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An Atomistic Approach to Conduction Between Nanoelectrodes Through a Single Molecule


Capacitance and other properties of nanoelectrodes, finite-size metal clusters envisaged for use in complex molecular-electronic devices, are discussed. The applicability of classical electrostatics (Coulomb's and Gauss' law, Poisson's equation, etc.) to atomistic systems is investigated and the self-energy necessary to store a finite charge on an atom is found to be of central importance. In particular, the neglect of electron exchange is found to introduce severe limitations, with quantum calculations predicting fundamentally different electronic structures. Also, the well-known poor representation of the atomic self-energy inherent to modern DFT is discussed, along with its implications for molecular electronics calculations. An INDO/S method is introduced with new parameters for gold. This is the simplest approximate computational scheme that correctly includes quantum electrostatic, resonance, and spin effects, and is capable of describing arbitrary excited electronic states. Encouraging results are obtained for some trial problems. In particular, voltage differential between the electrodes in electrode-molecule-electrode conduction is obtained, not through an a priori prescription but rather by moving whole electrons between the electrodes and analyzing the response. The voltage drops across the molecule-electrode junctions and the central molecular region are then deduced. This alternative to the current Landauer-based 1-particle transmission equations for electrode-molecule-electrode conduction is discussed in terms of the use of the electronic states of the system. It provides a proper description not only of conduction via electrode-to-molecule charge or hole transfer but also of conduction via simultaneous charge and hole transfer via low-lying excited molecular electronic states, including the ability to account for electroluminescence and other chemical effects. In addition, various aspects of our research on the quantitative prediction of the I(V) curves for electrode-molecule-electrode conduction are reviewed, including demonstration of the equivalence of the formalisms generated by the Datta and the Mujica-Ratner groups, and the development of analytically solvable paradigms, including the conduction through a linear-chain Hueckel wire.......

【作者名称】: JEFFREY R. REIMERS, WARWICK A. SHAPLEY, NICHOLAS LAMBROPOULOS, NOEL S. HUSH
【作者单位】: School of Chemistry, University of Sydney, Sydney, NSW 2006, Australia
【关 键 词】: nanoelectrode, self-energy, atomistic, gauss' law, molecular electronics, molecular capacitance
【会议名称】: Conference on Molecular Electronics II, Dec 10-14, 2000, Kailua-kona, Hawaii
【期刊论文数据库】: [DBS_Articles_01]
【期刊论文编号】: 100,835,277
【摘要长度】: 2,292
【会议地点】: Kailua-Kona, HI(US)
【会议组织】: School of Chemistry, University of Sydney, Sydney, NSW 2006, Australia
【会议时间】: 2000
【上篇论文】: 外文会议 - NEW GENERATION OF OPTICAL ULTRASONIC SENSORS ADAPTED TO INDUSTRIAL CONSTRAINTS
【下篇论文】: 外文会议 - Numerical Simulation and Mechanism Analysis of a Slender Delta Wing Undergoing Combined Free-roll and Free-sideslip Motion

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