Institute of Chemistry, Physical Chemistry, University of Potsdam, Karl-Liebknecht-Strasse 24-25, 14476 Potsdam, Germany.
Department of Analytical Chemistry, Institute of Chemistry, State University of Campinas (UNICAMP), P.O. Box 6154, 13083-970, Campinas São Paulo, Brazil.
ACS Nano. 2021 Dec 28;15(12):20562-20573. doi: 10.1021/acsnano.1c09176. Epub 2021 Dec 7.
Using hot charge carriers far from a plasmonic nanoparticle surface is very attractive for many applications in catalysis and nanomedicine and will lead to a better understanding of plasmon-induced processes, such as hot-charge-carrier- or heat-driven chemical reactions. Herein we show that DNA is able to transfer hot electrons generated by a silver nanoparticle over several nanometers to drive a chemical reaction in a molecule nonadsorbed on the surface. For this we use 8-bromo-adenosine introduced in different positions within a double-stranded DNA oligonucleotide. The DNA is also used to assemble the nanoparticles into nanoparticles ensembles enabling the use of surface-enhanced Raman scattering to track the decomposition reaction. To prove the DNA-mediated transfer, the probe molecule was insulated from the source of charge carriers, which hindered the reaction. The results indicate that DNA can be used to study the transfer of hot electrons and the mechanisms of advanced plasmonic catalysts.
利用远离等离子体纳米粒子表面的热电荷载流子对于催化和纳米医学中的许多应用非常有吸引力，并且将有助于更好地理解等离子体诱导的过程，例如热电荷载流子或热驱动的化学反应。在此，我们表明 DNA 能够将由银纳米粒子产生的热电子转移到几个纳米之外，以驱动非吸附在表面上的分子中的化学反应。为此，我们使用在双链 DNA 寡核苷酸中不同位置引入的 8-溴-腺苷。DNA 还用于将纳米粒子组装成纳米粒子集合体，从而可以使用表面增强拉曼散射来跟踪分解反应。为了证明 DNA 介导的转移，将探针分子与电荷载流子的源隔离开，这阻碍了反应。结果表明，DNA 可用于研究热电子的转移和先进等离子体催化剂的机理。
