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Investigation techniques based on tip-enhanced optical effects, capable to yield spatial resolutions down to nanometers level, have enabled a wide palette of important discoveries over the past twenty years. Recently, their underlying optical setups are beginning to emerge as useful tools to modify and manipulate matter with nanoscale spatial resolution. We try to contribute to these efforts by reporting a method that we found viable to modify the surface refractive index of polymethyl methacrylate (PMMA), an acrylic polymer material. The changes in the refractive index are accomplished by focusing a femtosecond pulsed near-infrared laser beam on the apex of a metalized nano-sized tip, traditionally used in scanning probe microscopy (SPM) applications. The adopted illumination strategy yields circular-shaped modifications of the refractive index occurring at the surface of the PMMA sample, exhibiting a lateral size <200 nm, under 790 nm illumination, representing a four-fold increase in precision compared to the current state-of-the-art. The light intensity enhancement effects taking place at the tip apex makes possible achieving refractive index changes at low laser pulse energies (<0.5 nJ), which represents two orders of magnitude advantage over the current state-of-the art. The presented nanoimprinting method is very flexible, as it can be used with different power levels and can potentially be operated with other materials. Besides enabling modifications of the refractive index with high lateral resolution, this method can pave the way towards other important applications such the fabrication of photonic crystal lattices or surface waveguides.

A thorough understanding of biological species and of emerging nanomaterials requires, among others, their in-depth characterization with optical techniques capable of nano-resolution. Nanoscopy techniques based on tip-enhanced optical effects have gained over the past years tremendous interest given their potential to probe various optical properties with resolutions depending on the size of a sharp probe interacting with focused light, irrespective of the illumination wavelength. Although their popularity and number of applications is rising, tip-enhanced nanoscopy techniques (TEN) still largely rely on probes that are not specifically developed for such applications, but for Atomic Force Microscopy. This cages their potential in many regards, e.g. in terms of signal-to-noise ratio, attainable image quality, or extent of applications. In this article we place first steps towards next-gen TEN, demonstrating the fabrication and modelling of specialized TEN probes with known optical properties. The proposed framework is highly flexible and can be easily adjusted to be of o benefit to various types of TEN techniques, for which probes with known optical properties could potentially enable faster and more accurate imaging via different routes, such as direct signal enhancement or novel signal modulation strategies. We consider that the reported development can pave the way for a vast number of novel TEN imaging protocols and applications, given the many advantages that it offers., Comment: 24 pages, 9 figures

Second Harmonic Generation Microscopy (SHG) is generally acknowledged as a powerful tool for the label-free 3D visualization of tissues and advanced materials, with one of its most popular applications being collagen imaging. Although the great need, progress in super-resolved SHG imaging lags behind the developments reported over the past years in fluorescence-based optical nanoscopy. In this work, we quantitatively show on collagenous tissues that by combining SHG imaging with re-scan microscopy resolutions that surpass the diffraction limit with ~1.4x become available. Besides Re-scan Second Harmonic Generation Microscopy (rSHG), we demonstrate as well super-resolved Re-scan Two-Photon Excited Fluorescence Microscopy (rTPEF). These two techniques are implemented by modifying a Re-scan Confocal Microscope (RCM), retaining its initial function, resulting thus in a multimodal rSHG/rTPEF/RCM system. Given the simplicity and flexibility of re-scan microscopy, we consider that the reported results are likely to augment the number and nature of applications relying on super-resolved non-linear optical imaging.