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 incoherent transport through a finite system. We compute the transport properties of short sequences of DNA by expanding the diagrammatic theory up to second order in the hopping parameters. The correlations qualitatively modify the I-V characteristics as compared to those approaches where correlations are dealt with in a mean-field type approximation only.
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…
Quantum transport in disordered systems is studied using a polaron-based master equation. The polaron approach is capable of bridging the results from the coherent band-like transport regime governed by the Redfield equation to incoherent hopping transport in the classical regime. A non-monotonic dependence of the diffusion coefficient is observed both as a function of temperature and system-phonon coupling strength. In the band-like transport regime, the diffusion coefficient is shown to be linearly proportional to the system-phonon coupling strength, and vanishes at zero coupling due to Ande…
The small polaron theory is applied to describe the vibron dynamics in an adsorbed nanowire with a special emphasis onto finite size effects. It is shown that the finite size of the nanowire discriminates between side molecules and core molecules which experience a different dressing mechanism. Moreover, the inhomogeneous behavior of the polaron hopping constant is established and it is shown that the core hopping constant depends on the lattice size. However, the property of a lattice with translational invariance is recovered when the size of the nanowire is greater than a critical value. Fi…
Motivated by recent experiments on electric transport through single molecules and quantum dots, we investigate a model for transport that allows for significant coupling between the electrons and a boson mode isolated on the molecule or dot. We focus our attention on the temperature dependent properties of the transport. In the Holstein picture for polaronic transport in molecular crystals the temperature dependence of the conductivity exhibits a crossover from coherent (band) to incoherent (hopping) transport. Here, the temperature dependence of the differential conductance on resonance does…
The theory of exciton coupling to photons and LO phonons in quantum dots (QDs) and quantum-dot molecules (QDMs) is presented. Resonant-round trips of the exciton between the ground (bright) and excited (dark or bright) states mediated by the LO-phonon alter the decay time and yield the Rabi oscillation. The initial distributions of the population in the ground and the excited states dominate the oscillating amplitude and frequency. This property provides a detectable signature to the information stored in a qubit made from QD or QDM for a wide range of temperature T. Our results presented here…
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…
We present a microscopic semi-analytical theory for the description of organic molecules interacting strongly with a cavity mode. Exciton-vibration coupling within the molecule and exciton-cavity interaction are treated on an equal footing by employing a temperature-dependent variational approach. The interplay between strong exciton-vibration coupling and strong exciton-cavity coupling gives rise to a hybrid ground state, which we refer to as the lower polaron polariton. Explicit expressions for the ground-state wave function, the zero-temperature quasiparticle weight of the lower polaron pol…
Fractons are a type of emergent quasiparticle which cannot move freely in isolation, but can easily move in bound pairs. Similar phenomenology is found in boson-affected hopping models, encountered in the study of polaron systems and hole-doped Ising antiferromagnets, in which motion of a particle requires the creation or absorption of bosonic excitations. We show that boson-affected hopping models can provide a natural realization of fractons, either approximately or exactly, depending on the details of the system. We first consider a generic one-dimensional boson-affected hopping model, in w…
The coherent dynamics of a Holstein polaron in strong electric fields is considered under different regimes. Using analytical and numerical analysis, we show that even for small hopping constant and weak electron-phonon interaction, the original discrete Wannier-Stark (WS) ladder electronic states are each replaced by a semi-continuous band if a resonance condition is satisfied between the phonon frequency and the ladder spacing. In this regime, the original localized WS states can become {\em delocalized}, yielding both `tunneling' and `stretched' polarons. The transport properties of such a …
A polaron model proposed as a possible mechanism for nonlinear conductance [Galperin M, Ratner M A, and Nitzan A 2005 Nano Lett. 5 125-30] is revisited with focus on the differences between the weak and strong molecule-lead coupling cases. Within the one-molecular level model we present an approximate expression for the electronic Green function corresponding to inelastic transport case, which in the appropriate limits reduces to expressions presented previously for the isolated molecule and for molecular junction coupled to a slow vibration (static limit). The relevance of considerations base…
Here we study the polaronic transport through molecules weakly connected to metallic electrodes in the nonlinear response regime. Molecule itself is treated as a quantum dot with discrete energy levels, its connection to the electrodes is described within the wide-band approximation, while the charging is incorporated by means of the self-consistent potential. Nonperturbative computational scheme, used in this work, is based on the Green's function theory within the framework of mapping technique (GFT-MT). This method transforms the many-body electron-phonon interaction problem into a one-body…
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…
We consider resonant transport through a molecular quantum dot coupled to a local vibration mode. Applying the non-equilibrium Green function technique in the polaron representation, we develop a non-perturbative scheme to calculate the electron spectral function of the molecule in the regime of intermediate electron-phonon coupling. With increasing tunneling coupling to the leads, correlations between polaron clouds become more important at relatively high temperature leading to a strong sharpening of the peak structure in the spectral function. The detection of such features in the current-v…
For defining the conductance of single molecule junctions with a redox functionality in an electrochemical cell, two conceptually different electron transport mechanisms, namely coherent tunnelling and vibrationally induced hopping compete with each other, where implicit parameters of the setup such as the length of the molecule and the applied gate voltage decide which mechanism is the dominant one. Although coherent tunnelling is most efficiently described within Landauer theory, while the common theoretical treatment of electron hopping is based on Marcus theory, both theories are adequate …
In the regime of strong coupling between molecular excitons and confined optical modes, the intra-molecular degrees of freedom are profoundly affected, leading to a reduced vibrational dressing of polaritons compared to bare electronically excited states. However, existing models only describe a single vibrational mode in each molecule, while actual molecules possess a large number of vibrational degrees of freedom and additionally interact with a continuous bath of phononic modes in the host medium in typical experiments. In this work, we investigate a small ensemble of molecules with an arbi…
