Photophysical Behavior of Self-Organizing Derivatives of 10- and 12-Vertex p-Carboranes, and their Bicyclo[2.2.2]octane and Benzene Analogues.

DFT calculations UV spectroscopy boron clusters fluorescence liquid crystals molecular structure synthesis

Journal

Chemistry (Weinheim an der Bergstrasse, Germany)
ISSN: 1521-3765
Titre abrégé: Chemistry
Pays: Germany
ID NLM: 9513783

Informations de publication

Date de publication:
26 May 2023
Historique:
received: 16 12 2022
medline: 23 2 2023
pubmed: 23 2 2023
entrez: 22 2 2023
Statut: ppublish

Résumé

Four series of isostructural derivatives of 3-ring liquid crystalline derivatives containing p-carboranes (12-vertex A, and 10-vertex B), bicyclo[2.2.2]octane (C), or benzene (D) as the variable structural element were investigated for their mesogenic behavior and electronic interactions. Comparative studies demonstrated that the effectiveness of elements A-D in stabilization of the mesophase typically increases in the order: B<A<C<D. Absorption and emission spectroscopy for the four series and reference compounds augmented with DFT computational results revealed that the degree of electronic interactions with the connected benzene π system increases in the order C<A<B<D. Emission spectra exhibit large Stokes' shifts for 10-vertex derivatives (B) in solutions and in the solid state. Spectroscopic characterization was supplemented with polarization electronic spectroscopy and solvatochromic studies of selected series. Overall, 12-vertex p-carborane A acts as an electron withdrawing auxochromic substituent with interactions similar to those of bicyclo[2.2.2]octane, although capable of accepting some electron density in the excited state. In contrast, 10-vertex p-carborane B is much more interactive with the π-aromatic electron manifold and exhibits greater ability to participate in photo-induced CT processes. Absorption and emission energies and quantum yields (1-51 %) for carborane derivatives, representing the D-A-D system, were compared to those of their isoelectronic zwitterionic analogues (the A-D-A system). The analysis is supplemented with four single-crystal XRD structures.

Identifiants

pubmed: 36813741
doi: 10.1002/chem.202203948
doi:

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

e202203948

Subventions

Organisme : Fundacja na rzecz Nauki Polskiej
ID : TEAM/2016-3/24

Informations de copyright

© 2023 Wiley-VCH GmbH.

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Auteurs

Rafał Jakubowski (R)

Centre of Molecular and Macromolecular Studies, Polish Academy of Sciences, Sienkiewicza 112, 90-363, Łódź, Poland.

Adam Januszko (A)

Department of Chemistry, Vanderbilt University, Nashville, TN 37212, USA.

R William Tilford (R)

Department of Chemistry, Vanderbilt University, Nashville, TN 37212, USA.

George J Radziszewski (GJ)

Department of Chemistry, Colorado School of Mines, Golden, CO 80401, USA.

Anna Pietrzak (A)

Faculty of Chemistry, Łódź University of Technology, 90-924, Łódź, Poland.

Victor G Young (VG)

Department of Chemistry, University of Minnesota, Twin Cities, MN 55455, USA.

Piotr Kaszyński (P)

Centre of Molecular and Macromolecular Studies, Polish Academy of Sciences, Sienkiewicza 112, 90-363, Łódź, Poland.
Department of Chemistry, Vanderbilt University, Nashville, TN 37212, USA.
Faculty of Chemistry, University of Łódź, Tamka 12, 91-403 Łódź, Poland.
Department of Chemistry, Middle Tennessee State University, Murfreesboro, TN 37132, USA.

Classifications MeSH