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Extending the Self-Discharge Time of Dicke Quantum Batteries Using Molecular Triplets

Daniel J. Tibben1, Enrico Della Gaspera1, Joel van Embden1, Philipp Reineck1, James Q. Quach2, Francesco Campaioli1,3,4,*, and Daniel E. Gómez1,†

  • *Contact author: francesco.campaioli@unipd.it
  • †Contact author: daniel.gomez@rmit.edu.au
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PRX Energy 4, 023012 – Published 23 June, 2025

DOI: https://doi.org/10.1103/bhyh-53np

Abstract

Quantum batteries, quantum systems for energy storage, have gained interest due to their potential scalable charging power density. A quantum battery proposal based on the Dicke model has been explored using organic microcavities, which enable a cavity-enhanced energy-transfer process called superabsorption. However, energy-storage lifetime in these devices is limited by fast radiative emission losses, worsened by superradiance. Here, we demonstrate a promising approach to extend the energy-storage lifetime of Dicke quantum batteries using molecular triplet states. We examine a type of multilayer microcavity where an active absorption layer transfers energy to the molecular triplets of a storage layer, identifying two regimes based on exciton-polariton resonances. We tested one of these mechanisms by fabricating and characterizing five devices across a triplet-polariton resonance, showing that triplet population is maximized when the lower polariton and triplet state are isoenergetic. We found that one of these devices can store energy for 40.3 ± 0.4 μs, a 103-fold increase in storage time compared to previous demonstrations. We conclude by discussing potential optimization outlooks for this class of devices.

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Quantum batteries may offer scalable charging power density. Those based on the Dicke model enable a cavity-enhanced energy transfer process called superabsorption, but the lifetime is limited by fast radiative emission losses and super radiance. Here, the authors show a promising approach to extend the energy storage lifetime using molecular triplet states, which they test on five devices across a triplet-polariton resonance. One device shows a 1000-fold increase in storage time compared to previous demonstrations.

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References (75)

