arXiv subjects

C. A. Stafford

Publications and source records attributed to C. A. Stafford.

At least 19 recordsLinked to original sources

arXiv2013

Local Temperature of Out-of-Equilibrium Quantum Electron Systems

We show how the local temperature of out-of-equilibrium, quantum electron systems can be consistently defined with the help of an external voltage and temperature probe. We determine sufficient conditions under which the temperature measured by the probe (i) is independent of details of the system-probe coupling, (ii) is equal to the temperature obtained from an independent current-noise measurement, (iii) satisfies the transitivity condition expressed by the zeroth law of thermodynamics, and (iv) is consistent with Carnot's theorem. This local temperature therefore characterizes the system in the common sense of equilibrium thermodynamics, but remains well defined even in out-of-equilibrium situations with no local equilibrium.

cond-mat.stat-mech↗

arXiv2010

The number of transmission channels through a single-molecule junction

We calculate transmission eigenvalue distributions for Pt-benzene-Pt and Pt-butadiene-Pt junctions using realistic state-of-the-art many-body techniques. An effective field theory of interacting $π$-electrons is used to include screening and van der Waals interactions with the metal electrodes. We find that the number of dominant transmission channels in a molecular junction is equal to the degeneracy of the molecular orbital closest to the metal Fermi level.

cond-mat.mes-hall↗

arXiv2010

Coherent Destruction of Coulomb Blockade Peaks in Molecular Junctions

Coherent electronic transport in single-molecule junctions is investigated in the Coulomb blockade regime. Both the transmission phase and probability are calculated for junctions with various contact symmetries. A dramatic suppression of the Coulomb blockade peaks is predicted for junctions where multiple atomic orbitals of the molecule couple to a single electrode although the charging steps are unaffected.

cond-mat.mes-hall↗

arXiv2010

A nanoscale transistor based on gate-induced stochastic transitions

A nanoscale device consisting of a metal nanowire, a dielectric, and a gate is proposed. A combination of quantum and thermal stochastic effects enable the device to have multiple functionalities, serving alternately as a transistor, a variable resistor, or a simple resistive element with $I-V$ characteristics that can switch between ohmic and non-ohmic. By manipulating the gate voltage, stochastic transitions between different conducting states of the nanowire can be induced, with a switching time as short as picoseconds. With an appropriate choice of dielectric, the transconductance of the device can significantly exceed the conductance quantum $G_0=2e^2/h$, a remarkable figure of merit for a device at this lengthscale.

cond-mat.mes-hall↗

arXiv2010

The Nanoscale Free-Electron Model

A brief review of the nanoscale free-electron model of metal nanowires is presented. This continuum description of metal nanostructures allows for a unified treatment of cohesive and conducting properties. Conductance channels act as delocalized chemical bonds whose breaking is responsible for jumps in the conductance and force oscillations. It is argued that surface and quantum-size effects are the two dominant factors in the energetics of a nanowire, and much of the phenomenology of nanowire stability and structural dynamics can be understood based on the interplay of these two competing factors. A linear stability analysis reveals a sequence of ``magic'' conductance values for which the underlying nanowire geometry is exceptionally stable. The stable configurations include Jahn-Teller deformed wires of broken axial symmetry. The model naturally explains the experimentally observed shell and supershell structures.

cond-mat.mes-hall↗

arXiv2010

The importance of intra-molecular electron spin relaxation in small molecular semiconductors

Electron spin relaxation rate (eSR) is investigated on several organic semiconductors of different morphologies and molecular structures, using avoided level crossing muon spectroscopy as a local spin probe. We find that two functionalized acenes (polycrystalline tri(isopropyl)silyl-pentacene and amorphous 5,6,11,12-tetraphenyltetracene) exhibit eSRs with an Arrhenius-like temperature dependence, each with two characteristic energy scales similar to those expected from vibrations. Polycrystalline tris(8-hydroxyquinolate)gallium shows a similar behavior. The observed eSR for these molecules is no greater than 0.85 MHz at 300 K. The variety of crystal structures and transport regimes that these molecules possess, as well as the local nature of the probe, strongly suggest an intra-molecular phenomenon general to many organic semiconductors, contrasting the commonly assumed spin relaxation models based on inter-molecular charge carrier transport.

