Time-dependent quantum transport: causal superfermions, exact fermion-parity protected decay mode, and Pauli exclusion principle for mixed quantum states

We extend the recently developed causal superfermion approach to the real-time transport theory to time-dependent decay problems.Its usefulness is illustrated for the Anderson model of a quantum dot with tunneling rates depending on spin due to the ferromagnetic electrodes and/or spin polarization of the tunnel junction. We set up a second quantization scheme for density operators in the Liouville-Fock space constructing causal field superoperators using the fundamental physical principles of causality/probability conservation and the fermion-parity superselection (univalence). The time-dependent perturbation series for the time-evolution is renormalized by explicitly performing the wide-band limit on the superoperator level. The short and long-time reservoir correlations are shown to be tightly linked to the occurrence of causal field destruction and creation superoperators, respectively. The effective theory takes as a reference a damped local system, providing an interesting starting point for numerical calculations of memory kernels in real-time. A remarkable feature of this approach is the natural appearance of a measurable fermion-parity protected decay mode. It already can be calculated exactly in the Markovian, infinite temperature limit by leading order perturbation theory, yet persists unaltered for the finite temperature, interaction and tunneling spin polarization. Furthermore, we show how a Liouville-space analog of the Pauli principle directly leads to the exact result in the noninteracting limit: surprisingly, it is obtained in finite (second) order renormalized perturbation theory, both for the self-energy as well as the time-evolution propagator. For this limit we calculate the time-evolution of the full density operator starting from an arbitrary initial state on the quantum dot, including spin and pairing coherences and two-particle correlations.Comment: This version contains the more extensive introduction and the conclusion, discussing an experimental relevance of the obtained exact result for the new decay mode. A lot of new references have been added. The more detailed comparison of the results obtained for the noninteracting case with the known results has been done. Small typos have been fixe

Transport signature of pseudo-Jahn-Teller dynamics in a single-molecule transistor

We calculate the electronic transport through a molecular dimer, in which an excess electron is delocalized over equivalent monomers, which can be locally distorted. In this system the Born-Oppenheimer approximation breaks down resulting in quantum entanglement of the mechanical and electronic motion. We show that pseudo Jahn-Teller (pJT) dynamics of the molecule gives rise to conductance peaks that indicate this violation. Their magnitude, sign and position sharply depend on the electro-mechanical properties of the molecule, which can be varied in recently developed three-terminal junctions with mechanical control. The predicted effect depends crucially on the degree of intramolecular delocalization of the excess electron, a parameter which is also of fundamental importance in physical chemistry.Comment: 6 pages, 3 figure

Fermion-parity duality and energy relaxation in interacting open systems

We study the transient heat current out of a confined electron system into a weakly coupled electrode in response to a voltage switch. We show that the decay of the Coulomb interaction energy for this repulsive system exhibits signatures of electron-electron attraction, and is governed by an interaction-independent rate. This can only be understood from a general duality that relates the non-unitary evolution of a quantum system to that of a dual model with inverted energies. Deriving from the fermion-parity superselection postulate, this duality applies to a large class of open systems.Comment: 5 pages + 19 pages of Supplementary Materia

Coherent and incoherent pumping of electrons in double quantum dots

We propose a new mode of operation of an electron pump consisting of two weakly coupled quantum dots connected to reservoirs. An electron can be transferred within the device at zero bias voltage when it is subjected to electromagnetic radiation, thereby exciting the double dot. The excited state can decay by transferring charge from one lead and to the other lead in one direction. Depending on the energies of the intermediate states in the pumping cycle, which are controlled by the gate voltages, this transport is either incoherent via well-known sequential tunneling processes, or coherent via a inelastic co-tunneling process. The latter novel mode of operation is possible only when interdot Coulomb charging is important. The D.C. transport through the system can be controlled by the frequency of the applied radiation. We concentrate on the resonant case, when the frequency matches the energy difference for exciting an electron from one dot into the other. The resonant peaks in the pumping current should be experimentally observable. We have developed a density matrix approach which describes the dynamics of the system on timescales much larger than the period of the applied irradiation. In contrast to previous works we additionally consider the case of slow modulation of the irradiation amplitude. Harmonic modulation produces additional sidepeaks in the photoresponse, and pulsed modulation can be used to resolve the Rabi frequency in the time-averaged current.Comment: 5 pages, 6 figures. This is an extension of cond-mat/9707310 "A coherent double-quantum-dot electron pump" This version has been accepted for publication in Phys. Rev. B. Changes: Added references. Corrected typos. Changed content mainly the introduction. Regime of device operation is now specified more precisely. A stability diagram has been added as a figure has been adde

