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Register a new userNonequilibrium transport through magnetic vibrating molecules
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Pablo Roura-Bas Dr.
Publication date
2013
fields
Physics
and research's language is
English
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We calculate the nonequilibrium conductance through a molecule or a quantum dot in which the occupation of the relevant electronic level is coupled with intensity $lambda$ to a phonon mode, and also to two conducting leads. The system is described by the Anderson-Holstein Hamiltonian. We solve the problem using the Keldysh formalism and the non-crossing approximation (NCA) for both, the electron-electron and the electron-phonon interactions. We obtain a moderate decrease of the Kondo temperature $T_K$ with $lambda$ for fixed renormalized energy of the localized level $tilde{E_d}$. The meaning and value of $tilde{E_d}$ are discussed. The spectral density of localized electrons shows in addition to the Kondo peak of width $2 T_K$, satellites of this peak shifted by multiples of the phonon frequency $ omega_0$. The nonequilibrium conductance as a function of bias voltage $V_b$ at small temperatures, also displays peaks at multiples of $omega_0$ in addition to the central dominant Kondo peak near $V_b=0$.
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We employ the functional renormalization group to study the effects of phonon-assisted tunneling on the nonequilibrium steady-state transport through a single level molecular quantum dot coupled to electronic leads. Within the framework of the spinless Anderson-Holstein model, we focus on small to intermediate electron-phonon couplings, and we explore the evolution from the adiabatic to the antiadiabatic limit and also from the low-temperature non-perturbative regime to the high temperature perturbative one. We identify the phononic signatures in the bias-voltage dependence of the electrical current and the differential conductance. Considering a temperature gradient between the electronic leads, we further investigate the interplay between the transport of charge and heat. Within the linear response regime, we compare the temperature dependence of various thermoelectric coefficients to our earlier results obtained within the numerical renormalization group [Phys.~Rev.~B {bf 96}, 195156 (2017)]. Beyond the linear response regime, in the context of thermoelectric generators, we discuss the influence of molecular vibrations on the output power and the efficiency. We find that the molecular energy dissipation, which is inevitable in the presence of phonons, is significantly suppressed in the antiadiabatic limit resulting in the enhancement of the thermoelectric efficiency.
Nonequilibrium properties of correlated quantum matter are being intensively investigated because of the rich interplay between external driving and the many-body correlations. Of particular interest is the nonequilibrium behavior near a quantum critical point (QCP), where the system is delicately balanced between different ground states. We present both an analytical calculation of the nonequilibrium steady-state current in a critical system and experimental results to which the theory is compared. The system is a quantum dot coupled to resistive leads: a spinless resonant level interacting with an ohmic dissipative environment. A two channel Kondo-like QCP occurs when the level is on resonance and symmetrically coupled to the leads, conditions achieved by fine-tuning using electrostatic gates. We calculate and measure the nonlinear current as a function of bias ($I$-$V$ curve) at the critical values of the gate voltages corresponding to the QCP. The quantitative agreement between the experimental data and the theory, with no fitting parameter, is excellent. As our system is fully accessible to both theory and experiment, it provides an ideal setting for addressing nonequilibrium phenomena in correlated quantum matter.
We study the transport through a molecular junction exhibiting interference effects. We show that these effects can still be observed in the presence of molecular vibrations if Coulomb repulsion is taken into account. In the Kondo regime, the conductance of the junction can be changed by several orders of magnitude by tuning the levels of the molecule, or displacing a contact between two atoms, from nearly perfect destructive interference to values of the order of 2e 2 /h expected in Kondo systems. We also show that this large conductance change is robust for reasonable temperatures and voltages for symmetric and asymmetric tunnel couplings between the source-drain electrodes and the molecular orbitals. This is relevant for the development of quantum interference effect transistors based on molecular junctions.
We propose a novel approach to nonequilibrium real-time dynamics of quantum impurities models coupled to biased non-interacting leads, such as those relevant to quantum transport in nanoscale molecular devices. The method is based on a Diagrammatic Monte Carlo sampling of the real-time perturbation theory along the Keldysh contour. We benchmark the method on a non-interacting resonant level model and, as a first non-trivial application, we study zero temperature non-equilibrium transport through a vibrating molecule.
Magnetic oscillation is a generic property of electronic conductors under magnetic fields and widely appreciated as a useful probe of their electronic band structure, i.e., the Fermi surface geometry. However, the usage of the strong static magnetic field makes the measurement insensitive to the magnetic order of the target material. That is, the magnetic order is anyhow turned into a forced ferromagnetic one. Here we theoretically propose an experimental method of measuring the magnetic oscillation in a magnetic-order-resolved way by using the azimuthal cylindrical vector (CV) beam, an example of topological lightwaves. The azimuthal CV beam is unique in that when focused tightly, it develops a pure longitudinal magnetic field. We argue that this characteristic focusing property and the discrepancy in the relaxation timescale between conduction electrons and localized magnetic moments allow us to develop the nonequilibrium analog of the magnetic oscillation measurement. Our optical method would be also applicable to metals the under ultra-high pressure of diamond anvil cells.
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