# Physics - Atomic and Molecular Clusters Publications (50)

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## Physics - Atomic and Molecular Clusters Publications

The bound states of two identical dipoles in a harmonic waveguide are investigated. In the regime of weak dipole-dipole interactions, the local frame transformation (LFT) method is applied to determine the spectrum of dipolar confinement-induced bound states analytically. The accuracy of the LFT approach is discussed by comparing the analytical results with the numerical ones based on a solution of the close-coupling equations. Read More

Rabi oscillations typify the inherent nonlinearity of optical excitations in quantum dots. Using an integral kernel formulation to solve the 3D Maxwell-Bloch equations in ensembles of up to $10^4$ quantum dots, we observe features in Rabi oscillations due to the interplay of nonlinearity, non-equilibrium excitation, and electromagnetic coupling between the dots. This approach allows us to observe the dynamics of each dot in the ensemble without resorting to spatial averages. Read More

We review recent experimental and theoretical progress in understanding the microscopic details of clustering in nuclei. We discuss recent experimental results on alpha-conjugate systems, alpha-states in heavy systems, molecular structures in neutron-rich nuclei, and constraints for ab initio theory. We then examine nuclear clustering in a wide range of theoretical methods, including the resonating group and generator coordinate methods, antisymmetrized molecular dynamics, fermionic molecular dynamics, Tohsaki-Horiuchi-Schuck-R\"opke wave function and container model, no-core shell model methods, continuum quantum Monte Carlo, lattice effective field theory, and several approaches to clustering in heavier systems. Read More

We report on the Doppler-free saturation spectroscopy of the nitrous oxide (N$_2$O) overtone transition at 1.28~$\mu$m. This measurement is performed by the noise-immune cavity-enhanced optical heterodyne molecular spectroscopy (NICE-OHMS) technique based on the quantum-dot (QD) laser. Read More

Lowest bound S-state energy of Coulomb three-body systems ($N^{Z+}\mu^-e^-$) having a positively charged nucleus of charge number Z ($N^{Z+}$), a negatively charged muon ($\mu^-$) and an electron ($e^-$), is investigated in the framework of hyperspherical harmonics expansion method. A Yukawa type Coulomb potential with an adjustable screening parameter ($\lambda$) is chosen for the 2-body subsystems. In the resulting Schr\"odinger equation (SE), the three-body relative wave function is expanded in the complete set of hyperspherical harmonics (HH). Read More

We report on studies of collisions between 3 keV Ar$^+$ projectile ions and neutral targets of isolated 1,3-butadiene (C$_4$H$_6$) molecules and cold, loosely bound clusters of these molecules. We identify molecular growth processes within the molecular clusters that appears to be driven by knockout processes and that could result in the formation of (aromatic) ring structures. These types of reactions are not unique to specific projectile ions and target molecules, but will occur whenever atoms or ions with suitable masses and kinetic energies collide with aggregates of matter, such as carbonaceous grains in the interstellar medium or aerosol nanoparticles in the atmosphere. Read More

We examine time-resolved X-ray diffraction from molecules in the gas phase which undergo nonadiabatic avoided-crossing dynamics involving strongly coupled electrons and nuclei. Several contributions to the signal are identified, representing (in decreasing strength) elastic scattering, contributions of the electronic coherences created by nonadiabatic couplings in the avoided crossing regime, and inelastic scattering. The former probes the charge density and delivers direct information on the evolving molecular geometry. Read More

We show a unified second-order scheme for constructing simple, robust and accurate algorithms for typical thermostats for configurational sampling for the canonical ensemble. When Langevin dynamics is used, the scheme leads to the BAOAB algorithm that has been recently investigated. We show that the scheme is also useful for other types of thermostat, such as the Andersen thermostat and Nos\'e-Hoover chain. Read More

The spin-1 Haldane chain is an example of the symmetry-protected-topological (SPT) phase in one dimension. Experimental realization of the spin chain materials usually involves both the uniaxial-type, $D(S^z)^2$, and the rhombic-type, $E[(S^x)^2-(S^y)^2]$, single-ion anisotropies. Here, we provide a precise ground-state phase diagram for spin-1 Haldane chain with these single-ion anisotropies. Read More

