04441 Abstracts Collection -- Mobile Information Management

From 24.10.04 to 29.10.04, the Dagstuhl Seminar 04441 ``Mobile Information Management\u27\u27 was held in the International Conference and Research Center (IBFI), Schloss Dagstuhl. During the seminar, several participants presented their current research, and ongoing work and open problems were discussed. Abstracts of the presentations given during the seminar as well as abstracts of seminar results and ideas are put together in this paper. The first section describes the seminar topics and goals in general. Links to extended abstracts or full papers are provided, if available

Using Permuted States of Validated Simulation to Analyze Conflict Rates in Optimistic Replication

Optimistic replication provides high data availability in the presence of network outages. Although widely deployed, this relaxed consistency model introduces concurrent updates, whose behavior is poorly understood due to the vast state space. This paper introduces the notion of permuted states to eliminate system states that are redundant and unreachable, which can constitute the majority of states (4069 out of 4096 for four replicas). With the aid of permuted states, we are for the first time able to construct analytical models beyond the two-replica case. By examining the analysis for 2 to 4 replicas, we can demystify the process of forming identical conflicts—the most common conflict type at high replication factors. Additionally, we have automated and optimized the generation of permuted states, which allows us to explore higher replication factors (up to 10 replicas) using hybrid techniques. It also allows us to validate our results with existing simulations based on actual replication mechanisms, which previously were analytically validated with only one pair of replicas. Finally, we have discovered that update locality and bimodal access patterns are the primary factors contributing to the formation of identical conflicts

Complete-Graph Tensor Network States: A New Fermionic Wave Function Ansatz for Molecules

We present a new class of tensor network states that are specifically designed to capture the electron correlation of a molecule of arbitrary structure. In this ansatz, the electronic wave function is represented by a Complete-Graph Tensor Network (CGTN) ansatz which implements an efficient reduction of the number of variational parameters by breaking down the complexity of the high-dimensional coefficient tensor of a full-configuration-interaction (FCI) wave function. We demonstrate that CGTN states approximate ground states of molecules accurately by comparison of the CGTN and FCI expansion coefficients. The CGTN parametrization is not biased towards any reference configuration in contrast to many standard quantum chemical methods. This feature allows one to obtain accurate relative energies between CGTN states which is central to molecular physics and chemistry. We discuss the implications for quantum chemistry and focus on the spin-state problem. Our CGTN approach is applied to the energy splitting of states of different spin for methylene and the strongly correlated ozone molecule at a transition state structure. The parameters of the tensor network ansatz are variationally optimized by means of a parallel-tempering Monte Carlo algorithm

Accurate ab initio spin densities

We present an approach for the calculation of spin density distributions for molecules that require very large active spaces for a qualitatively correct description of their electronic structure. Our approach is based on the density-matrix renormalization group (DMRG) algorithm to calculate the spin density matrix elements as basic quantity for the spatially resolved spin density distribution. The spin density matrix elements are directly determined from the second-quantized elementary operators optimized by the DMRG algorithm. As an analytic convergence criterion for the spin density distribution, we employ our recently developed sampling-reconstruction scheme [J. Chem. Phys. 2011, 134, 224101] to build an accurate complete-active-space configuration-interaction (CASCI) wave function from the optimized matrix product states. The spin density matrix elements can then also be determined as an expectation value employing the reconstructed wave function expansion. Furthermore, the explicit reconstruction of a CASCI-type wave function provides insights into chemically interesting features of the molecule under study such as the distribution of $\alpha$- and $\beta$-electrons in terms of Slater determinants, CI coefficients, and natural orbitals. The methodology is applied to an iron nitrosyl complex which we have identified as a challenging system for standard approaches [J. Chem. Theory Comput. 2011, 7, 2740].Comment: 37 pages, 13 figure

Sequential decoupling of negative-energy states in Douglas-Kroll-Hess theory

Here, we review the historical development, current status, and prospects of Douglas--Kroll--Hess theory as a quantum chemical relativistic electrons-only theory.Comment: 15 page

Block-Diagonalization of Operators with Gaps, with Applications to Dirac Operators

We present new results on the block-diagonalization of Dirac operators on three-dimensional Euclidean space with unbounded potentials. Classes of admissible potentials include electromagnetic potentials with strong Coulomb singularities and more general matrix-valued potentials, even non-self-adjoint ones. For the Coulomb potential, we achieve an exact diagonalization up to nuclear charge Z=124 and prove the convergence of the Douglas-Kroll-He\ss\ approximation up to Z=62, thus improving the upper bounds Z=93 and Z=51, respectively, by H.\ Siedentop and E.\ Stockmeyer considerably. These results follow from abstract theorems on perturbations of spectral subspaces of operators with gaps, which are based on a method of H.\ Langer and C.\ Tretter and are also of independent interest

Semi- and Non-relativistic Limit of the Dirac Dynamics with External Fields

We show how to approximate Dirac dynamics for electronic initial states by semi- and non-relativistic dynamics. To leading order, these are generated by the semi- and non-relativistic Pauli hamiltonian where the kinetic energy is related to $\sqrt{m^2 + \xi^2}$ and $\xi^2 / 2m$, respectively. Higher-order corrections can in principle be computed to any order in the small parameter v/c which is the ratio of typical speeds to the speed of light. Our results imply the dynamics for electronic and positronic states decouple to any order in v/c << 1. To decide whether to get semi- or non-relativistic effective dynamics, one needs to choose a scaling for the kinetic momentum operator. Then the effective dynamics are derived using space-adiabatic perturbation theory by Panati et. al with the novel input of a magnetic pseudodifferential calculus adapted to either the semi- or non-relativistic scaling.Comment: 42 page

Quantum information analysis of electronic states at different molecular structures

We have studied transition metal clusters from a quantum information theory perspective using the density-matrix renormalization group (DMRG) method. We demonstrate the competition between entanglement and interaction localization. We also discuss the application of the configuration interaction based dynamically extended active space procedure which significantly reduces the effective system size and accelerates the speed of convergence for complicated molecular electronic structures to a great extent. Our results indicate the importance of taking entanglement among molecular orbitals into account in order to devise an optimal orbital ordering and carry out efficient calculations on transition metal clusters. We propose a recipe to perform DMRG calculations in a black-box fashion and we point out the connections of our work to other tensor network state approaches

Entanglement Measures for Single- and Multi-Reference Correlation Effects

Electron correlation effects are essential for an accurate ab initio description of molecules. A quantitative a priori knowledge of the single- or multi-reference nature of electronic structures as well as of the dominant contributions to the correlation energy can facilitate the decision regarding the optimum quantum chemical method of choice. We propose concepts from quantum information theory as orbital entanglement measures that allow us to evaluate the single- and multi-reference character of any molecular structure in a given orbital basis set. By studying these measures we can detect possible artifacts of small active spaces.Comment: 14 pages, 4 figure