We study the electrical conductance $G$ and the thermopower $S$ of single-molecule junctions, and reveal signatures of different transport mechanisms: off-resonant tunneling, on-resonant coherent (ballistic) motion, and multi-step hopping. These mechanisms are identified by studying the behavior of $G$ and $S$ while varying molecular length and temperature. Based on a simple one-dimensional model for molecular junctions, we derive approximate expressions for the thermopower in these different regimes. Analytical results are compared to numerical simulations, performed using a variant of Büttiker's probe technique, the so-called voltage-temperature probe, which allows us to phenomenologically introduce environmentally-induced elastic and inelastic electron scattering effects, while applying both voltage and temperature biases across the junction. We further simulate the thermopower of GC-rich DNA molecules with mediating A:T blocks, and manifest the tunneling-to-hopping crossover in both the electrical conductance and the thermopower, in accord with measurements by Y. Li et al., Nature Comm. 7, 11294 (2016).
We investigate the electrical conductance and thermopower of a quantum dot tunnel coupled to external leads described by an extension of the Anderson impurity model which takes into account the assisted hopping processes, i.e., the occupancy-dependence of the tunneling amplitudes. We provide analytical understanding based on scaling arguments and the Schrieffer-Wolff transformation, corroborated by detailed numerical calculations using the numerical renormalization group (NRG) method. The assisted hopping modifies the coupling to the two-particle state, which shifts the Kondo exchange coupling…
It is shown that for the hopping regime, the thermopowers in both finite two-terminal and three-terminal systems are governed by the edges of the samples. This is due to the fact that the energy transfer between a transport electron and a conducting terminal is determined by the site most strongly coupled to that terminal. One-dimensional systems with both nearest-neighbor and variable-range transport as well as certain types of two-dimensional systems, are considered. For a given sample, the changes in the thermopowers due to modifying the bulk are quite limited, compared with those of the co…
We study the thermopower of a disordered nanowire in the field effect transistor configuration. After a first paper devoted to the elastic coherent regime (Bosisio R., Fleury G. and Pichard J.-L. 2014 \textit{New J. Phys.} \textbf{16} 035004), we consider here the inelastic activated regime taking place at higher temperatures. In the case where charge transport is thermally assisted by phonons (Mott Variable Range Hopping regime), we use the Miller-Abrahams random resistor network model as recently adapted by Jiang et al. for thermoelectric transport. This approach previously used to study the…
Ultrathin layers of semiconducting molybdenum disulfide (MoS2) offer significant prospects in future electronic and optoelectronic applications. Although an increasing number of experiments bring light into the electronic transport properties of these crystals, their thermoelectric properties are much less known. In particular, thermoelectricity in chemical vapor deposition grown MoS2, which is more practical for wafer-scale applications, still remains unexplored. Here, for the first time, we investigate these properties in grown single layer MoS2. Micro-fabricated heaters and thermometers are…
The current - voltage dependence of the transverse tunneling current through the electron or hole traps in a DNA is investigated. The hopping of the charge between the sites of the trap and the charge-phonon coupling results in a staircase structure of the I-V curve. For typical parameters of the DNA molecule the energy characteristics of a DNA trap can be extracted from the I-V dependence, viz., for a small gate voltage the phonon frequency and for a large gate voltage the hopping integral can be found from the positions of the steps in the I-V curve. Formation of the polaronic state also res…
We study the electronic transport through short DNA chains with various sequences of base pairs between voltage-biased leads. The strong coupling of the charge carriers to local vibrations of the base pairs leads to the formation of polarons, and in the relevant temperature range the transport is accomplished by sequential polaron hopping. We calculate the rates for these processes, extending what is known as the $P(E)$-theory of single-electron tunneling to the situation with site-specific local oscillators. The non-equilibrium charge rearrangement along the DNA leads to sequence-dependent cu…
A theoretical study is presented to quantitatively analyze the transport experiment through individual DNA molecules reported recently by Porath {\it et al.} [Nature {\bf 403}, 635 (2000)]. A variety of valuable quantities are identified by contacting the theoretical model with the measured data. The partially decoherent nature on the GC pairs of DNA is elaborated in contrast to the completely incoherent hopping mechanism discussed in the context of charge transfer experiments.
