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At least 145 records · Page 8Linked to original sources

arXiv2014

Exchange interaction between the triplet exciton and the localized spin in copper-phthalocyanine

Triplet excitonic state in the organic molecule may arise from a singlet excitation and the following inter-system crossing. Especially for a spin-bearing molecule, an exchange interaction between the triplet exciton and the original spin on the molecule can be expected. In this paper, such exchange interaction in copper-phthalocyanine (CuPc, spin-$\frac{1}{2}$) was investigated from first-principles by using density-functional theory within a variety of approximations to the exchange correlation, ranging from local-density approximation to long-range corrected hybrid-exchange functional. The magnitude of the computed exchange interaction is in the order of meV with the minimum value (1.5 meV, ferromagnetic) given by the long-range corrected hybrid-exchange functional CAM-B3LYP. This exchange interaction can therefore give rise to a spin coherence with an oscillation period in the order of picoseconds, which is much shorter than the triplet lifetime in CuPc (typically tens of nanoseconds). This implies that it might be possible to manipulate the localised spin on Cu experimentally using optical excitation and inter-system crossing well before the triplet state disappears.

quant-ph↗

arXiv2018

Resonant electron attachment to mixed hydrogen/oxygen and deuterium/oxygen clusters

Low energy electron attachment to mixed (H$_2$)$_x$/(O$_2$)$_y$ clusters and their deuterated analogues has been investigated for the first time. These experiments were carried out using liquid helium nanodroplets to form the clusters, and the effect of the added electron was then monitored via mass spectrometry. There are some important differences between electron attachment to the pure clusters and to the mixed clusters. A particularly notable feature is the formation of HO$_2$$^{-}$ and H$_2$O$^{-}$ ions from an electron-induced chemical reaction between the two dopants. The chemistry leading to these anions appears to be driven by electron resonances associated with H$_2$ rather than O$_2$. The electron resonances for H$_2$ can lead to dissociative electron attachment (DEA), just as for the free H$_2$ molecule. However, there is evidence that the resonance in H$_2$ can also lead to rapid electron transfer to O$_2$, which then induces DEA of the O$_2$. This kind of excitation transfer has not, as far as we are aware, been reported previously

physics.atm-clus↗

arXiv2018

General theory of photoexcitation induced photoelectron circular dichroism

The photoionization of chiral molecules prepared in a coherent superposition of excited states can give access to the underlying chiral coherent dynamics in a procedure known as photoexcitation induced photoelectron circular dichroism (PXECD). This exclusive dependence on coherence can also be seen in a different part of the angular spectrum, where it is not contingent on the chirality of the molecule, thus allowing extension of PXECD's sensitivity to tracking coherence to non-chiral molecules. Here we present a general theory of PXECD based on angular momentum algebra and derive explicit expressions for all pertinent asymmetry parameters which arise for arbitrary polarisation of pump and probe pulses. The theory is developed in a way that clearly and simply separates chiral and non-chiral contributions to the photoelectron angular distribution, and also demonstrates how PXECD and PECD-type contributions, which may be distinguished by whether pump or ionizing probe enables chiral response, are mixed when arbitrary polarization is used.

physics.atm-clus↗

arXiv2018

Time-resolved double-resonance spectroscopy: Lifetime measurement of the $6\,^1Σ_g^+(7,31)$ electronic state of molecular sodium

We report on the lifetime measurement of the $6\,^1Σ_g^+ (7,31)$ state of Na$_2$ molecules, produced in a heat-pipe oven, using a time-resolved spectroscopic technique. The $6\,^1Σ_g^+ (7,31)$ level was populated by two-step two-color double resonance excitation via the intermediate $A\,^1Σ_u^+ (8,30)$ state. The excitation scheme was done using two synchronized pulsed dye lasers pumped by a Nd:YAG laser operating at the second harmonics. The fluorescence emitted upon decay to the final state was measured using a time-correlated photon counting technique, as a function of argon pressure. From this the radiative lifetime was extracted by extrapolating the plot to collision-free zero pressure. We also report calculated radiative lifetimes of the Na$_2$ $6\,^1Σ_g^+$ ro-vibrational levels in the range of $v=0-200$ with $J=1$ and $J=31$ using the LEVEL program for bound-bound and the BCONT program for bound-free transitions. Our calculations reveal the importance of the bound-free transitions on the lifetime calculations and a large difference of about a factor of three between the $J=1$ and $J=31$ for the $v=40$ and $v=100$, due to the wavefunction alternating between having predominantly inner and outer well amplitude.