Neutral metal-containing molecules and clusters present a particular challenge to velocity map imaging techniques. Common methods of choice for producing such species such as laser ablation or magnetron sputtering typically generate a wide variety of metal-containing species and, without the possibility of mass-selection, even determining the identity of the dissociating moiety can be challenging. In recent years, we have developed a velocity map imaging spectrometer equipped with a laser ablation source explicitly for studying neutral metal-containing species. Read More

There is considerable interest in collective effects in hybrid systems formed by molecular or atomic ensembles strongly coupled by an electromagnetic resonance. For analyzing such collective effects, we develop an efficient and general theoretical formalism based on the natural modes of the resonator. The main strength of our approach is its generality and the high level of analyticity enabled by modal analysis, which allows one to model complex hybrid systems without any restriction on the resonator shapes or material properties, and to perform statistical computations to predict general properties that are robust to spatial and polarization disorders. Read More

Reflection Nebula NGC2023 shows specific interstellar infrared spectrum due to polycyclic aromatic hydrocarbon (PAH) in a wide wavelength range from 5 to 20 micrometer. By our previous quantum chemistry calculation, it was suggested that a molecule group having hydrocarbon pentagon-hexagon combined skeleton could reproduce ubiquitous interstellar infrared spectrum. In this paper, observed NGC2023 spectrum was compared in detail with such carrier candidates. Read More

From microscopic point-dipole model calculations of the screening of the Coulomb interaction in non-polar systems by polarizable atoms, it is known that screening strongly depends on dimensionality. For example, in one dimensional systems the short range interaction is screened, while the long range interaction is anti-screened. This anti-screening is also observed in some zero dimensional structures, i. Read More

In this Letter we explore the potential of probing new light force-carriers, with spin-independent couplings to the electron and the neutron, using precision isotope shift spectroscopy. We develop a formalism to interpret linear King plots as bounds on new physics with minimal theory inputs. We focus only on bounding the new physics contributions that can be calculated independently of the Standard Model nuclear effects. Read More

Iodine (I$_2$) molecules embedded in He nanodroplets are aligned by a 160 ps long laser pulse. The highest degree of alignment, occurring at the peak of the pulse and quantified by $\langle \cos^2 \theta_{2D} \rangle$, is measured as a function of the laser intensity. The results are well described by $\langle \cos^2 \theta_{2D} \rangle$ calculated for a gas of isolated molecules each with an effective rotational constant of 0. Read More

The process of wave propagation in an infinite linear chain is analyzed. Established, that dispersion relation between the angular frequency and the wave number for transverse waves differs from similar dependencies for longitudinal. Read More

The radiative lifetime of molecules or atoms can be increased by placing them within a tuned conductive cavity that inhibits spontaneous emission. This was examined as a possible means of enhancing three-body, singlet-based upconversion, known as energy pooling. Achieving efficient upconversion of light has potential applications in the fields of photovoltaics, biofuels, and medicine. Read More

A recent rejuvenation of experimental and theoretical interest in the physics of few- body systems has provided deep, fundamental insights into a broad range of problems. Few-body physics is a cross-cutting discipline not restricted to conventional subject ar- eas such as nuclear physics or atomic or molecular physics. To a large degree, the recent explosion of interest in this subject has been sparked by dramatic enhancements of experimental capabilities in ultracold atomic systems over the past decade, which now permit atoms and molecules to be explored deep in the quantum mechanical limit with controllable two-body interactions. Read More

We investigate the transient photoexcited lattice dynamics in a layered perovskite Mott insulator Sr2IrO4 by femtosecond X-ray diffraction using a laser plasma-based X-ray source. Ultrafast structural dynamics of Sr2IrO4 thin films are determined by observing the shift and broadening of the (0012) Bragg diffraction after excitation by 1.5 eV and 3. Read More

The calculation of minimum energy paths for transitions such as atomic and/or spin re-arrangements is an important task in many contexts and can often be used to determine the mechanism and rate of transitions. An important challenge is to reduce the computational effort in such calculations, especially when ab initio or electron density functional calculations are used to evaluate the energy since they can require large computational effort. Gaussian process regression is used here to reduce significantly the number of energy evaluations needed to find minimum energy paths of atomic rearrangements. Read More

