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Strong two-photon circular dichroism in helicenes: A theoretical investigation
KTH, School of Biotechnology (BIO), Theoretical Chemistry.ORCID iD: 0000-0002-1763-9383
2008 (English)In: Journal of Chemical Theory and Computation, ISSN 1549-9618, E-ISSN 1549-9626, Vol. 4, no 3, 457-467 p.Article in journal (Refereed) Published
Abstract [en]

Using a recently derived origin-invariant quadratic response approach combined with time-dependent density functional theory, four representative helicenes are shown to present a very strong two-photon circular dichroism (TPCD) response, which makes them candidates for the first experimental observation of a TPCD effect. The large response is attributed to the unique combination of chirality and electron delocalization. Comparison with electronic circular dichroism and two-photon absorption (TPA) shows that the three effects exhibit complementary features for unravelling the molecular structures. In particular, for the four (M)-helicenes studied here, the first, i.e., low-energy, dominant Cotton band is always negative, whereas for TPCD it is positive. From an analysis of the frontier orbitals describing most of the one-electron excitation vectors, the largest TPCD response of tetramethoxy-bisquinone-dithia-[7]-helicene has been attributed to the charge-transfer character of the excited state, like for the parent TPA effect. Moreover, the TPCD intensities are found to be mostly governed by the electric and magnetic dipole contributions, while the electric quadrupole terms are, on a relative basis, less important.

Place, publisher, year, edition, pages
2008. Vol. 4, no 3, 457-467 p.
Keyword [en]
density-functional theory, bridged triarylamine helicenes, nonlinear-optical properties, absorption cross-sections, multiphoton, absorption, 2nd-harmonic generation, organic-molecules, permanent, moments, chiral molecules, liquid-crystal
URN: urn:nbn:se:kth:diva-17398DOI: 10.1021/ct700329aISI: 000254277900009ScopusID: 2-s2.0-42949135428OAI: diva2:335442
QC 20100525Available from: 2010-08-05 Created: 2010-08-05Bibliographically approved

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Ågren, Hans
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