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Optical activity tensor for radiating atomic and molecular systems

The optical activity tensor (OAT) is explicitly derived. It is shown that to evaluate a large number of effects related to optical activity of some atomic/molecular system at arbitrary frequency $ω$ of the incident light, one needs to know only four optical activity tensors which have twelve irreducible (tensor) components. An additional amplification factor contains one $3 \times 3$ tensor of light scattering with three irreducible components. The explicit dependence of all irreducible components of OAT upon $ω$ and some molecular parameters is derived and discussed. We apply OAT to explain the dispersion of optical rotation in dilute solutions of organic molecules. This study opens a new avenue in application of methods of modern Quantum Electrodynamics to the optical activity.

physics.atm-clus↗

Energy absorption of quasineutral plasmas through electronic edge-modes

Ultracold quasineutral plasmas generated in the laboratory are generically inhomogeneous and ex- hibit small charge imbalances. As will be demonstrated, via a hydrodynamic theory as well as microscopic simulations, the latter lead to efficient energy absorption at the plasma boundary. This proposed "edge-mode" is shown to provide a unified explanation for observed absorption spectra measured in different experiments. Understanding the response of the electronic plasma compo- nent to weak external driving is essential since it grants experimental access to the density and temperature of ultracold plasmas.

physics.plasm-ph↗

Complete dynamics of H2+ in strong laser fields

Based on a combined quantum-classical treatment, a complete study of the strong field dynamics of H2+, i.e. including all nuclear and electronic DOF as well as dissociation and ionization, is presented. We find that the ro-vibrational nuclear dynamics enhances dissociation and, at the same time, suppresses ionization, confirming experimental observations by I. Ben-Itzhak et al. [Phys. Rev. Lett. 95, 073002 (2005)]. In addition and counter-intuitively, it is shown that for large initial vibrational excitation ionization takes place favorably at large angles between the laser polarization and molecular axis. A local ionization model delivers a transparent explanation of these findings.

physics.atm-clus↗

Observation of (N2)2 dimers in free nitrogen and argon-nitrogen clusters

Supersonic-jet luminescence spectroscopy was applied to study vibronic transitions in icosahedral N2 and Ar-N2 clusters having from 100 to 400 particles per cluster. In the case of mixed Ar-N2 clusters, the w->X transitions were observed to occur in single N2 molecules in an Ar environment, that is very much in the same way as in Ar-N2 bulk samples. In N2 clusters, however, a band series was detected which was never observed earlier. In the spectra of Ar-N2 clusters, this new series coexisted with the 'bulk' w->X transitions. Our analysis demonstrated that the series should be assigned to emission of van der Waals (N2)2 dimers from inside clusters. Earlier, such dimers were only observed in molecular beams and gaseous nitrogen, this paper reports their observation in the solid phase of nitrogen suggesting that they may be the basic building blocks of small N2 clusters. Our results can be of interest from the viewpoint of producing polymeric nitrogen since (N2)2 dimers can be considered to be a starting species for its synthesis.

physics.atm-clus↗

Atomic fragments from the nuclear reaction of the ${}^{6}$Li atom with slow neutrons

Approximate probabilities of formation of various atoms and ions in different bound states are determined for the exothermic nuclear $(n,{}^{6}$Li$;t,{}^{4}$He)-reaction of atomic lithium-6 with slow neutrons. In our calculations of the final state probabilities we have assumed that the incident lithium atom is in its ground (doublet) atomic ${}^2S(L = 0)-$state. It is straightforward to generalize our analysis to other bound states of the three-electron Li atom.

physics.atom-ph↗

Revisiting Zeno's paradox: Flying arrows for atom-diatom reactions

The possibility to observe quantum Zeno and anti-Zeno scenarios for atom-diatom reactive collisions is investigated for two diferent processes (F+HD and H+O_2) by means of time-dependent wave packet propagations. A novel approach is proposed in which the survival probabilities investigated are those obtained when the initial state is redefined after time intervals tau at which measurements are performed on the system. The comparison with the actual probability for the unperturbed system reveals the existence of a regime in which the decay from the initial state appears to be inhibited (the quantum Zeno effect) or accelerated (the anti-Zeno effect). In contrast with preceding interpretations, given that the time-evolving wave packet is not affected at any time ("flying arrow"), the present procedure does not require to invoke to counterintuitive hindered evolutions ("stopping arrow") to explain the results. On the contrary the consecutive update of the reference state of the system solves the apparent modern version of Zeno's paradox.

