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N. D. Drummond

Publications and source records attributed to N. D. Drummond.

At least 37 records · Page 2Linked to original sources

Ground-state properties of electron-electron biwire systems

The correlation between electrons in different quantum wires is expected to affect the electronic properties of quantum electron-electron biwire systems. Here, we use the variational Monte Carlo method to study the ground-state properties of parallel, infinitely thin electron-electron biwires for several electron densities ($r_\text{s}$) and interwire separations ($d$). Specifically, the ground-state energy, the correlation energy, the interaction energy, the pair-correlation function (PCF), the static structure factor (SSF), and the momentum distribution (MD) function are calculated. We find that the interaction energy increases as $\ln(d)$ for $d\to 0$ and it decreases as $d^{-2}$ when $d\to \infty$. The PCF shows oscillatory behavior at all densities considered here. As two parallel wires approach each other, interwire correlations increase while intrawire correlations decrease as evidenced by the behavior of the PCF, SSF, and MD. The system evolves from two monowires of density parameter $r_\text{s}$ to a single monowire of density parameter $r_\text{s}/2$ as $d$ is reduced from infinity to zero. The MD reveals Tomonaga-Luttinger (TL) liquid behavior with a power-law nature near $k_\text{F}$ even in the presence of an extra interwire interaction between the electrons in biwire systems. It is observed that when $d$ is reduced the MD decreases for $k k_\text{F}$, similar to its behavior with increasing $r_\text{s}$. The TL liquid exponent is extracted by fitting the MD data near $k_\text{F}$, from which the TL liquid interaction parameter $K_ρ$ is calculated. The value of the TL parameter is found to be in agreement with that of a single wire for large separation between the two wires.

cond-mat.quant-gas↗

Structures of bulk hexagonal post-transition-metal chalcogenides from dispersion-corrected density-functional theory

We use dispersion-corrected density-functional theory to determine the relative energies of competing polytypes of bulk layered hexagonal post-transition-metal chalcogenides, to search for the most stable structures of these potentially technologically important semiconductors. We show that there is some degree of consensus among dispersion-corrected exchange-correlation functionals regarding the energetic orderings of polytypes, but we find that for each material there are multiple stacking orders with relative energies of less than 1 meV per monolayer unit cell, implying that stacking faults are expected to be abundant in all post-transition-metal chalcogenides. By fitting a simple model to all our energy data, we predict that the most stable hexagonal structure has P$6_3$/mmc space group in each case, but that the stacking order differs between GaS, GaSe, GaTe, and InS on the one hand and InSe and InTe on the other. At zero pressure, the relative energies obtained with different functionals disagree by around 1-5 meV per monolayer unit cell, which is not sufficient to identify the most stable structure unambiguously; however, multi-GPa pressures reduce the number of competing phases significantly. At higher pressures, an AB$'$-stacked structure of the most stable monolayer polytype is found to be the most stable bulk structure; this structure has not been reported in experiments thus far.

cond-mat.mtrl-sci↗

Diffusion quantum Monte Carlo and GW study of the electronic properties of monolayer and bulk hexagonal boron nitride

We report diffusion quantum Monte Carlo (DMC) and many-body $GW$ calculations of the electronic band gaps of monolayer and bulk hexagonal boron nitride (hBN). We find the monolayer band gap to be indirect. $GW$ predicts much smaller quasiparticle gaps at both the single-shot $G_0W_0$ and the partially self-consistent $GW_0$ levels. In contrast, solving the Bethe-Salpeter equation on top of the $GW_0$ calculation yields an exciton binding energy for the direct exciton at the $K$ point in close agreement with the DMC value. Vibrational renormalization of the electronic band gap is found to be significant in both the monolayer and the bulk. Taking vibrational effects into account, DMC overestimates the band gap of bulk hBN, while $GW$ theory underestimates it.

cond-mat.mtrl-sci↗

Variational and Diffusion Quantum Monte Carlo Calculations with the CASINO Code

We present an overview of the variational and diffusion quantum Monte Carlo methods as implemented in the CASINO program. We particularly focus on developments made in the last decade, describing state-of-the-art quantum Monte Carlo algorithms and software and discussing their strengths and their weaknesses. We review a range of recent applications of CASINO.