  1. D. Larcher and J.-M. Tarascon, Towards greener and more sustainable batteries for electrical energy storage, Nat. Chem. 7, 19 (2015).
  2. M. Armand and J. M. Tarascon, Building better batteries, Nature 451, 652 (2008).
  3. Y. Ye, et al., Quadruple the rate capability of high-energy batteries through a porous current collector design, Nat. Energy 9, 643 (2024).
  4. M. N. Leuenberger and D. Loss, Quantum computing in molecular magnets, Nature 410, 789 (2001).
  5. F. Campaioli, S. Gherardini, J. Q. Quach, M. Polini, and G. M. Andolina, Colloquium: Quantum batteries, Rev. Mod. Phys. 96, 031001 (2024).
  6. F. C. Binder, S. Vinjanampathy, K. Modi, and J. Goold, Quantacell: Powerful charging of quantum batteries, New J. Phys. 17, 075015 (2015).
  7. F. Campaioli, F. A. Pollock, F. C. Binder, L. Céleri, J. Goold, S. Vinjanampathy, and K. Modi, Enhancing the charging power of quantum batteries, Phys. Rev. Lett. 118, 150601 (2017).
  8. C.-K. Hu, J. Qiu, P. J. P. Souza, J. Yuan, Y. Zhou, L. Zhang, J. Chu, X. Pan, L. Hu, J. Li, Y. Xu, Y. Zhong, S. Liu, F. Yan, D. Tan, R. Bachelard, C. J. Villas-Boas, A. C. Santos, and D. Yu, Optimal charging of a superconducting quantum battery, Quantum Sci. Technol. 7, 045018 (2022).
  9. G. M. Andolina, M. Keck, A. Mari, V. Giovannetti, and M. Polini, Quantum versus classical many-body batteries, Phys. Rev. B 99, 1 (2019).
  10. S. Julià-Farré, T. Salamon, A. Riera, M. N. Bera, and M. Lewenstein, Bounds on the capacity and power of quantum batteries, Phys. Rev. Res. 2, 023113 (2020).
  11. D. Ferraro, M. Campisi, G. M. Andolina, V. Pellegrini, and M. Polini, High-power collective charging of a solid-state quantum battery, Phys. Rev. Lett. 120, 117702 (2018).
  12. S. Haroche, Nobel lecture: Controlling photons in a box and exploring the quantum to classical boundary, Rev. Mod. Phys. 85, 1083 (2013).
  13. K. Cong, Q. Zhang, Y. Wang, G. T. Noe, A. Belyanin, and J. Kono, Dicke superradiance in solids, JOSA B 33, C80 (2016).
  14. L. Fusco, M. Paternostro, and G. De Chiara, Work extraction and energy storage in the Dicke model, Phys. Rev. E 94, 052122 (2016).
  15. K. Higgins, S. Benjamin, T. Stace, G. Milburn, B. W. Lovett, and E. Gauger, Superabsorption of light via quantum engineering, Nat. Commun. 5, 4705 (2014).
  16. P. A. Erdman, G. M. Andolina, V. Giovannetti, and F. Noé, Reinforcement learning optimization of the charging of a Dicke quantum battery, Phys. Rev. Lett. 133, 243602 (2024).
  17. A. Crescente, M. Carrega, M. Sassetti, and D. Ferraro, Ultrafast charging in a two-photon Dicke quantum battery, Phys. Rev. B 102, 1 (2020).
  18. F.-Q. Dou, Y.-Q. Lu, Y.-J. Wang, and J.-A. Sun, Extended Dicke quantum battery with interatomic interactions and driving field, Phys. Rev. B 105, 115405 (2022).
  19. G. Gemme, G. M. Andolina, F. M. D. Pellegrino, M. Sassetti, and D. Ferraro, Off-resonant Dicke quantum battery: Charging by virtual photons, Batteries 9, 197 (2023).
  20. J. Q. Quach, K. E. McGhee, L. Ganzer, D. M. Rouse, B. W. Lovett, E. M. Gauger, J. Keeling, G. Cerullo, D. G. Lidzey, and T. Virgili, Superabsorption in an organic microcavity: Toward a quantum battery, Sci. Adv. 8, eabk3160 (2022).
  21. X.-W. Chen, V. Sandoghdar, and M. Agio, Coherent interaction of light with a metallic structure coupled to a single quantum emitter: From superabsorption to cloaking, Phys. Rev. Lett. 110, 153605 (2013).
  22. R. W. Crisp, J. N. Schrauben, M. C. Beard, J. M. Luther, and J. C. Johnson, Coherent exciton delocalization in strongly coupled quantum dot arrays, Nano Lett. 13, 4862 (2013).
  23. A. A. Svidzinsky, L. Yuan, and M. O. Scully, Quantum amplification by superradiant emission of radiation, Phys. Rev. X 3, 041001 (2013).
  24. S. Aberra Guebrou, C. Symonds, E. Homeyer, J. C. Plenet, Y. N. Gartstein, V. M. Agranovich, and J. Bellessa, Coherent emission from a disordered organic semiconductor induced by strong coupling with surface plasmons, Phys. Rev. Lett. 108, 066401 (2012).
  25. B. M. Garraway, The Dicke model in quantum optics: Dicke model revisited, Philos. Trans. R. Soc. A: Math. Phys. Eng. Sci. 369, 1137 (2011).
  26. S. Prasad and R. J. Glauber, Coherent radiation by a spherical medium of resonant atoms, Phys. Rev. A 82, 063805 (2010).
