Recent developments in the method of different orbitals for different spins

Alternate molecular orbital and nonpaired spatial orbital methods compared for conjugate organic compound

Three-electron anisotropic quantum dots in variable magnetic fields: exact results for excitation spectra, spin structures, and entanglement

Exact-diagonalization calculations for N=3 electrons in anisotropic quantum dots, covering a broad range of confinement anisotropies and strength of inter-electron repulsion, are presented for zero and low magnetic fields. The excitation spectra are analyzed as a function of the strength of the magnetic field and for increasing quantum-dot anisotropy. Analysis of the intrinsic structure of the many-body wave functions through spin-resolved two-point correlations reveals that the electrons tend to localize forming Wigner molecules. For certain ranges of dot parameters (mainly at strong anisotropy), the Wigner molecules acquire a linear geometry, and the associated wave functions with a spin projection S_z=1/2 are similar to the representative class of strongly entangled states referred to as W-states. For other ranges of parameters (mainly at intermediate anisotropy), the Wigner molecules exhibit a more complex structure consisting of two mirror isosceles triangles. This latter structure can be viewed as an embryonic unit of a zig-zag Wigner crystal in quantum wires. The degree of entanglement in three-electron quantum dots can be quantified through the use of the von Neumann entropy.Comment: To appear in Physical Review B. REVTEX4. 13 pages with 16 color figures. To download a copy with higher-quality figures, go to publication #78 in http://www.prism.gatech.edu/~ph274cy

Time-dependent restricted active space Configuration Interaction for the photoionization of many-electron atoms

We introduce the time-dependent restricted active space Configuration Interaction method to solve the time-dependent Schr\"odinger equation for many-electron atoms, and particularly apply it to the treatment of photoionization processes in atoms. The method is presented in a very general formulation and incorporates a wide range of commonly used approximation schemes, like the single-active electron approximation, time-dependent Configuration Interaction with single-excitations, or the time-dependent R-matrix method. We proof the applicability of the method by calculating the photoionization cross sections of Helium and Beryllium, as well as the X-ray--IR pump-probe ionization in BerylliumComment: 12 pages, 9 figure

Approximating a Wavefunction as an Unconstrained Sum of Slater Determinants

The wavefunction for the multiparticle Schr\"odinger equation is a function of many variables and satisfies an antisymmetry condition, so it is natural to approximate it as a sum of Slater determinants. Many current methods do so, but they impose additional structural constraints on the determinants, such as orthogonality between orbitals or an excitation pattern. We present a method without any such constraints, by which we hope to obtain much more efficient expansions, and insight into the inherent structure of the wavefunction. We use an integral formulation of the problem, a Green's function iteration, and a fitting procedure based on the computational paradigm of separated representations. The core procedure is the construction and solution of a matrix-integral system derived from antisymmetric inner products involving the potential operators. We show how to construct and solve this system with computational complexity competitive with current methods.Comment: 30 page

Quasipinning and selection rules for excitations in atoms and molecules

Postulated by Pauli to explain the electronic structure of atoms and molecules, the exclusion principle establishes an upper bound of 1 for the fermionic natural occupation numbers $\{n_i\}$. A recent analysis of the pure $N$-representability problem provides a wide set of inequalities for the $\{n_i\}$, leading to constraints on these numbers. This has a strong potential impact on reduced density matrix functional theory as we know it. In this work we continue our study the nature of these inequalities for some atomic and molecular systems. The results indicate that (quasi)saturation of some of them leads to selection rules for the dominant configurations in configuration interaction expansions, in favorable cases providing means for significantly reducing their computational requirements.Comment: 12 pages, 15 figures, new references, some typos corrected and a new section adde