In this work we investigate the interplay between coherent and incoherent charge transport in cytosine-guanine (GC) rich DNA molecules. Our objective is to introduce physically grounded approach to dephasing in large molecules and to understand the length dependent charge transport characteristics and especially the crossover from coherent tunneling to incoherent hopping regime at different temperatures. Therefore, we apply the vibronic dephasing model and compare the results to the Büttiker probe model which is commonly used to describe decoherence effects in charge transport. Using the full …
We investigate the thermopower of a metal-molecule-metal junction taking into account thermal effects on the junction. Based on analytical expressions and numerical simulations we show that the thermoelectric potential reveals valuable information on the mechanisms controlling the electron transfer process, including coherent transmission and thermalized hopping. We also show that at high temperatures the position of the Fermi energy relative to the molecular states can be easily deduced from the thermoelectric potential. Standard current-voltage measurements are insensitive to this informatio…
The electrical conductance of molecular junctions may strongly depend on the temperature, and weakly on molecular length, under two distinct mechanisms: phase-coherent resonant conduction, with charges proceeding via delocalized molecular orbitals, and incoherent thermally-assisted multi-step hopping. While in the case of coherent conduction the temperature dependence arises from the broadening of the Fermi distribution in the metal electrodes, in the latter case it corresponds to electron-vibration interaction effects on the junction. With the objective to distill the thermally-activated hopp…
Recent studies indicated that helical organic molecules, such as DNA and $α$-helical protein, can behave as Thouless quantum pumps when a rotating electric field is applied perpendicularly to their helical axes. Here we investigate the influence of long-range hoppings on this topological pumping of electrons in single-helical organic molecules. Under variation of the long-range hoppings governed by a decay exponent $μ$, we find an energy gap in the molecular band structure closes at a critical value $μ_c$ of the decay exponent and reopens for $μ$ deviating from $μ_c$. The relevant bulk bands i…
In many organic molecules the strong coupling of excess charges to vibrational modes leads to the formation of polarons, i.e., a localized state of a charge carrier and a molecular deformation. Incoherent hopping of polarons along the molecule is the dominant mechanism of transport at room temperature. We study the far-from-equilibrium situation where, due to the applied bias, the induced number of charge carriers on the molecule is high enough such that charge correlations become relevant. We develop a diagrammatic theory that exactly accounts for all many-particle correlations functions for …
First principle calculations of charge transfer in DNA molecules are computationally expensive given that charge carriers migrate in interaction with intra- and inter-molecular atomic motion. Screening sequences, e.g. to identify excellent electrical conductors is challenging even when adopting coarse-grained models and effective computational schemes that do not explicitly describe atomic dynamics. In this work, we present a machine learning (ML) model that allows the inexpensive prediction of the electrical conductance of millions of {\it long} double-stranded DNA (dsDNA) sequences, reducing…
This dissertation presents an investigation into the electrical properties of two types of G4-DNA and several DNA-based molecules, targeting them as candidates for molecular wires and devices. Atomic force microscopy (AFM) and electrostatic force microscopy (EFM) comparison of co-deposited tetra- and intra-molecular G4-DNA reveals variations in morphology and different sensitivity to the applied electric field, suggesting that the folding orientation of the strands affects the molecular structure, i.e. either the tetrad unit or the tetrad-tetrad stacking or both, and therefore the charge mobil…
We consider a polaron model where molecular \emph{rotations} are important. Here, the usual hopping between neighboring sites is affected directly by the electron-phonon interaction via a {\em twist-dependent} hopping amplitude. This model may be of relevance for electronic transport in complex molecules and polymers with torsional degrees of freedom, such as DNA, as well as in molecular electronics experiments where molecular twist motion is significant. We use a tight-binding representation and find that very different polaronic properties are already exhibited by a two-site model -- these a…
