Beyond Marcus theory and the Landauer-Büttiker approach in molecular junctions: A unified framework

Sowa, Jakub K.; Mol, Jan A.; Briggs, G. Andrew D.; Gauger, Erik M.

doi:10.1063/1.5049537

Cited by 80 publications

(87 citation statements)

References 100 publications

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“…One is then generally interested in the steady-state current through the junction as a function of the voltage applied to the leads. Current approaches include quantum master equations have successfully simulated situations with weak molecule-lead coupling via a pertubative treatment 13,14 . Another promising approach is that of hierarchical equations of motion, which works well for high temperatures and unstructured spectral densities 15,64 .…”

Section: Discussionmentioning

confidence: 99%

Efficient simulation of open quantum systems coupled to a fermionic bath

et al. 2020

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We present and analyze the fermionic time evolving density matrix using orthogonal polynomials algorithm (fTEDOPA), which enables the numerically exact simulation of open quantum systems coupled to a fermionic environment. The method allows for simulating the time evolution of open quantum systems with arbitrary spectral densities at zero or finite temperatures with controllable and certified error. We demonstrate the efficacy of the method towards the simulation of quintessential fermionic open quantum systems including the resonant level model and quantum dot coupled to an impurity and towards simulating hitherto intractable problems in quantum transport. Furthermore, we demonstrate significant efficiency gains in the computational costs by performing simulations in the Heisenberg picture. Finally, we compare different approaches for simulating finite-temperature situations and provide guidelines for choosing between these approaches. arXiv:1909.09589v1 [quant-ph]

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Section: Discussionmentioning

confidence: 99%

Efficient simulation of open quantum systems coupled to a fermionic bath

et al. 2020

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“…It would be interesting to generate datasets using other (relatively cheap) methods that perturbatively include electron-vibration interaction effects, see e.g. [72][73][74] and explore the ability of the ML technique to reproduce other transport mechanisms.…”

Section: Discussionmentioning

confidence: 99%

Machine Learning Prediction of DNA Charge Transport

Korol¹,

Segal²

2019

J. Phys. Chem. C

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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 long double-stranded DNA (dsDNA) sequences, reducing computational costs by orders of magnitude. The algorithm is trained on short DNA nanojunctions with n = 3 − 7 base pairs. The electrical conductance of the training set is computed with a quantum scattering method, which captures charge-nuclei scattering processes. We demonstrate that the ML method accurately predicts the electrical conductance of varied dsDNA junctions tracing different transport mechanisms: coherent (short-range) quantum tunneling, onresonance (ballistic) transport, and incoherent site-to-site hopping. Furthermore, the ML approach supports physical observations that clusters of nucleotides regulate DNA transport behavior. The input features tested in this work could be used in other ML studies of charge transport in complex polymers, in the search for promising electronic and thermoelectric materials.

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“…The phonon interaction (20) is already partitioned into system (21a)-(21c) and environment (22a)-(22c) operators. In the weak coupling (or lab) frame, the phonon rates scale with the phonon coupling strength.…”

Section: Master Equation Formalismmentioning

confidence: 99%

“…The spectral densities of organic molecules are generally composed of a series of sharp peaks [20]. The chosen form of (36) captures the envelope of this structure whilst retaining a form that can be integrated easily.…”

Section: Antisymmetric Eigenstate Photon Ratesmentioning

confidence: 99%

“…We assume that photon temperature has negligible effect. We choose identical phonon spectral densities for the two baths given by (36) and keep ω c =0.3 eV fixed, which gives a realistic range of vibrational modes in organic molecules [20]. Both phonon baths are at identical temperature, T pn =300 K. These phonon bath properties are used throughout the paper.…”

Section: Minimization Of the Emission Ratementioning

confidence: 99%

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Optimal power generation using dark states in dimers strongly coupled to their environment

2019

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Dark state protection has been proposed as a mechanism to increase the power output of light harvesting devices by reducing the rate of radiative recombination. Indeed many theoretical studies have reported increased power outputs in dimer systems which use quantum interference to generate dark states. These models have typically been restricted to particular geometries and to weakly coupled vibrational baths. Here we consider the experimentally-relevant strong vibrational coupling regime with no geometric restrictions on the dimer. We analyze how dark states can be formed in the dimer by numerically minimizing the emission rate of the lowest energy excited eigenstate, and then calculate the power output of the molecules with these dark states. We find that there are two distinct types of dark states depending on whether the monomers form homodimers, where energy splittings and dipole strengths are identical, or heterodimers, where there is some difference. Homodimers, which exploit destructive quantum interference, produce high power outputs but strong phonon couplings and perturbations from ideal geometries are extremely detrimental. Heterodimers, which are closer to the classical picture of a distinct donor and acceptor molecule, produce an intermediate power output that is relatively stable to these changes. The strong vibrational couplings typically found in organic molecules will suppress destructive interference and thus favor the dark-state enhancement offered by heterodimers.

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Beyond Marcus theory and the Landauer-Büttiker approach in molecular junctions: A unified framework

Cited by 80 publications

References 100 publications

Efficient simulation of open quantum systems coupled to a fermionic bath

Efficient simulation of open quantum systems coupled to a fermionic bath

Machine Learning Prediction of DNA Charge Transport

Optimal power generation using dark states in dimers strongly coupled to their environment

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