[en] We present a comprehensive experimental and theoretical study of the optical properties of matrix-isolated molecules of the two perylene derivatives N,N'-dimethylperylene-3,4,9,10-dicarboximide (MePTCDI) and 3,4,9,10-perylenetetracarboxylic dianhydride (PTCDA). A solid solution of the dyes in an SiO2 matrix exhibits monomer-like behavior. Transient absorption pump-probe spectroscopy in the range 1.2-2.6 eV has been performed on an ultrafast time scale. The differential transmittance reveals contributions from ground-state bleaching, stimulated emission, and excited-state absorption. Both systems exhibit broad excited-state absorption features below 2.0 eV with a clear peak around 1.8 eV. The spectra can be consistently explained by the results of quantum-chemical calculations. We have applied both the coupled cluster singles and doubles (CCSD) model and the multireference-determinant single and double configuration-interaction (MRD-CI) technique on the basis of the intermediate neglect of differential overlap (INDO) Hamiltonian. The results are insensitive to whether the geometry is optimized for the electronic ground state or first excited state. The experimental polarization anisotropies for the two major transitions are in agreement with the calculated polarizations.
Disciplines :
Physics
Author, co-author :
Engel, E.
Schmidt, K.
Beljonne, David ; Université de Mons > Faculté des Sciences > Chimie des matériaux nouveaux
Brédas, Jean-Luc ; Université de Mons > Faculté des Sciences > Chimie des matériaux nouveaux
Assa, J.
Fröb, H.
Leo, K.
Hoffmann, M.
Language :
English
Title :
Transient Absorption Spectroscopy and Quantum-Chemical Studies of Matrix-Isolated Perylene Derivatives
Publication date :
29 June 2006
Journal title :
Physical Review. B, Condensed Matter
ISSN :
0163-1829
Publisher :
American Physical Society, Moldova
Volume :
73
Issue :
24
Pages :
245216
Peer reviewed :
Peer Reviewed verified by ORBi
Research unit :
S817 - Chimie des matériaux nouveaux
Research institute :
R400 - Institut de Recherche en Science et Ingénierie des Matériaux
Commentary :
Lecture en ligne: http://www.hemica.de/HoffmannScientific/Pdf/Engel06b_web.pdf
Publié en ligne le 7 avril 2006
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