- Open Access
Energy transfer between localized emitters in photonic cavities from first principles
Phys. Rev. Research 7, 033229 – Published 9 September, 2025
DOI: https://doi.org/10.1103/8h8j-b79r
Abstract
Radiative and nonradiative resonant couplings between defects are ubiquitous phenomena in photonic devices used in classical and quantum information technology applications. In this work, we present a first-principles approach to enable quantitative predictions of the energy transfer between defects in photonic cavities, beyond the dipole-dipole approximation and including the many-body nature of the electronic states. As an example, we discuss the energy transfer from a dipolelike emitter to an center in MgO in a spherical cavity. We show that the cavity can be used to controllably enhance or suppress specific spin-flip and spin-conserving transitions. Specifically, we predict that an ∼10–100 enhancement in the resonant energy transfer rate can be gained in the case of the center in MgO at ∼10 nm distances from a dipolar source, using rather moderate cavity with quality factor ∼ 400. We also show that a similar suppression in the transfer rate can be achieved by off-tuning the cavity resonance relative to the emitter transition energy. The framework presented here is general and readily applicable to a wide range of devices where localized emitters are embedded in microspheres, core-shell nanoparticles, and dielectric Mie resonators. Hence, our approach paves the way to predict how to control energy transfer in quantum memories and in ultrahigh-density optical memories, and in a variety of quantum information platforms.
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References (81)
- Th. Forster, Zwischenmolekulare Energiewanderung und Fluoreszenz, Ann. Phys. 437, 55 (1948).
- D. L. Dexter, A theory of sensitized luminescence in solids, J. Chem. Phys. 21, 836 (1953).
- D. L. Dexter and J. H. Schulman, Theory of concentration quenching in inorganic phosphors, J. Chem. Phys. 22, 1063 (1954).
- A. Salam, The unified theory of resonance energy transfer according to molecular quantum electrodynamics, Atoms 6, 56 (2018).
- G. A. Jones and D. S. Bradshaw, Resonance energy transfer: From fundamental theory to recent applications, Front. Phys. 7, 100 (2019).
- S. Chattaraj, S. Guha, and G. Galli, First-principles investigation of near-field energy transfer between localized quantum emitters in solids, Phys. Rev. Res. 6, 033170 (2024).
- D. Awschalom et al., Development of quantum interconnects (QuICs) for next-generation information technologies, PRX Quantum 2, 017002 (2021).
- G. Wolfowicz, F. J. Heremans, C. P. Anderson, S. Kanai, H. Seo, A. Gali, G. Galli, and D. D. Awschalom, Quantum guidelines for solid-state spin defects, Nat. Rev. Mater. 6, 906 (2021).
- M. Pompili et al., Realization of a multinode quantum network of remote solid-state qubits, Science 372, 259 (2021).
- K. Azuma, S. E. Economou, D. Elkouss, P. Hilaire, L. Jiang, H.-K. Lo, and I. Tzitrin, Quantum repeaters: From quantum networks to the quantum internet, Rev. Mod. Phys. 95, 045006 (2023).
- V. M. Kenkre and R. S. Knox, Generalized-master-equation theory of excitation transfer, Phys. Rev. B 9, 5279 (1974).
- G. D. Grant et al., Optical and microstructural characterization of doped epitaxial cerium oxide on silicon, APL Mater. 12, 021121 (2024).
- E. A. Power and T. Thirunamachandran, Quantum electrodynamics with nonrelativistic sources. III. Intermolecular interactions, Phys. Rev. A 28, 2671 (1983).
- D. L. Andrews, A unified theory of radiative and radiationless molecular energy transfer, Chem. Phys. 135, 195 (1989).
- G. J. Daniels, R. D. Jenkins, D. S. Bradshaw, and D. L. Andrews, Resonance energy transfer: The unified theory revisited, J. Chem. Phys. 119, 2264 (2003).
- L.-Y. Hsu, W. Ding, and G. C. Schatz, Plasmon-coupled resonance energy transfer, J. Phys. Chem. Lett. 8, 2357 (2017).
- W. Ding, L.-Y. Hsu, and G. C. Schatz, Plasmon-coupled resonance energy transfer: A real-time electrodynamics approach, J. Chem. Phys. 146, 064109 (2017).
- M.-W. Lee and L.-Y. Hsu, Polariton-assisted resonance energy transfer beyond resonant dipole-dipole interaction: A transition-current-density approach, Phys. Rev. A 107, 053709 (2023).
- P. Lodahl, S. Mahmoodian, and S. Stobbe, Interfacing single photons and single quantum dots with photonic nanostructures, Rev. Mod. Phys. 87, 347 (2015).
