dc.contributor.author | Cort Barrada, Luis | |
dc.contributor.author | Nielsen, Soeren Ersbak Bang | |
dc.contributor.author | van Leeuwen, Robert | |
dc.date.accessioned | 2019-02-25T12:49:18Z | |
dc.date.available | 2019-02-25T12:49:18Z | |
dc.date.issued | 2019 | |
dc.identifier.citation | Cort Barrada, L., Nielsen, S. E. B., & van Leeuwen, R. (2019). Strictly-correlated-electron approach to excitation energies of dissociating molecules. <i>Physical Review A</i>, <i>99</i>(2), Article 022501. <a href="https://doi.org/10.1103/PhysRevA.99.022501" target="_blank">https://doi.org/10.1103/PhysRevA.99.022501</a> | |
dc.identifier.other | CONVID_28935557 | |
dc.identifier.uri | https://jyx.jyu.fi/handle/123456789/62962 | |
dc.description.abstract | In this work we consider a numerically solvable model of a two-electron diatomic molecule to study a recently
proposed approximation based on the density functional theory of so-called strictly correlated electrons (SCE).
We map out the full two-particle wave function for a wide range of bond distances and interaction strengths
and obtain analytic results for the two-particle states and eigenenergies in various limits of strong and weak
interactions, and in the limit of large bond distance. We then study the so-called Hartree-exchange-correlation
(Hxc) kernel of time-dependent density functional theory which is a key ingredient in calculating excitation
energies. We study an approximation based on adiabatic SCE (ASCE) theory which was shown to display a
particular feature of the exact Hxc kernel, namely, a spatial divergence as function of the bond distance. This
makes the ASCE kernel a candidate for correcting a notorious failure of the commonly used adiabatic local
density approximation (ALDA) in the calculation of excitation energies of dissociating molecules. Unlike the
ALDA, we obtain nonzero excitation energies from the ASCE kernel in the dissociation regime but they do not
correspond to those of the true spectrum unless the interaction strength is taken to be very large such that the
SCE theory has the right regime of validity, in which case the excitation energies become exact and represent the
so-called zero-point oscillations of the strictly correlated electrons. The commonly studied physical dissociation
regime, namely, large molecular separation at intermediate interaction strength, therefore remains a challenge
for density functional approximations based on SCE theory. | fi |
dc.format.mimetype | application/pdf | |
dc.language.iso | eng | |
dc.publisher | American Physical Society | |
dc.relation.ispartofseries | Physical Review A | |
dc.rights | CC BY 4.0 | |
dc.subject.other | two-electron diatomic molecule | |
dc.subject.other | strictly correlated electrons | |
dc.title | Strictly-correlated-electron approach to excitation energies of dissociating molecules | |
dc.type | research article | |
dc.identifier.urn | URN:NBN:fi:jyu-201902221625 | |
dc.contributor.laitos | Fysiikan laitos | fi |
dc.contributor.laitos | Department of Physics | en |
dc.contributor.oppiaine | Nanoscience Center | fi |
dc.contributor.oppiaine | Nanoscience Center | en |
dc.type.uri | http://purl.org/eprint/type/JournalArticle | |
dc.date.updated | 2019-02-22T16:15:10Z | |
dc.type.coar | http://purl.org/coar/resource_type/c_2df8fbb1 | |
dc.description.reviewstatus | peerReviewed | |
dc.relation.issn | 2469-9926 | |
dc.relation.numberinseries | 2 | |
dc.relation.volume | 99 | |
dc.type.version | publishedVersion | |
dc.rights.copyright | © 2019 American Physical Society | |
dc.rights.accesslevel | openAccess | fi |
dc.type.publication | article | |
dc.subject.yso | molekyylit | |
dc.subject.yso | tiheysfunktionaaliteoria | |
dc.subject.yso | approksimointi | |
dc.format.content | fulltext | |
jyx.subject.uri | http://www.yso.fi/onto/yso/p2984 | |
jyx.subject.uri | http://www.yso.fi/onto/yso/p28852 | |
jyx.subject.uri | http://www.yso.fi/onto/yso/p4982 | |
dc.rights.url | https://creativecommons.org/licenses/by/4.0/ | |
dc.relation.doi | 10.1103/PhysRevA.99.022501 | |
dc.type.okm | A1 | |