Please use this identifier to cite or link to this item: http://dx.doi.org/10.14279/depositonce-5247
|Main Title:||Size and shape dependent photoluminescence and excited state decay rates of diamondoids|
Dahl, Jeremy E.
Carlson, Robert M. K.
|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.|
|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|
|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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