- J. Lee, V. Leong, D. Kalashnikov, J. Dai, A. Gandhi, and L. A. Krivitsky, Integrated single photon emitters, AVS Quantum Sci. 2, 031701 (2020).
- C. Ji et al., Nanocavity-mediated Purcell enhancement of Er in thin films grown via atomic layer deposition, ACS Nano 18, 9929 (2024).
- S. Chakravarthi, N. S. Yama, A. Abulnaga, D. Huang, C. Pederson, K. Hestroffer, F. Hatami, N. P. De Leon, and K.-M. C. Fu, Hybrid integration of GaP photonic crystal cavities with silicon-vacancy centers in diamond by stamp-transfer, Nano Lett. 23, 3708 (2023).
- G. Ya. Slepyan, S. Vlasenko, and D. Mogilevtsev, Quantum antennas, Adv. Quantum Technol. 3, 1900120 (2020).
- P. Bharadwaj, B. Deutsch, and L. Novotny, Optical antennas, Adv. Opt. Photonics 1, 438 (2009).
- S. Chattaraj, J. Zhang, S. Lu, and A. Madhukar, On-chip integrated single photon source-optically resonant metastructure based scalable quantum optical circuits, IEEE J. Quantum Electron. 56, 9300109 (2019).
- M. Petruzzella, S. Birindelli, F. M. Pagliano, D. Pellegrino, Ž. Zobenica, L. H. Li, E. H. Linfield, and A. Fiore, Quantum photonic integrated circuits based on tunable dots and tunable cavities, APL Photonics 3, 106103 (2018).
- J.-H. Kim, S. Aghaeimeibodi, C. J. K. Richardson, R. P. Leavitt, and E. Waks, Super-radiant emission from quantum dots in a nanophotonic waveguide, Nano Lett. 18, 4734 (2018).
- A. D. Logan, N. S. Yama, and K.-M. C. Fu, Selective active resonance tuning for multi-mode nonlinear photonic cavities, Opt. Express 32, 13396 (2024).
- A. Majumdar, A. Rundquist, M. Bajcsy, V. D. Dasika, S. R. Bank, and J. Vučković, Design and analysis of photonic crystal coupled cavity arrays for quantum simulation, Phys. Rev. B 86, 195312 (2012).
- D. M. Lukin, M. A. Guidry, J. Yang, M. Ghezellou, S. Deb Mishra, H. Abe, T. Ohshima, J. Ul-Hassan, and J. Vučković, Two-emitter multimode cavity quantum electrodynamics in thin-film silicon carbide photonics, Phys. Rev. X 13, 011005 (2023).
- C. Carlson, D. Dalacu, C. Gustin, S. Haffouz, X. Wu, J. Lapointe, R. L. Williams, P. J. Poole, and S. Hughes, Theory and experiments of coherent photon coupling in semiconductor nanowire waveguides with quantum dot molecules, Phys. Rev. B 99, 085311 (2019).
- K. N. Avanaki and G. C. Schatz, Entangled photon resonance energy transfer in arbitrary media, J. Phys. Chem. Lett. 10, 3181 (2019).
- Y.-C. Wei, M.-W. Lee, P.-T. Chou, G. D. Scholes, G. C. Schatz, and L.-Y. Hsu, Can nanocavities significantly enhance resonance energy transfer in a single donor–acceptor pair? J. Phys. Chem. C 125, 18119 (2021).
- T. Mohamadian, J. Negro, L. M. Nieto, and H. Panahi, Tavis-Cummings models and their quasi-exactly solvable Schrödinger Hamiltonians, Eur. Phys. J. Plus 134, 363 (2019).
- J. Flick, C. Schäfer, M. Ruggenthaler, H. Appel, and A. Rubio, Ab initio optimized effective potentials for real molecules in optical cavities: Photon contributions to the molecular ground state, ACS Photonics 5, 992 (2018).
- M. K. Svendsen, Y. Kurman, P. Schmidt, F. Koppens, I. Kaminer, and K. S. Thygesen, Combining density functional theory with macroscopic QED for quantum light-matter interactions in 2D materials, Nat. Commun. 12, 2778 (2021).
- M. Ruggenthaler, J. Flick, C. Pellegrini, H. Appel, I. V. Tokatly, and A. Rubio, Quantum-electrodynamical density-functional theory: Bridging quantum optics and electronic-structure theory, Phys. Rev. A 90, 012508 (2014).
- J. Flick, N. Rivera, and P. Narang, Strong light-matter coupling in quantum chemistry and quantum photonics, Nanophotonics 7, 1479 (2018).
