Show simple item record

dc.contributor.authorMyöhänen, Petri
dc.contributor.authorTuovinen, Riku
dc.contributor.authorKorhonen, Topi
dc.contributor.authorStefanucci, G.
dc.contributor.authorvan Leeuwen, Robert
dc.date.accessioned2016-02-16T12:34:20Z
dc.date.available2016-02-16T12:34:20Z
dc.date.issued2012
dc.identifier.citationMyöhänen, P., Tuovinen, R., Korhonen, T., Stefanucci, G., & van Leeuwen, R. (2012). Image charge dynamics in time-dependent quantum transport. <em>Physical Review B</em>, 85 (7). <a href="http://dx.doi.org/10.1103/PhysRevB.85.075105">doi:10.1103/PhysRevB.85.075105</a> Retrieved from <a href="http://arxiv.org/abs/1111.6104">http://arxiv.org/abs/1111.6104</a>
dc.identifier.otherTUTKAID_55748
dc.identifier.urihttps://jyx.jyu.fi/handle/123456789/48799
dc.description.abstractIn this work, we investigate the effects of the electron-electron interaction between a molecular junction and the metallic leads in time-dependent quantum transport. We employ the recently developed embedded Kadanoff-Baym method [Phys. Rev. B 80, 115107 (2009)] and show that the molecule-lead interaction changes substantially the transient and steady-state transport properties. We first show that the mean-field Hartree-Fock (HF) approximation does not capture the polarization effects responsible for the renormalization of the molecular levels neither in nor out of equilibrium. Furthermore, due to the time-local nature of the HF self-energy, there exists a region in parameter space for which the system does not relax after the switch-on of a bias voltage. These and other artifacts of the HF approximation disappear when including correlations at the second-Born or GW levels. Both these approximations contain polarization diagrams, which correctly account for the screening of the charged molecule. We find that by changing the molecule-lead interaction, the ratio between the screening and relaxation time changes, an effect which must be properly taken into account in any realistic time-dependent simulation. Another important finding is that while in equilibrium the molecule-lead interaction is responsible for a reduction of the highest occupied molecular orbital-lowest unoccupied molecular orbital (HOMO-LUMO) gap and for a substantial redistribution of the spectral weight between the main spectral peaks and the induced satellite spectrum, in the biased system it can have the opposite effect, i.e., it sharpens the spectral peaks and opens the HOMO-LUMO gap.
dc.language.isoeng
dc.publisherAmerican Physical Society
dc.relation.ispartofseriesPhysical Review B
dc.subject.otherquantum transport
dc.titleImage charge dynamics in time-dependent quantum transport
dc.typearticle
dc.identifier.urnURN:NBN:fi:jyu-201601191161
dc.contributor.laitosFysiikan laitosfi
dc.contributor.laitosDepartment of Physicsen
dc.contributor.oppiaineFysiikka
dc.type.urihttp://purl.org/eprint/type/JournalArticle
dc.date.updated2016-01-19T16:15:21Z
dc.type.coarjournal article
dc.description.reviewstatuspeerReviewed
dc.relation.issn1098-0121
dc.relation.volume85
dc.type.versionpublishedVersion
dc.rights.copyright© 2012 American Physical Society. Published in this repository with the kind permission of the publisher.
dc.rights.accesslevelopenAccessfi
dc.relation.doi10.1103/PhysRevB.85.075105


Files in this item

Thumbnail

This item appears in the following Collection(s)

Show simple item record