Frequency-Resolved Purcell Effect for the Dissipative Generation of Steady-State Entanglement.

We report a driven-dissipative mechanism to generate stationary entangled W states among strongly interacting quantum emitters placed within a cavity. Driving the ensemble into the highest energy state-whether coherently or incoherently-enables a subsequent cavity-enhanced decay into an entangled steady state consisting of a single deexcitation shared coherently among all emitters, i.e.

Random matrix theory approach to quantum Fisher information in quantum ergodic systems.

We theoretically investigate quantum parameter estimation in quantum chaotic systems. Our analysis is based on an effective description of quantum ergodic systems in terms of a random matrix Hamiltonian. Based on this approach, we derive an analytical expression for the time evolution of the quantum Fisher information (QFI), which we find to have three distinct timescales.

Microsolvation of a Proton by Ar Atoms: Structures and Energetics of ArH Clusters.

We present a computational investigation on the structural arrangements and energetic stabilities of small-size protonated argon clusters, Ar nH +. Using high-level ab initio electronic structure computations, we determined that the linear symmetric triatomic ArH +Ar ion serves as the molecular core for all larger clusters studied. Through harmonic normal-mode analysis for clusters containing up to seven argon atoms, we observed that the proton-shared vibration shifts to lower frequencies, consistent with measurements in gas-phase IRPD and solid Ar-matrix isolation experiments.

CO2 inside sI clathrate-like cages: Automated construction of neural network/machine learned guest-host potential and quantum spectra computations.

We present new results on the underlying guest-host interactions and spectral characterization of a CO2 molecule confined in the cages of the sI clathrate hydrate. Such types of porous solids raise computational challenges, as they are of practical interest as gas storage/capture materials. Accordingly, we have directed our efforts toward addressing their modeling in a proper manner, ensuring the quality of the input data and the efficiency of the computational approaches.

Converting Long-Range Entanglement into Mixture: Tensor-Network Approach to Local Equilibration.

In the out-of-equilibrium evolution induced by a quench, fast degrees of freedom generate long-range entanglement that is hard to encode with standard tensor networks. However, local observables only sense such long-range correlations through their contribution to the reduced local state as a mixture. We present a tensor network method that identifies such long-range entanglement and efficiently transforms it into mixture, much easier to represent.

A kernel-based machine learning potential and quantum vibrational state analysis of the cationic Ar hydride (ArH).

One of the most fascinating discoveries in recent years, in the cold and low pressure regions of the universe, was the detection of ArH and HeH species. The identification of such noble gas-containing molecules in space is the key to understanding noble gas chemistry. In the present work, we discuss the possibility of [ArH] existence as a potentially detectable molecule in the interstellar medium, providing new data on possible astronomical pathways and energetics of this compound.

Analysing the stability of He-filled hydrates: how many He atoms fit in the sII crystal?

Clathrate hydrates have the ability to encapsulate atoms and molecules within their cavities, and thus they could be potentially large storage capacity materials. The present work studies the multiple cage occupancy effects in the recently discovered He@sII crystal. On the basis of previous theoretical and experimental findings, the stability of He@sII, He@sII and He@sII crystals was analysed in terms of structural, mechanical and energetic properties.

Confining He Atoms in Diverse Ice-Phases: Examining the Stability of He Hydrate Crystals through DFT Approaches.

In the realm of solid water hydrostructures, helium atoms have a tendency to occupy the interstitial spaces formed within the crystal lattice of ice structures. The primary objective of this study is to examine the stability of various ice crystals when influenced by the presence of He atoms. Presenting a first attempt at a detailed computational description of the whole energy components (guest-water, water-water, guest-guest) in the complete crystal unit cells contributes to enhancing the knowledge available about these relatively unexplored helium-water systems, which could potentially benefit future experiments.

Computational Energy Spectra of the H O@C Endofullerene.

A water molecule confined inside the C fullerene was quantum-mechanically described using a computational approach within the MCTDH framework. Such procedure involves the development of a full-dimensional coupled hamiltonian, with an exact kinetic energy operator, including all rotational, translational and vibrational degrees of freedom of the endofullerene system. In turn, through an effective pairwise potential model, the ground and rotationally excited states of the encapsulated H O inside the C cage were calculated, and traced back to the isotropic case of the H O@C endofullerene in order to understand the nature and physical origin of the symmetry breaking observed experimentally in the latter system.

Variational Quantum Simulators Based on Waveguide QED.

