Light-Harvesting Nanoparticle Core-Shell Clusters with Controllable Optical Output.
We used DNA self-assembly methods to fabricate a series of core-shell gold nanoparticle-DNA-colloidal quantum dot (AuNP-DNA-Qdot) nanoclusters with satellite-like architecture to modulate optical (photoluminescence) response. By varying the intercomponent distance through the DNA linker length designs, we demonstrate precise tuning of the plasmon-exciton interaction and the optical behavior of the nanoclusters from regimes characterized by photoluminescence quenching to photoluminescence enhancement. The combination of detailed X-ray scattering probing with photoluminescence intensity and lifetime studies revealed the relation between the cluster structure and its optical output. Compared to conventional light-harvesting systems like conjugated polymers and multichromophoric dendrimers, the proposed nanoclusters bring enhanced flexibility in controlling the optical behavior toward a desired application, and they can be regarded as controllable optical switches via the optically pumped color.
†Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, United States.|‡Department of Materials Science and Engineering, South University of Science and Technology of China, Shenzhen, Guangdong 518055, China.
Dazhi
D
Sun
†Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, United States.
Ye
Y
Tian
†Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, United States.
Yugang
Y
Zhang
†Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, United States.|§Department of Chemical Engineering, University of Minnesota, Duluth, Minnesota 55812, United States.
Zhihua
Z
Xu
†Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, United States.
Matthew Y
MY
Sfeir
†Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, United States.
Mircea
M
Cotlet
†Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, United States.
Oleg
O
Gang
D003102:Colloids / Q000737:chemistry; D004247:DNA / Q000737:chemistry*; D006046:Gold / Q000737:chemistry*; D008027:Light; D049449:Luminescence; D053768:Metal Nanoparticles / Q000737:chemistry*; D055668:Photochemical Processes; D045663:Quantum Dots
D003102:Colloids; D006046:Gold; D004247:DNA
DNA; cluster; fluorescence; nanoparticle; quantum dots; self-assembly