Light-matter interactions at the nanoscale

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Nanoantenna enhanced fluorescence

Antennas in nanobiophotonics

Principal investigator: Jerome Wenger

Nanophotonics can improve single molecule optical detection beyond the diffraction limit. The main goal is to tailor the electromagnetic environment by the use of an optical antenna to concentrate the light on a tiny spot and simultaneously enhance the molecular emission. Single molecule spectroscopy techniques, FRET and FCS can greatly benefit from photonic nanoantennas to enter a new dimension of higher sensitivities at molecular concentrations reaching physiological conditions.

In a collaboration with ICFO and EPFL, we develop a novel “antenna-in-box” platform for single molecule fluorescence detection with unprecedented resolutions and sensitivity. The innovative approach combines a plasmonic gap antenna for ultra-high fluorescence enhancement with a metal nanoaperture for optimized background-free operation. It allows for 1100-fold fluorescence brightness enhancement together with detection volumes down to 58 zeptoliters (1 zL = 1e-21L), realizing a gain of four orders of magnitude as compared to classical microscopes. The antenna-in-box offers a highly efficient platform for nanoscale biochemical assays with single molecule sensitivity at physiological conditions. This research is done in close collaboration with the groups of Niek Van Hulst and Maria Garcia-Parajo at ICFO, and is part of the NANO-VISTA project, funded by the European Commission’s 7th research Framework programme.

Photonic engineering of fluorescent dyes Designing fluorescent dyes typically relies on a molecular engineering approach in which photophysical properties are tuned by chemical modifications. We present a novel way of engineering the luminescence by changing the photonic environment of a chromophore while maintaining its solubility. We produce purified suspensions of gold nanoparticle dimers linked by a single DNA double strand exhibiting one a single dye molecule. Tuning the electromagnetic field enables unprecedented photophysical properties, such as decay rates and excitation cross-sections enhanced by more than one order of magnitude compared to an optimized, commercial chromophore. This research is done in close collaboration with the group of Sebastien Bidault at Institut Langevin.

