Coherent laser control of the current through molecular junctions

The electron tunneling through a molecular junction modeled by a single site weakly coupled to two leads is studied in the presence of a time-dependent external field using a master equation approach. In the case of small bias voltages and high carrier frequencies of the external field, we observe the phenomenon of coherent destruction of tunneling, i.e. the current through the molecular junction vanishes completely for certain parameters of the external field. In previous studies the tunneling within isolated and open multi-site systems was suppressed; it is shown here that the tunneling between a single site and electronic reservoirs, i.e. the leads, can be suppressed as well. For larger bias voltages the current does not vanish any more since further tunneling channels participate in the electron conduction and we also observe photon-assisted tunneling which leads to steps in the current-voltage characteristics. The described phenomena are demonstrated not only for monochromatic fields but also for laser pulses and therefore could be used for ultrafast optical switching of the current through molecular junctions.Comment: 6 pages and 4 figure

Switching the current through molecular wires

The influence of Gaussian laser pulses on the transport through molecular wires is investigated within a tight-binding model for spinless electrons including correlation. Motivated by the phenomenon of coherent destruction of tunneling for monochromatic laser fields, situations are studied in which the maximum amplitude of the electric field fulfills the conditions for the destructive quantum effect. It is shown that, as for monochromatic laser pulses, the average current through the wire can be suppressed. For parameters of the model, which do not show a net current without any optical field, a Gaussian laser pulse can establish a temporary current. In addition, the effect of electron correlation on the current is investigated.Comment: 8 pages, 6 figure

Comparison of two models for bridge-assisted charge transfer

Based on the reduced density matrix method, we compare two different approaches to calculate the dynamics of the electron transfer in systems with donor, bridge, and acceptor. In the first approach a vibrational substructure is taken into account for each electronic state and the corresponding states are displaced along a common reaction coordinate. In the second approach it is assumed that vibrational relaxation is much faster than the electron transfer and therefore the states are modeled by electronic levels only. In both approaches the system is coupled to a bath of harmonic oscillators but the way of relaxation is quite different. The theory is applied to the electron transfer in ${\rm H_2P}-{\rm ZnP}-{\rm Q}$ with free-base porphyrin (${\rm H_2P}$) being the donor, zinc porphyrin (${\rm ZnP}$) being the bridge and quinone (${\rm Q}$) the acceptor. The parameters are chosen as similar as possible for both approaches and the quality of the agreement is discussed.Comment: 12 pages including 4 figures, 1 table, 26 references. For more info see http://eee.tu-chemnitz.de/~kili

The size of two-body weakly bound objects : short versus long range potentials

The variation of the size of two-body objects is investigated, as the separation energy approaches zero, with both long range potentials and short range potentials having a repulsive core. It is shown that long range potentials can also give rise to very extended systems. The asymptotic laws derived for states with angular momentum l=1,2 differ from the ones obtained with short range potentials. The sensitivity of the asymptotic laws on the shape and length of short range potentials defined by two and three parameters is studied. These ideas as well as the transition from the short to the long range regime for the l=0 case are illustrated using the Kratzer potential.Comment: 5 pages, 3 figures, submitted to Physical Review Letter

To wet or not to wet: that is the question

Wetting transitions have been predicted and observed to occur for various combinations of fluids and surfaces. This paper describes the origin of such transitions, for liquid films on solid surfaces, in terms of the gas-surface interaction potentials V(r), which depend on the specific adsorption system. The transitions of light inert gases and H2 molecules on alkali metal surfaces have been explored extensively and are relatively well understood in terms of the least attractive adsorption interactions in nature. Much less thoroughly investigated are wetting transitions of Hg, water, heavy inert gases and other molecular films. The basic idea is that nonwetting occurs, for energetic reasons, if the adsorption potential's well-depth D is smaller than, or comparable to, the well-depth of the adsorbate-adsorbate mutual interaction. At the wetting temperature, Tw, the transition to wetting occurs, for entropic reasons, when the liquid's surface tension is sufficiently small that the free energy cost in forming a thick film is sufficiently compensated by the fluid- surface interaction energy. Guidelines useful for exploring wetting transitions of other systems are analyzed, in terms of generic criteria involving the "simple model", which yields results in terms of gas-surface interaction parameters and thermodynamic properties of the bulk adsorbate.Comment: Article accepted for publication in J. Low Temp. Phy

Atoms to phenotypes: Molecular design principles of cellular energy metabolism

We report a 100-million atom-scale model of an entire cell organelle, a photosynthetic chromatophore vesicle from a purple bacterium, that reveals the cascade of energy conversion steps culminating in the generation of ATP from sunlight. Molecular dynamics simulations of this vesicle elucidate how the integral membrane complexes influence local curvature to tune photoexcitation of pigments. Brownian dynamics of small molecules within the chromatophore probe the mechanisms of directional charge transport under various pH and salinity conditions. Reproducing phenotypic properties from atomistic details, a kinetic model evinces that low-light adaptations of the bacterium emerge as a spontaneous outcome of optimizing the balance between the chromatophore’s structural integrity and robust energy conversion. Parallels are drawn with the more universal mitochondrial bioenergetic machinery, from whence molecular-scale insights into the mechanism of cellular aging are inferred. Together, our integrative method and spectroscopic experiments pave the way to first-principles modeling of whole living cells