Tight-Binding Modeling of Charge Migration in DNA Devices

Cuniberti, Gianaurelio; Maciá, Enrique; Rodríguez, Ana Alonso; Römer, Rudolf A.

doi:10.1007/978-3-540-72494-0_1

Cited by 37 publications

(46 citation statements)

References 117 publications

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“…A more accurate description requires us to model each nucleobase in a bp as an independent site as well as including the sugarphosphate backbone. 8 The hydrogen bonding between complementary bases is then described as an additional hopping term perpendicular to the DNA stack, [9][10][11][12][13] and appropriate on-site energies and hopping parameters for the backbone must be included as well. [14][15][16] The resulting models are essentially a planar projection ͑two dimensions͒ of the DNA structure with its double helix unwound, so that the successive bp's are lined up face to face along the strand.…”

Section: Introductionmentioning

confidence: 99%

Electrical conductance in duplex DNA: Helical effects and low-frequency vibrational coupling

Maciá

2007

Phys. Rev. B

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In this work we consider the combined effect of helical structure and base-pair twist motion on charge transfer through duplex DNA at low temperatures. We present a fully analytical treatment of charge-lattice coupled dynamics in terms of nearest-neighbor tight-binding equations describing the propagation of the charge through an effective linear lattice for certain frequency values. The corresponding effective hopping terms include both helicoidal and dynamical effects in a unified way. Although base-pair motion generally reduces -stack overlapping, the coupling to certain normal modes gives rise to a significant improvement of the Landauer conductance.

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Section: Introductionmentioning

confidence: 99%

Electrical conductance in duplex DNA: Helical effects and low-frequency vibrational coupling

Maciá

2007

Phys. Rev. B

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“…is the Hamiltonian of usual two-leg ladder model including spin degree of freedom [17], with N the DNA length, c † jn = (c † jn↑ , c † jn↓ ) the creation operator of the spinor at the nth site of the jth chain of the ds-DNA, ε jn the on-site energy, t jn the intrachain hopping integral, and λ n the interchain hybridization interaction. +H.c.]…”

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confidence: 99%

Spin-Selective Transport of Electrons in DNA Double Helix

Guo¹,

Sun²

2012

Phys. Rev. Lett.

296

476

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The experiment that the high spin selectivity and the length-dependent spin polarization are observed in double-stranded DNA [Science 331, 894 (2011)], is elucidated by considering the combination of the spin-orbit coupling, the environment-induced dephasing, and the helical symmetry. We show that the spin polarization in double-stranded DNA is significant even in the case of weak spin-orbit coupling, while no spin polarization appears in single-stranded DNA. Furthermore, the underlying physical mechanism and the parameters-dependence of the spin polarization are studied.PACS numbers: 87.14.gk, 87.15.Pc, Molecular spintronics, by combining molecular electronics with spintronics to manipulate the transport of electron spins in organic molecular systems, is regarded as one of the most promising research fields and is now attracting extensive interest [1][2][3][4], owing to the long spin relaxation time and the flexibility of organic materials. Unconventional magnetic properties of molecular systems reported in organic spin valves and magnetic tunnel junctions, are attributed to the hybrid states in the organicmagnetic interfaces [5][6][7][8][9] and to single-molecule magnet [4]. Organic molecules would not be suitable candidates for spin-selective transport because of their nonmagnetic properties and weak spin-orbit coupling (SOC) [10].However, very recently, Göhler et al. reported the spin selectivity of photoelectron transmission through selfassembled monolayers of double-stranded DNA (dsDNA) deposited on gold substrate [11]. They found that wellorganized monolayers of the dsDNA act as very efficient spin filters with high spin polarization at room temperature for long dsDNA, irrespective of the polarization of the incident light. The spin filtration efficiency increases with increasing length of the dsDNA and contrarily no spin polarization could be observed for single-stranded DNA (ssDNA). These results were further substantiated by direct charge transport measurements of single ds-DNA connected between two leads [12]. Although several theoretical models were put forward to investigate the spin-selective properties of DNA molecule based on single helical chain-induced Rashba SOC [13,14], the models neglect the double helix feature of the dsDNA and are somewhat inconsistent with the experimental results that the ssDNA could not be a spin filter. Until now the underlying physical mechanism remains unclear for high spin selectivity observed in the dsDNA [15,16].In this Letter, a model Hamiltonian, including the small environment-induced dephasing, the weak SOC, and the helical symmetry, is proposed to investigate the quantum spin transport through the ssDNA and dsDNA connected to nonmagnetic leads. We interpret the experimental results that the electrons transmitted through the dsDNA exhibit high spin polarization, the spin filtration efficiency will be enhanced by increasing the DNA length, and no spin polarization appears for the ssDNA. The physical mechanism arises from the combination of the dephasing, the S...

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“…Unfortunately, systematic investigations (within a given experimental setup) on base sequence, length, and the temperature dependence of charge transport are still missing, so that the theoretical analysis of possible charge transport pathways faces big challenges [40]. Initial modeling of charge transport was mainly based on effective Hamiltonians with fixed electronic parameters and describing e.g hole transport through the highest occupied molecular orbitals (HOMO) of the bases [41][42][43][44][45][46][47] (see also [48,49] for recent reviews). Model Hamiltonians clearly offer the possibility to explore different charge transport scenarios in a relatively flexible way, but they also contain usually many parameters which are difficult to estimate.…”

Section: Introductionmentioning

confidence: 99%

Modeling Charge Transport and Dynamics in Biomolecular Systems

Gutiérrez

Cuniberti

2023

JSAME

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Charge transport at the molecular scale builds the cornerstone of molecular electronics (ME), a novel paradigm aiming at the realization of nanoscale electronics via tailored molecular functionalities. Biomolecular electronics, lying at the borderline between physics, chemistry and biology, can be considered as a sub-field of ME. In particular, the potential applications of DNA oligomers either as template or as active device element in ME have strongly drawn the attention of both experimentalist and theoreticians in the past years. While exploiting the self-assembling and self-recognition properties of DNA based molecular systems is meanwhile a well-established field, the potential of such biomolecules as active devices is much less clear mainly due to the poorly understood charge conduction mechanisms. One key component in any theoretical description of charge migration in biomolecular systems, and hence in DNA oligomers, is the inclusion of conformational fluctuations and their coupling to the transport process. The treatment of such a problem affords to consider dynamical effects in a non-perturbative way in contrast to, e.g., conventional bulk materials. Here we present an overview of recent work aiming at combining molecular dynamic simulations and electronic structure calculations with charge transport in coarse-grained effective model R. Gutierrez and G. CunibertiHamiltonians. This hybrid methodology provides a common theoretical starting point to treat charge transfer/transport in strongly structurally fluctuating molecular-scale physical systems.

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Tight-Binding Modeling of Charge Migration in DNA Devices

Cited by 37 publications

References 117 publications

Electrical conductance in duplex DNA: Helical effects and low-frequency vibrational coupling

Electrical conductance in duplex DNA: Helical effects and low-frequency vibrational coupling

Spin-Selective Transport of Electrons in DNA Double Helix

Modeling Charge Transport and Dynamics in Biomolecular Systems

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