Abstract
Single-molecule fluorescence has revealed a wealth of biochemical processes but does not give access to submillisecond dynamics involved in transient interactions and molecular dynamics. Here we overcome this bottleneck and demonstrate record-high photon count rates of >107 photons/s from single plasmon-enhanced fluorophores. This is achieved by combining two conceptual novelties: first, we balance the excitation and decay rate enhancements by the antenna’s volume, resulting in maximum fluorescence intensity. Second, we enhance the triplet decay rate using a multicomponent surface chemistry that minimizes microsecond blinking. We demonstrate applications to two exemplary molecular processes: we first reveal transient encounters and hybridization of DNA with a 1 μs temporal resolution. Second, we exploit the field gradient around the nanoparticle as a molecular ruler to reveal microsecond intramolecular dynamics of multivalent complexes. Our results pave the way toward real-time microsecond studies of biochemical processes using an implementation compatible with existing single-molecule fluorescence methods.
| Original language | English |
|---|---|
| Journal | Nano Letters |
| Volume | 24 |
| Issue | 37 |
| Pages (from-to) | 11641-11647 |
| Number of pages | 7 |
| ISSN | 1530-6984 |
| DOIs | |
| Publication status | Published - 18 Sept 2024 |
Keywords
- nanoscale sensing
- plasmon-enhanced fluorescence
- single gold nanoparticles
- single-molecule detection