Molecular Junctions Inspired by Nature: Electrical Conduction through Noncovalent Nanobelts

Jones, Leighton O.; Mosquera, Martín A.; Schatz, George C.; Ratner, Mark A.

doi:10.1021/acs.jpcb.9b06255

Title: Molecular Junctions Inspired by Nature: Electrical Conduction through Noncovalent Nanobelts

Journal Article · Thu Sep 05 00:00:00 EDT 2019 · Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

DOI:https://doi.org/10.1021/acs.jpcb.9b06255· OSTI ID:1591989

^[1];

^[1]; Ratner, Mark A. ^[1]

Northwestern Univ., Evanston, IL (United States)

Charge transport has long been known to occur naturally in a range of bio molecular systems, from enzymes to neurotransmitters whose structures have covalent and non covalent bonds. Understanding from these systems have yet to translate into molecular junction devices. In this work, we design junctions which have hydrogen bonds between the edges of a series of prototype noncovalent nanobelts (NCNs) and vary the number of donor acceptors to study their electrical properties. From frontier molecular orbitals (FMOs) and projected density of states (DOS) calculations, we found these NCN dimer junctions (bridging Au electrodes) to be gapless systems, with eigenvalues of occupied and unoccupied levels between -5.8 and -5.1 eV respectively, and states at the Fermi level suggesting these are metallic like systems. Their conductance properties were studied with non equilibrium Green’s functions density functional theory (NEGF-DFT) and conductance was found to decrease with cooperative H bonding, that is, the conductance decreased as the alternating donors and acceptors around the nanobelts attenuates to a uniform distribution in the H-bonding arrays. The highest conductance was 51.3 × 10 6 S (τ=0.662 at the Fermi level), with a pair of NCN dimers having only donors on one nanobelt and acceptors on the other in the NCN junction. The Seebeck coefficient showed that these are n type (-36 to 39 µV K 1), while the lower conductors with alternating H bonds are p type (49.7 to 204 µV K 1). In addition, the NCNs have appreciable binding energies (19.8 to 46.1 kcal/mol), implying that in practice, they could form self-assembled monolayer (SAM) heterojunctions, and future systems could be designed to yield a noncovalent polymeric network of nanobelts for long range charge transport.

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Research Organization:: Northwestern Univ., Evanston, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0004752

OSTI ID:: 1591989

Alternate ID(s):: OSTI ID: 1592225

Journal Information:: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry, Vol. 123, Issue 38; ISSN 1520-6106

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 9 works

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