Highly reproducible near-field optical imaging with sub-20-nm resolution based on template-stripped gold pyramids.

With a template-stripping fabrication technique, we demonstrate the mass fabrication of high-quality, uniform, ultrasharp (10 nm) metallic probes suitable for single-molecule fluorescence imaging, tip-enhanced Raman spectroscopy (TERS), and other near-field imaging techniques. We achieve reproducible single-molecule imaging with sub-20-nm spatial resolution and an enhancement in the detected fluorescence signal of up to 200. Similar results are obtained for TERS imaging of carbon nanotubes. We show that the large apex angle (70.5°) of our pyramidal tip is well suited to scatter the near-field optical signal into the far-field, leading to larger emission enhancement and hence to a larger quantum yield. Each gold or silver pyramidal probe is used on-demand, one at a time, and the unused tips can be stored for extended times without degradation or contamination. The high yield (>95%), reproducibility, durability, and massively parallel fabrication (1.5 million identical probes over a wafer) of the probes hold promise for reliable optical sensing and detection and for cementing near-field optical imaging and spectroscopy as a routine characterization technique.

[1]  Duane C. Karns,et al.  Heat-assisted magnetic recording by a near-field transducer with efficient optical energy transfer , 2009 .

[2]  B. Hecht,et al.  Principles of nano-optics , 2006 .

[3]  Olivier J. F. Martin,et al.  Scanning near-field optical microscopy with aperture probes: Fundamentals and applications , 2000 .

[4]  Sang‐Hyun Oh,et al.  Ultrasmooth Patterned Metals for Plasmonics and Metamaterials , 2009, Science.

[5]  X. Xie,et al.  Near-field fluorescence microscopy based on two-photon excitation with metal tips , 1999 .

[6]  R. Zenobi,et al.  Nanoscale chemical analysis by tip-enhanced Raman spectroscopy , 2000 .

[7]  A. Jorio,et al.  Mechanism of near-field Raman enhancement in one-dimensional systems. , 2009, Physical review letters.

[8]  Lukas Novotny,et al.  Principles of Nano-Optics by Lukas Novotny , 2006 .

[9]  Benjamin J Wiley,et al.  Mid-IR plasmonics: near-field imaging of coherent plasmon modes of silver nanowires. , 2009, Nano letters.

[10]  M. Stockman,et al.  Nanofocusing of optical energy in tapered plasmonic waveguides. , 2004, Physical review letters.

[11]  Zachary J. Lapin,et al.  Self-similar gold-nanoparticle antennas for a cascaded enhancement of the optical field. , 2012, Physical review letters.

[12]  D. E. Chang,et al.  Strong coupling of single emitters to surface plasmons , 2006, quant-ph/0603221.

[13]  M. Garcia-Parajo,et al.  Optical antennas focus in on biology , 2008 .

[14]  T G Brown,et al.  Longitudinal field modes probed by single molecules. , 2001, Physical review letters.

[15]  R. Hillenbrand,et al.  Infrared spectroscopic near-field mapping of single nanotransistors , 2010, Nanotechnology.

[16]  Vahid Sandoghdar,et al.  Enhancement of single-molecule fluorescence using a gold nanoparticle as an optical nanoantenna. , 2006, Physical review letters.

[17]  L. Novotný,et al.  Enhancement and quenching of single-molecule fluorescence. , 2006, Physical review letters.

[18]  Reinhard Guckenberger,et al.  High-resolution imaging of single fluorescent molecules with the optical near-field of a metal tip. , 2004, Physical review letters.

[19]  Sang‐Hyun Oh,et al.  Engineering metallic nanostructures for plasmonics and nanophotonics , 2012, Reports on progress in physics. Physical Society.

[20]  Reinhard Guckenberger,et al.  Fluorescence near metal tips: The roles of energy transfer and surface plasmon polaritons. , 2007, Optics express.

[21]  Lukas Novotny,et al.  Near-field optical microscopy and spectroscopy with pointed probes. , 2006, Annual review of physical chemistry.

[22]  S. Kawata,et al.  Tip-enhanced coherent anti-stokes Raman scattering for vibrational nanoimaging. , 2004, Physical review letters.

[23]  K. Karrai,et al.  Piezoelectric tip‐sample distance control for near field optical microscopes , 1995 .

[24]  Martin Schnell,et al.  Nanofocusing of mid-infrared energy with tapered transmission lines , 2011 .

[25]  Prashant Nagpal,et al.  Three-dimensional plasmonic nanofocusing. , 2010, Nano letters.

[26]  Stephen R Quake,et al.  Tip-enhanced fluorescence microscopy at 10 nanometer resolution. , 2004, Physical review letters.

[27]  Lukas Novotny,et al.  Plasmon-Enhanced Photoemission from a Single Y3N@C80 Fullerene† , 2010 .

[28]  F. Keilmann,et al.  Near-field microscopy by elastic light scattering from a tip , 2004, Philosophical Transactions of the Royal Society of London. Series A: Mathematical, Physical and Engineering Sciences.

[29]  Xue-Wen Chen,et al.  Resolution and enhancement in nanoantenna-based fluorescence microscopy. , 2009, Nano letters.

[30]  Lukas Novotny,et al.  Nanoscale vibrational analysis of single-walled carbon nanotubes. , 2005, Journal of the American Chemical Society.

[31]  T. Elsaesser,et al.  Grating-coupling of surface plasmons onto metallic tips: a nanoconfined light source. , 2007, Nano letters.

[32]  T. J. Watson,et al.  Apertureless near-field optical microscope , 1999 .

[33]  Martin Hegner,et al.  Ultralarge atomically flat template-stripped Au surfaces for scanning probe microscopy , 1993 .

[34]  Harald Giessen,et al.  Near-field dynamics of optical Yagi-Uda nanoantennas. , 2011, Nano letters.

[35]  Teri W. Odom,et al.  Mesoscale metallic pyramids with nanoscale tips. , 2005, Nano letters.