Exciton-exciton interaction and biexciton formation in bilayer systems

We report quantum Monte Carlo calculations of biexciton binding energies in ideal two-dimensional bilayer systems with isotropic electron and hole masses. We have also calculated exciton-exciton interaction potentials, and pair distribution functions for electrons and holes in bound biexcitons. Comparing our data with results obtained in a recent study using a model exciton-exciton potential [C. Schindler and R. Zimmermann, Phys. Rev. B \textbf{78}, 045313 (2008)], we find a somewhat larger range of layer separations at which biexcitons are stable. We find that individual excitons retain their identity in bound biexcitons for large layer separations.Comment: 7 pages, 11 figures, 2 table

Dissociation energy of the water dimer from Quantum Monte Carlo calculations

We report a study of the electronic dissociation energy of the water dimer using quantum Monte Carlo (QMC) techniques. We have performed variational quantum Monte Carlo (VMC) and diffusion quantum Monte Carlo (DMC) calculations of the electronic ground state of the water monomer and dimer using all-electron and pseudopotential approaches. We have used Slater-Jastrow trial wave functions with B3LYP-like single-particle orbitals, into which we have incorporated backflow correlations. When backflow correlations are introduced, the total energy of the water monomer decreases by about 4-5 mHa, yielding a DMC energy of -76.42830(5) Ha, which is only 10 mHa above the experimental value. In our pseudopotential DMC calculations, we have compared the total energies of the water monomer and dimer obtained using the locality approximation with those from the variational scheme recently proposed by Casula [Phys. Rev. B 74, 161102(R) (2006)]. The time step errors in the Casula scheme are larger and the extrapolation of the energy to zero time step always lies above the result obtained with the locality approximation. However, the errors cancel when energy differences are taken, yielding electronic dissociation energies within error bars of each other. The dissociation energies obtained in our various all-electron and pseudopotential calculations range between 5.03(7) and 5.47(9) kcal/mol and are in good agreement with experiment. Our calculations give monomer dipole moments which range between 1.897(2) and 1.909(4) Debye and dimer dipole moments which range between 2.628(6) and 2.672(5) Debye.Comment: 31 pages, 7 figures, 5 tables. See Journal reference belo

Diffusion quantum Monte Carlo calculation of the quasiparticle effective mass of the two-dimensional homogeneous electron gas

The quasiparticle effective mass is a key quantity in the physics of electron gases, describing the renormalization of the electron mass due to electron-electron interactions. Two-dimensional electron gases are of fundamental importance in semiconductor physics, and there have been numerous experimental and theoretical attempts to determine the quasiparticle effective mass in these systems. In this work we report quantum Monte Carlo results for the quasiparticle effective mass of a two-dimensional homogeneous electron gas. Our calculations differ from previous quantum Monte Carlo work in that much smaller statistical error bars have been achieved, allowing for an improved treatment of finite-size effects. In some cases we have also been able to use larger system sizes than previous calculations

Pressure-induced s-band ferromagnetism in alkali metals

First-principles density-functional-theory calculations show that compression of alkali metals stabilizes open structures with localized interstitial electrons which may exhibit a Stoner-type instability towards ferromagnetism. We find ferromagnetic phases of the lithium-IV-type, simple cubic, and simple hexagonal structures in the heavier alkali metals, which may be described as s-band ferromagnets. We predict that the most stable phases of potassium at low temperatures and pressures around 20 GPa are ferromagnets.Comment: 5 pages, 3 figure

Comparison of Smooth Hartree-Fock Pseudopotentials

The accuracy of two widely used scalar-relativistic Hartree-Fock pseudopotentials, the Trail-Needs-Dirac-Fock (TNDF) and the Burkatzki-Filippi-Dolg (BFD) pseudopotentials, is assessed. The performance of the pseudopotentials is tested for a chemically representative set of 34 first-row molecules. All comparisons are made at the Hartree-Fock level of theory, and both sets of pseudopotentials give good results. The all-electron equilibrium geometries, molecular dissociation energies, and zero-point vibrational energies are reproduced a little more accurately by the TNDF pseudopotentials than the BFD ones.Comment: 9 pages, 3 figures, 1 tabl

Electron Emission from Diamondoids: A Diffusion Quantum Monte Carlo Study

We present density-functional theory (DFT) and quantum Monte Carlo (QMC) calculations designed to resolve experimental and theoretical controversies over the optical properties of H-terminated C nanoparticles (diamondoids). The QMC results follow the trends of well-converged plane-wave DFT calculations for the size dependence of the optical gap, but they predict gaps that are 1-2 eV higher. They confirm that quantum confinement effects disappear in diamondoids larger than 1 nm, which have gaps below that of bulk diamond. Our QMC calculations predict a small exciton binding energy and a negative electron affinity (NEA) for diamondoids up to 1 nm, resulting from the delocalized nature of the lowest unoccupied molecular orbital. The NEA suggests a range of possible applications of diamondoids as low-voltage electron emitters

A variance-minimization scheme for optimizing Jastrow factors

We describe a new scheme for optimizing many-electron trial wave functions by minimizing the unreweighted variance of the energy using stochastic integration and correlated-sampling techniques. The scheme is restricted to parameters that are linear in the exponent of a Jastrow correlation factor, which are the most important parameters in the wave functions we use. The scheme is highly efficient and allows us to investigate the parameter space more closely than has been possible before. We search for multiple minima of the variance in the parameter space and compare the wave functions obtained using reweighted and unreweighted variance minimization.Comment: 19 pages; 12 figure

Correlated Electron Pseudopotentials for 3d-Transition Metals

A recently published correlated electron pseudopotentials (CEPPs) method has been adapted for application to the 3d-transition metals, and to include relativistic effects. New CEPPs are reported for the atoms Sc$-$Fe, constructed from atomic quantum chemical calculations that include an accurate description of correlated electrons. Dissociation energies, molecular geometries, and zero-point vibrational energies of small molecules are compared with all electron results, with all quantities evaluated using coupled cluster singles doubles and triples (CCSD(T)) calculations. The CEPPs give better results in the correlated-electron calculations than Hartree-Fock-based pseudopotentials available in the literature.Comment: 12 pages, 6 figure

Quantum Monte Carlo study of the ground state of the two-dimensional Fermi fluid

We have used the variational and diffusion quantum Monte Carlo methods to calculate the energy, pair correlation function, static structure factor, and momentum density of the ground state of the two-dimensional homogeneous electron gas. We have used highly accurate Slater-Jastrow-backflow trial wave functions and twist averaging to reduce finite-size effects where applicable. We compare our results with others in the literature and construct a local-density-approximation exchange-correlation functional for 2D systems