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Charles A. Stafford

Publications and source records attributed to Charles A. Stafford.

27 records · Page 2Linked to original sources

On Transmission Node Structure in Interacting Systems

We provide a series of generic results regarding the structure of nodes in the retarded Green's function G of an interacting system, as exemplified by the extended Hubbard model. In particular: (1) due to an incompatibility between interactions of nearly any form and a precise definition of series propagation, degenerate geometric nodes are split or lifted by interactions; (2) degenerate nodes generically exist at the boundary between regimes of node splitting and node lifting and, in the presence of interactions, they require fine-tuning; (3) degenerate nodes are highly sensitive to perturbation and their sensitivity increases with their degeneracy. Moreover, for high degeneracies there is a tendency toward lifting rather than splitting. We also propose a characterization of the node structure in extended Hubbard models at arbitrary filling in terms of either the eigenvalues of G, or equivalently, the roots of a polynomial. This shows that "Mott nodes" previously predicted to occur in the transmission spectra of molecular radicals are fundamentally associated with nodes in the eigenvalues of the retarded Green's function that occur in open-shelled systems. This is accompanied by a low-energy two-pole approximation wherein each of the eigenvalues of G are mapped onto a Fermi-liquid-like renormalization of the Anderson model, for which the exact self-energy is provided.

cond-mat.mes-hall↗

Probing Maxwell's Demon with a Nanoscale Thermometer

A precise definition for a quantum electron thermometer is given, as an electron reservoir coupled locally (e.g., by tunneling) to a sample, and brought into electrical and thermal equilibrium with it. A realistic model of a scanning thermal microscope with atomic resolution is then developed, where the resolution is limited in ultrahigh vacuum by thermal coupling to the electromagnetic environment. We show that the temperatures of individual atomic orbitals or bonds in a conjugated molecule with a temperature gradient across it exhibit quantum oscillations, whose origin can be traced to a realization of Maxwell's demon at the single-molecule level. These oscillations may be understood in terms of the rules of covalence describing bonding in π-electron systems. Fourier's law of heat conduction is recovered as the resolution of the temperature probe is reduced, indicating that the macroscopic law emerges as a consequence of coarse graining.

cond-mat.mes-hall↗

Effective Field Theory of Interacting π-Electrons

We develop a π-electron effective field theory (π-EFT) wherein the two-body Hamiltonian for a π-electron system is expressed in terms of three effective parameters: the π-orbital quadrupole moment, the on-site repulsion, and a dielectric constant. As a first application of this π-EFT, we develop a model of screening in molecular junctions based on image multipole moments, and use this to investigate the reduction of the HOMO-LUMO gap of benzene. Beyond this, we also use π-EFT to calculate the differential conductance spectrum of the prototypical benzenedithiol-Au single-molecule junction and the π-electron contribution to the van der Waals interaction between benzene and a metallic electrode.

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Accuracy of density functionals for molecular electronics: the Anderson junction

The exact ground-state exchange-correlation functional of Kohn-Sham density functional theory yields the exact transmission through an Anderson junction at zero bias and temperature. The exact impurity charge susceptibility is used to construct the exact exchange-correlation potential. We analyze the successes and limitations of various types of approximations, including smooth and discontinuous functionals of the occupation, as well as symmetry-broken approaches.

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Kondo effect given exactly by density functional theory

Transport through an Anderson junction (two macroscopic electrodes coupled to an Anderson impurity) is dominated by a Kondo peak in the spectral function at zero temperature. The exact single-particle Kohn-Sham potential of density functional theory reproduces the linear transport exactly, despite the lack of a Kondo peak in its spectral function. Using Bethe ansatz techniques, we calculate this potential exactly for all coupling strengths, including the cross-over from mean-field behavior to charge quantization caused by the derivative discontinuity. A simple and accurate interpolation formula is also given.

cond-mat.mes-hall↗

Transmission eigenvalue distributions in highly-conductive molecular junctions

The transport through a quantum-scale device may be characterized by the transmission eigenvalues. These values constitute a junction PIN code where, for example, in single-atom metallic contacts the number of transmission channels is also the chemical valence of the atom. Recently, highly conductive single-molecule junctions (SMJ) with multiple transport channels have been formed from benzene molecules between Pt electrodes. Transport through these multi-channel SMJs is a probe of both the bonding properties at the lead-molecule interface and of the molecular symmetry. Here we utilize a many-body theory that properly describes the complementary nature of the charge carrier to calculate transport distributions through Pt-benzene-Pt junctions. We develop an effective field theory of interacting pi-electrons to accurately model the electrostatic influence of the leads and an ab initio tunneling model to describe the lead-molecule bonding. With this state-of-the-art many-body technique we calculate the transport using the full molecular spectrum and using an `isolated resonance approximation' for the molecular Green's function. We confirm that the number of transmission channels in a SMJ is equal to the degeneracy of the relevant molecular orbital. In addition, we demonstrate that the isolated resonance approximation is extremely accurate and determine that transport occurs predominantly via the HOMO orbital in Pt-benzene-Pt junctions. Finally, we show that the transport occurs in a lead-molecule coupling regime where the charge carriers are both particle-like and wave-like simultaneously, requiring a many-body description.

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The Quantum Interference Effect Transistor: Principles and Perspectives

We give a detailed discussion of the Quantum Interference Effect Transistor (QuIET), a proposed device which exploits interference between electron paths through aromatic molecules to modulate current flow. In the off state, perfect destructive interference stemming from the molecular symmetry blocks current, while in the on state, current is allowed to flow by locally introducing either decoherence or elastic scattering. Details of a model calculation demonstrating the efficacy of the QuIET are presented, and various fabrication scenarios are proposed, including the possibility of using conducting polymers to connect the QuIET with multiple leads.

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Quantum-Dot Cascade Laser: Proposal for an Ultra-Low-Threshold Semiconductor Laser

We propose a quantum-dot version of the quantum-well cascade laser of Faist et al. [Science {\bf 264}, 553 (1994)]. The elimination of single phonon decays by the three-dimensional confinement implies a several order-of-magnitude reduction in the threshold current. The requirements on dot size (10-20nm) and on dot density and uniformity [one coupled pair of dots per (180nm)^3 with 5% nonuniformity] are close to current technology.

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Resonant Photon-Assisted Tunneling Through a Double Quantum Dot: An Electron Pump From Spatial Rabi Oscillations

The time average of the fully nonlinear current through a double quantum dot, subject to an arbitrary combination of ac and dc voltages, is calculated exactly using the Keldysh nonequilibrium Green function technique. When driven on resonance, the system functions as an efficient electron pump due to Rabi oscillation between the dots. The pumping current is maximum when the coupling to the leads equals the Rabi frequency.

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