Publications

[17] P. M. Winkler, R. Regmi, V. Flauraud, J. Brugger, H. Rigneault, J. Wenger, M. F. García-Parajo, Optical Antenna-based Fluorescence Correlation Spectroscopy to Probe the Nanoscale Dynamics of Biological Membranes, J. Phys. Chem. Lett. 9, 110-119 (2018). DOI: 10.1021/acs.jpclett.7b02818, arXiv 1712.06817
[16] R. Regmi, P. M. Winkler, V. Flauraud, J. Brugger, H. Rigneault, J. Wenger, M. F. García-Parajo, Planar Optical Nanoantennas Resolve Cholesterol-Dependent Nanoscale Heterogeneities in the Plasma Membrane of Living Cells, Nano Lett. 17, 6295–6302 (2017). DOI: 10.1021/acs.nanolett.7b02973, arXiv 1711.06617
[15] P. M. Winkler, R. Regmi, V. Flauraud, J. Brugger, H. Rigneault, J. Wenger, M. F. García-Parajo, Transient Nanoscopic Phase Separation in Biological Lipid Membranes Resolved by Planar Plasmonic Antennas, ACS Nano 11, 7241-7250 (2017). DOI: 10.1021/acsnano.7b03177, arXiv 1711.07729
[14] V. Flauraud, R. Regmi, P. M. Winkler, D. T. L. Alexander, H. Rigneault, N. F. van Hulst, M. F. Garcia-Parajo, J. Wenger, J. Brugger, In-Plane Plasmonic Antenna Arrays with Surface Nanogaps for Giant Fluorescence Enhancement, Nano Lett. 17, 1703-1710 (2017). DOI: 10.1021/acs.nanolett.6b04978
[13] R. Regmi, J. Berthelot, P. M. Winkler, M. Mivelle, J. Proust, F. Bedu, I. Ozerov, T. Begou, J. Lumeau, H. Rigneault, M. F. García-Parajó, S. Bidault, J. Wenger, N. Bonod, All-Dielectric Silicon Nanogap Antennas To Enhance the Fluorescence of Single Molecules, Nano Lett. 16, 5143-5151 (2016).
[12] S. Bidault, A. Devilez, V. Maillard, L. Lermusiaux, J.M. Guigner, N. Bonod, J. Wenger, Picosecond lifetimes with high quantum yields from single-photon emitting colloidal nanostructures at room temperature, ACS Nano 10, 4806-4815 (2016).
[11] J. Wenger, R. Regmi, H. Rigneault, Plasmonic-enhanced fluorescence detection of single molecules at high concentrations in Roadmap on biosensing and photonics with advanced nano-optical methods, edited by E. Di Fabrizio, J. Optics 18, 063003 (2016).
[10] R. Regmi, A. A. Al Balushi, H. Rigneault, R. Gordon, J. Wenger, Nanoscale volume confinement and fluorescence enhancement with double nanohole aperture, Sci. Rep. 5, 15852 (2015).
[9] D. Punj, R. Regmi, A. Devilez, R. Plauchu, S. B. Moparthi, B. Stout, N. Bonod, H. Rigneault, J. Wenger, Self-Assembled Nanoparticle Dimer Antennas for Plasmonic-Enhanced Single-Molecule Fluorescence Detection at Micromolar Concentrations, ACS Photonics 2, 1099-1107 (2015).
[8] D. Punj, P. Ghenuche, S. B. Moparthi, J. de Torres, V. Grigoriev, H. Rigneault, J. Wenger, Plasmonic antennas and zero-mode waveguides to enhance single molecule fluorescence detection and fluorescence correlation spectroscopy toward physiological concentrations, WIREs Nanomed Nanobiotechnol 6, 268 (2014).
[7] D. Punj, J. de Torres, H. Rigneault, J. Wenger, Gold nanoparticles for enhanced single molecule fluorescence analysis at micromolar concentration, Opt. Express 21, 27338-27343 (2013).
[6] D. Punj, M. Mivelle, S. B. Moparthi, T. van Zanten, H. Rigneault, N. F. van Hulst, M. F. Garcia-Parajo, J. Wenger, A plasmonic ‘antenna-in-box’ platform for enhanced single-molecule analysis at micromolar concentrations, Nature Nanotech. 8, 512-516 (2013).
[5] M. P. Busson, B. Rolly, B. Stout, N. Bonod, J. Wenger, S. Bidault, Photonic engineering of hybrid metal-organic chromophores, Angew. Chem. Int. Ed. 51, 11083-11087 (2012).
[4] E. Bermúdez Ureña, M. P. Kreuzer, S. Itzhakov, H. Rigneault, R. Quidant, D. Oron, J. Wenger, Excitation enhancement of a quantum dot coupled to a plasmonic antenna, Adv. Mater. 24, OP314-OP-320 (2012).
[3] J. Wenger, Fluorescence Enhancement Factors on Optical Antennas: Enlarging the Experimental Values without Changing the Antenna Design, Int. J. Optics 2012, 828121 (2012).
[2] H. Aouani, S. Itzhakov, D. Gachet, E. Devaux, T. W. Ebbesen, H. Rigneault, D. Oron, J. Wenger, Colloidal Quantum Dots as Probes of Excitation Field Enhancement in Photonic Antennas, ACS Nano 4, 4571-4578 (2010)
[1] J. Wenger, H. Rigneault, Photonic Methods to Enhance Fluorescence Correlation Spectroscopy and Single Molecule Fluorescence Detection, Int. J. Mol. Sci. 11, 206-221 (2010)

The research leading to these results has received funding from the European Research Council under the European Union’s Seventh Framework Programme (FP7/2007-2013) / ERC Grant agreements 278242 (ExtendFRET).