physics.chem-ph↗

Velocity distribution of neutral particles ejected from biological material under ultra short laser radiation

Neutral particles ejected from biological material under ultra short laser ablation have been investigated by laser post-ionization time-of-flight mass spectrometry. It could be shown, that beside ionized species, a substantial amount of neutral particles is ejected. A temporal study of the ablation plume is carried out by recording neutral particle time-of- flight mass spectra as a function of delay time between the ablation and post-ionization pulse. Close the ablation threshold, the mechanism of ejection is found to be of predominantely mechanical nature, driven by the relaxation of the laser-induced pressure. In this regime of stress confinement, the ejection results in very broad velocity distributions and extremely low velocities.

physics.bio-ph↗

Phase-Controlled Atom-Photon Entanglement in a Three-Level lambda-Type Closed-Loop Atomic System

The atom-photon entanglement is studied in a three-level lambda-type closed-loop atomic system in multi-photon resonance condition and beyond it. It is shown that the von Neumann entropy in such a system is phase dependent, and it can be controlled by either intensity or relative phase of applied fields. It is demonstrated that for the special case of Rabi frequency of applied fields, the system is disentangled.

physics.atm-clus↗

Phase-controlled transparent superluminal light propagation in a Doppler-broadened four-level N-type system

The propagation of a weak probe field in a four-level N-type quantum system in the presence of spontaneously generated coherence (SGC) is theoretically investigated. The optical properties of the system are studied and it is shown that the group velocity of light pulse can be controlled by relative phase of applied fields. By changing the relative phase of applied fields, the group velocity of light pulse changes from transparent subluminal to the transparent superluminal light propagation. Thus, the phase-controlled absorption-free superluminal light propagation is obtained without applying an incoherent laser fields to the system. The propagation of a weak probe light pulse is studied by solving the Maxwell's wave equation on numerical grid in space and time. Moreover, we study the third order self- and cross-Kerr susceptibility of probe field and calculate the nonlinear cross-phase shift for different values of intensity of applied fields. In addition, we take into account the effect of Doppler broadening on the light pulse propagation and it is found that a suitable choice of laser propagation directions allows us to preserve our results even in the presence of Doppler effect. It is demonstrated that by increasing the Doppler width of distribution to the room temperature, the dispersion changes from transparent subluminal to transparent superluminal light propagation which is our major motivation for this work.

physics.atm-clus↗

Effect of Ni on Cu precipitation kinetics in α-Fe by AKMC study

The kinetics of coherent Cu rich precipitation in Fe-Cu and Fe-Cu-Ni alloys during thermal ageing have been modeled by Atomic Kinetic Monte Carlo method (AKMC). The AKMC is parameterized by existing ab-inito data to treat vacancy mediated diffusion which is depend on local atomic environment. A nonlinear semi-empirical time adjusting method is proposed to rescaled the MC time. The combining AKMC and time adjusting method give a good agreement with experiments and other simulations, including advancement factor and the Cu cluster mobility. Simulations of ternary alloys reveal Ni has a temporal delay effect on Cu precipitation. This effect is caused by the decreasing of diffusion coefficient of Cu clusters. And the reduction effect of diffusion coefficient weakens with larger Cu cluster size. The simulation results can be used to explain the experimental phenomenon that ternary Fe-Cu-Ni alloys have higher cluster number density than corresponding binary during coarsening stage, which is related to cluster mobility.

