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arXiv:2601.20700 · The Journal of Chemical Physics

Entangled photon pair excitation and time-frequency filtered multidimensional photon correlation spectroscopy as a probe for dissipative exciton kinetics

Arunangshu Debnath, Shaul Mukamel

quant-phSubmitted Jan 28, 2026• Announced Jan 29, 2026• 0 citations• Revised Feb 7, 2026 (v3)
v1 · Jan 28, 2026v2 · Feb 5, 2026v3 · Feb 7, 2026v4 · Apr 23, 2026v5 · Jul 15, 2026v6 · Sep 10, 2026
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Abstract

In molecular aggregates, multiple delocalized exciton states interact with phonons, making the state-resolved spectroscopic monitoring of dynamics challenging. We propose a protocol that combines photon-entanglement-enhanced narrowband excitation of two-exciton states with time-frequency-filtered two-photon coincidence counting. This approach alleviates bottlenecks associated with probing exciton dynamics spread across multiple spectral and temporal windows. We demonstrate that non-classical correlations of entangled photon pairs can be used to prepare narrowband two-exciton population distributions, thereby circumventing transport in mediating one-exciton states. The evolution of these population distributions and cascading transitions can be monitored using time-frequency-filtered photon coincidence counting. Numerical simulations for a light-harvesting aggregate highlight the ability of this protocol to achieve selectivity by suppressing or amplifying specific pathways. Combining entangled photonic sources with multidimensional photon correlation spectroscopy allows promising applications in spectroscopy and sensing.

Comments
Submitted 14/04/2025 (under review). Updates: Corrected typos; Formatted equations

