Near-fi eld optical microscopies and spectroscopies seek to investigate materials by combining the best aspects of optical characterization and scan-probe microscopy techniques. In principle, this provides access to chemical, morphological, physical and dynamical information at nanometer length scales that is impossible to access by other means. But a number of challenges, particularly on the scan-probe front, have limited the widespread application of near-fi eld investigations. This work describes how recent probe engineering and technique innovation have addressed many of these challenges. This Feature Article begins with a short overview of the fi eld, providing perspective and motivation for these developments and highlighting some key improvements. This is followed by a more in-depth description of the near-fi eld advances developed at the Molecular Foundry, a national nanoscience User Facility-advances that provide groundwork for generally-applicable nano-optical studies. Finally, a discussion is provided of what progress is still needed in order to realize the ultimate objective of translating all optical measurements to the nanoscale.
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FEATURE ARTICLEdiameter and not by the wavelength of the light. By scanning this aperture over a surface, it is possible to build up an optical image with resolution determined by the aperture diameter. Several review articles and texts have been written on this subject; readers interested in more details are directed to [ 1 , 7 ] and references therein. The idea for aperture-based sub-diffraction-limited optical imaging originated with Synge [ 8 ] in 1928, though the fi rst experimental results at optical frequencies were not published until 1984 by Pohl et al. [ 9 ] and Lewis et al. [ 10 ] Approximately eight years later, the fi rst fl uorescence images of single molecules were acquired using aperture NSOM. [ 11 ] In the most widely-adapted approach, a fi ber probe-consisting of a metal-coated tapered optical fi ber with the small aperture at the apex-is raster-scanned over the sample while maintaining a small tip-sample distance. [ 12 ] From a practical standpoint, however, this approach presents many complications. While aperture probes enable "background-free" imaging, where sample illumination occurs only within the nanoscale light spot created by the aperture probe, the boundary conditions for this type of waveguiding tip unfortunately demand that all propagating modes within the taper get cut off before reaching the aperture. This causes only evanescent waves to leak out from the end (see Figure 1 ). [ 13 ] Also, there is not signifi cant local electric fi eld enhancement at the aperture. These factors ultimately result in low optical throughput and signal strength. [ 13 , 14 ] In addition, because throughput is inversely proportional to the fourth power of the aperture radius, [ 14 ] signal-to-noise considerations in aperture NSOM ultimately constrain aperture size, and resolution, to ≈ 50-100 nm. In typical operation, the sample is either locally excited wi...