A Dynamical Theory of Electron Transfer: Crossover from Weak to Strong Electronic Coupling

We present a real-time path integral theory for the rate of electron transfer reactions. Using graph theoretic techniques, the dynamics is expressed in a formally exact way as a set of integral equations. With a simple approximation for the self-energy, the rate can then be computed analytically to all orders in the electronic coupling matrix element. We present results for the crossover region between weak (nonadiabatic) and strong (adiabatic) electronic coupling and show that this theory provides a rigorous justification for the salient features of the rate expected within conventional electron transfer theory. Nonetheless, we find distinct characteristics of quantum behavior even in the strongly adiabatic limit where classical rate theory is conventionally thought to be applicable. To our knowledge, this theory is the first systematic dynamical treatment of the full crossover region.Comment: 11 pages, LaTeX, 8 Postscript figures to be published in J. Chem. Phy

Is the direct observation of electronic coherence in electron transfer reactions possible?

The observability of electronic coherence in electron transfer reactions is discussed. We show that under appropriate circumstances large-amplitude oscillations can be found in the electronic occupation probabilities. The initial preparation of the system is of crucial importance for this effect, and we discuss conditions under which experiments detecting electronic coherence should be feasible. The Feynman-Vernon influence functional formalism is extended to examine more general and experimentally relevant initial preparations. Analytical expressions and path integral quantum dynamics simulations were developed to study the effects of various initial preparations on the observability of electronic coherence.Comment: 14 pages, 9 figures, to be published in J. Chem. Phy

Exact c-number Representation of Non-Markovian Quantum Dissipation

The reduced dynamics of a quantum system interacting with a linear heat bath finds an exact representation in terms of a stochastic Schr{\"o}dinger equation. All memory effects of the reservoir are transformed into noise correlations and mean-field friction. The classical limit of the resulting stochastic dynamics is shown to be a generalized Langevin equation, and conventional quantum state diffusion is recovered in the Born--Markov approximation. The non-Markovian exact dynamics, valid at arbitrary temperature and damping strength, is exemplified by an application to the dissipative two-state system.Comment: 4 pages, 2 figures. To be published in Phys. Rev. Let

Magnetic Field Dependent Tunneling in Glasses

We report on experiments giving evidence for quantum effects of electromagnetic flux in barium alumosilicate glass. In contrast to expectation, below 100 mK the dielectric response becomes sensitive to magnetic fields. The experimental findings include both, the complete lifting of the dielectric saturation by weak magnetic fields and oscillations of the dielectric response in the low temperature resonant regime. As origin of these effects we suggest that the magnetic induction field violates the time reversal invariance leading to a flux periodicity in the energy levels of tunneling systems. At low temperatures, this effect is strongly enhanced by the interaction between tunneling systems and thus becomes measurable.Comment: 4 pages, 4 figure

Real-Time-RG Analysis of the Dynamics of the Spin-Boson Model

Using a real-time renormalization group method we determine the complete dynamics of the spin-boson model with ohmic dissipation for coupling strengths $\alpha\lesssim 0.1-0.2$. We calculate the relaxation and dephasing time, the static susceptibility and correlation functions. Our results are consistent with quantum Monte Carlo simulations and the Shiba relation. We present for the first time reliable results for finite cutoff and finite bias in a regime where perturbation theory in $\alpha$ or in tunneling breaks down. Furthermore, an unambigious comparism to results from the Kondo model is achieved.Comment: 4 pages, 5 figures, 1 tabl

Spin Star as Switch for Quantum Networks

Quantum state transfer is an important task in quantum information processing. It is known that one can engineer the couplings of a one-dimensional spin chain to achieve the goal of perfect state transfer. To leverage the value of these spin chains, a spin star is potentially useful for connecting different parts of a quantum network. In this work, we extend the spin-chain engineering problem to the problems with a topology of a star network. We show that a permanently coupled spin star can function as a network switch for transferring quantum states selectively from one node to another by varying the local potentials only. Together with one-dimensional chains, this result allows applications of quantum state transfer be applied to more general quantum networks.Comment: 10 pages, 2 figur

Dynamical simulation of current fluctuations in a dissipative two-state system

Current fluctuations in a dissipative two-state system have been studied using a novel quantum dynamics simulation method. After a transformation of the path integrals, the tunneling dynamics is computed by deterministic integration over the real-time paths under the influence of colored noise. The nature of the transition from coherent to incoherent dynamics at low temperatures is re-examined.Comment: 4 pages, 4 figures; to appear in Phys. Rev. Letter

Dynamical control of correlated states in a square quantum dot

In the limit of low particle density, electrons confined to a quantum dot form strongly correlated states termed Wigner molecules, in which the Coulomb interaction causes the electrons to become highly localized in space. By using an effective model of Hubbard-type to describe these states, we investigate how an oscillatory electric field can drive the dynamics of a two-electron Wigner molecule held in a square quantum dot. We find that, for certain combinations of frequency and strength of the applied field, the tunneling between various charge configurations can be strongly quenched, and we relate this phenomenon to the presence of anti-crossings in the Floquet quasi-energy spectrum. We further obtain simple analytic expressions for the location of these anti-crossings, which allows the effective parameters for a given quantum dot to be directly measured in experiment, and suggests the exciting possibility of using ac-fields to control the time evolution of entangled states in mesoscopic devices.Comment: Replaced with version to be published in Phys. Rev.