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First-principles quantum transport modeling of thermoelectricity in single-molecule nanojunctions with graphene nanoribbon electrodes

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Abstract

We overview the nonequilibrium Green function combined with density functional theory (NEGF-DFT) approach to modeling of independent electronic and phononic quantum transport in nanoscale thermoelectrics with examples focused on a new class of devices where a single organic molecule is attached to two metallic zigzag graphene nanoribbons (ZGNRs) via highly transparent contacts. Such contacts make possible injection of evanescent wavefunctions from the ZGNR electrodes, so that their overlap within the molecular region generates a peak in the electronic transmission around the Fermi energy of the device. Additionally, the spatial symmetry properties of the transverse propagating states in the semi-infinite ZGNR electrodes suppress hole-like contributions to the thermopower. Thus optimized thermopower, together with diminished phonon thermal conductance in a ZGNR|molecule|ZGNR inhomogeneous heterojunctions, yields the thermoelectric figure of merit ZT≃0.4 at room temperature with maximum ZT≃3 reached at very low temperatures T≃10 K (so that the latter feature could be exploited for thermoelectric cooling of, e.g., infrared sensors). The reliance on evanescent mode transport and symmetry of propagating states in the electrodes makes the electronic-transport-determined power factor in this class of devices largely insensitive to the type of sufficiently short organic molecule, which we demonstrate by showing that both 18-annulene and C10 molecule sandwiched by the two ZGNR electrodes yield similar thermopower. Thus, one can search for molecules that will further reduce the phonon thermal conductance (in the denominator of ZT) while keeping the electronic power factor (in the nominator of ZT) optimized. We also show how the often employed Brenner empirical interatomic potential for hydrocarbon systems fails to describe phonon transport in our single-molecule nanojunctions when contrasted with first-principles results obtained via NEGF-DFT methodology.

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Notes

  1. We should mention here that the Lorenz ratio κ el/GT calculated for transport of noninteracting electrons through several single-molecule nanojunctions shows variations by tens of percent from the Wiedemann-Franz law as the chemical potential crosses a transmission resonance, and much larger deviation around the transmission nodes [18, 19].

  2. For comparison between Boltzmann semiclassical and Landauer quantum transport approaches applied to thermoelectric transport coefficients of conventional translationally invariant systems see Ref. [55].

  3. For example, in the case of either bulk graphene [64] or GNRs [65] one has to employ TB Hamiltonian with up to third-nearest-neighbor hopping in order to match the DFT-computed band structure.

  4. For an example of the peak in T el(E) induced by the overlap of evanescent wavefunctions originating from two CNT electrodes sandwiching 18-annulene molecule see Supplemental Material of Ref. [93].

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Acknowledgements

We thank K. Esfarjani, V. Meunier and M. Paulsson for illuminating discussions. Financial support under DOE Grant No. DE-FG02-07ER46374 (K.K.S. and B.K.N.) and FTP Grants No. 274-08-0408 and No. 11-104592 (T.M. and K.S.T.) is gratefully acknowledged. The supercomputing time was provided in part by the NSF through TeraGrid resource TACC Ranger under Grant No. TG-DMR100002 and NSF Grant No. CNS-0958512.

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  1. Department of Physics and Astronomy, University of Delaware, Newark, DE, 19716, USA

    Branislav K. Nikolić & Kamal K. Saha

  2. Center for Atomic-scale Materials Design (CAMD), Department of Physics, Technical University of Denmark, 2800, Kongens Lyngby, Denmark

    Troels Markussen & Kristian S. Thygesen

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  1. Branislav K. Nikolić
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  2. Kamal K. Saha
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  3. Troels Markussen
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  4. Kristian S. Thygesen
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Correspondence to Branislav K. Nikolić.

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Nikolić, B.K., Saha, K.K., Markussen, T. et al. First-principles quantum transport modeling of thermoelectricity in single-molecule nanojunctions with graphene nanoribbon electrodes. J Comput Electron 11, 78–92 (2012). https://doi.org/10.1007/s10825-012-0386-y

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