physics.chem-ph↗

arXiv2017

Infrared observation of OC-C2H2, OC-(C2H2)2 and their isotopologues

The fundamental band for the OC-C2H2 dimer and two combination bands involving the intermolecular bending modes nu9 and nu8 in the carbon monoxide CO stretch region are re-examined. Spectra are obtained using a pulsed supersonic slit jet expansion probed with a mode-hop free tunable infrared quantum cascade laser. Analogous bands for OC-C2D2 and the fundamental for OC-DCCH as an impurity are also observed and analysed. A much weaker band in the same spectral region is assigned to a new mixed trimer, CO-(C2H2)2. The trimer band is composed uniquely of a-type transitions, establishing that the CO monomer is nearly aligned with the a-inertial axis. The observed rotational constants agree well with ab initio calculations and a small inertial defect value indicates that the trimer is planar. The structure is a compromise between the T-shaped structure of free acetylene dimer and the linear geometry of free OC-C2H2. A similar band for the fully deuterated isotopologue CO-(C2D2)2 confirms our assignment.

physics.atm-clus↗

arXiv2018

First principles absorption spectra of Au nanoparticles: from quantum to classical

Absorption cross-section spectra for gold nanoparticles were calculated using fully quantum Stochastic Density Functional Theory and a classical Finite-Difference Time Domain (FDTD) Maxwell solver. Spectral shifts were monitored as a function of size (1.3-3.1 nm) and shape (octahedron, cubeoctahedron, and truncated cube). Even though the classical approach is forced to fit the quantum TDDFT at 3.1nm, at smaller sizes there is a significant deviation as the classical theory is unable to account for peak splitting and spectral blue shifts even after quantum spectral corrections. We attribute the failure of classical methods at predicting these features to quantum effects and low density of states in small nanoparticles. Classically, plasmon resonances are modeled as collective conduction electron excitations, but at small nanoparticle size these excitations transition to few or even individual conductive electron excitations, as indicated by our results.

physics.atm-clus↗

arXiv2013

Formation of silicon oxide grains at low temperature

The formation of grains in the interstellar medium, i.e., at low temperature, has been proposed as a possibility to solve the lifetime problem of cosmic dust. This process lacks a firm experimental basis, which is the goal of this study. We have investigated the condensation of SiO molecules at low temperature using neon matrix and helium droplet isolation techniques. The energies of SiO polymerization reactions have been determined experimentally with a calorimetric method and theoretically with calculations based on the density functional theory. The combined experimental and theoretical values have revealed the formation of cyclic (SiO)$_k$ ($k$ = 2--3) clusters inside helium droplets at $T$ = 0.37 K. Therefore, the oligomerization of SiO molecules is found to be barrierless and is expected to be fast in the low-temperature environment of the interstellar medium on the surface of dust grains. The incorporation of numerous SiO molecules in helium droplets leads to the formation of nanoscale amorphous SiO grains. Similarly, the annealing and evaporation of SiO-doped Ne matrices lead to the formation of solid amorphous SiO on the substrate. The structure and composition of the grains were determined by infrared absorption spectroscopy, transmission electron microscopy, and energy-dispersive X-ray spectroscopy. Our results support the hypothesis that interstellar silicates \textbf{can be formed} in the low temperature regions of the interstellar medium by accretion through barrierless reactions.

astro-ph.GA↗

arXiv2014

Formation of classical crystals of dipolar particles in a helical geometry

We consider crystal formation of particles with dipole-dipole interactions that are confined to move in a one-dimensional helical geometry with their dipole moments oriented along the symmetry axis of the confining helix. The stable classical lowest energy configurations are found to be chain structures for a large range of pitch-to-radius ratios for relatively low density of dipoles and a moderate total number of particles. The classical normal mode spectra support the chain interpretation both through structure and the distinct degeneracies depending discretely on the number of dipoles per revolution. A larger total number of dipoles leads to a clusterization where the dipolar chains move closer to each other. This implies a change in the local density and the emergence of two length scales, one for the cluster size and one for the inter-cluster distance along the helix. Starting from three dipoles per revolution, this implies a breaking of the initial periodicity to form a cluster of two chains close together and a third chain removed from the cluster. This is driven by the competition between in-chain and out-of-chain interactions, or alternatively the side-by-side repulsion and the head-to-tail attraction in the system. The speed of sound propagates along the chains. It is independent of the number of chains although depending on geometry.

