Single-emitter super-resolved imaging of radiative decay rate enhancement in dielectric gap nanoantennas

R. Margoth Córdova-Castro; Bart van Dam; Alberto Lauri; Stefan A. Maier; Riccardo Sapienza; Yannick De Wilde; Ignacio Izeddin; Valentina Krachmalnicoff

doi:10.1038/s41377-023-01349-2

Your Location：

Home >

Browse articles >

Single-emitter super-resolved imaging of radiative decay rate enhancement in dielectric gap nanoantennas

Article

- Single-emitter super-resolved imaging of radiative decay rate enhancement in dielectric gap nanoantennas
- Light: Science & Applications Vol. 13, Issue 1, Pages: 47-54(2024)
- Affiliations：
- Author bio：
  
  gignacio.izeddin@espci.fr
  hvalentina.krachmalnicoff@espci.fr
- Funds：
- DOI：10.1038/s41377-023-01349-2
  CLC：
- Received：27 June 2023，
  
  Revised：20 November 2023，
  
  Accepted：2023-11-29，
  
  Published Online：02 January 2024，
  
  Published：2024-12
- Accepted：
Scan QR Code
R. Margoth Córdova-Castro, Bart van Dam, Alberto Lauri, et al. Single-emitter super-resolved imaging of radiative decay rate enhancement in dielectric gap nanoantennas[J]. Light: science & applications, 2024, 13(1): 47-54.
DOI：

R. Margoth Córdova-Castro, Bart van Dam, Alberto Lauri, et al. Single-emitter super-resolved imaging of radiative decay rate enhancement in dielectric gap nanoantennas[J]. Light: science & applications, 2024, 13(1): 47-54. DOI： 10.1038/s41377-023-01349-2.

摘要

Abstract

High refractive index dielectric nanoantennas strongly modify the decay rate via the Purcell effect through the design of radiative channels. Due to their dielectric nature

the field is mainly confined inside the nanostructure and in the gap

which is hard to probe with scanning probe techniques. Here we use single-molecule fluorescence lifetime imaging microscopy (smFLIM) to map the decay rate enhancement in dielectric GaP nanoantenna dimers with a median localization precision of 14 nm. We measure

in the gap of the nanoantenna

decay rates that are almost 30 times larger than on a glass substrate. By comparing experimental results with numerical simulations we show that this large enhancement is essentially radiative

contrary to the case of plasmonic nanoantennas

and therefore has great potential for applications such as quantum optics and biosensing.

Single-molecule fluorescence lifetime imaging microscopy (smFLIM) measures the radiative decay rate of single molecules in the near field of dielectric nanoantennas providing super-resolved information of the local density of states.

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=70079287&type=

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=70079287&type=small

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=70079287&type=middle

关键词

Keywords

references

Novotny, L. & Hecht, B. Principles of Nano-Optics . (New York: Cambridge University Press, 2012).

L. Novotny , N. van Hulst , Antennas for light . Nat. Photon 5 , 83 - 90 ( 2011 ). http://doi.org/10.1038/nphoton.2010.237 http://doi.org/10.1038/nphoton.2010.237

H. Duan , A.I. Fernández-Domínguez , M. Bosman , S.A. Maier , J.K.W. Yang , Nanoplasmonics: classical down to the nanometer scale . Nano Lett. 12 , 1683 - 1689 ( 2012 ). http://doi.org/10.1021/nl3001309 http://doi.org/10.1021/nl3001309

V. Giannini , A.I. Fernández-Domínguez , S.C. Heck , S.A. Maier , Plasmonic nanoantennas: fundamentals and their use in controlling the radiative properties of nanoemitters . Chem. Rev. 111 , 3888 - 3912 ( 2011 ). http://doi.org/10.1021/cr1002672 http://doi.org/10.1021/cr1002672

M.E. Nasir et al. , Mode engineering in large arrays of coupled plasmonic–dielectric nanoantennas . Adv. Optical Mater. 9 , 2001467 ( 2021 ). http://doi.org/10.1002/adom.202001467 http://doi.org/10.1002/adom.202001467

R.M. Córdova-Castro , A.V. Krasavin , M.E. Nasir , A.V. Zayats , W. Dickson , Nanocone-based plasmonic metamaterials . Nanotechnology 30 , 055301 ( 2019 ). http://doi.org/10.1088/1361-6528/aaea39 http://doi.org/10.1088/1361-6528/aaea39