- T. W. Ebbesen, A. Rubio, and G. D. Scholes, Introduction: Polaritonic chemistry, Chem. Rev. 123, 12037 (2023).
- F. P. Bonafé, E. I. Albar, S. T. Ohlmann, V. P. Kosheleva, C. M. Bustamante, F. Troisi, A. Rubio, and H. Appel, Full minimal coupling Maxwell-TDDFT: An ab initio framework for light-matter phenomena beyond the dipole approximation, Phys. Rev. B 111, 085114 (2025).
- D. L. Andrews and D. S. Bradshaw, The role of virtual photons in nanoscale photonics: The role of virtual photons in nanoscale photonics, Ann. Phys. (Berlin) 526, 173 (2014).
- L.-Y. Hsu, Chemistry meets plasmon polaritons and cavity photons: A perspective from macroscopic quantum electrodynamics, J. Phys. Chem. Lett. 16, 1604 (2025).
- Y.-T. Chuang, M.-W. Lee, and L.-Y. Hsu, Tavis-Cummings model revisited: A perspective from macroscopic quantum electrodynamics, Front. Phys. 10, 980167 (2022).
- N. Westerberg and R. Bennett, Perturbative light–matter interactions; from first principles to inverse design, Phys. Rep. 1026, 1 (2023).
- T. Hümmer, F. J. García-Vidal, L. Martín-Moreno, and D. Zueco, Weak and strong coupling regimes in plasmonic QED, Phys. Rev. B 87, 115419 (2013).
- B. Yuen and A. Demetriadou, Exact quantum electrodynamics of radiative photonic environments, Phys. Rev. Lett. 133, 203604 (2024).
- P. Tighineanu, The mesoscopic nature of quantum dots in photon emission, in Quantum Dots for Quantum Information Technologies, Nano-Optics and Nanophotonics, edited by P. Michler (Springer International Publishing, Cham, 2017), Chap. 5, pp. 165–198.
- J. Feist, A. I. Fernández-Domínguez, and F. J. García-Vidal, Macroscopic QED for quantum nanophotonics: Emitter-centered modes as a minimal basis for multiemitter problems, Nanophotonics 10, 477 (2020).
- W. Kohn and L. J. Sham, Self-consistent equations including exchange and correlation effects, Phys. Rev. 140, A1133 (1965).
- P. Hohenberg and W. Kohn, Inhomogeneous electron gas, Phys. Rev. 136, B864 (1964).
- P. Giannozzi et al., QUANTUM ESPRESSO: A modular and open-source software project for quantum simulations of materials, J. Phys.: Condens. Matter 21, 395502 (2009).
- H. Ma, N. Sheng, M. Govoni, and G. Galli, Quantum embedding theory for strongly correlated states in materials, J. Chem. Theory Comput. 17, 2116 (2021).
- N. Sheng, C. Vorwerk, M. Govoni, and G. Galli, Green’s function formulation of quantum defect embedding theory, J. Chem. Theory Comput. 18, 3512 (2022).
- C. Vorwerk and G. Galli, Disentangling photoexcitation and photoluminescence processes in defective MgO, Phys. Rev. Mater. 7, 033801 (2023).
- S. Verma, A. Mitra, Y. Jin, S. Haldar, C. Vorwerk, M. R. Hermes, G. Galli, and L. Gagliardi, Optical properties of neutral centers in bulk MgO with density matrix embedding, J. Phys. Chem. Lett. 14, 7703 (2023).
- Y. Jin, V. W. Yu, M. Govoni, A. C. Xu, and G. Galli, Excited state properties of point defects in semiconductors and insulators investigated with time-dependent density functional theory, J. Chem. Theory Comput. 19, 8689 (2023).
- R. R. Chance, A. Prock, and R. Silbey, Molecular fluorescence and energy transfer near interfaces, in Advances in Chemical Physics, edited by I. Prigogine and S. A. Rice (Wiley, 1978), Vol. 37, 1st ed., pp. 1–65.
- B. P. Krueger, G. D. Scholes, and G. R. Fleming, Calculation of couplings and energy-transfer pathways between the pigments of LH2 by the ab initio transition density cube method, J. Phys. Chem. B 102, 5378 (1998).
- E. A. Power and T. Thirunamachandran, On the nature of the Hamiltonian for the interaction of radiation with atoms and molecules: (/mc)p⋅A, −µ⋅E, and all that, Am. J. Phys. 46, 370 (1978).
- M. Wubs, L. G. Suttorp, and A. Lagendijk, Multiple-scattering approach to interatomic interactions and superradiance in inhomogeneous dielectrics, Phys. Rev. A 70, 053823 (2004).