cond-mat.quant-gas↗

arXiv2018

Medium-sized Sin- (n=14-20) clusters: a combined study of photoelectron spectroscopy and DFT calculations

Size-selected anionic silicon clusters, Sin- (n=14-20), have been investigated by photoelectron spectroscopy and density functional theory (DFT) calculations. Low-energy structures of the clusters are globally searched for by using a genetic algorithm based on DFT calculations. The electronic density of states and VDEs have been simulated by using ten DFT functionals and compared to the experimental results. We systematically evaluated the DFT functionals for the calculation of the energetics of silicon clusters. CCSD(T) single-point energies based on MP2 optimized geometries for selected isomers of Sin- are also used as benchmark for the energy sequence. The HSE06 functional with aug-cc-pVDZ basis set is found to show the best performance. Our global minimum search corroborates that most of the lowest-energy structures of Sin- (n=14-20) clusters can be derived from assembling tricapped trigonal prisms (TTP) in various ways. For most sizes previous structures are confirmed, whereas for Si20- a new structure has been found.

physics.atm-clus↗

arXiv2013

Quantum-classical hybrid dynamics - a summary

A summary of a recently proposed description of quantum-classical hybrids is presented, which concerns quantum and classical degrees of freedom of a composite object that interact directly with each other. This is based on notions of classical Hamiltonian mechanics suitably extended to quantum mechanics.

quant-ph↗

arXiv2012

About disposition of energy levels

The unique properties of central potential of the form $-βe^{-r}r^γ$ were studied using the recently developed critical parameter technique. The particular cases of $γ=0$ and $γ=-1$ yield, respectively, the exponential and Yukawa potentials widely used in the atomic, molecular and nuclear physics. We found different behavior of the energy levels of this potential for three different ranges of the value of $γ$. For $γ\geq0$ it was found that the energy of bound states with the same principal quantum number $N$ decreases with increasing angular momentum $\ell$. The Gaussian and Woods-Saxon potentials also show this behavior. On the contrary, for $-2\leqγ\leq-1$ increasing $\ell$ gives a higher energy, resembling the Hulthen potential. However, a potential with $-1<γ<0$ possesses mixed properties, which give rise to several interesting results. For one, the order of energy levels with different quantum numbers is not preserved when varying the parameter $β$. This leads to a quantum degeneracy of the states, and in fact, for a given value of $γ$ we can find the values $β_{thr}$ for which two energy levels with different quantum numbers coincide. Another interesting phenomena is the possibility, for some values of $γ$ in this range, for two new energy levels with different quantum numbers to appear simultaneously when $β$ reaches their common critical value.

physics.comp-ph↗

arXiv2014

Do cement nanoparticles exist in space ?

The calcium-silicate-hydrate is used to model properties of cement on Earth. We study cementitious nanoparticles and propose these structures as components of cosmic dust grains. Quantum density functional theory methods are applied for the calculation of infrared spectra of Ca4Si4O14H4, Ca6Si3O13H2, and Ca12Si6O26H4 clusters. We find bands distributed over the near, mid and far-infrared region. A specific calcium-silicate-hydrate spectral feature at 14 microns, together with the bands at 10 and 18 microns which exist for other silicates as well, could be used for a detection of cosmic cement. We compare calculated bands with the 14 microns features in the spectra of HD 45677, HD 44179, and IRC+10420 which were observed by Infrared Space Observatory and classified as remaining. High abundance of oxygen atoms in cementitious nanoparticles could partially explain observed depletion of this element from the interstellar medium into dust grains.

astro-ph.SR↗

arXiv2022

Dynamical preparation of an atomic condensate in a Hofstadter band

The creation of a Hamiltonian in the quantum regime which has non-trivial topological features is a central goal of the cold-atom community, enabling widespread exploration of novel phases of quantum matter. A general scheme to synthesize such Hamiltonians is based on dynamical modulation of optical lattices which thereby generate vector potentials. At the same time the modulation can lead to heating and serious difficulties with equilibration. Here we show that these challenges can be overcome by demonstrating how a Hofstadter Bose-Einstein condensate (BEC) can be dynamically realized, using experimental protocols. From Gross-Pitaevskii simulations our study reveals a complex, multistage evolution; this includes a chaotic intermediate "heating" stage followed by a spontaneous reentrance to the BEC. The observed behavior is reminiscent of evolution in cosmological models.