J.J. Baumberg , J. Aizpurua , M.H. Mikkelsen , D.R. Smith , Extreme nanophotonics from ultrathin metallic gaps . Nat. Mater. 18 , 668 - 678 ( 2019 ). http://doi.org/10.1038/s41563-019-0290-y http://doi.org/10.1038/s41563-019-0290-y

O.L. Muskens , V. Giannini , J.A. Sanchez-Gil , J. Gómez Rivas , Strong enhancement of the radiative decay rate of emitters by single plasmonic nanoantennas . Nano Lett. 7 , 2871 - 2875 ( 2007 ). http://doi.org/10.1021/nl0715847 http://doi.org/10.1021/nl0715847

K. Matsuzaki et al. , Strong plasmonic enhancement of biexciton emission: controlled coupling of a single quantum dot to a gold nanocone antenna . Sci. Rep. 7 ,( 2017 ). http://doi.org/10.1038/srep42307 http://doi.org/10.1038/srep42307

S. Kühn , U. Håkanson , L. Rogobete , V. Sandoghdar , Enhancement of single-molecule fluorescence using a gold nanoparticle as an optical nanoantenna . Phys. Rev. Lett. 97 , 017402 ( 2006 ). http://doi.org/10.1103/PhysRevLett.97.017402 http://doi.org/10.1103/PhysRevLett.97.017402

K. Matsuzaki , H.-W. Liu , S. Götzinger , V. Sandoghdar , On quantum efficiency measurements and plasmonic antennas . ACS Photonics 8 , 1508 - 1521 ( 2021 ). http://doi.org/10.1021/acsphotonics.1c00169 http://doi.org/10.1021/acsphotonics.1c00169

A.F. Koenderink , Single-photon nanoantennas . ACS Photonics 4 , 710 - 722 ( 2017 ). http://doi.org/10.1021/acsphotonics.7b00061 http://doi.org/10.1021/acsphotonics.7b00061

R. Carminati et al. , Electromagnetic density of states in complex plasmonic systems . Surf. Sci. Rep. 70 , 1 - 41 ( 2015 ). http://doi.org/10.1016/j.surfrep.2014.11.001 http://doi.org/10.1016/j.surfrep.2014.11.001

J. Wenger et al. , Emission and excitation contributions to enhanced single molecule fluorescence by gold nanometric apertures . Opt. Express, OE 16 , 3008 - 3020 ( 2008 ). http://doi.org/10.1364/OE.16.003008 http://doi.org/10.1364/OE.16.003008

P.R. West et al. , Searching for better plasmonic materials . Laser Photonics Rev. 4 , 795 - 808 ( 2010 ). http://doi.org/10.1002/lpor.200900055 http://doi.org/10.1002/lpor.200900055

J.B. Khurgin , How to deal with the loss in plasmonics and metamaterials . Nat. Nanotech 10 , 2 - 6 ( 2015 ). http://doi.org/10.1038/nnano.2014.310 http://doi.org/10.1038/nnano.2014.310

P. Anger , P. Bharadwaj , L. Novotny , Enhancement and quenching of single-molecule fluorescence . Phys. Rev. Lett. 96 , 113002 ( 2006 ). http://doi.org/10.1103/PhysRevLett.96.113002 http://doi.org/10.1103/PhysRevLett.96.113002

D. Cao et al. , Mapping the radiative and the apparent nonradiative local density of states in the near field of a metallic nanoantenna . ACS Photonics 2 , 189 - 193 ( 2015 ). http://doi.org/10.1021/ph500431g http://doi.org/10.1021/ph500431g

Bohren, C. F. & Huffman, D. R. Absorption and Scattering of Light by Small Particles . (John Wiley & Sons, 1998).

A.I. Kuznetsov , A.E. Miroshnichenko , M.L. Brongersma , Y.S. Kivshar , B. Luk’yanchuk , Optically resonant dielectric nanostructures . Science 354 , aag2472 ( 2016 ). http://doi.org/10.1126/science.aag2472 http://doi.org/10.1126/science.aag2472

M. Caldarola et al. , Non-plasmonic nanoantennas for surface enhanced spectroscopies with ultra-low heat conversion . Nat. Commun. 6 ,( 2015 ). http://doi.org/10.1038/ncomms8915 http://doi.org/10.1038/ncomms8915

D. Bouchet et al. , Enhancement and Inhibition of Spontaneous Photon Emission by Resonant Silicon Nanoantennas . Phys. Rev. Appl. 6 , 064016 ( 2016 ). http://doi.org/10.1103/PhysRevApplied.6.064016 http://doi.org/10.1103/PhysRevApplied.6.064016