When matter is exposed to a high-intensity x-ray free-electron-laser pulse, the x rays excite inner-shell electrons leading to the ionization of the electrons through various atomic processes and creating high-energy-density plasma, i.e., warm dense matter. Read More

The influence of the surface curvature on the surface tension of small droplets in equilibrium with a surrounding vapour, or small bubbles in equilibrium with a surrounding liquid, can be expanded as $\gamma(R) = \gamma_0 + c_1\gamma_0/R + O(1/R^2)$, where $R = R_\gamma$ is the radius of the surface of tension and $\gamma_0$ is the surface tension of the planar interface, corresponding to zero curvature. According to Tolman's law, the first-order coefficient in this expansion is assumed to be related to the planar limit $\delta_0$ of the Tolman length, i.e. Read More

In several settings of physics and chemistry one has to deal with molecules interacting with some kind of an external environment, be it a gas, a solution, or a crystal surface. Understanding molecular processes in the presence of such a many-particle bath is inherently challenging, and usually requires large-scale numerical computations. Here, we present an alternative approach to the problem - that based on the notion of the angulon quasiparticle. Read More

The degree of thermalization of electronically excited state manifolds of an absorber can be tested via optical spectroscopy. In the thermalized-manifold case, the ratio of absorption and emission is expected to follow a universal Boltzmann-type frequency scaling, known as the Kennard-Stepanov relation. Here, we investigate absorption and emission spectral profiles of rubidium, cesium, and potassium molecular dimers in a high-pressure argon buffer-gas environment and study the effect of collisionally induced redistribution. Read More

High-order harmonic generation (HHG) from aligned acetylene molecules interacting with mid infra-red (IR), linearly polarized laser pulses is studied theoretically using a mixed quantum-classical approach in which the electrons are described using time-dependent density functional theory while the ions are treated classically. We find that for molecules aligned perpendicular to the laser polarization axis, HHG arises from the HOMO orbital while for molecules aligned along the laser polarization axis, HHG is dominated by the HOMO-1 orbital. In the parallel orientation the harmonic spectrum comprises a double plateau structure with the inner plateau arising from excitation of an autoionizing state. Read More

We find that negative charges on an armchair single-walled carbon nanotube (SWCNT) can significantly enhance the migration of a carbon adatom on the external surfaces of SWCNTs, along the direction of the tube axis. Nanotube charging results in stronger binding of adatoms to SWCNTs and consequent longer lifetimes of adatoms before desorption, which in turn increases their migration distance several orders of magnitude. These results support the hypothesis of diffusion enhanced SWCNT growth in the volume of arc plasma. Read More

We study plasmonic excitations in the limit of few electrons, in one-atom thick sodium chains, and characterize them based on collectivity. We also compare the excitations to classical localised plasmon modes and find for the longitudinal mode a quantum-classical transition around 10 atoms. The transverse mode appears at much higher energies than predicted classically for all chain lengths. Read More

The molecular absorption of photons with angular momentum can result in twisted excitons with a well-defined quasi-angular momentum. Although they represent different physical properties, photonic and excitonic quanta can both be described in terms of topological charge, a conserved quantity. Multiple absorption events can be used to create a wide range of excitonic topological charges. Read More

This work takes inspiration from chemistry where the spectral characteristics of the molecules are determined by hybridization of electronic states evolving from the individual atomic orbitals. Based on analogy between quantum mechanics and the classical electrodynamics, we sorted dielectric microspheres with almost identical positions of their whispering gallery mode (WGM) resonances. Using these microspheres as classical photonic atoms, we assembled them in a wide range of structures including linear chains and planar photonic molecules. Read More

High harmonic generation in the interaction of femtosecond lasers with atoms and molecules opens the path to molecular orbital tomography and to probe the electronic dynamics with attosecond-{\AA}ngstr\"{o}m resolutions. Molecular orbital tomography requires both the amplitude and phase of the high harmonics. Yet the measurement of phases requires sophisticated techniques and represents formidable challenges at present. Read More

