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arXiv:2607.20333

Collective Electronic Entanglement via Infrared Cavity-Induced Vibronic Transduction

Vivek Yadav, Bar Cohn, Shmuel Sufrin, Uri Peskin, Lev Chuntonov

quant-phphysics.chem-phSubmitted Jul 22, 2026• Announced Jul 23, 2026
arXivHTMLPDF

Abstract

Polaritonic architectures seek to engineer molecular properties by hybridizing localized degrees of freedom with delocalized optical cavity fields. However, scaling laws impose a severe bottleneck on N-molecule collective strong coupling: because each molecule contributes only a fractional share to the collective state, localized responses undergo O(1/N) ensemble dilution. We demonstrate a violation of this scaling using fluorescence-encoded infrared spectroscopy of molecular ensembles under vibrational strong coupling, where macroscopically synchronized electronic responses scale as O(1). This scale-invariance reveals a regime of vibronic quantum transduction, where non-local vibrational entanglement is translated into collective electronic entanglement. By demonstrating the generation of macroscopically entangled electronic states from vibro-polaritons without an O(1/N) penalty, these results provide a scalable framework for room-temperature quantum technologies and coherent steering of non-adiabatic chemical pathways.

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Polaritonic architectures seek to engineer molecular properties by hybridizing localized degrees of freedom with delocalized optical cavity fields. However, scaling laws impose a severe bottleneck on N-molecule collective strong coupling: because each molecule contributes only a fractional share to the collective state, localized responses undergo O(1/N) ensemble dilution. We demonstrate a violation of this scaling using fluorescence-encoded infrared spectroscopy of molecular ensembles under vibrational strong coupling, where macroscopically synchronized electronic responses scale as O(1). This scale-invariance reveals a regime of vibronic quantum transduction, where non-local vibrational entanglement is translated into collective electronic entanglement. By demonstrating the generation of macroscopically entangled electronic states from vibro-polaritons without an O(1/N) penalty, these results provide a scalable framework for room-temperature quantum technologies and coherent steering of non-adiabatic chemical pathways.
Strong coupling between molecular excitations and quantized electromagnetic fields in optical cavities provides a powerful means to control the physical and chemical properties of molecular systems. Here, we study electron transfer (ET) dynamics in cavity-coupled molecules using the numerically exact hierarchical equations of motion (HEOM) method, which captures nonperturbative and non-Markovian effects beyond standard perturbative theories. We identify distinct resonance and collective effects associated with polariton formation and show that the ET rate saturates in the strong-coupling regime, a feature not captured by perturbative approaches. We further extend the cavity-modified ET model by incorporating the nuclear-coordinate dependence of molecular electric dipole moments, which gives rise to a three-body interaction involving molecular electronic and vibrational degrees of freedom and cavity photons. This vibronic polariton formation leads to non-monotonic, oscillatory dependencies of the ET rate on the light-matter coupling strength and cavity frequency, which we attribute to quantum interference among multiple transfer pathways. These findings establish cavity-modified electron transfer as a multichannel quantum process governed by the interplay of electronic, vibrational, and photonic degrees of freedom.
The demonstration of strong and ultrastrong coupling regimes of cavity QED with polyatomic molecules has opened new routes to control chemical dynamics at the nanoscale. We show that strong resonant coupling of a cavity field with an electronic transition can effectively decouple collective electronic and nuclear degrees of freedom in a disordered molecular ensemble, even for molecules with high-frequency quantum vibrational modes having strong electron-vibration interactions. This type of polaron decoupling can be used to control chemical reactions. We show that the rate of electron transfer reactions in a cavity can be orders of magnitude larger than in free space for a wide class of organic molecular species.
We theoretically investigate a single fluorescent molecule as a hybrid quantum optical device, in which multiple external laser sources exert control of the vibronic states. In the high-saturation regime, a coherent interaction is established between the vibrational and electronic degrees of freedom, and molecules can simulate several cavity QED models, whereby a specific vibrational mode plays the role of the cavity mode. Focusing on the specific example where the system is turned into an analogue simulator of the quantum Rabi model, the steady state exhibits vibrational bi-modality resulting in a statistical mixture of highly non-classical vibronic cat states. Applying our paradigm to molecules with prominent spatial asymmetry and combining an optical excitation with a THz(IR) driving, the system can be turned into a single photon transducer. Two possible implementations are discussed based on the coupling to a subwavelength THz patch antenna or a resonant metamaterial. In a nutshell, this work assesses the role of molecules as an optomechanical quantum toolbox for creating hybrid entangled states of electrons, photons, and vibrations, hence enabling frequency conversion over very different energy scales.
We study the polaritonic states and dynamics of multiple Jahn-Teller (JT) active molecules coupled to the modes of a Fabry-Perot cavity. We find that collective effects dramatically alter the interplay of electronic, vibrational and cavity angular momenta, giving rise to markedly different polaritonic spectra and dynamics even when going from one to two JT molecules. Starting from the ground vibronic state, we find that JT molecules collectively coupled to a common cavity can access a cascade of high-angular-momentum vibronic states in the presence of a single cavity photon, in sharp contrast to the single molecule case where the range of accessible vibronic angular momentum values are bounded. The observable consequences are a broadening of the cavity-molecular polariton spectrum and a suppression of photon polarization dynamics under broadband excitation of the system. Our results uncover new pathways for vibronic angular momentum transfer unique to collective molecular polaritonics with potential implications for cavity-assisted photo-physics and photo-chemistry.
We theoretically investigate a single fluorescent molecule as a hybrid quantum optical device, in which multiple external laser sources exert control of the vibronic states. In the high-saturation regime, a coherent interaction is established between the vibrational and electronic degrees of freedom, and molecules can simulate several cavity QED models, whereby a specific vibrational mode plays the role of the cavity mode. Focusing on the specific example where the system is turned into an analogue simulator of the quantum Rabi model, the steady state exhibits vibrational bi-modality resulting in a statistical mixture of highly non-classical vibronic cat states. Applying our paradigm to molecules with prominent spatial asymmetry and combining an optical excitation with a THz(IR) driving, the system can be turned into a single photon transducer. Two possible implementations are discussed based on the coupling to a subwavelength THz patch antenna or a resonant metamaterial. In a nutshell, this work assesses the role of molecules as an optomechanical quantum toolbox for creating hybrid entangled states of electrons, photons, and vibrations, hence enabling frequency conversion over very different energy scales.
Abstract We theoretically investigate a single fluorescent molecule as a hybrid quantum optical device, in which multiple external laser sources exert control of the vibronic states. In the high-saturation regime, a coherent interaction is established between the vibrational and electronic degrees of freedom, and molecules can simulate several cavity QED models, whereby a specific vibrational mode plays the role of the cavity mode. Focusing on the specific example where the system is turned into an analogue simulator of the quantum Rabi model, the steady state exhibits vibrational bi-modality resulting in a statistical mixture of highly non-classical vibronic cat states. Applying our paradigm to molecules with prominent spatial asymmetry and combining an optical excitation with a THz(IR) driving, the system can be turned into a single photon transducer. Two possible implementations are discussed based on the coupling to a subwavelength THz patch antenna or a resonant metamaterial. In a nutshell, this work assesses the role of molecules as an optomechanical quantum toolbox for creating hybrid entangled states of electrons, photons, and vibrations, hence enabling frequency conversion over very different energy scales.