Blanquer, Guillaume

Cordova-Castro, R. Margoth

De Wilde, Yannick

Izeddin, Ignacio

Jonker, Dirk

Krachmalnicoff, Valentina

Susarrey-Arce, Arturo

van Dam, Bart

English

The direct measurement of a single emitter decay rate and the simultaneous knowledge of their position is a powerful tool for the study of light-matter interaction at the nanometer scale. In particular, the decay rate is directly related to the local density of states (LDOS) which measures the number of modes of the electromagnetic environment available for the decay of an emitter.</p

University of Twente Research Information

   Single-molecule imaging of LDOS modification  by an array of plasmonic nanochimneys  R. Margoth Córdova-Castro1, Dirk Jonker 2, Bart van Dam1, Guillaume Blanquer, Yannick De Wilde1, Ignacio Izeddin1, Arturo Susarrey-Arce2, Valentina Krachmalnicoff1.  1. Institut Langevin, ESPCI Paris, Université PSL, CNRS, 75005 Paris, France. 2. Mesoscale Chemical Systems, MESA+ Institute, University of Twente, Enschede 7500AE, The Netherlands.       The direct measurement of a single emitter decay rate and the simultaneous knowledge of their position is a powerful tool for the study of light-matter interaction at the nanometer scale. In particular, the decay rate is directly related to the local density of states (LDOS) which measures the number of modes of the electromagnetic environment available for the decay of an emitter.   In this work we study the modification of fluorescence emission and decay rate of single fluorescent molecules in the near field of a periodic plasmonic nanostructure formed by a square lattice of Au nanochimneys (hollow conical pillars). Such nanostructure can be fabricated on a large area with a wafer-scale (15cm2) fabrication method by sputter redeposition on a hybrid mask [1]. It behaves as a metamaterial in the near-IR and supports rich optical properties with tunable dipolar and quadrupolar plasmonic resonances in the visible spectral range with angular illumination dependence.   Fig. 1 Scanning electron microscopy image of the nanochimneys array and calculated field enhancement (Finite Element Method) for a Au nanochimneys square array with unitary cell as described at a 620 nm wavelength under the illumination with p-polarised plane wave at a 45°angle..    We perform nanometer-resolved imaging of the LDOS by simultaneously mapping the position and the decay rate of photoactivatable single-molecules with a novel super-resolved microscopy approach [2] which enables multiplexed and super-resolved fluorescence lifetime imaging at the single-molecule level (smFLIM) with a field of view of ~10 µm2. Our method combines the use of an EMCCD camera for spatial measurements and a linear array of single-photon avalanche diodes (SPADs) for time-resolved measurements [3]. We observe the field enhancement and the LDOS modification of such optically rich material at different illumination conditions, for TM and TE polarization at different angles of illumination, and we measure a large Purcell factor enhancement which increases for oblique illumination of the nanostructure.   [1] D. Jonker, Z. Jafari, J.P. Winczewski, C. Eyovge, J. G. E. Gardeniers, I. De Leon and A. Susarrey-Arce, “A Wafer-scale Fabrication Method for Three-Dimensional Plasmonic Hollow Nanopillars” to be published (2021). [2] D. Bouchet, J. Scholler, G. Blanquer, Y. De Wilde, I. Izeddin, and V. Krachmalnicoffl, “Probing near-field light–matter interactions with single-molecule lifetime imaging,” Optica 6, 135 (2019). [3] G. Blanquer, B. van Dam, A. Gulinatti, G. Acconcia, Y. De Wilde, I. Izeddin, and V. Krachmalnicoff, “Relocating Single Molecules in Super-Resolved Fluorescence Lifetime Images near a Plasmonic Nanostructure,”ACS Photonics 7, 393-400  (2020).    978-1-6654-1876-8/21/$31.00 c©2021 European Union2021 Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC) | 978-1-6654-1876-8/21/$31.00 ©2021 IEEE | DOI: 10.1109/CLEO/Europe-EQEC52157.2021.9541896Authorized licensed use limited to: UNIVERSITY OF TWENTE.. Downloaded on November 23,2021 at 08:45:31 UTC from IEEE Xplore.  Restrictions apply. 

Single-molecule imaging of LDOS modification by an array of plasmonic nanochimneys

R. Margoth Cordova-Castro

Dirk Jonker

Bart van Dam

Guillaume Blanquer

Yannick De Wilde

Ignacio Izeddin

Arturo Susarrey-Arce

Valentina Krachmalnicoff

Crossref

https://research.utwente.nl/en/publications/5e0a1290-4404-474e-bb97-50302d62e16f

Single-molecule imaging of LDOS modification by an array of plasmonic nanochimneys

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