cond-mat.mtrl-sci↗

arXiv2010

Giant Thermoelectric Effect from Transmission Supernodes

We predict an enormous order-dependent quantum enhancement of thermoelectric effects in the vicinity of a higher-order `supernode' in the transmission spectrum of a nanoscale junction. Single-molecule junctions based on 3,3'-biphenyl and polyphenyl ether (PPE) are investigated in detail. The nonequilibrium thermodynamic efficiency and power output of a thermoelectric heat engine based on a 1,3-benzene junction are calculated using many-body theory, and compared to the predictions of the figure-of-merit ZT.

cond-mat.mes-hall↗

arXiv2009

Determining the Energy Barrier for Decay out of Superdeformed Bands

An asymptotically exact quantum mechanical calculation of the matrix elements for tunneling through an asymmetric barrier is combined with the two-state statistical model for decay out of superdeformed bands to determine the energy barrier (as a function of spin) separating the superdeformed and normal-deformed wells for several nuclei in the 190 and 150 mass regions. The spin-dependence of the barrier leading to sudden decay out is shown to be consistent with the decrease of a centrifugal barrier with decreasing angular momentum. Values of the barrier frequency in the two mass regions are predicted.

nucl-th↗

arXiv2008

Many-body treatment of quantum transport through single molecules

We develop a theoretical approach to quantum transport through single conjugated organic molecules that accurately accounts for all molecular excited and ground states via a semi-empirical many-body molecular Hamiltonian. We then calculate the linear and non-linear transport properties of a benzenedithiol molecule covalently bonded to two gold electrodes at room temperature, eliminating all free parameters by comparing the calculated thermopower and linear-conductance with experiment. The resulting `molecular diamond' structure exhibits experimentally observed many-body effects inaccessible to mean-field approaches.

cond-mat.mtrl-sci↗

arXiv2008

Many-body theory of electronic transport in single-molecule heterojunctions

A many-body theory of molecular junction transport based on nonequilibrium Green's functions is developed, which treats coherent quantum effects and Coulomb interactions on an equal footing. The central quantity of the many-body theory is the Coulomb self-energy matrix $Σ_{\rm C}$ of the junction. $Σ_{\rm C}$ is evaluated exactly in the sequential tunneling limit, and the correction due to finite tunneling width is evaluated self-consistently using a conserving approximation based on diagrammatic perturbation theory on the Keldysh contour. Our approach reproduces the key features of both the Coulomb blockade and coherent transport regimes simultaneously in a single unified transport theory. As a first application of our theory, we have calculated the thermoelectric power and differential conductance spectrum of a benzenedithiol-gold junction using a semi-empirical $π$-electron Hamiltonian that accurately describes the full spectrum of electronic excitations of the molecule up to 8--10eV.

cond-mat.mes-hall↗

arXiv2008

Proposal for a nanoscale variable resistor/electromechanical transistor

A nanoscale variable resistor consisting of a metal nanowire (active element), a dielectric, and a gate, is proposed. By means of the gate voltage, stochastic transitions between different conducting states of the nanowire can be induced, with a switching time as fast as picoseconds. With an appropriate choice of dielectric, the transconductance of the device, which may also be considered an ``electromechanical transistor,'' is shown to significantly exceed the conductance quantum G_0=2e^2/h, a remarkable figure of merit for a nanoscale device.

cond-mat.mes-hall↗

arXiv2008

The Order of Phase Transitions in Barrier Crossing

A spatially extended classical system with metastable states subject to weak spatiotemporal noise can exhibit a transition in its activation behavior when one or more external parameters are varied. Depending on the potential, the transition can be first or second-order, but there exists no systematic theory of the relation between the order of the transition and the shape of the potential barrier. In this paper, we address that question in detail for a general class of systems whose order parameter is describable by a classical field that can vary both in space and time, and whose zero-noise dynamics are governed by a smooth polynomial potential. We show that a quartic potential barrier can only have second-order transitions, confirming an earlier conjecture [1]. We then derive, through a combination of analytical and numerical arguments, both necessary conditions and sufficient conditions to have a first-order vs. a second-order transition in noise-induced activation behavior, for a large class of systems with smooth polynomial potentials of arbitrary order. We find in particular that the order of the transition is especially sensitive to the potential behavior near the top of the barrier.

