On the Munn-Silbey approach to polaron transport with off-diagonal coupling

Improved results using a method similar to the Munn-Silbey approach have been obtained on the temperature dependence of transport properties of an extended Holstein model incorporating simultaneous diagonal and off-diagonal exciton-phonon coupling. The Hamiltonian is partially diagonalized by a canonical transformation, and optimal transformation coefficients are determined in a self-consistent manner. Calculated transport properties exhibit substantial corrections on those obtained previously by Munn and Silbey for a wide range of temperatures thanks to a numerically exact evaluation and an added momentum-dependence of the transformation matrix. Results on the diffusion coefficient in the moderate and weak coupling regime show distinct band-like and hopping-like transport features as a function of temperature.Comment: 12 pages, 6 figures, accpeted in Journal of Physical Chemistry B: Shaul Mukamel Festschrift (2011

Symphony on strong field approximation

This paper has been prepared by the Symphony collaboration (University of Warsaw, Uniwersytet Jagiellonski, DESY/CNR and ICFO) on the occasion of the 25th anniversary of the 'simple man's models' which underlie most of the phenomena that occur when intense ultrashort laser pulses interact with matter. The phenomena in question include high-harmonic generation (HHG), above-threshold ionization (ATI), and non-sequential multielectron ionization (NSMI). 'Simple man's models' provide both an intuitive basis for understanding the numerical solutions of the time-dependent Schrodinger equation and the motivation for the powerful analytic approximations generally known as the strong field approximation (SFA). In this paper we first review the SFA in the form developed by us in the last 25 years. In this approach the SFA is a method to solve the TDSE, in which the non-perturbative interactions are described by including continuum-continuum interactions in a systematic perturbation-like theory. In this review we focus on recent applications of the SFA to HHG, ATI and NSMI from multi-electron atoms and from multi-atom molecules. The main novel part of the presented theory concerns generalizations of the SFA to: (i) time-dependent treatment of two-electron atoms, allowing for studies of an interplay between electron impact ionization and resonant excitation with subsequent ionization; (ii) time-dependent treatment in the single active electron approximation of 'large' molecules and targets which are themselves undergoing dynamics during the HHG or ATI processes. In particular, we formulate the general expressions for the case of arbitrary molecules, combining input from quantum chemistry and quantum dynamics. We formulate also theory of time-dependent separable molecular potentials to model analytically the dynamics of realistic electronic wave packets for molecules in strong laser fields. We dedicate this work to the memory of Bertrand Carre, who passed away in March 2018 at the age of 60

Wannier-Bloch Approach to Localization in High-Harmonics Generation in Solids

Emission of high-order harmonics from solids provides a new avenue in attosecond science. On the one hand, it allows us to investigate fundamental processes of the nonlinear response of electrons driven by a strong laser pulse in a periodic crystal lattice. On the other hand, it opens new paths toward efficient attosecond pulse generation, novel imaging of electronic wave functions, and enhancement of high-order harmonic-generation (HHG) intensity. A key feature of HHG in a solid (as compared to the well-understood phenomenon of HHG in an atomic gas) is the delocalization of the process, whereby an electron ionized from one site in the periodic lattice may recombine in any other. Here, we develop an analytic model, based on the localized Wannier wave functions in the valence band and delocalized Bloch functions in the conduction band. This Wannier-Bloch approach assesses the contributions of individual lattice sites to the HHG process and hence precisely addresses the question of localization of harmonic emission in solids. We apply this model to investigate HHG in a ZnO crystal for two different orientations, corresponding to wider and narrower valence and conduction bands, respectively. Interestingly, for narrower bands, the HHG process shows significant localization, similar to harmonic generation in atoms. For all cases, the delocalized contributions to HHG emission are highest near the band-gap energy. Our results pave the way to controlling localized contributions to HHG in a solid crystal

Finite size effects on transport coefficients for models of atomic wires coupled to phonons

We consider models of quasi-1-d, planar atomic wires consisting of several, laterally coupled rows of atoms, with mutually non-interacting electrons. This electronic wire system is coupled to phonons, corresponding, e.g., to some substrate. We aim at computing diffusion coefficients in dependence on the wire widths and the lateral coupling. To this end we firstly construct a numerically manageable linear collision term for the dynamics of the electronic occupation numbers by following a certain projection operator approach. By means of this collision term we set up a linear Boltzmann equation. A formula for extracting diffusion coefficients from such Boltzmann equations is given. We find in the regime of a few atomic rows and intermediate lateral coupling a significant and non-trivial dependence of the diffusion coefficient on both, the width and the lateral coupling. These results, in principle, suggest the possible applicability of such atomic wires as electronic devices, such as, e.g., switches.Comment: 9 pages, 5 figures, accepted for publication in Eur. Phys. J.

Identifying the Azobenzene/Aniline reaction intermediate on TiO2-(110) : a DFT Study

Density functional theory (DFT) calculations, both with and without dispersion corrections, have been performed to investigate the nature of the common surface reaction intermediate that has been shown to exist on TiO2(110) as a result of exposure to either azobenzene (C6H5N═NC6H5) or aniline (C6H5NH2). Our results confirm the results of a previous DFT study that dissociation of azobenzene into two adsorbed phenyl imide (C6H5N) fragments, as was originally proposed, is not energetically favorable. We also find that deprotonation of aniline to produce this surface species is even more strongly energetically disfavored. A range of alternative surface species has been considered, and while dissociation of azobenzene to form surface C6H4NH species is energetically favored, the same surface species cannot form from adsorbed aniline. On the contrary, adsorbed aniline is much the most stable surface species. Comparisons with experimental determinations of the local adsorption site, the Ti–N bond length, the molecular orientation, and the associated C 1s and N 1s photoelectron core level shifts are all consistent with the DFT results for adsorbed aniline and are inconsistent with other adsorbed species considered. Possible mechanisms for the hydrogenation of azobenzene required to produce this surface species are discussed

Exploring CEvNS with NUCLEUS at the Chooz Nuclear Power Plant

Coherent elastic neutrino-nucleus scattering (CE$\nu$NS) offers a unique way to study neutrino properties and to search for new physics beyond the Standard Model. Nuclear reactors are promising sources to explore this process at low energies since they deliver large fluxes of (anti-)neutrinos with typical energies of a few MeV. In this paper, a new-generation experiment to study CE$\nu$NS is described. The NUCLEUS experiment will use cryogenic detectors which feature an unprecedentedly low energy threshold and a time response fast enough to be operated in above-ground conditions. Both sensitivity to low-energy nuclear recoils and a high event rate tolerance are stringent requirements to measure CE$\nu$NS of reactor antineutrinos. A new experimental site, denoted the Very-Near-Site (VNS) at the Chooz nuclear power plant in France is described. The VNS is located between the two 4.25 GW$_{\mathrm{th}}$ reactor cores and matches the requirements of NUCLEUS. First results of on-site measurements of neutron and muon backgrounds, the expected dominant background contributions, are given. In this paper a preliminary experimental setup with dedicated active and passive background reduction techniques is presented. Furthermore, the feasibility to operate the NUCLEUS detectors in coincidence with an active muon-veto at shallow overburden is studied. The paper concludes with a sensitivity study pointing out the promising physics potential of NUCLEUS at the Chooz nuclear power plant