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Register a new userElectron transfer in the nonadiabatic regime: Crossover from quantum-mechanical to classical behaviour
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Authors
G. Lang
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We study nonadiabatic electron transfer within the biased spin-boson model. We calculate the incoherent transfer rate in analytic form at all temperatures for a power law form of the spectral density of the solvent coupling. In the Ohmic case, we present the exact low temperature corrections to the zero temperature rate for arbitrarily large bias energies between the two redox sites. Both for Ohmic and non-Ohmic coupling, we give the rate in the entire regime extending from zero temperature, where the rate depends significantly on the detailed spectral behaviour, via the crossover region, up to the classical regime. For low temperatures, the rate shows characteristic quantum features, in particular the shift of the rate maximum to a bias value below the reorganization energy, and the asymmetry of the rate around the maximum. We study in detail the gradual extinction of the quantum features as temperature is increased.
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We discuss the semiclassical and classical character of the dynamics of a single spin 1/2 coupled to a bath of noninteracting spins 1/2. On the semiclassical level, we extend our previous approach presented in D. Stanek, C. Raas, and G. S. Uhrig, Phys. Rev. B 88, 155305 (2013) by the explicit consideration of the conservation of the total spin. On the classical level, we compare the results of the classical equations of motions in absence and presence of an external field to the full quantum result obtained by density-matrix renormalization (DMRG). We show that for large bath sizes and not too low magnetic field the classical dynamics, averaged over Gaussian distributed initial spin vectors, agrees quantitatively with the quantum-mechanical one. This observation paves the way for an efficient approach for certain parameter regimes.
The two-dimensional cage model for polymer motion is discussed with an emphasis on the effect of sideways motions, which cross the barriers imposed by the lattice. Using the Density Matrix Method as a solver of the Master Equation, the renewal time and the diffusion coefficient are calculated as a function of the strength of the barrier crossings. A strong crossover influence of the barrier crossings is found and it is analyzed in terms of effective exponents for a given chain length. The crossover scaling functions and the crossover scaling exponents are calculated.
Recently, macroscopic mechanical oscillators have been coaxed into a regime of quantum behavior, by direct refrigeration [1] or a combination of refrigeration and laser-like cooling [2, 3]. This exciting result has encouraged notions that mechanical oscillators may perform useful functions in the processing of quantum information with superconducting circuits [1, 4-7], either by serving as a quantum memory for the ephemeral state of a microwave field or by providing a quantum interface between otherwise incompatible systems [8, 9]. As yet, the transfer of an itinerant state or propagating mode of a microwave field to and from a mechanical oscillator has not been demonstrated owing to the inability to agilely turn on and off the interaction between microwave electricity and mechanical motion. Here we demonstrate that the state of an itinerant microwave field can be coherently transferred into, stored in, and retrieved from a mechanical oscillator with amplitudes at the single quanta level. Crucially, the time to capture and to retrieve the microwave state is shorter than the quantum state lifetime of the mechanical oscillator. In this quantum regime, the mechanical oscillator can both store and transduce quantum information.
We study a simple quantum mechanical symmetric donor-acceptor model for electron transfer (ET) with coupling to internal deformations. The model contains several basic properties found in biological ET in enzymes and photosynthetic centers; it produces tunnelling with hysteresis thus providing a simple explanation for the slowness of the reversed rate and the near 100% efficiency of ET in many biological systems. The model also provides a conceptual framework for the development of molecular electronics memory elements based on electrostatic architectures.
The competition between reptation and Rouse Dynamics is incorporated in the Rubinstein-Duke model for polymer motion by extending it with sideways motions, which cross barriers and create or annihilate hernias. Using the Density-Matrix Renormalization-Group Method as solver of the Master Equation, the renewal time and the diffusion coefficient are calculated as function of the length of the chain and the strength of the sideways motion. These new types of moves have a strong and delicate influence on the asymptotic behavior of long polymers. The effects are analyzed as function of the chain length in terms of effective exponents and crossover scaling functions.
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