Abstract
We develop a numerical approach for simulating light-induced charge transport dynamics across a metal-molecule-metal conductance junction. The finite-difference time-domain method is used to simulate the plasmonic response of the metal structures. The Huygens subgridding technique, as adapted to Lorentz media, is used to bridge the vastly disparate length scales of the plasmonic metal electrodes and the molecular system, maintaining accuracy. The charge and current densities calculated with classical electrodynamics are transformed to an electronic wavefunction, which is then propagated through the molecular linker via the Heisenberg equations of motion. We focus mainly on development of the theory and exemplify our approach by a numerical illustration of a simple system consisting of two silver cylinders bridged by a three-site molecular linker. The electronic subsystem exhibits fascinating light driven dynamics, wherein the charge density oscillates at the driving optical frequency, exhibiting also the natural system timescales, and a resonance phenomenon leads to strong conductance enhancement.
| Original language | English |
|---|---|
| Article number | 224104 |
| Journal | Journal of Chemical Physics |
| Volume | 141 |
| Issue number | 22 |
| DOIs | |
| Publication status | Published - Dec 14 2014 |
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ASJC Scopus subject areas
- Physics and Astronomy(all)
- Physical and Theoretical Chemistry
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Modeling light-induced charge transfer dynamics across a metal-molecule-metal junction : Bridging classical electrodynamics and quantum dynamics. / Hu, Zixuan; Ratner, Mark A; Seideman, Tamar.
In: Journal of Chemical Physics, Vol. 141, No. 22, 224104, 14.12.2014.Research output: Contribution to journal › Article
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TY - JOUR
T1 - Modeling light-induced charge transfer dynamics across a metal-molecule-metal junction
T2 - Bridging classical electrodynamics and quantum dynamics
AU - Hu, Zixuan
AU - Ratner, Mark A
AU - Seideman, Tamar
PY - 2014/12/14
Y1 - 2014/12/14
N2 - We develop a numerical approach for simulating light-induced charge transport dynamics across a metal-molecule-metal conductance junction. The finite-difference time-domain method is used to simulate the plasmonic response of the metal structures. The Huygens subgridding technique, as adapted to Lorentz media, is used to bridge the vastly disparate length scales of the plasmonic metal electrodes and the molecular system, maintaining accuracy. The charge and current densities calculated with classical electrodynamics are transformed to an electronic wavefunction, which is then propagated through the molecular linker via the Heisenberg equations of motion. We focus mainly on development of the theory and exemplify our approach by a numerical illustration of a simple system consisting of two silver cylinders bridged by a three-site molecular linker. The electronic subsystem exhibits fascinating light driven dynamics, wherein the charge density oscillates at the driving optical frequency, exhibiting also the natural system timescales, and a resonance phenomenon leads to strong conductance enhancement.
AB - We develop a numerical approach for simulating light-induced charge transport dynamics across a metal-molecule-metal conductance junction. The finite-difference time-domain method is used to simulate the plasmonic response of the metal structures. The Huygens subgridding technique, as adapted to Lorentz media, is used to bridge the vastly disparate length scales of the plasmonic metal electrodes and the molecular system, maintaining accuracy. The charge and current densities calculated with classical electrodynamics are transformed to an electronic wavefunction, which is then propagated through the molecular linker via the Heisenberg equations of motion. We focus mainly on development of the theory and exemplify our approach by a numerical illustration of a simple system consisting of two silver cylinders bridged by a three-site molecular linker. The electronic subsystem exhibits fascinating light driven dynamics, wherein the charge density oscillates at the driving optical frequency, exhibiting also the natural system timescales, and a resonance phenomenon leads to strong conductance enhancement.
UR - http://www.scopus.com/inward/record.url?scp=84916217156&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84916217156&partnerID=8YFLogxK
U2 - 10.1063/1.4903046
DO - 10.1063/1.4903046
M3 - Article
AN - SCOPUS:84916217156
VL - 141
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
SN - 0021-9606
IS - 22
M1 - 224104
ER -