The fragmentation dynamics of 2,6- and 3,5-difluoroiodobenzene after iodine 4$d$ inner-shell photoionization with soft X-rays are studied using coincident electron and ion momentum imaging. By analyzing the momentum correlation between iodine and fluorine cations in three-fold ion coincidence events, we can distinguish the two isomers experimentally. Classical Coulomb explosion simulations are in overall agreement with the experimentally determined fragment ion kinetic energies and momentum correlations and point toward different fragmentation mechanisms and time scales. Read More

A robust potential wherein is embedded the crucial core polarization interaction is used in the Regge Pole methodology to calculate low energy electron elastic scattering total cross section (TCS) for the C60 fullerene in the electron impact energy range 0.02 through 10.0 eV. Read More

We report a theoretical analysis showing that Rayleigh scattering could be used to monitor the growth of nanoparticles under arc discharge conditions. We compute the Rayleigh scattering cross sections of the nanoparticles by combining light scattering theory for gas-particle mixtures with calculations of the dynamic electronic polarizability of the nanoparticles. We find that the resolution of the Rayleigh scattering probe is adequate to detect nanoparticles as small as C60 at the expected concentrations of synthesis conditions in the arc periphery. Read More

Morphology and its stability are essential features to address physicochemical properties of metallic nanoparticles. By means of Molecular Dynamics based simulations we show a complex dependence on the size and material of common structural mechanisms taking place in mono-metallic nanoparticles at icosahedral magic sizes. We show that the well known Lipscomb s Diamond Square Diamond mechanisms, single step screw dislocation motions of the whole cluster, take place only below a given size which is material dependent. Read More

We present the results of classical molecular dynamics simulations of collision-induced fusion and fragmentation of C$_{60}$ fullerenes, performed by means of the MBN Explorer software package. The simulations provide information on the structural differences of the fused compound depending on kinematics of the collision process. The analysis of fragmentation dynamics at different initial conditions shows that the size distributions of molecular fragments produced are peaked for dimers, which is in agreement with a well-established mechanism of C$_{60}$ fragmentation via preferential C$_2$ emission. Read More

Tributyl-phosphate (TBP), a ligand used in the PUREX liquid-liquid separation process of spent nuclear fuel, can form explosive mixture in contact with nitric acid, that might lead to violent explosive thermal runaway. In the context of safety of a nuclear reprocessing plant facility, it is crucial to predict the stability of TBP at elevated temperatures. So far, only the enthalpies of formation of TBP is available in the literature with a rather large uncertainties, while those of its degradation products, di-(HDBP) and mono-(H$_2$MBP}) are unknown. Read More

The mechanisms of phase change of argon during picosecond laser internal ablation are studied using molecular dynamics simulations. It is found that propagation of stress wave and fluctuation of temperature are periodical. The phase change process from solid to liquid to supercritical fluid then back to solid occurs as combined results of heating and the propagation of tensile stress wave induced by the laser pulse and the limited internal space. Read More

We present a comprehensive analysis of photon emission and atomic collision processes in two-phase argon doped with xenon and nitrogen. The dopants are aimed to convert the VUV emission of pure Ar to the UV emission of the Xe dopant in the liquid phase and to the near UV emission of the N2 dopant in the gas phase. Such a mixture is relevant to two-phase dark matter and low energy neutrino detectors, with enhanced photon collection efficiency for primary and secondary scintillation signals. Read More

The momentum density, $n(k)$ of interacting many-body Fermionic systems is studied (for $k>k_F)$ using examples of several well-known two-body interaction models. This work shows that $n(k)$ can not be approximated by a zero-range model for momenta $k$ greater than about $1/(a r_e^2)^{1/3}$, where $a$ is the scattering length, and $r_e$ the effective range. However, if the scattering length is large and one includes the effects of a fixed value of $r_e\ne0$, $n(k)$ is universal for momenta $k$ up to about $2/r_e$. Read More

Accurate prediction of the electronic and hydrogen storage properties of linear carbon chains (Cn) and Li-terminated linear carbon chains (Li2Cn), with n carbon atoms (n = 5 - 10), has been very challenging for traditional electronic structure methods, due to the presence of strong static correlation effects. To meet the challenge, we study these properties using our newly developed thermally-assisted-occupation density functional theory (TAO-DFT), a very efficient electronic structure method for the study of large systems with strong static correlation effects. Owing to the alteration of the reactivity of Cn and Li2Cn with n, odd-even oscillations in their electronic properties are found. Read More