cond-mat.quant-gas↗

arXiv2005

Two-Photon Excitation of Low-Lying Electronic Quadrupole States in Atomic Clusters

A simple scheme of population and detection of low-lying electronic quadrupole modes in free small deformed metal clusters is proposed. The scheme is analyzed in terms of the TDLDA (time-dependent local density approximation) calculations. As test case, the deformed cluster $Na^+_{11}$ is considered. Long-living quadrupole oscillations are generated via resonant two-photon (two-dipole) excitation and then detected through the appearance of satellites in the photoelectron spectra generated by a probe pulse. Femtosecond pump and probe pulses with intensities $I = 2\cdot 10^{10} - 2\cdot 10^{11} W/cm^2$ and pulse duration $T = 200 - 500$ fs are found to be optimal. The modes of interest are dominated by a single electron-hole pair and so their energies, being combined with the photoelectron data for hole states, allow to gather new information about mean-field spectra of valence electrons in the HOMO-LUMO region. Besides, the scheme allows to estimate the lifetime of electron-hole pairs and hence the relaxation time of electronic energy into ionic heat.

physics.atm-clus↗

arXiv2013

Multiphoton-double-ionization probability linearly depends on laser intensity: Experimental studies of barium

Despite inherently complex multiphoton dynamics, our observations show that Ba double ionization with an infrared laser (8800-8920 cm^{-1}) resembles a single-photon process; namely, its probability is proportional to the laser intensity. In this regime, single-electron ionization is due to a four-photon resonant transition through the highly perturbed state 6p^2 1D_2, whereas double ionization is realized by the two-electron mechanism. Furthermore, we argue that these conclusions are valid for other alkaline-earth-metal atoms and other parameters of laser radiation.

physics.atom-ph↗

arXiv2013

Ion impact induced Interatomic Coulombic Decay in neon and argon dimers

We investigate the contribution of Interatomic Coulombic Decay induced by ion impact in neon and argon dimers (Ne$_2$ and Ar$_2$) to the production of low energy electrons. Our experiments cover a broad range of perturbation strengths and reaction channels. We use 11.37 MeV/u S$^{14+}$, 0.125 MeV/u He$^{1+}$, 0.1625 MeV/u He$^{1+}$ and 0.150 MeV/u He$^{2+}$ as projectiles and study ionization, single and double electron transfer to the projectile as well as projectile electron loss processes. The application of a COLTRIMS reaction microscope enables us to retrieve the three-dimensional momentum vectors of the ion pairs of the fragmenting dimer into Ne$^{q+}$/Ne$^{1+}$ and Ar$^{q+}$/Ar$^{1+}$ (q = 1, 2, 3) in coincidence with at least one emitted electron.

physics.atm-clus↗

arXiv2013

Revisiting the physics of Fano resonances for nanoparticle oligomers

We present a new and robust approach for interpreting the physics of Fano resonances in planar oligomer structures of both metallic and dielectric nanoparticles. We reveal a key mechanism for Fano resonances by demonstrating that such resonances can be generated purely from the interference of nonorthogonal collective eigenmodes, which are clearly identified based on the coupled-dipole approximation. We prove analytically a general theorem to identify the number of collective eigenmodes that can be excited in ring-type nanoparticle oligomers and further demonstrate that no dark mode excitation is necessary for existence of Fano resonances in symmetric oligomers. As a consequence, we unify the understanding of Fano resonances for both plasmonic and all-dielectric oligomers.

physics.optics↗

arXiv2013

Dynamically corrected gates for qubits with always-on Ising couplings: Error model and fault-tolerance with the toric code

We describe how a universal set of dynamically-corrected quantum gates can be implemented using sequences of shaped decoupling pulses on any qubit network forming a sparse bipartite graph with always-on Ising interactions. These interactions are constantly decoupled except when they are needed for two-qubit gates. We analytically study the error operators associated with the constructed gates up to third order in the Magnus expansion, analyze these errors numerically in the unitary time evolution of small qubit clusters, and give a bound on high-order errors for qubits on a large square lattice. We prove that with a large enough toric code the present gate set can be used to implement a fault-tolerant quantum memory.

quant-ph↗