physics.comp-ph↗

Comparing many-body approaches against the helium atom exact solution

Over time, many different theories and approaches have been developed to tackle the many-body problem in quantum chemistry, condensed-matter physics, and nuclear physics. Here we use the helium atom, a real system rather than a model, and we use the exact solution of its Schrödinger equation as a benchmark for comparison between methods. We present new results beyond the random-phase approximation (RPA) from a renormalized RPA (r-RPA) in the framework of the self-consistent RPA (SCRPA) originally developed in nuclear physics, and compare them with various other approaches like configuration interaction (CI), quantum Monte Carlo (QMC), time-dependent density-functional theory (TDDFT), and the Bethe-Salpeter equation on top of the GW approximation. Most of the calculations are consistently done on the same footing, e.g. using the same basis set, in an effort for a most faithful comparison between methods.

physics.atom-ph↗

One-dimensional electron fluid at high density

We calculate the ground-state energy, pair correlation function, static structure factor, and momentum density of the one-dimensional electron fluid at high density using variational quantum Monte Carlo simulation. For an infinitely thin cylindrical wire the predicted correlation energy is found to fit nicely with a quadratic function of coupling parameter $r_s$. The extracted exponent $α$ of the momentum density for $k\sim k_F$ is used to determine the Tomonaga-Luttinger parameter $K_ρ$ as a function of $r_s$ in the high-density regime for the first time. We find that the simulated static structure factor and pair correlation function for infinitely thin wires agree with our recent high-density theory [K. Morawetz et al., Phys. Rev. B 97, 155147 (2018)].

cond-mat.str-el↗

Stability of trions in coupled quantum wells modelled by two-dimensional bilayers

We report variational and diffusion quantum Monte Carlo calculations of the binding energies of indirect trions and biexcitons in ideal two-dimensional bilayer systems within the effective-mass approximation, and with a Coulomb $1/r$ interaction between charge carriers. The critical layer separation at which trions become unbound has been studied for various electron-hole mass ratios, and found to be over an order of magnitude larger than the critical layer separation for biexcitons.

cond-mat.mes-hall↗

Diffusion quantum Monte Carlo study of excitonic complexes in two-dimensional transition-metal dichalcogenides

Excitonic effects play a particularly important role in the optoelectronic behavior of two-dimensional semiconductors. To facilitate the interpretation of experimental photoabsorption and photoluminescence spectra we provide (i) statistically exact diffusion quantum Monte Carlo binding-energy data for a Mott-Wannier model of (donor/acceptor-bound) excitons, trions, and biexcitons in two-dimensional semiconductors in which charges interact via the Keldysh potential, (ii) contact pair-distribution functions to allow a perturbative description of contact interactions between charge carriers, and (iii) an analysis and classification of the different types of bright trion and biexciton that can be seen in single-layer molybdenum and tungsten dichalcogenides. We investigate the stability of biexcitons in which two charge carriers are indistinguishable, finding that they are only bound when the indistinguishable particles are several times heavier than the distinguishable ones. Donor/acceptor-bound biexcitons have similar binding energies to the experimentally measured biexciton binding energies. We predict the relative positions of all stable free and bound excitonic complexes of distinguishable charge carriers in the photoluminescence spectra of WSe$_2$ and MoSe$_2$.

cond-mat.mes-hall↗

Binding energies of trions and biexcitons in two-dimensional semiconductors from diffusion quantum Monte Carlo calculations

Excitonic effects play a particularly important role in the optoelectronic behavior of two-dimensional (2D) semiconductors. To facilitate the interpretation of experimental photoabsorption and photoluminescence spectra we provide statistically exact diffusion quantum Monte Carlo binding-energy data for Mott-Wannier models of excitons, trions, and biexcitons in 2D semiconductors. We also provide contact pair densities to allow a description of contact (exchange) interactions between charge carriers using first-order perturbation theory. Our data indicate that the binding energy of a trion is generally larger than that of a biexciton in 2D semiconductors. We provide interpolation formulas giving the binding energy and contact density of 2D semiconductors as functions of the electron and hole effective masses and the in-plane polarizability.

cond-mat.mes-hall↗

Trail-Needs pseudopotentials in quantum Monte Carlo calculations with plane-wave/blip basis sets