cond-mat.mtrl-sci↗

Raman and non Raman EIT resonances in a degenerate four level system

We study coherence effects in an atom having three metastable levels and single life-time broadened upper state. Two laser fields couple ground states to an excited one and an radio-frequency (rf) field operates between ground state levels. We consider the case when the common level for the rf-field and one of the laser field (to which we refer as the probing field) transitions is twice degenerate. We predict a novel type of dark states (we call them non Raman dark states), which in contrary to Raman resonances, do not require the fulfillment of the two-photon resonance condition. We realize the configuration in the atomic hydrogen and show that non Raman resonances are determined by the geometry of the rf and probing field's polarizations. For ultra-cold atoms non Raman resonances arise when the polarization vectors of the fields are parallel or perpendicular to each other. For an atomic gas at room temperatures electromagnetically induced transparency (EIT) resonances associated with Raman and non Raman dark states are studied by taking into account spin-exchange relaxation in the ground state of the hydrogen atom. We establish properties of non Raman dark states by investigating the relation of EIT resonances to the polarization geometry.

quant-ph↗

Complex-Scaling Calculation of Three-Body Resonances Using Complex-Range Gaussian Basis Functions --- Application to 3$α$ resonances in 12C ---

We propose to use the complex-range Gaussian basis functions, {r^l e^{-(1 \pm iω)(r/r_n)^2}Y_{lm}(\hat{r}); r_n in a geometric progression}, in the calculation of three-body resonances with the complex-scaling method (CSM) in which use is often made of the real-range Gaussian basis functions, {r^l e^{-(r/r_n)^2}Y_{lm}(\hat{r})}, that are suitable for describing the short-distance structure and the asymptotic decaying behavior of few-body systems. The former basis set is more powerful than the latter when describing the resonant and nonresonant continuum states with highly oscillating amplitude at large scaling angles θ. We applied the new basis functions to the CSM calculation of the 3αresonances with J=0^+, 2^+ and 4^+ in 12C. The eigenvalue distribution of the complex scaled Hamiltonian becomes more precise and the maximum scaling angle becomes drastically larger (θ_{max}=16 deg. \arrow 36 deg.) than those given by the use of the real-range Gaussians. Owing to these advantages, we were able to confirm the prediction by Kurokawa and Kato [Phys. Rev. C 71, 021301 (2005)] on the appearance of the new broad 0^+_3 state; we show it as an explicit resonance pole isolated from the 3$α$ continuum.

nucl-th↗

Manipulation of a continuous beam of molecules by light pulses

We experimentally observe the action of multiple light pulses on the transverse motion of a continuous beam of fullerenes. The light potential is generated by non-resonant ultra-short laser pulses in perpendicular spatial overlap with the molecule beam. We observe a small but clear enhancement of the number of molecules in the center fraction of the molecular beam. Relatively low light intensity and short laser pulse duration prevent the molecule from fragmentation and ionization. Experimental results are confirmed by Monte Carlo trajectory simulations.

physics.atm-clus↗

Nanodiamond Collective Electron States and their Localization

The existence and localization of collective electron states for nanodiamond particles were studied both by solving a one-particle one-dimensional Schrödinger equation in the Kronig-Penney potential and by ab initio computations of ground state wavefunctions of diamondoids C78H64, C123H100 and C211H140 at the DFT R-B3LYP/6-31G(d,p) level of theory. Three distinct classes of collective electron states have been found: collective bonding orbitals resembling the morphology of 3D-modulated particle in a box solutions; surface-localized non-bonding conductive Tamm states and subsurface-localized bonding states for non-uniformly compressed nanodiamond. Quantum-mechanical analysis shows that collective unpaired electrons are intrinsic to nanodiamond. Their subsurface localization is described in terms of surface compression arising from a self-consistency condition of the electron-nuclear wavefunction. Intrinsic spin existence is supposed to result from the collective and spread nature of subsurface orbitals, allowing spin-density fluctuation effects to become significant on this length scale. Suggested model allows to explain free spins of nanodiamond exhibited in experiments.

cond-mat.mtrl-sci↗

Low-energy electron holographic imaging of gold nanorods supported by ultraclean graphene