Waveguide QED simulators are analog quantum simulators made by quantum emitters interacting with one-dimensional photonic band gap materials. One of their remarkable features is that they can be used to engineer tunable-range emitter interactions. Here, we demonstrate how these interactions can be a resource to develop more efficient variational quantum algorithms for certain problems.

Computational investigations of stable multiple-cage-occupancy He clathrate-like hydrostructures.

One of the several possibilities offered by the interesting clathrate hydrates is the opportunity to encapsulate several atoms or molecules, in such a way that more efficient storage materials could be explored or new molecules that otherwise do not exist could be created. These types of applications are receiving growing attention from technologists and chemists, given the future positive implications that they entail. In this context, we investigated the multiple cage occupancy of helium clathrate hydrates, to establish stable novel hydrate structures or ones similar to those predicted previously by experimental and theoretical studies.

Modeling of Structure H Carbon Dioxide Clathrate Hydrates: Guest-Lattice Energies, Crystal Structure, and Pressure Dependencies.

We performed first-principles computations to investigate the complex interplay of molecular interaction energies in determining the lattice structure and stability of CO@sH clathrate hydrates. Density functional theory computations using periodic boundary conditions were employed to characterize energetics and the key structural properties of the sH clathrate crystal under pressure, such as equilibrium lattice volume and bulk modulus. The performance of exchange-correlation functionals together with recently developed dispersion-corrected schemes was evaluated in describing interactions in both short-range and long-range regions of the potential.

Tuning Long-Range Fermion-Mediated Interactions in Cold-Atom Quantum Simulators.

Engineering long-range interactions in cold-atom quantum simulators can lead to exotic quantum many-body behavior. Fermionic atoms in ultracold atomic mixtures can act as mediators, giving rise to long-range Ruderman-Kittel-Kasuya-Yosida-type interactions characterized by the dimensionality and density of the fermionic gas. Here, we propose several tuning knobs, accessible in current experimental platforms, that allow one to further control the range and shape of the mediated interactions, extending the existing quantum simulation toolbox.

Quantum molecular simulations of micro-hydrated halogen anions.

We report the results of a detailed and accurate investigation focused on structures and energetics of poly-hydrated halides employing first-principles polarizable halide-water potentials to describe the underlying forces. Following a bottom-up data-driven potential approach, we initially looked into the classical behavior of higher-order X(HO) clusters. We have located several low-lying energies, such as global and local minima, structures for each cluster, with various water molecules (up to = 8) surrounding the halide anion (X = F, Cl, Br, I), employing an evolutionary programming method.

Delving into guest-free and He-filled sI and sII clathrate hydrates: a first-principles computational study.

The dynamics of the formation of a specific clathrate hydrate as well as its thermodynamic transitions depend on the interactions between the trapped molecules and the host water lattice. The molecular-level understanding of the different underlying processes benefits not only the description of the properties of the system, but also allows the development of multiple technological applications such as gas storage, gas separation, energy transport, In this work we investigate the stability of periodic crystalline structures, such as He@sI and He@sII clathrate hydrates by first-principles computations. We consider such host water networks interacting with a guest He atom using selected density functional theory approaches, in order to explore the effects on the encapsulation of a light atom in the sI/sII crystals, by deriving all energy components (guest-water, water-water, guest-guest).

Tunable Directional Emission and Collective Dissipation with Quantum Metasurfaces.

Subwavelength atomic arrays, recently labeled as quantum metamaterials, have emerged as an exciting platform for obtaining novel quantum optical phenomena. The strong interference effects in these systems generate subradiant excitations that propagate through the atomic array with very long lifetimes. Here, we demonstrate that one can harness these excitations to obtain tunable directional emission patterns and collective dissipative couplings when placing judiciously additional atoms nearby the atomic array.

Unraveling the Origin of Symmetry Breaking in H O@C Endofullerene Through Quantum Computations.

We explore the origin of the anomalous splitting of the 1 levels reported experimentally for the H O@C endofullerene, in order to give some insight about the physical interpretations of the symmetry breaking observed. We performed fully-coupled quantum computations within the multiconfiguration time-dependent Hartree approach employing a rigorous procedure to handle such computationally challenging problems. We introduce two competing physical models, and discuss the observed unconventional quantum patterns in terms of anisotropy in the interfullerene interactions, caused by the change in the off-center position of the encapsulated water molecules inside the cage or the uniaxial C -cage distortion, arising from noncovalent bonding upon water's encapsulation, or exohedral fullerene perturbations.