  27. V. V. Temnov and U. Woggon, Superradiance and subradiance in an inhomogeneously broadened ensemble of two-level systems coupled to a low-q cavity, Phys. Rev. Lett. 95, 243602 (2005).
  28. S. Prasad and R. J. Glauber, Polarium model: Coherent radiation by a resonant medium, Phys. Rev. A 61, 063814 (2000).
  29. M. Gross and S. Haroche, Superradiance: An essay on the theory of collective spontaneous emission, Phys. Rep. 93, 301 (1982).
  30. R. H. Dicke, Coherence in spontaneous radiation processes, Phys. Rev. 93, 99 (1954).
  31. M. J. Tayebjee, S. N. Sanders, E. Kumarasamy, L. M. Campos, M. Y. Sfeir, and D. R. McCamey, Quintet multiexciton dynamics in singlet fission, Nat. Phys. 13, 182 (2017).
  32. M. I. Collins, F. Campaioli, M. J. Tayebjee, J. H. Cole, and D. R. McCamey, Quintet formation, exchange fluctuations, and the role of stochastic resonance in singlet fission, Commun. Phys. 6, 64 (2023).
  33. S. Davidson, A. Fruchtman, F. A. Pollock, and E. M. Gauger, The dark side of energy transport along excitonic wires: On-site energy barriers facilitate efficient, vibrationally mediated transport through optically dark subspaces, J. Chem. Phys. 153, 134701 (2020).
  34. S. Davidson, F. A. Pollock, and E. Gauger, Eliminating radiative losses in long-range exciton transport, PRX Quantum 3, 020354 (2022).
  35. J. Liu, D. Segal, and G. Hanna, Loss-free excitonic quantum battery, J. Phys. Chem. C 123, 18303 (2019).
  36. J. Q. Quach and W. J. Munro, Using dark states to charge and stabilize open quantum batteries, Phys. Rev. Appl. 14, 1 (2020).
  37. N. J. Hestand and F. C. Spano, Expanded theory of H- and J-molecular aggregates: The effects of vibronic coupling and intermolecular charge transfer, Chem. Rev. 118, 7069 (2018).
  38. S. R. Yost, E. Hontz, S. Yeganeh, and T. Van Voorhis, Triplet vs singlet energy transfer in organic semiconductors: The tortoise and the hare, J. Phys. Chem. C 116, 17369 (2012).
  39. Y.-C. Liang, S.-S. Gou, K.-K. Liu, W.-J. Wu, C.-Z. Guo, S.-Y. Lu, J.-H. Zang, X.-Y. Wu, Q. Lou, L. Dong, et al., Ultralong and efficient phosphorescence from silica confined carbon nanodots in aqueous solution, Nano Today 34, 100900 (2020).
  40. X. Zhong, T. Chervy, L. Zhang, A. Thomas, J. George, C. Genet, J. A. Hutchison, and T. W. Ebbesen, Energy transfer between spatially separated entangled molecules, Angew. Chem. Int. Ed. 56, 9034 (2017).
  41. In the Dicke model, each donor and acceptor molecule in the ensembles is treated as an individual system.
  42. D. Farina, G. M. Andolina, A. Mari, M. Polini, and V. Giovannetti, Charger-mediated energy transfer for quantum batteries: An open-system approach, Phys. Rev. B 99, 1 (2019).
  43. N. Carlon Zambon, Chirality and nonlinear dynamics in polariton microresonators, Theses, Université Paris-Saclay, 2020. https://theses.hal.science/tel-03035028.
  44. D. J. Tibben, G. O. Bonin, I. Cho, G. Lakhwani, J. Hutchison, and D. E. Gómez, Molecular energy transfer under the strong light–matter interaction regime, Chem. Rev. 123, 8044 (2023).
  45. When the exciton-photon couplings are small enough compared to the other energy scales, i.e., JD,JA≪ωC(θ),ωD,ωA, we can apply the rotating wave approximation to eliminate the counter-rotating terms arising from the exciton-cavity couplings.
  46. This represents the energy gap between ground S0 and excited S1 singlet, also known as the HOMO-LUMO gap [72].
  47. See Supplemental Material at http://link.aps.org/supplemental/10.1103/bhyh-53np for details on the transition operators, and the constructions and solution of Eq. (2). The Supplemental Material also contains Refs. [44, 49, 50, 51, 73, 74].
  48. T. W. Ebbesen, Hybrid light–matter states in a molecular and material science perspective, Acc. Chem. Res. 49, 2403 (2016).
  49. J. P. Zobel, J. J. Nogueira, and L. González, Mechanism of ultrafast intersystem crossing in 2-nitronaphthalene, Chem. - Eur. J. 24, 5379 (2018).
  50. J. S. Zugazagoitia, C. X. Almora-Díaz, and J. Peon, Ultrafast intersystem crossing in 1-nitronaphthalene. an experimental and computational study, J. Phys. Chem. A 112, 358 (2008).
  51. T. Okada, I. Karaki, E. Matsuzawa, N. Mataga, Y. Sakata, and S. Misumi, Ultrafast intersystem crossing in some intramolecular heteroexcimers, J. Phys. Chem. 85, 3957 (1981).
