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First-principles approach to the charge-transport characteristics of monolayer molecular-electronics devices: Application to hexanedithiolate devices

Kim, Yong-Hoon and Tahir-Kheli, Jamil and Schultz, Peter A. and Goddard, William A., III (2006) First-principles approach to the charge-transport characteristics of monolayer molecular-electronics devices: Application to hexanedithiolate devices. Physical Review B, 73 (23). Art. No. 235419. ISSN 1098-0121. doi:10.1103/PhysRevB.73.235419.

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We report on the development of an accurate first-principles computational scheme for the charge transport characteristics of molecular monolayer junctions and its application to hexanedithiolate (C6DT) devices. Starting from the Gaussian basis set density-functional calculations of a junction model in the slab geometry and corresponding two bulk electrodes, we obtain the transmission function using the matrix Green's function method and analyze the nature of transmission channels via atomic projected density of states. Within the developed formalism, by treating isolated molecules with the supercell approach, we can investigate the current-voltage characteristics of single and parallel molecular wires in a consistent manner. For the case of single C6DT molecules stretched between Au(111) electrodes, we obtain reasonable quantitative agreement of computed conductance with a recent scanning tunneling microscope experiment result. Comparing the charge transport properties of C6DT single molecules and their monolayer counterparts in the stretched and tilted geometries, we find that the effect of intermolecular coupling and molecule tilting on the charge transport characteristics is negligible in these devices. We contrast this behavior to that of the pi-conjugated biphenyldithiolate devices we have previously considered and discuss the relative importance of molecular cores and molecule-electrode contacts for the charge transport in those devices.

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Goddard, William A., III0000-0003-0097-5716
Additional Information:©2006 The American Physical Society (Received 5 December 2005; revised 10 April 2006; published 21 June 2006) Y.-H.K. was supported by the Korea Research Foundation Grant funded by the Korean Government (MOEHRD) (Grant No. KRF-2005-041-C00125), in which main calculations were performed by using the supercomputing resource of the Korea Institute of Science and Technology (KISTI). J.T.-K. and W.A.G. III were supported by NSF Nanotechnology and Interdisciplinary Research Initiative and MARCO Focus Centers on Functional Engineered NanoArchitectonics. W.A.G. III was also partially supported by Intel Components Research. The facilities of the MSC were supported by ONR-DURIP, ARO-DURIP, NSF-MRI, and the Beckman Institute. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the US DOE under Contract No. DE-AC04-94AL85000.
Subject Keywords:organic compounds; molecular electronics; ab initio calculations; density functional theory; Green's function methods; electronic density of states; electric admittance; scanning tunnelling microscopy; electrodes; electrical contacts
Issue or Number:23
Record Number:CaltechAUTHORS:KIMprb06
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:4706
Deposited By: Archive Administrator
Deposited On:03 Sep 2006
Last Modified:08 Nov 2021 20:19

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