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arXiv:2512.14964

Pulsed single-photon spectroscopy of an emitter with vibrational coupling

Sourav Das, Aiman Khan, Elnaz Darsheshdar, Francesco Albarelli, Animesh Datta

quant-phSubmitted Dec 16, 2025• Announced Dec 18, 2025• 0 citations
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Abstract

We analytically derive the quantum state of a single-photon pulse scattered from a single quantum two-level emitter interacting with a vibrational bath. This solution for the quadripartite system enables an information-theoretic characterization of vibrational effects in quantum light spectroscopy. We show that vibration-induced dephasing reduces the quantum Fisher information (QFI) for estimating the emitter's linewidth, largely reflecting the Franck-Condon suppression of light-matter coupling. Comparing time- and frequency-resolved photodetection, we find the latter to be more informative in estimating the emitter's linewidth for stronger vibrational coupling.

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We analytically derive the quantum state of a single-photon pulse scattered from a single quantum two-level emitter interacting with a vibrational bath. This solution for the quadripartite system enables an information-theoretic characterization of vibrational effects in quantum light spectroscopy. We show that vibration-induced dephasing reduces the quantum Fisher information (QFI) for estimating the emitter's linewidth, largely reflecting the Franck-Condon suppression of light-matter coupling. Comparing time- and frequency-resolved photodetection, we find the latter to be more informative in estimating the emitter's linewidth for stronger vibrational coupling.
We apply our recently developed theory of frequency-filtered and time-resolved N -photon correlations (del Valle et al 2012 Phys. Rev. Lett. 109 183601) to study the two-photon spectra of a variety of systems of increasing complexity: single-mode emitters with two limiting statistics (one harmonic oscillator or a two-level system) and the various combinations that arise from their coupling. We consider both the linear and nonlinear regimes under incoherent excitation. We find that even the simplest systems display a rich dynamics of emission, not accessible by simple single-photon spectroscopy. In the strong coupling regime, two-photon emission processes involving virtual states are revealed. Furthermore, two general results are unravelled by two-photon correlations with narrow linewidth detectors: (i) filtering-induced bunching and (ii) breakdown of the semi-classical theory. We show how to overcome the latter in a fully quantized picture.
We develop a theoretical framework to describe the scattering of photons against a two-level quantum emitter with arbitrary correlated dephasing noise.This is particularly relevant to waveguide-QED setups with solid-state emitters, such as superconducting qubits or quantum dots, which couple to complex dephasing environments in addition to the propagating photons along the waveguide.Combining input-output theory and stochastic methods, we predict the effect of correlated dephasing in single-photon transmission experiments with weak coherent inputs.We discuss homodyne detection and photon counting of the scattered photons and show that both measurements give the modulus and phase of the single-photon transmittance despite the presence of noise and dissipation.In addition, we demonstrate that these spectroscopic measurements contain the same information as standard time-resolved Ramsey interferometry, and thus they can be used to fully characterize the noise correlations without direct access to the emitter.The method is exemplified with paradigmatic correlated dephasing models such as colored Gaussian noise, white noise, telegraph noise, and 1/fnoise, as typically encountered in solid-state environments.
The interaction between quantum emitters leads to the formation of superradiant and subradiant states with possible applications in quantum technologies. To improve the characterization of light emission from these systems, we present here a systematic theoretical analysis of the intensity correlation from two strongly interacting quantum emitters at cryogenic temperatures as a function of the frequency and intensity of the excitation laser. This analysis effectively accounts for the effect of vibrational modes of the emitters and of phonons of the environment through the combined Debye-Waller/Franck-Condon factor. First, we analyze the color-blind intensity correlation and show that it can be tailored from strong antibunching to strong bunching by tuning the laser from the two-photon resonance to the transition frequency of the superradiant state. We also find a particularly complex behavior of the intensity correlation when the laser frequency is tuned to that of the transition of the subradiant state, giving raise to the possibility of emitting bunched and antibunched light depending on the laser intensity and the detuning between the two emitters. The numerical results are supported by analytical equations that can be used for the experimental characterization of the interacting emitters. Additionally, by selecting photons of particular frequencies, we analyze the rich landscape of frequency-resolved intensity correlations, which also depend on the laser detuning and intensity. The analysis of the frequency-resolved correlations provides further information about the different relaxation processes underlying the photon emission, unveiling one-photon and two-photon emission processes that cannot be resolved neither in the emission spectrum nor in the color-blind intensity correlation. These results show that two interacting emitters are a versatile and practical source of quantum light and highlight the usefulness of the intensity correlation to unveil complex dynamics in this system. Published by the American Physical Society 2024
Using second-order perturbation theory in the light-matter interaction, we derive an analytical approximation for the vibronic populations of a diatomic system excited by ultrabroadband frequency-entangled photons and evaluate the population dynamics for different degrees of entanglement between photon pairs. Our analytical approach makes the same predictions as previously derived via numerical solutions of the complete Schrödinger equation [H. Oka, ], with the added advantage of providing clear physical insights into the vibronic selectivity as a function of the degree of photon correlations while requiring significantly reduced computational effort. Specifically, our analytical expression for the probability of vibronic excitation includes a factor which predicts the enhancement of vibrational selectivity as a function of the degree correlation between the entangled photon pairs, the targeted vibrational energy level, and the vibrational molecular structure encoded in the Franck-Condon factors. Our results illustrate the importance of going beyond the usual approximations in second-order perturbation theory to capture the relevance of the vibrational structure of the molecular system of interest in order to gain a deeper understanding of the possible quantum-enhancement provided by the interaction between quantum light and matter.
Abstract. We apply our recently developed theory of frequency-filtered and time-resolved N-photon correlations [1] to study the two-photon spectra of a variety of systems of increasing complexity: single mode emitters with two limiting statistics (one harmonic oscillator or a two-level system) and the various combinations that arise from their coupling. We consider both the linear and nonlinear regimes under incoherent excitation. We find that even the simplest systems display a rich dynamics of emission, not accessible by simple single photon spectroscopy. In the strong coupling regime, novel two-photon emission processes involving virtual states are revealed. Furthermore, two general results are unraveled by two-photon correlations with narrow linewidth detectors: i) filtering induced bunching and ii) breakdown of the semi-classical theory. We show how to overcome this shortcoming in a fully-quantized picture. PACS numbers: 42.50.Ar,42.50.Lc,05.10.Gg,42.25.Kb,42.79.Pw ar X iv
Light emission from solid-state quantum emitters is inherently prone to environmental decoherence, which results in a line broadening and in the deterioration of photon indistinguishability. Here we employ photon correlation Fourier spectroscopy (PCFS) to study the temporal evolution of such a broadening in two prominent systems: GaAs and In(Ga)As quantum dots. Differently from previous experiments, the emitters are driven with short laser pulses as required for the generation of high-purity single photons, the time scales we probe range from a few nanoseconds to milliseconds and, simultaneously, the spectral resolution we achieve can be as small as ∼ 2µeV. We find pronounced differences in the temporal evolution of different optical transition lines, which we attribute to differences in their homogeneous linewidth and sensitivity to charge noise. We analyze the effect of irradiation with additional white light, which reduces blinking at the cost of enhanced charge noise. Due to its robustness against experimental imperfections and its high temporal resolution and bandwidth, PCFS outperforms established spectroscopy techniques, such as Michelson interferometry. We discuss its practical implementation and the possibility to use it to estimate the indistinguishability of consecutively emitted single photons for applications in quantum communication and photonic-based quantum information processing.