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O: Fachverband Oberflächenphysik
O 83: Focus Session: Novel Approaches to Surface Plasmon Generated Charges and Heat for Photocatalysis II (joint session O/CPP)
O 83.7: Talk
Thursday, March 21, 2024, 12:15–12:30, MA 141
Plasmonically generated low-energy electrons: the decomposition of DNA nucleobases derivatives study case — •Sergio Kogikoski Junior1, Janka Kopyra2, Janusz Rak3, and Ilko Bald1 — 1Institute of Chemistry, University of Potsdam, Germany — 2Faculty of Sciences, Siedlce University of Natural Sciences and Humanities, Poland — 3Faculty of Chemistry, University of Gdansk, Poland
One outcome of the excitation of plasmonic nanoparticles is the generation of low-energy charge carriers (E < 0.5 eV). Our group showed that such charge carriers could drive chemical reactions at the interface of Au and Ag nanoparticles using different probe molecules, such as bromoadenine. However, it is still unclear how such molecule activation happens and what the energy of these carriers is. Herein, we used modified DNA nucleobases as probes to understand the role of the support metal and the low-energy electrons generated. The activation mechanisms to drive reactions using low-energy electrons are already well-studied in the gas phase of such molecules, providing a suitable theoretical background. SERS was used to obtain the molecular fingerprint of the system during irradiation. Our results show that irradiated AgNPs can decompose uracil and adenine derivatives, possibly related to the higher amount and energy of the generated hot electrons. Also, adenines are readily decomposed, even though studies in the gas phase show that both molecules decompose. The results show an energy landscape of plasmonically generated hot charges and its relation to probe molecule structure.
Keywords: plasmonic nanoparticles; plasmonic catalysis; low energy electrons; hot electrons; DNA nanotechnology