Nonlinear optical response of endohedral all-metal electride cages 2e-Mg2+(M@E12)2-Ca2+ (M = Ni, Pd, and Pt; E = Ge, Sn, and Pb)
dc.contributor.author
dc.date.accessioned
2019-07-10T07:10:53Z
dc.date.available
2021-04-07T08:03:01Z
dc.date.issued
2019-01-21
dc.identifier.issn
2050-7526
dc.identifier.uri
dc.description.abstract
To extend the interesting new concept of the all-metal electride, a series of endohedral all-metal electride cages 2e-Mg2+(M@E12)2-Ca2+ (E = Ge, Sn, and Pb; M = Ni, Pd, and Pt) has been designed and investigated theoretically using the exchange-correlation functional CAM-B3LYP. In these electride cage molecules with excess electrons, interesting pull-push electron transfer relay occurs. The metal cage M@E12 first pulls valence electrons from Ca atom forming a polyanion (M@E12)2-, and then the formed polyanion pushes valence electrons of Mg atom out of its valence shell generating the isolated excess electrons that characterize this species as all-metal electrides. These endohedral all-metal electride cages display a large electronic first hyperpolarizability (beta^e_0) and so they could have a potential application as a new kind of second-order nonlinear optical (NLO) material. We have explored the structure-property relationships, which are significant. It is shown that, for a given central atom, the all-metal electrides with a Sn-cage correspond to the largest beta^e_0, whereas, for a given metal cage, the all-metal electrides with Ni as the central atom correspond to the largest beta^e_0. Owing to the two effects, the endohedral all-metal electride cage 2e-Mg2+(Ni@Sn12)2-Ca2+ exhibits the largest beta^e_0 value (16 893 a.u.). The same conclusions are also valid for the frequency-dependent be(2omega; omega, omgea) and be(2omea; omega, 0). Moreover, we have also explored the role of the vibrational contribution in the largest components (in x-axis) of static b for endohedral all-metal electride cages. The vibrational contributions are significant for new all-metal electride NLO properties and therefore should be considered in the design of new NLO all-metal electrides
dc.description.sponsorship
This study was supported by the National Natural Science Foundation of China (Grant
No. 21573089, 21603032), the Graduate Innovation Fund of Jilin University (Grant
No. 2017011), the Spanish Ministerio de Economıa y competividad (MINECO,
CTQ2014-52525-P), and the Generalitat de Catalunya (project number 2014SGR931)
dc.format.extent
9 p.
dc.format.mimetype
application/pdf
dc.language.iso
eng
dc.publisher
Royal Society of Chemistry (RSC)
dc.relation
info:eu-repo/grantAgreement/MINECO//CTQ2014-52525-P/ES/FUNCIONALES DFT PARA EL CALCULO DE PROPIEDADES OPTICAS NO LINEALES/
dc.relation.isformatof
Versió postprint del document publicat a: https://doi.org/10.1039/c8tc05647a
dc.relation.ispartof
© Journal of materials chemistry. C, 2019, vol. 7, núm. 3, p. 645-653
dc.relation.ispartofseries
Articles publicats (D-Q)
dc.rights
Tots els drets reservats
dc.source
He, Hui-Min Luis Luis, Josep Maria Chen, Wei-Hong Yu, Dan Li, Ying Wu, Di Sun, Wei-Ming Li, Zhi-Ru 2019 Nonlinear optical response of endohedral all-metal electride cages 2e-Mg2+(M@E12)2-Ca2+ (M = Ni, Pd, and Pt; E = Ge, Sn, and Pb) Journal of materials chemistry. C 7 3 645 653
dc.subject
dc.title
Nonlinear optical response of endohedral all-metal electride cages 2e-Mg2+(M@E12)2-Ca2+ (M = Ni, Pd, and Pt; E = Ge, Sn, and Pb)
dc.type
info:eu-repo/semantics/article
dc.rights.accessRights
info:eu-repo/semantics/openAccess
dc.embargo.terms
2020-01-21T00:00:00Z
dc.date.embargoEndDate
info:eu-repo/date/embargoEnd/2020-12-31
dc.type.version
info:eu-repo/semantics/acceptedVersion
dc.identifier.doi
dc.identifier.idgrec
029343
dc.contributor.funder
dc.type.peerreviewed
peer-reviewed
dc.relation.ProjectAcronym