arXiv subjects

Steven G. Louie

Publications and source records attributed to Steven G. Louie.

At least 199 records · Page 11Linked to original sources

arXiv2009

Mechanically-Controlled Binary Conductance Switching of a Single-Molecule Junction

Molecular-scale components are expected to be central to nanoscale electronic devices. While molecular-scale switching has been reported in atomic quantum point contacts, single-molecule junctions provide the additional flexibility of tuning the on/off conductance states through molecular design. Thus far, switching in single-molecule junctions has been attributed to changes in the conformation or charge state of the molecule. Here, we demonstrate reversible binary switching in a single-molecule junction by mechanical control of the metal-molecule contact geometry. We show that 4,4'-bipyridine-gold single-molecule junctions can be reversibly switched between two conductance states through repeated junction elongation and compression. Using first-principles calculations, we attribute the different measured conductance states to distinct contact geometries at the flexible but stable N-Au bond: conductance is low when the N-Au bond is perpendicular to the conducting pi-system, and high otherwise. This switching mechanism, inherent to the pyridine-gold link, could form the basis of a new class of mechanically-activated single-molecule switches.

cond-mat.mes-hall↗

arXiv2008

Electron-Phonon Interactions in Graphene, Bilayer Graphene, and Graphite

Using first-principles techniques, we calculate the renormalization of the electron Fermi velocity and the vibrational lifetimes arising from electron-phonon interactions in doped bilayer graphene and in graphite and compare the results with the corresponding quantities in graphene. For similar levels of doping, the Fermi velocity renormalization in bilayer graphene and in graphite is found to be approximately 30% larger than that in graphene. In the case of bilayer graphene, this difference is shown to arise from the interlayer interaction. We discuss our findings in the light of recent photoemission and Raman spectroscopy experiments.

cond-mat.mtrl-sci↗

arXiv2008

New Generation of Massless Dirac Fermions in Graphene under External Periodic Potentials

We show that new massless Dirac fermions are generated when a slowly varying periodic potential is applied to graphene. These quasiparticles, generated near the supercell Brillouin zone boundaries with anisotropic group velocity, are different from the original massless Dirac fermions. The quasiparticle wavevector (measured from the new Dirac point), the generalized pseudospin vector, and the group velocity are not collinear. We further show that with an appropriate periodic potential of triangular symmetry, there exists an energy window over which the only available states are these quasiparticles, thus, providing a good system to probe experimentally the new massless Dirac fermions. The required parameters of external potentials are within the realm of laboratory conditions.

cond-mat.mes-hall↗

arXiv2008

Electron Beam Supercollimation in Graphene Superlattices

Although electrons and photons are intrinsically different, importing useful concepts in optics to electronics performing similar functions has been actively pursued over the last two decades. In particular, collimation of an electron beam is a long-standing goal. We show that ballistic propagation of an electron beam with virtual no spatial spreading or diffraction, without a waveguide or external magnetic field, can be achieved in graphene under an appropriate class of experimentally feasible one-dimensional external periodic potentials. The novel chiral quasi-one-dimensional metallic state that the charge carriers are in originates from a collapse of the intrinsic helical nature of the charge carriers in graphene owing to the superlattice potential. Beyond providing a new way to constructing chiral one-dimensional states in two dimensions, our findings should be useful in graphene-based electronic devices (e.g., for information processing) utilizing some of the highly developed concepts in optics.

cond-mat.mes-hall↗

arXiv2008

Energy Gaps and Stark Effect in Boron Nitride Nanoribbons

A first-principles investigation of the electronic properties of boron nitride nanoribbons (BNNRs) having either armchair or zigzag shaped edges passivated by hydrogen with widths up to 10 nm is presented. Band gaps of armchair BNNRs exhibit family-dependent oscillations as the width increases and, for ribbons wider than 3 nm, converge to a constant value that is 0.02 eV smaller than the bulk band gap of a boron nitride sheet owing to the existence of very weak edge states. The band gap of zigzag BNNRs monotonically decreases and converges to a gap that is 0.7 eV smaller than the bulk gap due to the presence of strong edge states. When a transverse electric field is applied, the band gaps of armchair BNNRs decrease monotonically with the field strength. For the zigzag BNNRs, however, the band gaps and the carrier effective masses either increase or decrease depending on the direction and the strength of the field.

cond-mat.mtrl-sci↗

arXiv2008

Van Hove Singularity and Apparent Anisotropy in the Electron-Phonon Interaction in Graphene

We show that the electron-phonon coupling strength obtained from the slopes of the electronic energy vs. wavevector dispersion relations, as often done in analyzing angle-resolved photoemission data, can differ substantially from the actual electron-phonon coupling strength due to the curvature of the bare electronic bands. This effect becomes particularly important when the Fermi level is close to a van Hove singularity. By performing {\it ab initio} calculations on doped graphene we demonstrate that, while the apparent strength obtained from the slopes of experimental photoemission data is highly anisotropic, the angular dependence of the actual electron-phonon coupling strength in this material is negligible.

cond-mat.mtrl-sci↗

arXiv2008

Anisotropic behaviors of massless Dirac fermions in graphene under periodic potential