We report a systematic analysis of the performance of a widely used set of Dirac-Fock pseudopotentials for quantum Monte Carlo (QMC) calculations. We study each atom in the periodic table from hydrogen (Z=1) to mercury (Z=80), with the exception of the 4f elements (57 <= Z <= 70). We demonstrate that ghost states are a potentially serious problem when plane-wave basis sets are used in density functional theory (DFT) orbital-generation calculations, but that this problem can be almost entirely eliminated by choosing the s channel to be local in the DFT calculation; the d channel can then be chosen to be local in subsequent QMC calculations, which generally leads to more accurate results. We investigate the achievable energy variance per electron with different levels of trial wave function and we determine appropriate plane-wave cutoff energies for DFT calculations for each pseudopotential. We demonstrate that the so-called "T-move" scheme in diffusion Monte Carlo is essential for many elements. We investigate the optimal choice of spherical integration rule for pseudopotential projectors in QMC calculations. The information reported here will prove crucial in the planning and execution of QMC projects involving beyond-first-row elements.

cond-mat.mtrl-sci↗

Trion formation in a two-dimensional hole-doped electron gas

The interaction between a single hole and a two-dimensional, paramagnetic, homogeneous electron gas is studied using diffusion quantum Monte Carlo simulations. Calculations of the electron-hole correlation energy, pair-correlation function, and the electron-hole center-of-mass momentum density are reported for a range of electron--hole mass ratios and electron densities. We find numerical evidence of a crossover from a collective Mahan exciton to a trion-dominated state in a density range in agreement with that found in recent experiments on quantum well heterostructures.

cond-mat.str-el↗

Nature of the Metallization Transition in Solid Hydrogen

We present an accurate study of the static-nucleus electronic energy band gap of solid molecular hydrogen at high pressure. The excitonic and quasiparticle gaps of the $C2/c$, $Pc$, $Pbcn$, and $P6_3/m$ structures at pressures of 250, 300, and 350~GPa are calculated using the fixed-node diffusion quantum Monte Carlo (DMC) method. The difference between the mean-field and many-body band gaps at the same density is found to be almost independent of system size and can therefore be applied as a scissor correction to the mean-field gap of an infinite system to obtain an estimate of the many-body gap in the thermodynamic limit. By comparing our static-nucleus DMC energy gaps with available experimental results, we demonstrate the important role played by nuclear quantum effects in the electronic structure of solid hydrogen. Our DMC results suggest that the metallization of high-pressure solid hydrogen occurs via a structural phase transition rather than band gap closure.

cond-mat.mtrl-sci↗

Quasiparticle and excitonic gaps of one-dimensional carbon chains

We report diffusion quantum Monte Carlo (DMC) calculations of the quasiparticle and excitonic gaps of hydrogen-terminated oligoynes and polyyne. The electronic gaps are found to be very sensitive to the atomic structure in these systems. We have therefore optimised the geometry of polyyne by directly minimising the DMC energy with respect to the lattice constant and the Peierls-induced carbon-carbon bond-length alternation. We find the bond-length alternation of polyyne to be 0.136(2) Å and the excitonic and quasiparticle gaps to be 3.30(7) and 3.4(1) eV, respectively. The DMC zone-centre longitudinal optical phonon frequency of polyyne is 2084(5) cm$^{-1}$, which is consistent with Raman spectroscopic measurements for large oligoynes.

cond-mat.mes-hall↗

Quantum Monte Carlo study of the phase diagram of solid molecular hydrogen at extreme pressures

Establishing the phase diagram of hydrogen is a major challenge for experimental and theoretical physics. Experiment alone cannot establish the atomic structure of solid hydrogen at high pressure, because hydrogen scatters X-rays only weakly. Instead our understanding of the atomic structure is largely based on density functional theory (DFT). By comparing Raman spectra for low-energy structures found in DFT searches with experimental spectra, candidate atomic structures have been identified for each experimentally observed phase. Unfortunately, DFT predicts a metallic structure to be energetically favoured at a broad range of pressures up to 400 GPa, where it is known experimentally that hydrogen is nonmetallic. Here we show that more advanced theoretical methods (diffusion quantum Monte Carlo calculations) find the metallic structure to be uncompetitive, and predict a phase diagram in reasonable agreement with experiment. This greatly strengthens the claim that the candidate atomic structures accurately model the experimentally observed phases.

