Can optical spectroscopy directly elucidate the ground state of C20?

The optical response of the lowest energy members of the C20 family is calculated using time-dependent density functional theory within a real-space, real-time scheme. Significant differences are found among the spectra of the different isomers, and thus we propose optical spectroscopy as a tool for experimental investigation of the structure of these important clusters.Comment: 11 pages, 2 figures. To be published in J. Chem. Phy

Nonextensive thermodynamic functions in the Schr\"odinger-Gibbs ensemble

Schr\"odinger suggested that thermodynamical functions cannot be based on the gratuitous allegation that quantum-mechanical levels (typically the orthogonal eigenstates of the Hamiltonian operator) are the only allowed states for a quantum system [E. Schr\"odinger, Statistical Thermodynamics (Courier Dover, Mineola, 1967)]. Different authors have interpreted this statement by introducing density distributions on the space of quantum pure states with weights obtained as functions of the expectation value of the Hamiltonian of the system. In this work we focus on one of the best known of these distributions, and we prove that, when considered in composite quantum systems, it defines partition functions that do not factorize as products of partition functions of the noninteracting subsystems, even in the thermodynamical regime. This implies that it is not possible to define extensive thermodynamical magnitudes such as the free energy, the internal energy or the thermodynamic entropy by using these models. Therefore, we conclude that this distribution inspired by Schr\"odinger's idea can not be used to construct an appropriate quantum equilibrium thermodynamics.Comment: 32 pages, revtex 4.1 preprint style, 5 figures. Published version with several changes with respect to v2 in text and reference

The interplay between double exchange, super-exchange, and Lifshitz localization in doped manganites

Considering the disorder caused in manganites by the substitution of Mn by Fe or Ga, we accomplish a systematic study of doped manganites begun in previous papers. To this end, a disordered model is formulated and solved using the Variational Mean Field technique. The subtle interplay between double exchange, super-exchange, and disorder causes similar effects on the dependence of T_C on the percentage of Mn substitution in the cases considered. Yet, in La$_{2/3}$Ca$_{1/3}$Mn$_{1-y}$Ga$_y$O$_3$ our results suggest a quantum critical point (QCP) for $y\approx 0.1-0.2$, associated to the localization of the electronic states of the conduction band. In the case of La$_x$Ca$_x$Mn$_{1-y}$Fe$_y$O$_3$ (with $x=1/3,3/8$) no such QCP is expected.Comment: 6 pages + 3 postscript figures. Largely extended discussio

Statistics and Nos\'e formalism for Ehrenfest dynamics

Quantum dynamics (i.e., the Schr\"odinger equation) and classical dynamics (i.e., Hamilton equations) can both be formulated in equal geometric terms: a Poisson bracket defined on a manifold. In this paper we first show that the hybrid quantum-classical dynamics prescribed by the Ehrenfest equations can also be formulated within this general framework, what has been used in the literature to construct propagation schemes for Ehrenfest dynamics. Then, the existence of a well defined Poisson bracket allows to arrive to a Liouville equation for a statistical ensemble of Ehrenfest systems. The study of a generic toy model shows that the evolution produced by Ehrenfest dynamics is ergodic and therefore the only constants of motion are functions of the Hamiltonian. The emergence of the canonical ensemble characterized by the Boltzmann distribution follows after an appropriate application of the principle of equal a priori probabilities to this case. Once we know the canonical distribution of a Ehrenfest system, it is straightforward to extend the formalism of Nos\'e (invented to do constant temperature Molecular Dynamics by a non-stochastic method) to our Ehrenfest formalism. This work also provides the basis for extending stochastic methods to Ehrenfest dynamics.Comment: 28 pages, 1 figure. Published version. arXiv admin note: substantial text overlap with arXiv:1010.149

The IsoDAR high intensity H2+ transport and injection tests

This technical report reviews the tests performed at the Best Cyclotron Systems, Inc. facility in regards to developing a cost effective ion source, beam line transport system, and acceleration system capable of high H[subscript 2][superscript +] current output for the IsoDAR (Isotope Decay At Rest) experiment. We begin by outlining the requirements for the IsoDAR experiment then provide overviews of the Versatile Ion Source (VIS), Low Energy Beam Transport (LEBT) system, spiral inflector, and cyclotron. The experimental measurements are then discussed and the results are compared with a thorough set of simulation studies. Of particular importance we note that the VIS proved to be a reliable ion source capable of generating a large amount of H[subscript 2][superscript +] current. The results suggest that with further upgrades, the VIS could potentially be a suitable candidate for IsoDAR. The conclusion outlines the key results from our tests and introduces the forthcoming work this technical report has motivated.National Science Foundation (U.S.) (PHY-1148134)Massachusetts Institute of Technology (Seed Fund)Massachusetts Institute of Technology (Bose Fellowship

Ab Initio Molecular Dynamics on the Electronic Boltzmann Equilibrium Distribution

We prove that for a combined system of classical and quantum particles, it is possible to write a dynamics for the classical particles that incorporates in a natural way the Boltzmann equilibrium population for the quantum subsystem. In addition, these molecular dynamics do not need to assume that the electrons immediately follow the nuclear motion (in contrast to any adiabatic approach), and do not present problems in the presence of crossing points between different potential energy surfaces (conical intersections or spin-crossings). A practical application of this molecular dynamics to study the effect of temperature in molecular systems presenting (nearly) degenerate states - such as the avoided crossing in the ring-closure process of ozone - is presented.Comment: published in New J. Phy