cond-mat.stat-mech↗

arXiv2007

Universality of Decay out of Superdeformed Bands in the 190 Mass Region

Superdeformed nuclei in the 190 mass region exhibit a striking universality in their decay-out profiles. We show that this universality can be explained in the two-level model of superdeformed decay as related to a strong separation of energy scales: a higher scale related to the nuclear interactions, and a lower scale caused by electromagnetic decay. Furthermore, we present the results of the two-level model for all decays for which sufficient data are known, including statistical extraction of the matrix element for tunneling through the potential barrier.

nucl-th↗

arXiv2007

Scaling Theory of the Peierls-CDW in Metal Nanowires

The Peierls instability in multi-channel metal nanowires is investigated. Hyperscaling relations are established for the finite-size-, temperature-, and wavevector-scaling of the electronic free energy. It is shown that the softening of surface modes at wavevector $q=2k_{F,ν}$ leads to critical fluctuations of the wire's radius at zero temperature, where $k_{F,ν}$ is the Fermi wavevector of the highest occupied channel. This Peierls charge density wave emerges as the system size becomes comparable to the channel correlation length. Although the Peierls instability is weak in metal nanowires, in the sense that the correlation length is exponentially long, we predict that nanowires fabricated by current techniques can be driven into the charge-density-wave regime under strain.

cond-mat.mes-hall↗

arXiv2007

Electronic and atomic shell structure in aluminum nanowires

We report experiments on aluminum nanowires in ultra-high vacuum at room temperature that reveal a periodic spectrum of exceptionally stable structures. Two "magic" series of stable structures are observed: At low conductance, the formation of stable nanowires is governed by electronic shell effects whereas for larger contacts atomic packing dominates. The crossover between the two regimes is found to be smooth. A detailed comparison of the experimental results to a theoretical stability analysis indicates that while the main features of the observed electron-shell structure are similar to those of alkali and noble metals, a sequence of extremely stable wires plays a unique role in Aluminum. This series appears isolated in conductance histograms and can be attributed to "superdeformed" non-axisymmetric nanowires.

cond-mat.mes-hall↗

arXiv2006

Rabi Oscillations at Exceptional Points in Microwave Billiards

We experimentally investigated the decay behavior with time t of resonances near and at exceptional points, where two complex eigenvalues and also the associated eigenfunctions coalesce. The measurements were performed with a dissipative microwave billiard, whose shape depends on two parameters. The t^2-dependence predicted at the exceptional point on the basis of a two-state matrix model could be verified. Outside the exceptional point the predicted Rabi oscillations, also called quantum echoes in this context, were detected. To our knowledge this is the first time that quantum echoes related to exceptional points were observed experimentally.

cond-mat.other↗

arXiv2006

Cohesion, Conductance, and Charging Effects in a Metallic Nanocontact

The conducting and thermodynamic properties of ballistic metallic nanocontacts with smooth shapes are investigated. All properties are related to the electronic scattering matrix, which is evaluated in the WKB approximation for independent electrons and in the self-consistent Hartree approximation for interacting electrons. Mesoscopic oscillations of order 1nN in the cohesive force and of order e in the contact charge are predicted when a metallic nanocontact is pulled apart, which are synchronized with quantized jumps in the conductance.

cond-mat.mes-hall↗

arXiv2006

Universality in metallic nanocohesion: a quantum chaos approach

Convergent semiclassical trace formulae for the density of states and cohesive force of a narrow constriction in an electron gas, whose classical motion is either chaotic or integrable, are derived. It is shown that mode quantization in a metallic point contact or nanowire leads to universal oscillations in its cohesive force: the amplitude of the oscillations depends only on a dimensionless quantum parameter describing the crossover from chaotic to integrable motion, and is of order 1 nano-Newton, in agreement with recent experiments. Interestingly, quantum tunneling is shown to be described quantitatively in terms of the instability of the classical periodic orbits.

cond-mat.mes-hall↗