arXiv subjects

Valentina Notararigo

Publications and source records attributed to Valentina Notararigo.

4 recordsLinked to original sources

arXiv2024

Two-colour photon correlations probe coherent vibronic contributions to electronic excitation transport under incoherent illumination

Identifying signatures of quantum coherent behaviour in photoactive systems that are maintained in stationary states away from thermal equilibrium is an open problem of wide interest in a variety of physical scenarios, including single photosynthetic complexes subjected to continuous incoherent illumination. Here we consider a prototype light-harvesting heterodimer exhibiting coherent and collective exciton-vibration interactions and show that the second-order frequency-filtered correlations of fluorescence photons provide insightful information on the influence of such coherent interactions for different transitions, thereby yielding fundamentally different photon-counting statistics. Furthermore, we show that coherent vibronic mechanisms strongly affect the asymmetries characteristic of time-resolved photon cross-correlations and manifest themselves in a time-dependent violation of the Cauchy-Schwarz inequality bounding cross-correlations for classically fluctuating fields. We finally discuss how such second-order correlation asymmetry establishes important connections between coherent vibronic interactions, directional exciton population transport, and violation of quantum detailed balance. Our work then indicates that measurement of two-colour photon correlation asymmetry can be an important avenue to investigate quantum behaviour of single photoactive biomolecular and chemical systems under incoherent illumination conditions.

physics.chem-ph↗

arXiv2023

Multi-level Purcell effect and the impact of vibrational modes in molecular quantum optics

The increased decay rate of a two-level system weakly coupled to an optical cavity, known as the Purcell effect, is a cornerstone of cavity QED. However, the effect of cavity coupling is not well understood if the two-level system is replaced by a multi-level interacting system. Motivated by experiments looking to characterise molecular systems via exploiting a cavity interaction, we study a manifestation of the Purcell effect in a bio-inspired photosynthetic dimer. We focus in particular on how molecular vibrational modes, thought to play an important role in photosynthetic exciton transport, impact the system-cavity behaviour in the Purcell regime. We provide a theoretical picture in terms of an effective non-Hermitian Hamiltonian, which extends the simple picture of a Jaynes-Cummings model to the description of a `multi-level' Purcell effect, where different levels have differing Purcell factors, with effective cooperativities mediated by coherent vibrational interactions.

quant-ph↗

arXiv2018

Resonance interaction energy between two entangled atoms in a photonic bandgap environment

We consider the resonance interaction energy between two identical entangled atoms, where one is in the excited state and the other in the ground state. They interact with the quantum electromagnetic field in the vacuum state and are placed in a photonic-bandgap environment with a dispersion relation quadratic near the gap edge and linear for low frequencies, while the atomic transition frequency is assumed to be inside the photonic gap and near its lower edge. This problem is strictly related to the coherent resonant energy transfer between atoms in external environments. The analysis involves both an isotropic three-dimensional model and the one-dimensional case. The resonance interaction asymptotically decays faster with distance compared to the free-space case, specifically as $1/r^2$ compared to the $1/r$ free-space dependence in the three-dimensional case, and as $1/r$ compared to the oscillatory dependence in free space for the one-dimensional case. Nonetheless, the interaction energy remains significant and much stronger than dispersion interactions between atoms. On the other hand, spontaneous emission is strongly suppressed by the environment and the correlated state is thus preserved by the spontaneous-decay decoherence effects. We conclude that our configuration is suitable for observing the elusive quantum resonance interaction between entangled atoms.

quant-ph↗

arXiv2018

Perturbation approach for computing frequency- and time-resolved photon correlation functions

We propose an alternative formulation of the sensor method presented in [Phys. Rev. Lett 109, 183601 (2012)] for the calculation of frequency-filtered and time-resolved photon correlations. Our approach is based on an algebraic expansion of the joint steady state of quantum emitter and sensors with respect to the emitter-sensor coupling parameter ε. This allows us to express photon correlations in terms of the open quantum dynamics of the emitting system only and ensures that computation of correlations are independent on the choice of a small value of ε. Moreover, using time-dependent perturbation theory, we are able to express the frequency- and time- resolved second-order photon correlation as the addition of three components, each of which gives insight into the physical processes dominating the correlation at different time scales. We consider a bio-inspired vibronic dimer model to illustrate the agreement between the original formulation and our approach.

quant-ph↗