723 research outputs found
Large potential steps at weakly interacting metal-insulator interfaces
Potential steps exceeding 1 eV are regularly formed at metal|insulator
interfaces, even when the interaction between the materials at the interface is
weak physisorption. From first-principles calculations on metal|h-BN interfaces
we show that these potential steps are only indirectly sensitive to the
interface bonding through the dependence of the binding energy curves on the
van der Waals interaction. Exchange repulsion forms the main contribution to
the interface potential step in the weakly interacting regime, which we show
with a simple model based upon a symmetrized product of metal and h-BN wave
functions. In the strongly interacting regime, the interface potential step is
reduced by chemical bonding
Band gaps in pseudopotential self-consistent GW calculations
For materials which are incorrectly predicted by density functional theory to
be metallic, an iterative procedure must be adopted in order to perform GW
calculations. In this paper we test two iterative schemes based on the
quasi-particle and pseudopotential approximations for a number of inorganic
semiconductors whose electronic structures are well known from experiment.
Iterating just the quasi-particle energies yields a systematic, but modest
overestimate of the band gaps, confirming conclusions drawn earlier for CaB_6
and YH_3. Iterating the quasi-particle wave functions as well gives rise to an
imbalance between the Hartree and Fock potentials and results in bandgaps in
far poorer agreement with experiment.Comment: 5 pages, 2 figures, 2 table
Band gaps in incommensurable graphene on hexagonal boron nitride
Devising ways of opening a band gap in graphene to make charge-carrier masses
finite is essential for many applications. Recent experiments with graphene on
hexagonal boron nitride (h-BN) offer tantalizing hints that the weak
interaction with the substrate is sufficient to open a gap, in contradiction of
earlier findings. Using many-body perturbation theory, we find that the small
observed gap is what remains after a much larger underlying quasiparticle gap
is suppressed by incommensurability. The sensitivity of this suppression to a
small modulation of the distance separating graphene from the substrate
suggests ways of exposing the larger underlying gap
Ab initio study on the effects of transition metal doping of Mg2NiH4
Mg2NiH4 is a promising hydrogen storage material with fast (de)hydrogenation
kinetics. Its hydrogen desorption enthalpy, however, is too large for practical
applications. In this paper we study the effects of transition metal doping by
first-principles density functional theory calculations. We show that the
hydrogen desorption enthalpy can be reduced by ~0.1 eV/H2 if one in eight Ni
atoms is replaced by Cu or Fe. Replacing Ni by Co atoms, however, increases the
hydrogen desorption enthalpy. We study the thermodynamic stability of the
dopants in the hydrogenated and dehydrogenated phases. Doping with Co or Cu
leads to marginally stable compounds, whereas doping with Fe leads to an
unstable compound. The optical response of Mg2NiH4 is also substantially
affected by doping. The optical gap in Mg2NiH4 is ~1.7 eV. Doping with Co, Fe
or Cu leads to impurity bands that reduce the optical gap by up to 0.5 eV.Comment: 8 pages, 4 figure
Schottky barriers at hexagonal boron nitride/metal interfaces: a first principles study
The formation of a Schottky barrier at the interface between a metal and
hexagonal boron nitride (h-BN) is studied using density functional theory. For
metals whose work functions range from 4.2 to 6.0 eV, we find Schottky barrier
heights for holes between 1.2 and 2.3 eV. A central role in determining the
Schottky barrier height is played by a potential step of between 0.4 and 1.8 eV
that is formed at the metal|h-BN interface and effectively lowers the metal
work function. If h-BN is physisorbed, as is the case on fcc Cu, Al, Au, Ag and
Pt(111) substrates, the interface potential step is described well by a
universal function that depends only on the distance separating h-BN from the
metal surface. The interface potential step is largest when h-BN is
chemisorbed, which is the case for hcp Co and Ti (0001) and for fcc Ni and Pd
(111) substrates
First-principles calculations of the crystal structure, electronic structure, and thermodynamic stability of Be(BH4)2
Alanates and boranates are intensively studied because of their potential use as hydrogen storage materials. In this paper, we present a first-principles study of the electronic structure and the energetics of beryllium boranate BeBH42. From total energy calculations, we show that—in contrast to the other boranates and alanates—hydrogen desorption directly to the elements is likely and is at least competitive with desorption to the elemental hydride BeH2. The formation enthalpy of BeBH42 is only −0.14 eV/H2 at T=0 K. This low value can be rationalized by the participation of all atoms in the covalent bonding, which is in contrast to the ionic bonding observed in other boranates. From calculations of thermodynamic properties at finite temperature, we estimate a decomposition temperature of 162 K at a pressure of 1 bar
First-principles study of the interaction and charge transfer between graphene and metals
Measuring the transport of electrons through a graphene sheet necessarily
involves contacting it with metal electrodes. We study the adsorption of
graphene on metal substrates using first-principles calculations at the level
of density functional theory. The bonding of graphene to Al, Ag, Cu, Au and
Pt(111) surfaces is so weak that its unique "ultrarelativistic" electronic
structure is preserved. The interaction does, however, lead to a charge
transfer that shifts the Fermi level by up to 0.5 eV with respect to the
conical points. The crossover from p-type to n-type doping occurs for a metal
with a work function ~5.4 eV, a value much larger than the work function of
free-standing graphene, 4.5 eV. We develop a simple analytical model that
describes the Fermi level shift in graphene in terms of the metal substrate
work function. Graphene interacts with and binds more strongly to Co, Ni, Pd
and Ti. This chemisorption involves hybridization between graphene -states
and metal d-states that opens a band gap in graphene. The graphene work
function is as a result reduced considerably. In a current-in-plane device
geometry this should lead to n-type doping of graphene.Comment: 12 pages, 9 figure
Substrate-induced bandgap in graphene on hexagonal boron nitride
We determine the electronic structure of a graphene sheet on top of a
lattice-matched hexagonal boron nitride (h-BN) substrate using ab initio
density functional calculations. The most stable configuration has one carbon
atom on top of a boron atom, the other centered above a BN ring. The resulting
inequivalence of the two carbon sites leads to the opening of a gap of 53 meV
at the Dirac points of graphene and to finite masses for the Dirac fermions.
Alternative orientations of the graphene sheet on the BN substrate generate
similar band gaps and masses. The band gap induced by the BN surface can
greatly improve room temperature pinch-off characteristics of graphene-based
field effect transistors.Comment: 5 pages, 4 figures, Phys. Rev. B, in pres
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