184 research outputs found
Vibrational nonequilibrium effects in the conductance of single-molecules with multiple electronic states
Vibrational nonequilibrium effects in charge transport through
single-molecule junctions are investigated. Focusing on molecular bridges with
multiple electronic states, it is shown that electronic-vibrational coupling
triggers a variety of vibronic emission and absorption processes, which
influence the conductance properties and mechanical stability of
single-molecule junctions profoundly. Employing a master equation and a
nonequilibrium Green's function approach, these processes are analyzed in
detail for a generic model of a molecular junction and for
benzenedibutanethiolate bound to gold electrodes.Comment: 5 pages, 4 figure
Vibrational Instabilities in Resonant Electron Transport through Single-Molecule Junctions
We analyze various limits of vibrationally coupled resonant electron
transport in single-molecule junctions. Based on a master equation approach, we
discuss analytic and numerical results for junctions under a high bias voltage
or weak electronic-vibrational coupling. It is shown that in these limits the
vibrational excitation of the molecular bridge increases indefinitely, i.e. the
junction exhibits a vibrational instability. Moreover, our analysis provides
analytic results for the vibrational distribution function and reveals that
these vibrational instabilities are related to electron-hole pair creation
processes.Comment: 19 pages, 3 figure
Quantum Interference and Decoherence in Single-Molecule Junctions: How Vibrations Induce Electrical Current
Quantum interference effects and decoherence mechanisms in single-molecule
junctions are analyzed employing a nonequilibrium Green's function approach.
Electrons tunneling through quasi-degenerate states of a nanoscale molecular
junction exhibit interference effects. We show that electronic-vibrational
coupling, inherent to any molecular junction, strongly quenches such
interference effects. As a result, the electrical current can be significantly
larger than without electronic-vibrational coupling. The analysis reveals that
the quenching of quantum interference is particularly pronounced if the
junction is vibrationally highly excited, e.g. due to current-induced
nonequilibrium effects in the resonant transport regime.Comment: 11 pages, 4 figure
Switching the Conductance of a Molecular Junction using a Proton Transfer Reaction
A novel mechanism for switching a molecular junction based on a proton
transfer reaction triggered by an external electrostatic field is proposed. As
a specific example to demonstrate the feasibility of the mechanism, the
tautomers [2,5-(4-hydroxypyridine)] and {2,5-[4(1H)-pyridone]} are considered.
Employing a combination of first-principles electronic structure calculations
and Landauer transport theory, we show that both tautomers exhibit very
different conductance properties and realize the "on" and "off" states of a
molecular switch. Moreover, we provide a proof of principle that both forms can
be reversibly converted into each other using an external electrostatic field.Comment: 14 pages, 5 figure
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The use of the Continuously Regenerating Trap (CRT<sup>TM</sup>) and SCRT<sup>TM</sup> Systems to meet future emissions legislation
The progressive tightening of particulate matter (PM) legislation presents challenges to the engine development and aftertreatment communities. The Continuously Regenerating Trap (CRTTM) has been developed to enable diesel engines to meet the proposed future legislation. This passive filter system combines an oxidation catalyst with a Diesel Particulate Filter (DPF); the filter traps the PM and the oxidation catalyst generates NO2 which combusts the trapped PM at substantially lower temperatures than is possible using oxygen.
This paper outlines the operating principle of the CRTTM, and describes the performance of the system. It has been shown that the very high PM conversions obtained with the CRTTM can enable even Euro 1 engines to meet the PM limits proposed for introduction in Europe in 2005. In addition, the system removes PM across the whole particle size range, including ultrafine particulates. These results will be discussed, as will in-field durability studies which have shown that the system is still capable of converting 90% of PM after very high mileage operation (up to 600,000 km).
In addition to requiring very high PM conversion, the proposed future legislation requires substantial reductions in NOx emissions form heavy duty diesel vehicles. To meet these challenges the SCRTTM has been developed. This combines the CRTTM with SCR (Selective Catalytic Reduction) technology, and enables very high simultaneous conversions of CO, HC, PM and NOx to be achieved. The SCRTTM system is described, and its operating characteristics are discussed. It has been shown that the SCRTTM can potentially meet the legislative limits proposed for introduction in Europe in 2008
Resonant vibrations, peak broadening and noise in single molecule contacts: beyond the resonant tunnelling picture
We carry out experiments on single-molecule junctions at low temperatures,
using the mechanically controlled break junction technique. Analyzing the
results received with more than ten different molecules the nature of the first
peak in the differential conductance spectra is elucidated. We observe an
electronic transition with a vibronic fine structure, which is most frequently
smeared out and forms a broad peak. In the usual parameter range we find strong
indications that additionally fluctuations become active even at low
temperatures. We conclude that the electrical field feeds instabilities, which
are triggered by the onset of current. This is underscored by noise
measurements that show strong anomalies at the onset of charge transport
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