- K. Rustomji, M. Dubois, P. Jomin, S. Enoch, J. Wenger, C. M. De Sterke, and R. Abdeddaim, Complete electromagnetic dyadic Green function characterization in a complex environment—resonant dipole-dipole interaction and cooperative effects, Phys. Rev. X 11, 021004 (2021).
- F.-F. Kong, X.-J. Tian, Y. Zhang, Y. Zhang, G. Chen, Y.-J. Yu, S.-H. Jing, H.-Y. Gao, Y. Luo, J.-L. Yang, Z.-C. Dong, and J. G. Hou, Wavelike electronic energy transfer in donor–acceptor molecular systems through quantum coherence, Nat. Nanotechnol. 17, 729 (2022).
- A. Shukla, G. Kaur, K. J. Babu, A. Kaur, D. K. Yadav, and H. N. Ghosh, Defect-interceded cascading energy transfer and underlying charge transfer in europium-doped nanocrystals, J. Phys. Chem. Lett. 13, 83 (2022).
- A. Gibson, R. Haydock, and J. P. LaFemina, Stability of vacancy defects in MgO: The role of charge neutrality, Phys. Rev. B 50, 2582 (1994).
- G. P. Summers, T. M. Wilson, B. T. Jeffries, H. T. Tohver, Y. Chen, and M. M. Abraham, Luminescence from oxygen vacancies in MgO crystals thermochemically reduced at high temperatures, Phys. Rev. B 27, 1283 (1983).
- L. A. Kappers, R. L. Kroes, and E. B. Hensley, and F′ centers in magnesium oxide, Phys. Rev. B 1, 4151 (1970).
- P. Rinke, A. Schleife, E. Kioupakis, A. Janotti, C. Rödl, F. Bechstedt, M. Scheffler, and C. G. Van de Walle, First-principles optical spectra for F centers in MgO, Phys. Rev. Lett. 108, 126404 (2012).
- S. Sahoo, V. A. Davydov, V. N. Agafonov, and S. I. Bogdanov, Hybrid quantum nanophotonic devices with color centers in nanodiamonds [Invited], Opt. Mater. Express 13, 191 (2023).
- S. Kruk and Y. Kivshar, Functional meta-optics and nanophotonics governed by Mie resonances, ACS Photonics 4, 2638 (2017).
- V. Rutckaia, F. Heyroth, A. Novikov, M. Shaleev, M. Petrov, and J. Schilling, Quantum dot emission driven by Mie resonances in silicon nanostructures, Nano Lett. 17, 6886 (2017).
- E. E. Maslova, M. F. Limonov, and M. V. Rybin, Transition between a photonic crystal and a metamaterial with electric response in dielectric structures, JETP Lett. 109, 340 (2019).
- A. F. Koenderink, Single-photon nanoantennas, ACS Photonics 4, 710 (2017).
- S. Chattaraj and A. Madhukar, Multifunctional all-dielectric nano-optical systems using collective multipole Mie resonances: Toward on-chip integrated nanophotonics, J. Opt. Soc. Am. B 33, 2414 (2016).
- Spectroscopic Properties of Rare Earths in Optical Materials, Springer Series in Materials Science, edited by G. Liu and B. Jacquier (Springer, Berlin, 2005).
- P. Stevenson, C. M. Phenicie, I. Gray, S. P. Horvath, S. Welinski, A. M. Ferrenti, A. Ferrier, P. Goldner, S. Das, R. Ramesh, R. J. Cava, N. P. de Leon, and J. D. Thompson, Erbium-implanted materials for quantum communication applications, Phys. Rev. B 105, 224106 (2022).
- M. Govoni, M. Munakami, A. Tanikanti, J. H. Skone, H. B. Runesha, F. Giberti, J. De Pablo, and G. Galli, Qresp, a tool for curating, discovering and exploring reproducible scientific papers, Sci. Data 6, 190002 (2019).
- C. Butler and J. Van Bladel, Electromagnetic fields in a spherical cavity embedded in a dissipative medium, IEEE Trans. Antennas Propag. 12, 110 (1964).
- M. Schlipf and F. Gygi, Optimization algorithm for the generation of ONCV pseudopotentials, Comput. Phys. Commun. 196, 36 (2015).
- J. P. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77, 3865 (1996).
- J. H. Skone, M. Govoni, and G. Galli, Self-consistent hybrid functional for condensed systems, Phys. Rev. B 89, 195112 (2014).
- H. Somayaji, S. Wang, L.-Y. Hsu, and G. D. Scholes, Remarkable orientation dependence of plasmon-coupled resonance energy transfer, J. Phys. Chem. C 129, 4506 (2025).