@article{KogikoskiJuniorDuttaBald2021, author = {Kogikoski Junior, Sergio and Dutta, Anushree and Bald, Ilko}, title = {Spatial separation of plasmonic hot-electron generation and a hydrodehalogenation reaction center using a DNA wire}, series = {ACS nano}, volume = {15}, journal = {ACS nano}, number = {12}, publisher = {American Chemical Society}, address = {Washington}, issn = {1936-0851}, doi = {10.1021/acsnano.1c09176}, pages = {20562 -- 20573}, year = {2021}, abstract = {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.}, language = {en} } @article{HeckPrinzDatheetal.2017, author = {Heck, Christian and Prinz, Julia and Dathe, Andre and Merk, Virginia and Stranik, Ondrej and Fritzsche, Wolfgang and Kneipp, Janina and Bald, Ilko}, title = {Gold Nanolenses Self-Assembled by DNA Origami}, series = {ACS Photonics}, volume = {4}, journal = {ACS Photonics}, publisher = {American Chemical Society}, address = {Washington}, issn = {2330-4022}, doi = {10.1021/acsphotonics.6b00946}, pages = {1123 -- 1130}, year = {2017}, abstract = {Nanolenses are self-similar chains of metal nanoparticles, which can theoretically provide extremely high field enhancements. Yet, the complex structure renders their synthesis challenging and has hampered closer analyses so far. Here, DNA origami is used to self-assemble 10, 20, and 60 nm gold nanoparticles as plasmonic gold nanolenses (AuNLs) in solution and in billions of copies. Three different geometrical arrangements are assembled, and for each of the three designs, surface-enhanced Raman scattering (SERS) capabilities of single AuNLs are assessed. For the design which shows the best properties, SERS signals from the two different internal gaps are compared by selectively placing probe dyes. The highest Raman enhancement is found for the gap between the small and medium nanoparticle, which is indicative of a cascaded field enhancement.}, language = {en} } @article{EerqingSubramanianRubioJimenezetal.2021, author = {Eerqing, Narima and Subramanian, Sivaraman and Rubio Jimenez, Jesus and Lutz, Tobias and Wu, Hsin-Yu and Anders, Janet and Soeller, Christian and Vollmer, Frank}, title = {Comparing transient oligonucleotide hybridization kinetics using DNA-PAINT and optoplasmonic single-molecule sensing on gold nanorods}, series = {ACS photonics / American Chemical Society}, volume = {8}, journal = {ACS photonics / American Chemical Society}, number = {10}, publisher = {American Chemical Society}, address = {Washington}, issn = {2330-4022}, doi = {10.1021/acsphotonics.1c01179}, pages = {2882 -- 2888}, year = {2021}, abstract = {We report a comparison of two photonic techniques for single-molecule sensing: fluorescence nanoscopy and optoplasmonic sensing. As the test system, oligonucleotides with and without fluorescent labels are transiently hybridized to complementary "docking" strands attached to gold nanorods. Comparing the measured single-molecule kinetics helps to examine the influence of the fluorescent labels as well as factors arising from different sensing geometries. Our results demonstrate that DNA dissociation is not significantly altered by the fluorescent labels and that DNA association is affected by geometric factors in the two techniques. These findings open the door to exploiting plasmonic sensing and fluorescence nanoscopy in a complementary fashion, which will aid in building more powerful sensors and uncovering the intricate effects that influence the behavior of single molecules.}, language = {en} }