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In molecular aggregates, multiple delocalized exciton states interact with phonons, making the state-resolved spectroscopic monitoring of dynamics challenging. We propose a protocol that combines photon-entanglement-enhanced narrowband excitation of two-exciton states with time-frequency-filtered two-photon coincidence counting. This approach alleviates bottlenecks associated with probing exciton dynamics spread across multiple spectral and temporal windows. We demonstrate that non-classical correlations of entangled photon pairs can be used to prepare narrowband two-exciton population distributions, thereby circumventing transport in mediating one-exciton states. The evolution of these population distributions and cascading transitions can be monitored using time-frequency-filtered photon coincidence counting. Numerical simulations for a light-harvesting aggregate highlight the ability of this protocol to achieve selectivity by suppressing or amplifying specific pathways. Combining entangled photonic sources with multidimensional photon correlation spectroscopy allows promising applications in spectroscopy and sensing.
In quantum aggregates, delocalized exciton states across energy manifolds interact with phonon modes, making state-resolved spectroscopic monitoring of dynamics challenging. We propose a scheme that combines photon-entanglement-enhanced narrowband excitation of two-exciton states with time-frequency-filtered two-photon coincidence counting, which allows high-resolution probing of dissipative two-exciton dynamics spread across multiple spectral and temporal windows. We demonstrate that entangled photon pairs can be used to prepare narrowband two-exciton population distributions, circumventing transport in the mediating one-exciton manifold, and the redistributed two-exciton population can be monitored using time-frequency-filtered two-photon coincidence counting. Numerical simulations for a light-harvesting aggregate highlight the ability of this protocol to suppress or amplify specific pathways under a realistic scenario. Combining entangled photonic sources with multidimensional photon correlation techniques enables promising applications in spectroscopy and sensing.
Nonlinear spectroscopic techniques using entangled photon pairs can provide an opportunity to exploit non-classical correlations encoded in two-photon wavefunctions to manipulate two-exciton wavefunctions. We propose an entangled photon pair-enhanced multidimensional spectroscopic technique that is sensitive to exciton-exciton interactions and correlations at the femtosecond timescale. Simulations for a dissipative system, namely, the photosynthetic aggregate reveal the superior ability of entangled photon pairs, compared to both transform-limited and frequency-chirped laser pulses, to manipulate excited-state absorption pathways. The corresponding spectral features in the two-dimensional spectrogram are interpreted in terms of one- and two-exciton resonances. The signal scales linearly with the incoming intensity of the photon sources. We show that classifying these resonances using entangled photon source in the perturbative limit allow for probing exciton correlations at the natural energy scale. These insights can be used to explore multi-exciton dynamics in molecular systems using multiphoton entanglement.
We propose a photonic entanglement-enhanced multidimensional spectroscopic technique that is sensitive to exciton-exciton correlations at the ultrafast timescale. The signal demonstrates utility for monitoring the coherent signatures of exciton-exciton correlation dynamics in the presence of phonon-induced dissipation. Simulations of the signal for a photosynthetic aggregate is shown to reveal the superior ability of the entanglement-enhanced photonic sources to probe ultrafast dynamics while scaling linearly with the field intensity.The non-classical correlations are shown to aid in the exploration of hidden resonances originating from exciton correlations. Probing these resonances with high time-frequency resolution offers a distinctive advantage for nonlinear spectroscopy of molecular aggregates.
Recent advances in techniques for generating quantum light have stimulated research on novel spectroscopic measurements using quantum entangled photons. One such spectroscopy technique utilizes non-classical correlations among entangled photons to enable measurements with enhanced sensitivity and selectivity. Here, we investigate the spectroscopic measurement utilizing entangled three photons. In this measurement, time-resolved entangled photon spectroscopy with monochromatic pumping [A. Ishizaki, J. Chem. Phys. 153, 051102 (2020)] is integrated with the frequency-dispersed two-photon counting technique, which suppresses undesired accidental photon counts in the detector and thus allows one to separate the weak desired signal. This time-resolved frequency-dispersed two-photon counting signal, which is a function of two frequencies, is shown to provide the same information as that of coherent two-dimensional optical spectra. The spectral distribution of the phase-matching function works as a frequency filter to selectively resolve a specific region of the two-dimensional spectra, whereas the excited-state dynamics under investigation are temporally resolved in the time region longer than the entanglement time. The signal is not subject to Fourier limitations on the joint temporal and spectral resolution, and therefore, it is expected to be useful for investigating complex molecular systems in which multiple electronic states are present within a narrow energy range.
We theoretically propose a biphoton entanglement-enhanced multidimensional spectroscopic technique as a probe for the dissipative polariton dynamics in the ultrafast regime. It is applied to the cavity-confined monomeric photosynthetic complex that represents a prototypical multi-site excitonic quantum aggregate. The proposed technique is shown to be particularly sensitive to inter-manifold polariton coherence between the two and one-excitation subspaces. It is demonstrated to be able to monitor the dynamical role of cavity-mediated excitonic correlations, and dephasing in the presence of phonon-induced dissipation. The non-classicality of the entangled biphoton sources is shown to enhance the ultra-fast and broadband correlation features of the signal, giving an indication about the underlying state correlations responsible for long-range cavity-assisted exciton migration.
Quantum light is increasingly recognized as a promising resource for developing optical measurement techniques. Particular attention has been paid to enhancing the precision of the measurements beyond classical techniques by using nonclassical correlations between quantum entangled photons. Recent advances in the quantum optics technology have made it possible to manipulate spectral and temporal properties of entangled photons, and photon correlations can facilitate the extraction of matter information with relatively simple optical systems compared to conventional schemes. In these respects, the applications of entangled photons to time-resolved spectroscopy can open new avenues for unambiguously extracting information on dynamical processes in complex molecular and materials systems. Here, we propose time-resolved spectroscopy in which specific signal contributions are selectively enhanced by harnessing nonclassical correlations of entangled photons. The entanglement time characterizes the mutual delay between an entangled twin and determines the spectral distribution of photon correlations. The entanglement time plays a dual role as the knob for controlling the accessible time region of dynamical processes and the degrees of spectral selectivity. In this sense, the role of the entanglement time is substantially equivalent to the temporal width of the classical laser pulse. The results demonstrate that the application of quantum entangled photons to time-resolved spectroscopy leads to monitoring dynamical processes in complex molecular and materials systems by selectively extracting desired signal contributions from congested spectra. We anticipate that more elaborately engineered photon states would broaden the availability of quantum light spectroscopy.