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Spin Multiplicity Dependence of Nonlinear Optical Properties
KTH, School of Biotechnology (BIO), Theoretical Chemistry.
KTH, School of Biotechnology (BIO), Theoretical Chemistry.
KTH, School of Biotechnology (BIO), Theoretical Chemistry.ORCID iD: 0000-0002-1763-9383
2009 (English)In: ChemPhysChem, ISSN 1439-4235, E-ISSN 1439-7641, Vol. 10, no 5, 817-823 p.Article in journal (Refereed) Published
Abstract [en]

Open-shell spin-restricted time-dependent density functional theory is applied to explore the spin multiplicity dependence of linear and nonlinear optical properties. An open-shell neutral conjugated system, the CAN radical in the doublet X(2)A(2), quartet X(4)A(2), and sextet X(6)A(1) states, is chosen as a model system to illustrate various aspects of the theory. It is found that irrespective of the exchange-correlation functional employed, the components of the polarizability alpha(-omega,omega) and first hyperpolarizability beta(-2(omega,omega,omega) show very different dependency with respect to the multiplicity, with an increasing trend for higher spin states. This is rationalized by the decrease in conjugation and stability of the system with increasing multiplicity, and by the way the interaction between unpaired electrons and the external field is shielded by remaining electrons of the molecule. The study suggests the applicability of open-shell systems for frequency-dependent nonlinear optical properties and for the possibility of spin control for such properties.

Place, publisher, year, edition, pages
2009. Vol. 10, no 5, 817-823 p.
Keyword [en]
density functional calculations, nonlinear optics, open-shell systems, polarizability, spin multiplicity, 2nd hyperpolarizabilities, diradical character, density, exchange, system, gamma
URN: urn:nbn:se:kth:diva-18323DOI: 10.1002/cphc.200800671ISI: 000264774300013ScopusID: 2-s2.0-64249085026OAI: diva2:336369
QC 20100525Available from: 2010-08-05 Created: 2010-08-05 Last updated: 2011-01-10Bibliographically approved

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Jha, Prakash ChandraRinkevicius, ZilvinasÅgren, Hans
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