L. Abou-Hamdan et al. , Transition from phononic to geometrical mie modes measured in single subwavelength polar dielectric spheres . ACS Photonics 9 , 2295 - 2303 ( 2022 ). http://doi.org/10.1021/acsphotonics.2c00273 http://doi.org/10.1021/acsphotonics.2c00273

P. Albella et al. , Low-loss electric and magnetic field-enhanced spectroscopy with subwavelength . Silicon Dimers. J. Phys. Chem. C 117 , 13573 - 13584 ( 2013 ). http://doi.org/10.1021/jp4027018 http://doi.org/10.1021/jp4027018

J. Proust , F. Bedu , B. Gallas , I. Ozerov , N. Bonod , All-dielectric colored metasurfaces with silicon mie resonators . ACS Nano 10 , 7761 - 7767 ( 2016 ). http://doi.org/10.1021/acsnano.6b03207 http://doi.org/10.1021/acsnano.6b03207

J.M. Geffrin et al. , Magnetic and electric coherence in forward- and back-scattered electromagnetic waves by a single dielectric subwavelength sphere . Nat. Commun. 3 ,( 2012 ). http://doi.org/10.1038/ncomms2167 http://doi.org/10.1038/ncomms2167

A. García-Etxarri et al. , Strong magnetic response of submicron silicon particles in the infrared . Opt. Express 19 , 4815 - 4826 ( 2011 ). http://doi.org/10.1364/OE.19.004815 http://doi.org/10.1364/OE.19.004815

R. Regmi et al. , All-dielectric silicon nanogap antennas to enhance the fluorescence of single molecules . Nano Lett. 16 , 5143 - 5151 ( 2016 ). http://doi.org/10.1021/acs.nanolett.6b02076 http://doi.org/10.1021/acs.nanolett.6b02076

R. Camacho-Morales et al. , Resonant harmonic generation in AlGaAs nanoantennas probed by cylindrical vector beams . Nanoscale 11 , 1745 - 1753 ( 2019 ). http://doi.org/10.1039/C8NR08034H http://doi.org/10.1039/C8NR08034H

M.R. Hasan , O.G. Hellesø , Dielectric optical nanoantennas . Nanotechnology 32 , 202001 ( 2021 ). http://doi.org/10.1088/1361-6528/abdceb http://doi.org/10.1088/1361-6528/abdceb

G. Shambat , K. Rivoire , J. Lu , F. Hatami , J. Vucković , Tunable-wavelength second harmonic generation from GaP photonic crystal cavities coupled to fiber tapers . Opt. Express 18 , 12176 - 12184 ( 2010 ). http://doi.org/10.1364/OE.18.012176 http://doi.org/10.1364/OE.18.012176

R. Sanatinia , M. Swillo , S. Anand , Surface second-harmonic generation from vertical GaP nanopillars . Nano Lett. 12 , 820 - 826 ( 2012 ). http://doi.org/10.1021/nl203866y http://doi.org/10.1021/nl203866y

J. Cambiasso et al. , Bridging the gap between dielectric nanophotonics and the visible regime with effectively lossless gallium phosphide antennas . Nano Lett. 17 , 1219 - 1225 ( 2017 ). http://doi.org/10.1021/acs.nanolett.6b05026 http://doi.org/10.1021/acs.nanolett.6b05026

L. Sortino et al. , Enhanced light-matter interaction in an atomically thin semiconductor coupled with dielectric nano-antennas . Nat. Commun. 10 ,( 2019 ). http://doi.org/10.1038/s41467-019-12963-3 http://doi.org/10.1038/s41467-019-12963-3

L. Sortino et al. , Dielectric nanoantennas for strain engineering in atomically thin two-dimensional semiconductors . ACS Photonics 7 , 2413 - 2422 ( 2020 ). http://doi.org/10.1021/acsphotonics.0c00294 http://doi.org/10.1021/acsphotonics.0c00294

S. Mignuzzi et al. , Nanoscale design of the local density of optical states . Nano Lett. 19 , 1613 - 1617 ( 2019 ). http://doi.org/10.1021/acs.nanolett.8b04515 http://doi.org/10.1021/acs.nanolett.8b04515

D. Bouchet et al. , Probing near-field light-matter interactions with single-molecule lifetime imaging . Optica 6 , 135 - 138 ( 2019 ). http://doi.org/10.1364/OPTICA.6.000135 http://doi.org/10.1364/OPTICA.6.000135