Multi-Particle Pseudopotentials for Multi-Component Quantum Hall Systems

The Haldane pseudopotential construction has been an extremely powerful concept in quantum Hall physics --- it not only gives a minimal description of the space of Hamiltonians but also suggests special model Hamiltonians (those where certain pseudopotential are set to zero) that may have exactly solvable ground states with interesting properties. The purpose of this paper is to generalize the pseudopotential construction to situations where interactions are N-body and where the particles may have internal degrees of freedom such as spin or valley index. Assuming a rotationally invariant Hamiltonian, the essence of the problem is to obtain a full basis of wavefunctions for N particles with fixed relative angular momentum L. This basis decomposes into representations of SU(n) with n the number of internal degrees of freedom. We give special attention to the case where the internal degree of freedom has n=2 states, which encompasses the important cases of spin-1/2 particles and quantum Hall bilayers. We also discuss in some detail the cases of spin-1 particles (n=3) and graphene (n=4, including two spin and two valley degrees of freedom).Comment: 46 pages ; 9 tables ; no figures. (The revision fixes a number of typos and updates the formatting

Interpolated wave functions for nonadiabatic simulations with the fixed-node quantum Monte Carlo method

Simulating nonadiabatic effects with many-body wave function approaches is an open field with many challenges. Recent interest has been driven by new algorithmic developments and improved theoretical understanding of properties unique to electron-ion wave functions. Fixed-node diffusion Monte Caro is one technique that has shown promising results for simulating electron-ion systems. In particular, we focus on the CH molecule for which previous results suggested a relatively significant contribution to the energy from nonadiabatic effects. We propose a new wave function ansatz for diatomic systems which involves interpolating the determinant coefficients calculated from configuration interaction methods. We find this to be an improvement beyond previous wave function forms that have been considered. The calculated nonadiabatic contribution to the energy in the CH molecule is reduced compared to our previous results, but still remains the largest among the molecules under consideration.Comment: 7 pages, 3 figure

Symmetry breaking and quantum correlations in finite systems: Studies of quantum dots and ultracold Bose gases and related nuclear and chemical methods

Investigations of emergent symmetry breaking phenomena occurring in small finite-size systems are reviewed, with a focus on the strongly correlated regime of electrons in two-dimensional semicoductor quantum dots and trapped ultracold bosonic atoms in harmonic traps. Throughout the review we emphasize universal aspects and similarities of symmetry breaking found in these systems, as well as in more traditional fields like nuclear physics and quantum chemistry, which are characterized by very different interparticle forces. A unified description of strongly correlated phenomena in finite systems of repelling particles (whether fermions or bosons) is presented through the development of a two-step method of symmetry breaking at the unrestricted Hartree-Fock level and of subsequent symmetry restoration via post Hartree-Fock projection techniques. Quantitative and qualitative aspects of the two-step method are treated and validated by exact diagonalization calculations. Strongly-correlated phenomena emerging from symmetry breaking include: (I) Chemical bonding, dissociation, and entanglement (at zero and finite magnetic fields) in quantum dot molecules and in pinned electron molecular dimers formed within a single anisotropic quantum dot. (II) Electron crystallization, with particle localization on the vertices of concentric polygonal rings, and formation of rotating electron molecules (REMs) in circular quantum dots. (III) At high magnetic fields, the REMs are described by parameter-free analytic wave functions, which are an alternative to the Laughlin and composite-fermion approaches. (IV) Crystalline phases of strongly repelling bosons. In rotating traps and in analogy with the REMs, such repelling bosons form rotating boson molecules (RBMs).Comment: Review article published in Reports on Progress in Physics. REVTEX4. 95 pages with 37 color figures. To download a copy with high-quality figures, go to publication #82 in http://www.prism.gatech.edu/~ph274cy

Studies in molecular structure, symmetry and conformation I

Crystals of 1-aminocyclooctanecarboxylic acid hydrobromide are orthorhombic, with a = 26·026, b =7·087, c = 6·149, Z = 4 and space group P 2 1 2 1 2 1 .The structure was solved in projections by direct methods and later refined with three-dimensional data using a full-matrix least-squares treatment. All hydrogen atoms were located from a difference Fourier and the final R factor for the 1128 observed reflections was 8·62 %. The molecules are held together by a series of hydrogen bonds in a three-dimensional network. A detailed discussion of the intramolecular and the intermolecular features of the structure is presented. The cyclooctane ring is found to exist in the boat-chair conformation.Peer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/44829/1/10870_2005_Article_BF01198532.pd