An ideal support for electron microscopy shall be as thin as possible and interact as little as possible with the primary electrons. Since graphene is atomically thin and made up of carbon atoms arranged in a honeycomb lattice, the potential to use graphene as substrate in electron microscopy is enormous. Until now graphene has hardly ever been used for this purpose because the cleanliness of freestanding graphene before or after deposition of the objects of interest was insufficient. We demonstrate here by means of low-energy electron holographic imaging that freestanding graphene prepared with the Platinum-metal catalysis method remains ultraclean even after re-exposure to ambient conditions and deposition of gold-nanorods from the liquid phase. In the holographic reconstruction of the gold particles the organic shell surrounding the objects is imaged while it is not detectable in SEM images of the very same sample, demonstrating the tremendous potential of low-energy electron holography for the imaging of graphene-supported single biomolecules.

cond-mat.mtrl-sci↗

Charge-transfer from Regularized Symmetry-Adapted Perturbation Theory

The charge-transfer (CT) together with the polarization energy appears at second and higher orders in symmetry-adapted perturbation theory (SAPT). At present there is no theoretically compelling way of isolating the charge-transfer energy that is simultaneously basis-set independent and applicable for arbitrary intermolecular separation. We argue that the charge-transfer can be interpreted as a tunneling phenomenon, and can therefore be defined via regularized SAPT. This leads to a physically convincing, basis-independent definition of the charge-transfer energy that captures subtleties of the process, such as the asymmetry in the forward and backward charge transfer, as well as secondary transfer effects. With this definition of the charge-transfer the damping needed for polarization models can be determined with a level of confidence hitherto not possible.

physics.chem-ph↗

Spin Dynamics in Graphene and Graphene like Nanocarbon Doped with Nitrogen the ESR Analysis

Nano engineered spin degree of freedom in carbon system may offer desired exchange coupling with optimum spin orbit interaction which is essential, to construct solid state qubits, for fault tolerant quantum computation. The purpose of this communication is to analyze spin dynamics of, basically, four types of systems, (i) Graphene (system with inversion symmetry), (ii) Graphene like nanocarbons (GNCs, broken inversion symmetry and heterostructure, sp2 and sp3, environment), and (iii) their nitrogen doped derivatives. The spin transport data was obtained using the electron spin resonance spectroscopy (ESR) technique, carried out over 123 to 473K temperature range. Analysis of shape, linewidths of dispersion derivatives,, and g factor anisotropy has been carried out. Spin parameters such as, spin spin relaxation time, spin lattice relaxation time, spin flip parameter,spin relaxation rate,spin, momentum relaxation rate,pseudo chemical potential, density of states, effective magnetic moment, spin concentration, defect concentration, and Pauli susceptibility, has been estimated, and examined for their temperature as well as interdependence. Details of the analysis are presented. The quantitative study underlined the following facts: (i) by and large, spin dynamics in Graphene and GNCs is significantly different, (ii) transport of spin behaves in opposite fashion, after doping nitrogen, in both the systems, (iii) reduction in the magnetization has been observed for both GNCs and Graphene, after doping nitrogen, (iv) hyperfine interactions have been observed in all classes of systems except in GNCs, (v) nitrogen doped GNCs seems to be appropriate for qubit designing.

physics.atm-clus↗

{\it K}-Shell Photoionization of Be-like and Li-like Ions of Atomic Nitrogen: Experiment and Theory

Absolute cross sections for the {\it K}-shell photoionization of Be-like and Li-like atomic nitrogen ions were measured by employing the ion-photon merged-beam technique at the SOLEIL synchrotron radiation facility in Saint-Aubin, France. High-resolution spectroscopy at nominal resolutions of 38 meV, 56 meV, 111 meV, 133 meV FWHM for Be-like and 125 meV FWHM for Li-like atomic nitrogen ions was achieved for the photon energies ranging from 410 eV up to 460 eV. The experimental measurements are compared with theoretical estimates from the multi-configuration Dirac-Fock (MCDF), R-matrix and an empirical method. The interplay between experiment and theory enabled the identification and characterisation of the strong 1s $\rightarrow$ 2p resonances features observed in the {\it K}-shell spectra of each ion and the region around 460 eV for the 1s $\rightarrow$ 3p resonance of the N$^{3+}$ ion yielding suitable agreement with experiment.

physics.atom-ph↗