Charge carriers of graphene show neutrino-like linear energy dispersions as well as chiral behavior near the Dirac point. Here we report highly unusual and unexpected behaviors of these carriers in applied external periodic potentials, i.e., in graphene superlattices. The group velocity renormalizes highly anisotropically even to a degree that it is not changed at all for states with wavevector in one direction but is reduced to zero in another, implying the possibility that one can make nanoscale electronic circuits out of graphene not by cutting it but by drawing on it in a non-destructive way. Also, the type of charge carrier species (e.g. electron, hole or open orbit) and their density of states vary drastically with the Fermi energy, enabling one to tune the Fermi surface-dominant properties significantly with gate voltage. These results address the fundamental question of how chiral massless Dirac fermions propagate in periodic potentials and point to a new possible path for nanoscale electronics.

cond-mat.mtrl-sci↗

arXiv2007

Novel Orientational Ordering and Reentrant Metallicity in KxC60 Monolayers for 3 <= x <= 5

We have performed local STM studies on potassium-doped C60 (KxC60) monolayers over a wide regime of the phase diagram. As K content increases from x = 3 to 5, KxC60 monolayers undergo metal-insulator-metal reentrant phase transitions and exhibit a variety of novel orientational orderings. The most striking new structure has a pinwheel-like 7-molecule unit cell in insulating K4+dC60. We propose that the driving mechanism for the orientational ordering in KxC60 is the lowering of electron kinetic energy through maximization of the overlap of neighboring molecular orbitals over the entire doping range x = 3 to 5. In the insulating and metallic phases this gives rise to orbital versions of the superexchange and double-exchange interactions respectively.

cond-mat.mtrl-sci↗

arXiv2007

Electron-phonon interaction alone does not explain the photoemission kink in cuprate superconductors

Despite over two decades of intense research efforts, the origin of high-temperature superconductivity in the copper oxides remains elusive. Angle-resolved photoemission experiments (ARPES) revealed a kink in the dispersion relations (energy vs. wavevector) of electronic states in the cuprates at binding energies of 50-80 meV, and raised the hope that this anomaly could be key to understanding high-temperature superconductivity. The kink is often interpreted in terms of interactions between the electrons and a bosonic field. While there is no consensus on the nature of the bosons or even whether a boson model is appropriate, phonons and spin fluctuations have alternatively been proposed as possible candidates. Here we report state-of-the-art first-principles calculations of the role of phonons and the electron-phonon interaction in the photoemission spectra of La2-xSrxCuO4 (LSCO). Our study demonstrates that the phonon-induced renormalization of the electron energies and the Fermi velocity is almost one order of magnitude smaller than the effect observed in photoemission experiments. Hence, the present finding rules out electron-phonon interaction in bulk LSCO as the possible origin of the measured kink. This result should bear on several proposed theories of high temperature superconductivity in addition to theories concerning the origin of kinks in cuprate photoemission data.

cond-mat.supr-con↗

arXiv2007

Spatially-resolved electronic and vibronic properties of single diamondoid molecules

Diamondoids are a unique form of carbon nanostructure best described as hydrogen-terminated diamond molecules. Their diamond-cage structures and tetrahedral sp3 hybrid bonding create new possibilities for tuning electronic band gaps, optical properties, thermal transport, and mechanical strength at the nanoscale. The recently-discovered higher diamondoids (each containing more than three diamond cells) have thus generated much excitement in regards to their potential versatility as nanoscale devices. Despite this excitement, however, very little is known about the properties of isolated diamondoids on metal surfaces, a very relevant system for molecular electronics. Here we report the first molecular scale study of individual tetramantane diamondoids on Au(111) using scanning tunneling microscopy and spectroscopy. We find that both the diamondoid electronic structure and electron-vibrational coupling exhibit unique spatial distributions characterized by pronounced line nodes across the molecular surfaces. Ab-initio pseudopotential density functional calculations reveal that the observed dominant electronic and vibronic properties of diamondoids are determined by surface hydrogen terminations, a feature having important implications for designing diamondoid-based molecular devices.

cond-mat.mtrl-sci↗

arXiv2007

Excitonic Effects in the Optical Spectra of Graphene Nanoribbons

We present a first-principles calculation of the optical properties of armchair-edged graphene nanoribbons (AGNRs) with many-electron effects included. The reduced dimensionality of the AGNRs gives rise to an enhanced electron-hole binding energy for both bright and dark exciton states (0.8-1.4 eV for GNRs with width w ~ 1.2 nm) and dramatically changes the optical spectra owing to a near complete transfer of oscillator strength to the exciton states from the continuum transitions. The characteristics of the excitons of the three distinct families of AGNRs are compared and discussed. The enhanced excitonic effects found here are expected to be of importance in optoelectronic applications of graphene-based nanostructures.

