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Register a new userOn the theory of charge transport and entropic effects in solvated molecular junctions
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Experimental studies on single-molecule junctions are typically in need of a simple theoretical approach that can reproduce or be fitted to experimentally measured transport data. In this context, the single-level variant of the Landauer approach is most commonly used but methods based on Marcus theory are also gaining in popularity. Recently, a generalized theory unifying these two approaches has also been developed. In the present work, we extend this theory so that it includes entropic effects (which can be important when polar solvents are involved, but are likely minor for solid-state systems). We investigate the temperature-dependence of the electric current and compare it to the behavior predicted by the Landauer and the conventional Marcus theory. We argue that this generalized theory provides a simple yet effective framework for understanding charge transport through molecular junctions. Furthermore, we explore the role of the entropic effects in different transport regimes and suggest experimental criteria for detecting them in solvated molecular junctions. Lastly, in order to account for nuclear tunnelling effects, we also demonstrate how lifetime broadening can be introduced into the Marcus-Levich-Dogonadze-Jortner-type description of electron transport.
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Introduction (2) Experimental background: Test beds (8) Theoretical approaches: A microscopic model(10) The electron-phonon coupling(14)Time and energy scales(15) Theoretical methods(19)Numerical calculations(28) Incoherent vs. coherent transport (28) Inelastic tunneling spectroscopy: Experimental background(31) Theoretical considerations:the weak coupling limit(36) Theoretical considerations: moderately strong coupling(41)Comparison of approximation schemes(48)Asymmetry in IETS(51)The origin of dips in IETS signals(53)Computational approaches (56) Effects of electron-electron(e-e)interactions (63) Noise (66) Non-linear conductance phenomena (73) Heating and heat conduction: General considerations(77) Heat generation(81) Heat conduction(85) Junction temperature(88) Current induced reactions (91) Summary and outlook (91)
We present the results of theoretical study of Current-Phase Relations (CPR) in Josephson junctions of SIsFS type, where S is a bulk superconductor and IsF is a complex weak link consisting of a superconducting film s, a metallic ferromagnet F and an insulating barrier I. We calculate the relationship between Josephson current and phase difference. At temperatures close to critical, calculations are performed analytically in the frame of the Ginsburg-Landau equations. At low temperatures numerical method is developed to solve selfconsistently the Usadel equations in the structure. We demonstrate that SIsFS junctions have several distinct regimes of supercurrent transport and we examine spatial distributions of the pair potential across the structure in different regimes. We study the crossover between these regimes which is caused by shifting the location of a weak link from the tunnel barrier I to the F-layer. We show that strong deviations of the CPR from sinusoidal shape occur even in a vicinity of Tc, and these deviations are strongest in the crossover regime. We demonstrate the existence of temperature-induced crossover between 0 and pi states in the contact and show that smoothness of this transition strongly depends on the CPR shape.
We solve the coherent multiple Andreev reflection (MAR) problem and calculate current-voltage characteristics (IVCs) for Josephson SINIS junctions, where S are local-equilibrium superconducting reservoirs, I denotes tunnel barriers, and N is a short diffusive normal wire, the length of which is much smaller than the coherence length, and the resistance is much smaller than the resistance of the tunnel barriers. The charge transport regime in such junctions qualitatively depends on a characteristic value gamma = Delta tau_d of relative phase shifts between the electrons and retro-reflected holes accumulated during the dwell time tau_d. In the limit of small electron-hole dephasing gamma << 1, our solution recovers a known formula for a short mesoscopic connector extended to the MAR regime. At large dephasing, the subharmonic gap structure in the IVC scales with 1/ gamma, which thus plays the role of an effective tunneling parameter. In this limit, the even gap subharmonics are resonantly enhanced, and the IVC exhibits portions with negative differential resistance.
The conductance of single molecule junctions is calculated using a Landauer approach combined to many-body perturbation theory MBPT) to account for electron correlation. The mere correction of the density-functional theory eigenvalues, which is the standard procedure for quasiparticle calculations within MBPT, is found not to affect noticeably the zero-bias conductance. To reduce it and so improve the agreement with the experiments, the wavefunctions also need to be updated by including the non-diagonal elements of the self-energy operator.
We present a novel optical transient absorption and reflection microscope based on a diffraction-limited pump pulse in combination with a wide-field probe pulse, for the spatio-temporal investigation of ultrafast population transport in thin films. The microscope achieves a temporal resolution down to 12 fs and simultaneously provides sub-10 nm spatial accuracy. We demonstrate the capabilities of the microscope by revealing an ultrafast excited-state exciton population transport of up to 32 nm in a thin film of pentacene and by tracking the carrier motion in p-doped silicon. The use of few-cycle optical excitation pulses enables impulsive stimulated Raman micro-spectroscopy, which is used for in-situ verification of the chemical identity in the 100 - 2000 cm-1 spectral window. Our methodology bridges the gap between optical microscopy and spectroscopy allowing for the study of ultrafast transport properties down to the nanometer length scale.
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