Chiral Photomelting of DNA-Nanocrystal Assemblies Utilizing Plasmonic Photoheating
- Oscar Ávalos-Ovando*Oscar Ávalos-Ovando*Email: [email protected]Department of Physics and Astronomy, Ohio University, Athens, Ohio 45701, United StatesMore by Oscar Ávalos-Ovando
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- Lucas V. Besteiro
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- Artur MovsesyanArtur MovsesyanDepartment of Physics and Astronomy, Ohio University, Athens, Ohio 45701, United StatesInstitute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, ChinaMore by Artur Movsesyan
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- Gil MarkovichGil MarkovichSchool of Chemistry, Raymond and Beverly Sackler Faculty of Exact Sciences, Tel Aviv University, Tel Aviv, 6997801 IsraelMore by Gil Markovich
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- Tim LiedlTim LiedlFaculty of Physics and Center for NanoScience (CeNS), Ludwig-Maximilians-University, 80539 Munich, GermanyMore by Tim Liedl
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- Kevin MartensKevin MartensFaculty of Physics and Center for NanoScience (CeNS), Ludwig-Maximilians-University, 80539 Munich, GermanyMore by Kevin Martens
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- Zhiming WangZhiming WangInstitute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, ChinaMore by Zhiming Wang
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- Miguel A. Correa-DuarteMiguel A. Correa-DuarteCINBIO, Universidade de Vigo, 36310 Vigo, SpainMore by Miguel A. Correa-Duarte
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- Alexander O. Govorov*Alexander O. Govorov*Email: [email protected]Department of Physics and Astronomy, Ohio University, Athens, Ohio 45701, United StatesMore by Alexander O. Govorov
Abstract
Chiral plasmonic nanostructures exhibit anomalously strong chiroptical signals and offer the possibility to realize asymmetric photophysical and photochemical processes controlled by circularly polarized light. Here, we use a chiral DNA-assembled nanorod pair as a model system for chiral plasmonic photomelting. We show that both the enantiomeric excess and consequent circular dichroism can be controlled with chiral light. The nonlinear chiroptical response of our plasmonic system results from the chiral photothermal effect leading to selective melting of the DNA linker strands. Our study describes both the single-complex and collective heating regimes, which should be treated with different models. The chiral asymmetry factors of the calculated photothermal and photomelting effects exceed the values typical for the chiral molecular photochemistry at least 10-fold. Our proposed mechanism can be used to develop chiral photoresponsive systems controllable with circularly polarized light.
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