cond-mat.mtrl-sci↗

Quantum Monte Carlo Calculation of the Binding Energy of Bilayer Graphene

We report diffusion quantum Monte Carlo calculations of the interlayer binding energy of bilayer graphene. We find the binding energies of the AA- and AB-stacked structures at the equilibrium separation to be 11.5(9) and 17.7(9) meV/atom, respectively. The out-of-plane zone-center optical phonon frequency predicted by our binding-energy curve is consistent with available experimental results. As well as assisting the modeling of interactions between graphene layers, our results will facilitate the development of van der Waals exchange-correlation functionals for density functional theory calculations.

cond-mat.mes-hall↗

Finite-size errors in continuum quantum Monte Carlo calculations

We analyze the problem of eliminating finite-size errors from quantum Monte Carlo (QMC) energy data. We demonstrate that both (i) adding a recently proposed [S. Chiesa et al., Phys. Rev. Lett. 97, 076404 (2006)] finite-size correction to the Ewald energy and (ii) using the model periodic Coulomb (MPC) interaction [L. M. Fraser et al., Phys. Rev. B 53, 1814 (1996); P. R. C. Kent et al., Phys. Rev. B 59, 1917 (1999); A. J. Williamson et al., Phys. Rev. B 55, 4851 (1997)] are good solutions to the problem of removing finite-size effects from the interaction energy in cubic systems, provided the exchange-correlation (XC) hole has converged with respect to system size. However, we find that the MPC interaction distorts the XC hole in finite systems, implying that the Ewald interaction should be used to generate the configuration distribution. The finite-size correction of Chiesa et al. is shown to be incomplete in systems of low symmetry. Beyond-leading-order corrections to the kinetic energy are found to be necessary at intermediate and high densities, and we investigate the effect of adding such corrections to QMC data for the homogeneous electron gas. We analyze finite-size errors in two-dimensional systems and show that the leading-order behavior differs from that which has hitherto been supposed. We compare the efficiency of different twist-averaging methods for reducing single-particle finite-size errors and we examine the performance of various finite-size extrapolation formulas. Finally, we investigate the system-size scaling of biases in diffusion QMC.

cond-mat.mtrl-sci↗

Electrons and phonons in single layers of hexagonal indium chalcogenides from ab initio calculations

We use density functional theory to calculate the electronic band structures, cohesive energies, phonon dispersions, and optical absorption spectra of two-dimensional In$_2$X$_2$ crystals, where X is S, Se, or Te. We identify two crystalline phases (alpha and beta) of monolayers of hexagonal In$_2$X$_2$, and show that they are characterized by different sets of Raman-active phonon modes. We find that these materials are indirect-band-gap semiconductors with a sombrero-shaped dispersion of holes near the valence-band edge. The latter feature results in a Lifshitz transition (a change in the Fermi-surface topology of hole-doped In$_2$X$_2$) at hole concentrations $n_{\rm S}=6.86\times 10^{13}$ cm$^{-2}$, $n_{\rm Se}=6.20\times 10^{13}$ cm$^{-2}$, and $n_{\rm Te}=2.86\times 10^{13}$ cm$^{-2}$ for X=S, Se, and Te, respectively, for alpha-In$_2$X$_2$ and $n_{\rm S}=8.32\times 10^{13}$ cm$^{-2}$, $n_{\rm Se}=6.00\times 10^{13}$ cm$^{-2}$, and $n_{\rm Te}=8.14\times 10^{13}$ cm$^{-2}$ for beta-In$_2$X$_2$.

cond-mat.mes-hall↗

Electron-Phonon Coupling and the Metalization of Solid Helium at Terapascal Pressures

Solid He is studied in the pressure and temperature ranges 1-40 TPa and 0-10,000 K using first-principles methods. Anharmonic vibrational properties are calculated within a self-consistent field framework, including the internal and free energies, density-pressure relation, stress tensor, thermal expansion, and the electron-phonon coupling renormalization of the electronic band gap. We find that an accurate description of electron-phonon coupling requires us to use a non-perturbative approach. The metalization pressure of 32.9 TPa at 0 K is larger than found previously. The vibrational effects are large; for example at P=30 TPa the band gap is increased by 2.8 eV by electron-phonon coupling and a further 0.1 eV by thermal expansion compared to the static value. The implications of the calculated metalization pressure for the cooling of white dwarfs are discussed.

cond-mat.mtrl-sci↗