A Benchmark Protocol for DFT Approaches and Data-Driven Models for Halide-Water Clusters.

Dissolved ions in aqueous media are ubiquitous in many physicochemical processes, with a direct impact on research fields, such as chemistry, climate, biology, and industry. Ions play a crucial role in the structure of the surrounding network of water molecules as they can either weaken or strengthen it. Gaining a thorough understanding of the underlying forces from small clusters to bulk solutions is still challenging, which motivates further investigations.

Photon-Mediated Stroboscopic Quantum Simulation of a Z_{2} Lattice Gauge Theory.

Quantum simulation of lattice gauge theories, aiming at tackling nonperturbative particle and condensed matter physics, has recently received a lot of interest and attention, resulting in many theoretical proposals as well as several experimental implementations. One of the current challenges is to go beyond 1+1 dimensions, where four-body (plaquette) interactions, not contained naturally in quantum simulating devices, appear. In this Letter, we propose a method to obtain them based on a combination of stroboscopic optical atomic control and the nonlocal photon-mediated interactions appearing in nanophotonic or cavity QED setups.

Assessment of DFT approaches in noble gas clathrate-like clusters: stability and thermodynamics.

We have assessed the performance and accuracy of different wavefunction-based electronic structure methods, such as DFMP2 and domain-based local pair-natural orbital (DLPNO-CCSD(T)), as well as a variety of density functional theory (DFT) approaches on He@(HO) cage systems. We have selected representative clathrate-like structures corresponding to the building blocks present in each of the sI, sII and sH natural gas clathrate hydrates, and we have carefully studied the interaction between a He atom with each of their individual cages. We reported well-converged DFMP2 and DLPNO-CCSD(T) reference data, together with interaction and cohesive energies of four different density functionals (two GGA, revPBE and PW86PBE, and two hybrids, B3LYP and PBE0), including diverse dispersion correction schemes (D3(0), D3(BJ), D4 and XDM) for both He-filled and empty clathrate-like cages.

Encapsulation of a Water Molecule inside C Fullerene: The Impact of Confinement on Quantum Features.

We introduce an efficient quantum fully coupled computational scheme within the multiconfiguration time-dependent Hartree (MCTDH) approach to handle the otherwise extremely costly computations of translational-rotational-vibrational states and energies of light-molecule endofullenes. Quantum calculations on energy levels are reported for a water molecule inside C fullerene by means of such a systematic approach that includes all nine degrees of freedom of HO@C and does not consider restrictions above them. The potential energy operator is represented as a sum of natural potentials employing the -mode expansion, along with the exact kinetic energy operator, by introducing a set of Radau internal coordinates for the HO molecule.

Computational Characterization of Astrophysical Species: The Case of Noble Gas Hydride Cations.

Theoretical-computational studies together with recent astronomical observations have shown that under extreme conditions in the interstellar medium (ISM), complexes of noble gases may be formed. Such observations have generated a wide range of possibilities. In order to identify new species containing such atoms, the present study gathers spectroscopic data for noble gas hydride cations, NgH (Ng = He, Ne, Ar) from high-level quantum chemistry computations, aiming to contribute in understanding the chemical bonding and electron sharing in these systems.

Computational density-functional approaches on finite-size and guest-lattice effects in CO@sII clathrate hydrate.

We performed first-principles computations to investigate guest-host/host-host effects on the encapsulation of the CO molecule in sII clathrate hydrates from finite-size clusters up to periodic 3D crystal lattice systems. Structural and energetic properties were first computed for the individual and first-neighbors clathrate-like sII cages, where highly accurate ab initio quantum chemical methods are available nowadays, allowing in this way the assessment of the density functional (DFT) theoretical approaches employed. The performance of exchange-correlation functionals together with recently developed dispersion-corrected schemes was evaluated in describing interactions in both short-range and long-range regions of the potential.

Exploring CO @sI Clathrate Hydrates as CO Storage Agents by Computational Density Functional Approaches.

The formation of specific clathrate hydrates and their transformation at given thermodynamic conditions depends on the interactions between the guest molecule/s and the host water lattice. Understanding their structural stability is essential to control structure-property relations involved in different technological applications. Thus, the energetic aspects relative to CO @sI clathrate hydrate are investigated through the computation of the underlying interactions, dominated by hydrogen bonds and van der Waals forces, from first-principles electronic structure approaches.