The hydration of ions in nanoscale hydrated clusters is ubiquitous and essential in many physical and chemical processes. Here we show that the hydrolysis reaction is strongly affected by relative humidity. The hydrolysis of CO32- with n = 1-8 water molecules is investigated by ab initio method. Read More

Rotation of molecules embedded in He nanodroplets is explored by a combination of fs laser-induced alignment experiments and angulon quasiparticle theory. We demonstrate that at low fluence of the fs alignment pulse, the molecule and its solvation shell can be set into coherent collective rotation lasting long enough to form revivals. With increasing fluence, however, the revivals disappear -- instead, rotational dynamics as rapid as for an isolated molecule is observed during the first few picoseconds. Read More

A novel system containing nanoporous materials and carbonate ions is proposed, which is capable to capture CO2 from ambient air simply by controlling the amount of water (humidity) in the system. The system absorbs CO2 from the air when the surrounding is dry, whereas desorbs CO2 when wet. A design of such a CO2 absorption/desorption system is investigated in this paper using molecular dynamics and quantum mechanics simulations, and also verified by experiments. Read More

We investigate the impact of dissipation on the energy balance in the electron dynamics of metal clusters excited by strong electro-magnetic pulses. The dynamics is described theoretically by Time-Dependent Density-Functional Theory (TDDFT) at the level of Local Density Approximation (LDA) augmented by a self interaction correction term and a quantum collision term in Relaxation-Time Approximation (RTA). We evaluate the separate contributions to the total excitation energy, namely energy exported by electron emission, potential energy due to changing charge state, intrinsic kinetic and potential energy, and collective flow energy. Read More

Structural characterization of metalloporphyrins in complex systems such as native hydrocarbons is in the focus of scientific and industrial interests since many years. We describe electron-nuclear double resonance (ENDOR) of crude oil from the well without any additional sample treatment (i.e. Read More

In this research, we employ time-dependent density functional calculations for photoelectron spectroscopy of nitrogen molecule in short laser pulses. First, the optical absorption spectrum of nitrogen is calculated by using full time propagation and linear response techniques. Then laser pulses with different frequencies, intensities, and lengths are applied to the molecule and the resulting photoelectron spectra are analyzed. Read More

We theoretically analyze angle-resolved photo-electron spectra (ARPES) generated by the interaction of C$_{60}$ with intense, short laser pulses. In particular, we focus on the impact of the carrier-envelope phase (CEP) onto the angular distribution. The electronic dynamics is described by time-dependent density functional theory, and the ionic background of $\csixty$ is approximated by a particularly designed jellium model. Read More

Hydrogen storage by physisorption in carbon based materials is hindered by low adsorption energies. In the last decade doping of carbon materials with alkali, earth alkali or other metal atoms was proposed as a means to enhance adsorption energies, and some experiments have shown promising results. We investigate the upper bounds of hydrogen storage capacities of $C_{60}Cs$ clusters grown in ultracold helium nanodroplets by analyzing anomalies in the ion abundance that indicate shell closure of hydrogen adsorption shells. Read More

The interaction of a helium atom with intense short 800 nm laser pulse is studied theoretically beyond the single-active-electron approximation. For this purpose, the time-dependent Schr\"odinger equation for the two-electron wave packet driven by a linearly-polarized infrared pulse is solved by the time-dependent restricted-active-space configuration-interaction method (TD-RASCI) in the dipole velocity gauge. By systematically extending the space of active configurations, we investigate the role of the collective two-electron dynamics in the strong field ionization and high-order harmonic generation (HHG) processes. Read More

In this contribution I will review some of the researches that are currently being pursued in Padova (mainly within the In:Theory and Strength projects), focusing on the interdisciplinary applications of nuclear theory to several other branches of physics, with the aim of contributing to show the centrality of nuclear theory in the Italian scientific scenario and the prominence of this fertile field in fostering new physics. In particular, I will talk about: i) the recent solution of the long-standing "electron screening puzzle" that settles a fundamental controversy in nuclear astrophysics between the outcome of lab experiments on earth and nuclear reactions happening in stars; the application of algebraic methods to very diverse systems such as: ii) the supramolecular complex H2@C60, i.e. Read More