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Rosario Roberto Riso

Publications and source records attributed to Rosario Roberto Riso.

4 recordsLinked to original sources

Beyond ideal cavities: quantifying the impact of cavity dissipation on light-matter strong coupling

Cavity Quantum Electrodynamics (Cavity-QED) offers a powerful framework for controlling light-matter interactions, yet first-principles approaches commonly assume ideal, lossless cavity fields. Here, we introduce a minimal extension to the Pauli-Fierz Hamiltonian that accounts for cavity dissipation through the experimentally accessible cavity quality factor Q. The electromagnetic field is described as a damped harmonic oscillator within the very weak damping approximation. In this framework, cavity losses only enter the light-matter interaction and dipole self-energy terms, without introducing additional photonic degrees of freedom. A time-dependent unitary transformation yields a real-valued Hermitian Hamiltonian that can be incorporated into existing ab-initio QED methods without additional computational cost or changes in scaling. We combined the approach to the QED-CCSD method and investigated the effects of cavity dissipation on the optical spectrum of a p-nitroaniline molecule under strong light-matter coupling. We found that, for realistic quality factors, cavity dissipation can reduce the Rabi splitting by more than 20% compared to the ideal-cavity limit, even though the system remains in the strong-coupling regime. Convergence towards the ideal-cavity limit then requires substantially higher quality factors than those needed to establish strong coupling. These results demonstrate that cavity dissipation can significantly affect polaritonic energetics and highlight the importance of incorporating experimentally realistic cavity losses into quantitative ab-initio Cavity-QED simulations to accurately guide experimental protocols.

physics.chem-ph↗

Fast Quantum Gates for Neutral Atoms Separated by a Few Tens of Micrometers

We present a theoretical scheme for a family of fast and high-fidelity two-qubit iSWAP gates between neutral atoms separated by more than 20 um, enabled by resonant dipole-dipole spin-exchange interactions between Rydberg states. The protocol harnesses coherent excitation-exchange-deexcitation dynamics between the qubit and the Rydberg states within a single and smooth laser pulse, in the presence of strong dipole-dipole interactions. We utilize optimal control methods to achieve theoretical gate fidelities and durations comparable to blockade-based gates in the presence of relevant noise, while extending the effective interaction range by an order of magnitude. This enables entanglement well beyond the blockade radius, offering a route toward fast, high-connectivity quantum processors.

quant-ph↗

Polaritonic Bloch's Theorem beyond the Long-Wavelength Approximation

Cavity quantum electrodynamics provides a powerful tool to manipulate material properties, yet it remains a matter of debate whether and how quantized fields affect the periodicity of crystals. Here, we extend Bloch's theorem to crystals under strong light-matter coupling, revealing that polariton quasiparticles preserve lattice periodicity. We introduce a general framework to incorporate multimode cavity fields in a simple and tractable way, showing that additional modes contribute small energy corrections noticeable only at low frequencies. Within the single-photon approximation, these contributions reduce to a spatially uniform effective field in the crystal plane, providing a formal justification for the single-mode and long-wavelength approximations commonly used in molecular polaritonics. Together, these results establish a rigorous framework for describing polaritonic states in crystalline solids.

cond-mat.mtrl-sci↗

Electronic Transitions for a Fully Polarizable QM/MM Approach Based on Fluctuating Charges and Fluctuating Dipoles: Linear and Corrected Linear Response Regimes

Fully polarizable QM/MM approach based on fluctuating charges and fluctuating dipoles, named QM/FQFμ (J. Chem. Theory Comput. 2019, 15 2233-2245), is extended to the calculation of vertical excitation energies of solvated molecular systems. Excitation energies are defined within two different solvation regimes, i.e. linear response (LR), where the response of the MM portion is adjusted to the QM transition density, and corrected-Linear Response (cLR) in which the MM response is adjusted to the relaxed QM density, thus being able to account for charge equilibration in the excited state. The model, which is specified in terms of three physical parameters (electronegativity, chemical hardness, and polarizability) is applied to vacuo-to-water solvatochromic shifts of aqueous solutions of para-nitroaniline, pyridine and pyrimidine. The results show a good agreement with their experimental counterparts, thus highlighting the potentialities of this approach.

physics.chem-ph↗