cond-mat.mes-hall↗

arXiv2007

Amine-Gold Linked Single-Molecule Junctions: Experiment and Theory

The measured conductance distribution for single molecule benzenediamine-gold junctions, based on 59,000 individual conductance traces recorded while breaking a gold point contact in solution, has a clear peak at 0.0064 G$_{0}$ with a width of $\pm$ 40%. Conductance calculations based on density functional theory (DFT) for 15 distinct junction geometries show a similar spread. Differences in local structure have a limited influence on conductance because the amine-Au bonding motif is well-defined and flexible. The average calculated conductance (0.046 G$_{0}$) is seven times larger than experiment, suggesting the importance of many-electron corrections beyond DFT.

cond-mat.mtrl-sci↗

arXiv2007

Velocity Renormalization and Carrier Lifetime in Graphene from Electron-Phonon Interaction

We present a first-principles investigation of the phonon-induced electron self-energy in graphene. The energy dependence of the self-energy reflects the peculiar linear bandstructure of graphene and deviates substantially from the usual metallic behavior. The effective band velocity of the Dirac fermions is found to be reduced by 4-8%, depending on doping, by the interaction with lattice vibrations. Our results are consistent with the observed linear dependence of the electronic linewidth on the binding energy in photoemission spectra.

cond-mat.mtrl-sci↗

arXiv2007

Quasiparticle Energies and Band Gaps of Graphene Nanoribbons

We present calculations of the quasiparticle energies and band gaps of graphene nanoribbons (GNRs) carried out using a first-principles many-electron Green's function approach within the GW approximation. Because of the quasi-one-dimension nature of a GNR, electron-electron interaction effects due to the enhanced screened Coulomb interaction and confinement geometry greatly influence the quasiparticle band gap. Compared with previous tight-binding and density functional theory studies, our calculated quasiparticle band gaps show significant self-energy corrections for both armchair and zigzag GNRs, in the range of 0.5-3.0 eV for ribbons of width 2.4-0.4 nm. The quasiparticle band gaps found here suggest that use of GNRs for electronic device components in ambient conditions may be viable.

cond-mat.mes-hall↗

arXiv2007

Reversible Photomechanical Switching of Individual Engineered Molecules at a Surface

We have observed reversible light-induced mechanical switching for a single organic molecule bound to a metal surface. Scanning tunneling microscopy (STM) was used to image the features of an individual azobenzene molecule on Au(111) before and after reversibly cycling its mechanical structure between trans and cis states using light. Azobenzene molecules were engineered to increase their surface photomechanical activity by attaching varying numbers of tert-butyl (TB) ligands ("legs") to the azobenzene phenyl rings. STM images show that increasing the number of TB legs "lifts" the azobenzene molecules from the substrate, thereby increasing molecular photomechanical activity by decreasing molecule-surface coupling.

cond-mat.mtrl-sci↗

arXiv2007

Hole doping MgB$_2$ without chemical substitution

Structures for realizing hole-doped MgB$_2$ without appealing to chemical substitutions are proposed. These structures which consist of alternating MgB$_2$ and graphene layers have small excess energy compared to bulk graphite and MgB$_2$. Density functional theory based first-principles electronic structure calculations show significant charge transfer from the MgB$_2$ layer to graphene, resulting in effectively hole-doped MgB$_2$. Substantial enhancement in the density of states at the Fermi level of the proposed structure is predicted.

cond-mat.supr-con↗

arXiv2006

Half-Metallic Graphene Nanoribbons

Electrical current can be completely spin polarized in a class of materials known as half-metals, as a result of the coexistence of metallic nature for electrons with one spin orientation and insulating for electrons with the other. Such asymmetric electronic states for the different spins have been predicted for some ferromagnetic metals - for example, the Heusler compounds- and were first observed in a manganese perovskite. In view of the potential for use of this property in realizing spin-based electronics, substantial efforts have been made to search for half-metallic materials. However, organic materials have hardly been investigated in this context even though carbon-based nanostructures hold significant promise for future electronic device. Here we predict half-metallicity in nanometre-scale graphene ribbons by using first-principles calculations. We show that this phenomenon is realizable if in-plane homogeneous electric fields are applied across the zigzag-shaped edges of the graphene nanoribbons, and that their magnetic property can be controlled by the external electric fields. The results are not only of scientific interests in the interplay between electric fields and electronic spin degree of freedom in solids but may also open a new path to explore spintronics at nanometre scale, based on graphene.

cond-mat.mes-hall↗

arXiv2006

Energy Gaps in Graphene Nanoribbons

Based on a first-principles approach, we present scaling rules for the band gaps of graphene nanoribbons (GNRs) as a function of their widths. The GNRs considered have either armchair or zigzag shaped edges on both sides with hydrogen passivation. Both varieties of ribbons are shown to have band gaps. This differs from the results of simple tight-binding calculations or solutions of the Dirac's equation based on them. Our {\it ab initio} calculations show that the origin of energy gaps for GNRs with armchair shaped edges arises from both quantum confinement and the crucial effect of the edges. For GNRs with zigzag shaped edges, gaps appear because of a staggered sublattice potential on the hexagonal lattice due to edge magnetization. The rich gap structure for ribbons with armchair shaped edges is further obtained analytically including edge effects. These results reproduce our {\it ab initio} calculation results very well.

cond-mat.mes-hall↗