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Main Title: Size and shape dependent photoluminescence and excited state decay rates of diamondoids
Author(s): Richter, Robert
Wolter, David
Zimmermann, Tobias
Landt, Lasse
Knecht, Andre
Heidrich, Christoph
Merli, Andrea
Dopfer, Otto
Reiss, Philipp
Ehresmann, Arno
Petersen, Jens
Dahl, Jeremy E.
Carlson, Robert M. K.
Bostedt, Christoph
Möller, Thomas
Mitric, Roland
Rander, Torbjörn
Type: Article
Language Code: en
Abstract: We present photoluminescence spectra and excited state decay rates of a series of diamondoids, which represent molecular structural analogues to hydrogen-passivated bulk diamond. Specific isomers of the five smallest diamondoids (adamantane–pentamantane) have been brought into the gas phase and irradiated with synchrotron radiation. All investigated compounds show intrinsic photoluminescence in the ultraviolet spectral region. The emission spectra exhibit pronounced vibrational fine structure which is analyzed using quantum chemical calculations. We show that the geometrical relaxation of the first excited state of adamantane, exhibiting Rydberg character, leads to the loss of Td symmetry. The luminescence of adamantane is attributed to a transition from the delocalized first excited state into different vibrational modes of the electronic ground state. Similar geometrical changes of the excited state structure have also been identified in the other investigated diamondoids. The excited state decay rates show a clear dependence on the size of the diamondoid, but are independent of the particle geometry, further indicating a loss of particle symmetry upon electronic excitation.
Issue Date: 2014
Date Available: 23-Jun-2016
DDC Class: 540 Chemie und zugeordnete Wissenschaften
Sponsor/Funder: DFG, FOR 1282, Controlling the electronic structure of semiconductor nanoparticles by doping and hybrid formation
Journal Title: Physical chemistry, chemical physics
Publisher: Royal Society of Chemistry
Publisher Place: Cambridge
Volume: 16
Issue: 7
Publisher DOI: 10.1039/c3cp54570a
Page Start: 3070
Page End: 3076
EISSN: 1463-9076
Notes: Dieser Beitrag ist mit Zustimmung des Rechteinhabers aufgrund einer (DFG geförderten) Allianz- bzw. Nationallizenz frei zugänglich.
This publication is with permission of the rights owner freely accessible due to an Alliance licence and a national licence (funded by the DFG, German Research Foundation) respectively.
Appears in Collections:Inst. Optik und Atomare Physik » Publications

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