Two-photon absorption properties of two-dimensional π-conjugated chromophores: Combined experimental and theoretical study
Ohta K, Yamada S, Kamada K, Slepkov AD, Hegmann FA, Tykwinski R, Shirtcliff LD, Haley MM, Salek P, Gel'Mukhanov F, Agren H (2011)
Publication Type: Journal article, Original article
Publication year: 2011
Journal
Original Authors: Ohta K., Yamada S., Kamada K., Slepkov A.D., Hegmann F.A., Tykwinski R.R., Shirtcliff L.D., Haley M.M., Salek P., Gel'mukhanov F., Agren H.
Publisher: American Chemical Society
Book Volume: 115
Pages Range: 105-117
Journal Issue: 2
DOI: 10.1021/jp107044w
Abstract
The two-photon absorption (TPA) properties of four TPEB [tetrakis(phenylethynyl)benzene] derivatives (TD, para, ortho, and meta) with different donor/acceptor substitution patterns have been investigated experimentally by the femtosecond open-aperture Z-scan method and theoretically by the time-dependent density-functional theory (TDDFT) method. The four compounds show relatively large TPA cross sections, and the all-donor substituted species (TD) displays the largest TPA cross-section σ = 520 ± 30 GM. On the basis of the calculated electronic structure, TD shows no TPA band in the lower energy region of the spectrum because the transition density is concentrated on particular transitions due to the high symmetry of the molecular structure. The centrosymmetric donor-acceptor TPEB para shows excitations resulting from transitions centered on D-π-D and A-π-A moieties, as well as transition between the D-π-D and A-π-A moieties; this accounts for the broad nature of the TPA bands for this compound. Calculations for two noncentrosymmetric TPEBs (ortho and meta) reveal that the diminished TPA intensities of higher-energy bands result from destructive interference between the dipolar and three-state terms. The molecular orbitals (MOs) of the TPEBs are derivable with linear combinations of the MOs of the two crossing BPEB [bis(phenylethynyl) benzene] derivatives. Overall, the characteristics of the experimental spectra are well-described based on the theoretical analysis. © 2010 American Chemical Society.
Authors with CRIS profile
Involved external institutions
Royal Institute of Technology / Kungliga Tekniska Högskolan (KTH)
Sweden (SE)
University of Oregon (UO)
United States (USA) (US)
University of Alberta
Canada (CA)
National Institute of Advanced Industrial Science and Technology / 産業技術総合研究所 (AIST)
Japan (JP)
Sweden (SE)
University of Oregon (UO)
United States (USA) (US)
University of Alberta
Canada (CA)
National Institute of Advanced Industrial Science and Technology / 産業技術総合研究所 (AIST)
Japan (JP)
How to cite
APA:
Ohta, K., Yamada, S., Kamada, K., Slepkov, A.D., Hegmann, F.A., Tykwinski, R.,... Agren, H. (2011). Two-photon absorption properties of two-dimensional π-conjugated chromophores: Combined experimental and theoretical study. Journal of Physical Chemistry A, 115(2), 105-117. https://doi.org/10.1021/jp107044w
MLA:
Ohta, Koji, et al. "Two-photon absorption properties of two-dimensional π-conjugated chromophores: Combined experimental and theoretical study." Journal of Physical Chemistry A 115.2 (2011): 105-117.
BibTeX: Download