freyberger, W. Schleich, M. Bellini, A. Zavatta, G. Leuchs, C. Silberhorn, R. W. Boyd, L. L. Sánchez-Soto, A. Stefanov, M. Barbieri, A. Paterova, L. Krivitsky, S. Shwartz, K. Tamasaku, K. Dorfman, F. Schlawin, V. Sandoghdar, M. Raymer, A. Marcus, et al., Roadmap on quantum light spectroscopy, J. Phys. B: At. Mol. Opt. Phys. 53, 072002 (2020).
- K. E. Dorfman, F. Schlawin, and S. Mukamel, Nonlinear optical signals and spectroscopy with quantum light, Rev. Mod. Phys. 88, 045008 (2016).
- P. Lambropoulos, C. Kikuchi, and R. K. Osborn, Coherence and two-photon absorption, Phys. Rev. 144, 1081 (1966).
- B. Mollow, Two-photon absorption and field correlation functions, Phys. Rev. 175, 1555 (1968).
- P. Lambropoulos, Field-correlation effects in two-photon processes, Phys. Rev. 168, 1418 (1968).
- G. S. Agarwal, Field-correlation effects in multiphoton absorption processes, Phys. Rev. A 1, 1445 (1970).
- A. Jechow, M. Seefeldt, H. Kurzke, A. Heuer, and R. Menzel, Enhanced two-photon excited fluorescence from imaging agents using true thermal light, Nat. Photonics 7, 973 (2013).
- K. Y. Spasibko, D. A. Kopylov, V. L. Krutyanskiy, T. V. Murzina, G. Leuchs, and M. V. Chekhova, Multiphoton effects enhanced due to ultrafast photon-number fluctuations, Phys. Rev. Lett. 119, 223603 (2017).
- N. P. Georgiades, E. S. Polzik, K. Edamatsu, H. J. Kimble, and A. S. Parkins, Nonclassical excitation for atoms in a squeezed vacuum, Phys. Rev. Lett. 75, 3426 (1995).
- B. Dayan, A. Pe'Er, A. A. Friesem, and Y. Silberberg, Two photon absorption and coherent control with broadband down-converted light, Phys. Rev. Lett. 93, 023005 (2004).
- D.-I. Lee and T. Goodson, Entangled photon absorption in an organic porphyrin dendrimer, J. Phys. Chem. B 110, 25582 (2006).
- F. Schlawin and A. Buchleitner, Theory of coherent control with quantum light, New J. Phys. 19, 013009 (2017).
- E. S. Polzik, J. Carri, and H. J. Kimble, Spectroscopy with squeezed light, Phys. Rev. Lett. 68, 3020 (1992).
- S. Szoke, H. Liu, B. P. Hickam, M. He, and S. K. Cushing, Entangled light–matter interactions and spectroscopy, J. Mater. Chem. C 8, 10732 (2020).
- M. Gilaberte Basset, F. Setzpfandt, F. Steinlechner, E. Beckert, T. Pertsch, and M. Gräfe, Perspectives for applications of quantum imaging Laser Photonics Rev. 13, 1900097 (2019).
- J. C. López Carreño, C. Sánchez Muñoz, D. Sanvitto, E. Del Valle, and F. P. Laussy, Exciting polaritons with quantum light, Phys. Rev. Lett. 115, 196402 (2015).
- C. Sánchez Muñoz, G. Frascella, and F. Schlawin, Quantum metrology of two-photon absorption, Phys. Rev. Res. 3, 033250 (2021).
- A. Castro, H. Appel, and A. Rubio, Optimal control theory for quantum electrodynamics: An initial state problem, Eur. Phys. J. B 92, 223 (2019).
- F. Lindel, E. G. Carnio, S. Y. Buhmann, and A. Buchleitner, Quantized fields for optimal control in the strong coupling regime, Phys. Rev. Lett. 130, 133601 (2023).
- A. Gorlach, M. E. Tzur, M. Birk, M. Krüger, N. Rivera, O. Cohen, and I. Kaminer, High-harmonic generation driven by quantum light, Nat. Phys. 19, 1689 (2023).
- M. Even Tzur, M. Birk, A. Gorlach, M. Krüger, I. Kaminer, and O. Cohen, Photon-statistics force in ultrafast electron dynamics, Nat. Photonics 17, 501 (2023).
- E. G. Carnio, A. Buchleitner, and F. Schlawin, How to optimize the absorption of two entangled photons, SciPost Phys. Core 4, 028 (2021).
- G. S. Agarwal and S. Dutta Gupta, Dynamical interaction of an atomic oscillator with squeezed radiation inside a cavity, Phys. Rev. A 39, 2961 (1989).
- J. Ducuing and N. Bloembergen, Statistical fluctuations in nonlinear optical processes, Phys. Rev. 133, A1493 (1964).
- C. Lecompte, G. Mainfray, C. Manus, and F. Sanchez, Laser temporal-coherence effects on multiphoton ionization processes, Phys. Rev. A 11, 1009 (1975).
- E. Zubizarreta Casalengua, J. López Carreño, E. del Valle, and F. Laussy, Structure of the harmonic oscillator in the space of -particle Glauber correlators, J. Math. Phys. 58, 062109 (2017).
- R. Loudon, The Quantum Theory of Light (Oxford University Press, New York, 2000).
- Strictly speaking, the coherent state does not belong to the Hilbert space with maximally photons, since the upper tail of its photon-number distribution will extend beyond . The state (12) is therefore not the optimal state found by optimizing over the finite-dimensional Hilbert space .
- J. Janszky and Y. Yushin, Many-photon processes with the participation of squeezed light, Phys. Rev. A 36, 1288 (1987).