Alex Zunger

Bio: Alex Zunger is an academic researcher from University of Colorado Boulder. The author has contributed to research in topics: Band gap & Quantum dot. The author has an hindex of 128, co-authored 826 publications receiving 78798 citations. Previous affiliations of Alex Zunger include Tel Aviv University & University of Wisconsin-Madison.

Predicting Stable Stoichiometries of Compounds via Evolutionary Global Space-Group Optimization

Abstract: Whereas the Daltonian atom-to-atom ratios in ordinary molecules are well understood via the traditional theory of valence, the naturally occurring stoichiometries in intermetallic compounds ${A}_{p}{B}_{q}$, as revealed by phase-diagram compilations, are often surprising. Even equal-valence elements $A$ and $B$ give rise to unequal $(p,q)$ stoichiometries, e.g., the 1:2, 2:1, and 3:1 ratios in ${\text{Al}}_{p}{\text{Sc}}_{q}$. Moreover, sometimes different stoichiometries are associated with different lattice types and hence rather different physical properties. Here, we extend the fixed-composition global space-group optimization (GSGO) approach used to predict, via density-functional calculations, fixed-composition lattice types [G. Trimarchi and A. Zunger, J. Phys.: Condens. Matter 20, 295212 (2008)] to identify simultaneously all the minimum-energy lattice types throughout the composition range. Starting from randomly selected lattice vectors, atomic positions and stoichiometries, we construct the $T=0$ ``convex hull'' of energy vs composition. Rather than repeat a set of GSGO searches over a fixed list of stoichiometries, we minimize the distance to the convex hull. This approach is far more efficient than the former one as a single evolutionary search sequence simultaneously identifies the lowest-energy structures at each composition and among these it selects those that are ground states. For Al-Sc we correctly identify the stable stoichiometries and relative structure types: ${\text{AlSc}}_{2}\text{-B}{8}_{2}$, AlSc-B2, and ${\text{Al}}_{2}\text{Sc-C}15$ in the ${N}_{at}=6$ periodic cells, and ${\text{Al}}_{2}{\text{Sc}}_{6}\text{-D}{0}_{19}$, AlSc-B2, and ${\text{Al}}_{3}\text{Sc-L}{1}_{0}$ in the ${N}_{at}=8$ periodic cells. This extended evolutionary GSGO algorithm represents a step toward a fully ab initio materials synthesis, where compounds are predicted starting from sole knowledge of the chemical species of the constituents.

Quasi-Direct Optical Transitions in Silicon Nanocrystals with Intensity Exceeding the Bulk

Abstract: Comparison of the measured absolute absorption cross section on a per Si atom basis of plasma-synthesized Si nanocrystals (NCs) with the absorption of bulk crystalline Si shows that while near the band edge the NC absorption is weaker than the bulk, yet above ∼2.2 eV the NC absorbs up to 5 times more than the bulk. Using atomistic screened pseudopotential calculations we show that this enhancement arises from interface-induced scattering that enhances the quasi-direct, zero-phonon transitions by mixing direct Γ-like wave function character into the indirect X-like conduction band states, as well as from space confinement that broadens the distribution of wave functions in k-space. The absorption enhancement factor increases exponentially with decreasing NC size and is correlated with the exponentially increasing direct Γ-like wave function character mixed into the NC conduction states. This observation and its theoretical understanding could lead to engineering of Si and other indirect band gap NC materia...

Excited-state relaxation in PbSe quantum dots

Abstract: In solids the phonon-assisted, nonradiative decay from high-energy electronic excited states to low-energy electronic excited states is picosecond fast. It was hoped that electron and hole relaxation could be slowed down in quantum dots, due to the unavailability of phonons energy matched to the large energy-level spacings ("phonon-bottleneck"). However, excited-state relaxation was observed to be rather fast ( S electron Auger relaxation rate. We find that the Auger mechanism can explain the experimentally observed P-->S intraband decay time scale without the need to invoke any exotic relaxation mechanisms.

Compositional and size-dependent spectroscopic shifts in charged self-assembledInxGa1−xAs/GaAsquantum dots

Abstract: Atomistic pseudopotential many-body calculations of excitonic (X) recombination in charged, self-assembled ${\mathrm{In}}_{x}{\mathrm{Ga}}_{1\ensuremath{-}x}\mathrm{A}\mathrm{s}/\mathrm{G}\mathrm{a}\mathrm{A}\mathrm{s}$ dots predict and explain remarkable trends. (i) The redshift of the exciton energy upon negative charging is rapidly reduced with increasing the In content and increasing the dot height. The opposite behavior is observed upon positive charging. (ii) The recombination peak energies of different charge states show intriguing symmetries and alignments, e.g., ${X}^{\ensuremath{-}}$ aligns with ${X}^{2\ensuremath{-}}$ and ${X}^{3\ensuremath{-}}$ aligns with ${X}^{4\ensuremath{-}}.$ (iii) The ${X}^{3\ensuremath{-}}$ spectrum shows that a triplet initial state is lower in energy for flat dots (yielding two spectral lines), whereas the singlet state is lower in energy for taller dots (yielding a single line). These trends are explained theoretically in terms of a crossover occurring at a critical In concentration and dot height at which the electron wave functions becomes more localized than the hole wave functions.