  52. H. Sternlicht, G. Nieman, and G. Robinson, Triplet–triplet annihilation and delayed fluorescence in molecular aggregates, J. Chem. Phys. 38, 1326 (1963).
  53. P. Atkins and G. Evans, Magnetic field effects on chemiluminescent fluid solutions, Mol. Phys. 29, 921 (1975).
  54. R. Forecast, F. Campaioli, and J. H. Cole, Magnetic field effects in triplet–triplet annihilation upconversion: Revisiting atkins and evans’ theory, J. Chem. Theory Comput. 19, 7816 (2023).
  55. D. Dempster, T. Morrow, and M. Quinn, The photochemical characteristics of rhodamine 6g-ethanol solutions, J. Photochem. 2, 343 (1973).
  56. J. E. Rogers, K. A. Nguyen, D. C. Hufnagle, D. G. McLean, W. Su, K. M. Gossett, A. R. Burke, S. A. Vinogradov, R. Pachter, and P. A. Fleitz, Observation and interpretation of annulated porphyrins: Studies on the photophysical properties of meso-tetraphenylmetalloporphyrins, J. Phys. Chem. A 107, 11331 (2003).
  57. S. Wang, T. Chervy, J. George, J. A. Hutchison, C. Genet, and T. W. Ebbesen, Quantum yield of polariton emission from hybrid light-matter states, J. Phys. Chem. Lett. 5, 1433 (2014).
  58. A. E. Allahverdyan, R. Balian, and T. M. Nieuwenhuizen, Maximal work extraction from finite quantum systems, Europhys. Lett. 67, 565 (2004).
  59. M. Lostaglio, K. Korzekwa, D. Jennings, and T. Rudolph, Quantum coherence, time-translation symmetry, and thermodynamics, Phys. Rev. X 5, 021001 (2015).
  60. J. Goold, M. Huber, A. Riera, L. d. Rio, and P. Skrzypczyk, The role of quantum information in thermodynamics–a topical review, J. Phys. A: Math. Theor. 49, 143001 (2016).
  61. G. Francica, F. C. Binder, G. Guarnieri, M. T. Mitchison, J. Goold, and F. Plastina, Quantum coherence and ergotropy, Phys. Rev. Lett. 125, 180603 (2020).
  62. B. Çakmak, Ergotropy from coherences in an open quantum system, Phys. Rev. E 102, 042111 (2020).
  63. T. Biswas, M. Łobejko, P. Mazurek, K. Jałowiecki, and M. Horodecki, Extraction of ergotropy: free energy bound and application to open cycle engines, Quantum 6, 841 (2022).
  64. R. Castellano, D. Farina, V. Giovannetti, and A. Acin, Extended local ergotropy, Phys. Rev. Lett. 133, 150402 (2024).
  65. M. Alías-Rodríguez, C. de Graaf, and M. Huix-Rotllant, Ultrafast intersystem crossing in xanthone from wavepacket dynamics, J. Am. Chem. Soc. 143, 21474 (2021).
  66. Z. An, C. Zheng, Y. Tao, R. Chen, H. Shi, T. Chen, Z. Wang, H. Li, R. Deng, X. Liu, et al., Stabilizing triplet excited states for ultralong organic phosphorescence, Nat. Mater. 14, 685 (2015).
  67. J. Dutta, N. Yadav, P. Bhatt, K. Kaur, D. E. Gómez, and J. George, Enhanced energy transfer in cavity QED based phototransistors, J. Phys. Chem. Lett. 15, 8211 (2024).
  68. B. M. Maune, M. G. Borselli, B. Huang, T. D. Ladd, P. W. Deelman, K. S. Holabird, A. A. Kiselev, I. Alvarado-Rodriguez, R. S. Ross, A. E. Schmitz, et al., Coherent singlet-triplet oscillations in a silicon-based double quantum dot, Nature 481, 344 (2012).
  69. C. S. Adams, J. D. Pritchard, and J. P. Shaffer, Rydberg atom quantum technologies, J. Phys. B: At. Mol. Opt. Phys. 53, 012002 (2019).
  70. C. D. Bruzewicz, J. Chiaverini, R. McConnell, and J. M. Sage, Trapped-ion quantum computing: Progress and challenges, Appl. Phys. Rev. 6, 021314 (2019).
  71. A. Blais, A. L. Grimsmo, S. M. Girvin, and A. Wallraff, Circuit quantum electrodynamics, Rev. Mod. Phys. 93, 025005 (2021).
  72. S. S. Zade and M. Bendikov, From oligomers to polymer: Convergence in the HOMO-LUMO gaps of conjugated oligomers, Org. Lett. 8, 5243 (2006).
  73. L. V. Levshin, M. G. Reva, and B. D. Ryzhikov, Effect of intermolecular interactions on the electronic spectra of rhodamine 6G, J. Appl. Spectrosc. 26, 48 (1977).
  74. P. Bojarski, Concentration quenching and depolarization of rhodamine 6G in the presence of fluorescent dimers in polyvinyl alcohol films, Chem. Phys. Lett. 278, 225 (1997).
  75. https://github.com/danielgom3z/PRX_Energy_2025.

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PRX Energy 4, 023012– Published 23 June, 2025
  • Received 16 July 2024
  • Revised 29 November 2024
  • Accepted 23 May 2025
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