G. Blanquer et al. , Relocating single molecules in super-resolved fluorescence lifetime images near a plasmonic nanostructure . ACS Photonics 7 , 393 - 400 ( 2020 ). http://doi.org/10.1021/acsphotonics.9b01317 http://doi.org/10.1021/acsphotonics.9b01317

A.F. Koenderink , R. Tsukanov , J. Enderlein , I. Izeddin , V. Krachmalnicoff , Super-resolution imaging: when biophysics meets nanophotonics . Nanophotonics 11 , 169 - 202 ( 2022 ). http://doi.org/10.1515/nanoph-2021-0551 http://doi.org/10.1515/nanoph-2021-0551

M. Raab , C. Vietz , F.D. Stefani , G.P. Acuna , P. Tinnefeld , Shifting molecular localization by plasmonic coupling in a single-molecule mirage . Nat. Commun. 8 ,( 2017 ). http://doi.org/10.1038/ncomms13966 http://doi.org/10.1038/ncomms13966

E. Betzig et al. , Imaging intracellular fluorescent proteins at nanometer resolution . Science 313 , 1642 - 1645 ( 2006 ). http://doi.org/10.1126/science.1127344 http://doi.org/10.1126/science.1127344

S.T. Hess , T.P.K. Girirajan , M.D. Mason , Ultra-high resolution imaging by fluorescence photoactivation localization microscopy . Biophys. J. 91 , 4258 - 4272 ( 2006 ). http://doi.org/10.1529/biophysj.106.091116 http://doi.org/10.1529/biophysj.106.091116

M.J. Rust , M. Bates , X. Zhuang , Sub-diffraction-limit imaging by stochastic optical reconstruction microscopy (STORM) . Nat. Methods 3 , 793 - 796 ( 2006 ). http://doi.org/10.1038/nmeth929 http://doi.org/10.1038/nmeth929

D. Bouchet , V. Krachmalnicoff , I. Izeddin , Cramér-Rao analysis of lifetime estimations in time-resolved fluorescence microscopy . Opt. Express 27 , 21239 - 21252 ( 2019 ). http://doi.org/10.1364/OE.27.021239 http://doi.org/10.1364/OE.27.021239

C. Ropp et al. , Nanoscale imaging and spontaneous emission control with a single nano-positioned quantum dot . Nat. Commun. 4 ,( 2013 ). http://doi.org/10.1038/ncomms2477 http://doi.org/10.1038/ncomms2477

H. Groß et al. , Parallel mapping of optical near-field interactions by molecular motor-driven quantum dots . Nat. Nanotechnol. 13 , 691 - 695 ( 2018 ). http://doi.org/10.1038/s41565-018-0123-1 http://doi.org/10.1038/s41565-018-0123-1

A. Cuccato et al. , Complete and compact 32-channel system for time-correlated single-photon counting measurements . IEEE Photonics J. 5 , 6801514 - 6801514 ( 2013 ). http://doi.org/10.1109/JPHOT.2013.2284250 http://doi.org/10.1109/JPHOT.2013.2284250

D.E. Aspnes , A.A. Studna , Dielectric functions and optical parameters of Si, Ge, GaP, GaAs, GaSb, InP, InAs, and InSb from 1.5 to 6.0 eV . Phys. Rev. B 27 , 985 - 1009 ( 1983 ). http://doi.org/10.1103/PhysRevB.27.985 http://doi.org/10.1103/PhysRevB.27.985

E. Wertz , B.P. Isaacoff , J.D. Flynn , J.S. Biteen , Single-molecule super-resolution microscopy reveals how light couples to a plasmonic nanoantenna on the nanometer scale . Nano Lett. 15 , 2662 - 2670 ( 2015 ). http://doi.org/10.1021/acs.nanolett.5b00319 http://doi.org/10.1021/acs.nanolett.5b00319

M. Ovesný , P. Křížek , J. Borkovec , Z. Švindrych , G.M. Hagen , ThunderSTORM: a comprehensive ImageJ plug-in for PALM and STORM data analysis and super-resolution imaging . Bioinformatics 30 , 2389 - 2390 ( 2014 ). http://doi.org/10.1093/bioinformatics/btu202 http://doi.org/10.1093/bioinformatics/btu202

Views

Downloads

CSCD

Alert me when the article has been cited

Submit

Tools

Publicity Resources

Light | Single emitter superresolution imaging enhancement

No data

Related Author

No data

Related Institution

No data

⁰