Genetic design of enhanced valley splitting towards a spin qubit in silicon

Abstract: Electronic spins in Si are potentially useful in the development of solid-state quantum devices, but its degenerate valley states limits this potential. Zhang et al. use a genetic algorithm to identify a Ge/Si-multilayer-clad Si quantum structure whose valley splitting is increased by an order of magnitude.

Ab initio molecular-dynamics simulation of the liquid-metal-amorphous-semiconductor transition in germanium.

Abstract: We present ab initio quantum-mechanical molecular-dynamics simulations of the liquid-metal--amorphous-semiconductor transition in Ge. Our simulations are based on (a) finite-temperature density-functional theory of the one-electron states, (b) exact energy minimization and hence calculation of the exact Hellmann-Feynman forces after each molecular-dynamics step using preconditioned conjugate-gradient techniques, (c) accurate nonlocal pseudopotentials, and (d) Nos\'e dynamics for generating a canonical ensemble. This method gives perfect control of the adiabaticity of the electron-ion ensemble and allows us to perform simulations over more than 30 ps. The computer-generated ensemble describes the structural, dynamic, and electronic properties of liquid and amorphous Ge in very good agreement with experiment. The simulation allows us to study in detail the changes in the structure-property relationship through the metal-semiconductor transition. We report a detailed analysis of the local structural properties and their changes induced by an annealing process. The geometrical, bonding, and spectral properties of defects in the disordered tetrahedral network are investigated and compared with experiment.

Self-interaction correction to density-functional approximations for many-electron systems

Abstract: The exact density functional for the ground-state energy is strictly self-interaction-free (i.e., orbitals demonstrably do not self-interact), but many approximations to it, including the local-spin-density (LSD) approximation for exchange and correlation, are not. We present two related methods for the self-interaction correction (SIC) of any density functional for the energy; correction of the self-consistent one-electron potenial follows naturally from the variational principle. Both methods are sanctioned by the Hohenberg-Kohn theorem. Although the first method introduces an orbital-dependent single-particle potential, the second involves a local potential as in the Kohn-Sham scheme. We apply the first method to LSD and show that it properly conserves the number content of the exchange-correlation hole, while substantially improving the description of its shape. We apply this method to a number of physical problems, where the uncorrected LSD approach produces systematic errors. We find systematic improvements, qualitative as well as quantitative, from this simple correction. Benefits of SIC in atomic calculations include (i) improved values for the total energy and for the separate exchange and correlation pieces of it, (ii) accurate binding energies of negative ions, which are wrongly unstable in LSD, (iii) more accurate electron densities, (iv) orbital eigenvalues that closely approximate physical removal energies, including relaxation, and (v) correct longrange behavior of the potential and density. It appears that SIC can also remedy the LSD underestimate of the band gaps in insulators (as shown by numerical calculations for the rare-gas solids and CuCl), and the LSD overestimate of the cohesive energies of transition metals. The LSD spin splitting in atomic Ni and $s\ensuremath{-}d$ interconfigurational energies of transition elements are almost unchanged by SIC. We also discuss the admissibility of fractional occupation numbers, and present a parametrization of the electron-gas correlation energy at any density, based on the recent results of Ceperley and Alder.

A comprehensive review of zno materials and devices

Abstract: The semiconductor ZnO has gained substantial interest in the research community in part because of its large exciton binding energy (60meV) which could lead to lasing action based on exciton recombination even above room temperature. Even though research focusing on ZnO goes back many decades, the renewed interest is fueled by availability of high-quality substrates and reports of p-type conduction and ferromagnetic behavior when doped with transitions metals, both of which remain controversial. It is this renewed interest in ZnO which forms the basis of this review. As mentioned already, ZnO is not new to the semiconductor field, with studies of its lattice parameter dating back to 1935 by Bunn [Proc. Phys. Soc. London 47, 836 (1935)], studies of its vibrational properties with Raman scattering in 1966 by Damen et al. [Phys. Rev. 142, 570 (1966)], detailed optical studies in 1954 by Mollwo [Z. Angew. Phys. 6, 257 (1954)], and its growth by chemical-vapor transport in 1970 by Galli and Coker [Appl. Phys. ...