Charge fluctuations in nonlinear heat transport

We show that charge fluctuation processes are crucial for the nonlinear heat conductance through an interacting nanostructure, even far from a resonance. We illustrate this for an Anderson quantum dot accounting for the first two leading orders of the tunneling in a master equation. The often made assumption that off-resonant transport proceeds entirely by virtual occupation of charge states, underlying exchange-scattering models, can fail dramatically for heat transport. The identified energy-transport resonances in the Coulomb blockade regime provide new qualitative information about relaxation processes, for instance by strong negative differential heat conductance relative to the heat current. These can go unnoticed in the charge current, making nonlinear heat-transport spectroscopy with energy-level control a promising experimental tool

Vibrational detection and control of spin in mixed-valence molecular transistors

We investigate electron transport through a mixed-valence molecular complex in which an excess electron can tunnel between hetero-valent transition metal ions, each having a fixed localized spin. We show that in this class of molecules the interplay of the spins and the vibrational breathing modes of the ionic ligand-shells allows the total molecular spin to be detected as well as controlled by nonequilibrium transport. Due to a spin-dependent pseudo Jahn-Teller effect electronic transitions with different spin values can be distinguished by their vibronic conductance side peaks, without using an external magnetic field. Conversely, we show that the spin state of the entire molecule can also be controlled via the nonequilibrium quantized molecular vibrations due to a vibration-induced spin-blockade.Comment: 6 pages, 3 figure

Quantum dot occupation and electron dwell time in the cotunneling regime

We present comparative measurements of the charge occupation and conductance of a GaAs/AlGaAs quantum dot. The dot charge is measured with a capacitively coupled quantum point contact sensor. In the single-level Coulomb blockade regime near equilibrium, charge and conductance signals are found to be proportional to each other. We conclude that in this regime, the two signals give equivalent information about the quantum dot system. Out of equilibrium, we study the inelastic-cotunneling regime. We compare the measured differential dot charge with an estimate assuming a dwell time of transmitted carriers on the dot given by h/E, where E is the blockade energy of first-order tunneling. The measured signal is of a similar magnitude as the estimate, compatible with a picture of cotunneling as transmission through a virtual intermediate state with a short lifetime

Pumping of vibrational excitations in a Coulomb blockaded suspended carbon nanotube

Low-temperature transport spectroscopy measurements on a suspended few-hole carbon nanotube quantum dot are presented, showing a gate-dependent harmonic excitation spectrum which, strikingly, occurs in the Coulomb blockade regime. The quantized excitation energy corresponds to the scale expected for longitudinal vibrations of the nanotube. The electronic transport processes are identified as cotunnel-assisted sequential tunneling, resulting from non-equilibrium occupation of the mechanical mode. They appear only above a high-bias threshold at the scale of electronic nanotube excitations. We discuss models for the pumping process that explain the enhancement of the non-equilibrium occupation and show that it is connected to a subtle interplay between electronic and vibrational degrees of freedom

Electron transport through single Mn12 molecular magnets

We report transport measurements through a single-molecule magnet, the Mn12 derivative [Mn12O12(O2C-C6H4-SAc)16(H2O)4], in a single-molecule transistor geometry. Thiol groups connect the molecule to gold electrodes that are fabricated by electromigration. Striking observations are regions of complete current suppression and excitations of negative differential conductance on the energy scale of the anisotropy barrier of the molecule. Transport calculations, taking into account the high-spin ground state and magnetic excitations of the molecule, reveal a blocking mechanism of the current involving non-degenerate spin multiplets.Comment: Accepted for Phys. Rev. Lett., 5 pages, 4 figure