Graphene-based metal-induced energy transfer for sub-nanometre optical localization

Abstract

Single-molecule fluorescence imaging has become an indispensable tool for almost all fields of research, from fundamental physics to the life sciences. Among its most important applications is single-molecule localization super-resolution microscopy (SMLM) (for example, photoactivated localization microscopy (PALM)1, stochastic optical reconstruction microscopy (STORM)2, fluorescent PALM (fPALM)3, direct STORM (dSTORM)4 and point accumulation for imaging in nanoscale topography (PAINT)5), which uses the fact that the centre position of a single molecule’s image can be determined with much higher accuracy than the size of that image itself. However, a big challenge of SMLM is to achieve super-resolution along the third dimension as well. Recently, metal-induced energy transfer (MIET) was introduced to axially localize fluorescent emitters6,7,8,9. This exploits the energy transfer from an excited fluorophore to plasmons in a thin metal film. Here, we show that by using graphene as the ‘metal’ layer, one can increase the localization accuracy of MIET by nearly tenfold. We demonstrate this by axially localizing single emitters and by measuring the thickness of lipid bilayers with ångström accuracy.

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Fig. 1: Graphene-based MIET.
Fig. 2: Axial localization of single molecules with graphene-based MIET.
Fig. 3: Graphene-based MIET measurement of the thickness of SLBs.

Data availability

The data that support the plots within this paper and other findings of this study are available from the corresponding authors upon reasonable request.

Code availability

All Matlab routines and codes used for data analysis of this study are available from the corresponding authors upon request.

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Acknowledgements

We are grateful to the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) for financial support through projects A06 of SFB 803, A06 of SFB 860, A05 of SFB 937 and through Germany’s Excellence Strategy EXC 2067/1–390729940. We thank the Leibniz Association for financial support through project K76/2017. We also thank B. R. Brueckner for AFM measurements.

Author information

A.G. and N.K. co-designed the project. A.G., A.S. and I.G. performed all the lifetime and defocused imaging measurements. A.G. generated Figs. 2a,c and 3b in the main text. N.K. performed analysis of the defocused imaging data and lifetime data from SLB. A.I.C. carried out the quantum yield measurements with the nanocavity and D.R. performed the corresponding data analysis. S.I. conducted lifetime fitting of single-molecule data and wrote the corresponding section in the Supplementary Information. D.R. helped with writing the MIET routines in Matlab. R.T. designed the DNA origami sample. A.G., N.K. and J.E. carried out the final data analysis, generated all figures (except Figs. 2a,c and 3b) in the main text and wrote the main manuscript. All co-workers were involved with improving the manuscript and writing the Supplementary Information.

Correspondence to Narain Karedla or Jörg Enderlein.

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Supplementary Information

This file contains more information about the work and Supplementary Figs. 1–5.

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