Thesis (Ph. D.)--University of Texas at Austin, 2004. / Supervisor: David A. Vanden Bout. Vita. Includes bibliographical references. Also available from UMI.

Tip Enhanced Near-field Optical Microscopy (TENOM) is a method for optically imaging at resolutions far below the diffraction limit. This technique requires optical nano-probes with very specialized geometries, in order to obtain large, localized enhancements of the electromagnetic field, which is the driver behind this imaging method. Traditional methods for the fabrication of these nano-probes involve electrochemical etching and subsequent FIB milling. However, this milling process is non-trivial, requiring multiple cuts on each probe. This requires multiple rotations of the probe within the FIB system, which may not be possible in all systems, meaning the sample must be removed from vacuum, rotated by hand and placed back under vacuum. This is time consuming and costly and presents a problem with reproducibility. The method presented here is to replace multiple cuts from a side profile with a small number of cuts from a top down profile. This method uses the inherent imaging characteristics of the FIB, by assigning beam dwell times to specific locations on the sample, through the use of bitmap images. These bitmaps are placed over the sample while imaging and provide a lookup table for the beam while milling. These images are grayscale with the color of each pixel representing the dwell time at that pixel. This technique, combined with grayscale gradients, can provide probes with a symmetric geometry, making the system polarization independent.

Apertureless near-field scanning infrared microscopy is a technique in which an impinging infrared beam is scattered by a sharp atomic force microscopy (AFM) tip oscillating at the resonant frequency of the cantilever in close proximity to a sample. Several advantages offered by near-field imaging include nanoscale imaging with high spatial resolution (near-field imaging is not restricted by the diffraction limit of light) and the ability to differentiate between chemical properties of distinct compounds present in the sample under study due to differences in the scattered field. An overview of the assembly, tuning, and implementation of the near-field instrumentation is provided, as well as detailed descriptions about the samples probed and other instrumentation used. A description of the near-field phenomena, a comparison between aperture and apertureless-type near-field microscopy, and the coupled dipoles model explaining the origin of the chemical contrast present in near-field infrared imaging was discussed. Simultaneous topographic and chemical contrast images were collected at different wavelengths for the block copolymer thin film, polystyrene-b-poly(methyl ethacrylate) (PS-b-PMMA) and for amyloid fibrils synthesized from the #21-31 peptide of β2-microglobulin. In both cases it was observed that the experimental scattered field spectrum correlates strongly with that calculated using the far-field absorption spectrum, and using near-field microscopy, nanoscale structural and/or compositional variations were observed, which would not have been possible using ensemble FTIR measurements. Lastly, tip-enhanced Raman spectra of the #21-31 and #16-22 peptide fragments from the β2-microglobulin and Aβ(1-40) peptide were collected, examined, and an outline of the optimization conditions described.

This dissertation will demonstrate the synergy of nanoscopic materials and surface metrology methods by the fabrication and implementation of CNT atomic force microscopy (AFM) tips, CNT scanning tunneling microscopy (STM) tips, Pt spike AFM tips, and Pt spike near-field scanning optical microscopy (NSOM) tips for the methods of critical dimension metrology, STM, AFM phase imaging, scanning surface potential AFM (SSPM), NSOM, and three-dimensional AFM. Chapter 1 provides a general overview of the information that will be discussed in this dissertation. Chapter 2 describes two methods for the simultaneous fabrication of carbon nanotube atomic force microscopy and scanning tunneling microscopy probes. The fabrication of these high resolution probes, as well as their imaging characteristics, is described in detail. Resolution standards were used to characterize their behavior and resolution limits. In Chapter 3, the effect of high aspect ratio probe length on AFM phase imaging is studied by fabricating highly controllable Pt spike AFM tips. By monitoring phase shifts on homogenous surfaces as a function of Pt spike length, it is shown that attractive forces at the tip are significantly reduced when high aspect ratio structures are added to conventional AFM probes. In Chapter 4, the effect of probe geometry on scanning surface potential microscopy (SSPM) is described. By studying the effect of scan height in SSPM, it was found that large surface area probe geometries, such as conventional Pt coated AFM tips, have lower surface potential resolution because of contributions from the sides of the tip as well as the cantilever. Spatial resolution standards were probed to evaluate the effect of probe geometry on SSPM sensitivity and resolution. Chapter 5 describes the fabrication of specialized probes for three-dimensional atomic force microscopy, scanning near-field optical microscopy, and scanning electrochemical -- atomic force microscopy (SECM-AFM). Using techniques described in Chapters 2-4, high aspect ratio structures were added to conventional probes used in 3D AFM, NSOM and SECM-AFM to solve limitations inherent to current probe designs for each method. Preliminary data indicates that each probe will have a significant beneficial effect on the resolution limit of its technique.

Apertureless near-field scanning infrared microscopy is a technique in which an impinging infrared beam is scattered by a sharp atomic force microscopy (AFM) tip oscillating at the resonant frequency of the cantilever in close proximity to a sample. Several advantages offered by near-field imaging include nanoscale imaging with high spatial resolution (near-field imaging is not restricted by the diffraction limit of light) and the ability to differentiate between chemical properties of distinct compounds present in the sample under study due to differences in the scattered field. An overview of the assembly, tuning, and implementation of the near-field instrumentation is provided, as well as detailed descriptions about the samples probed and other instrumentation used. A description of the near-field phenomena, a comparison between aperture and apertureless-type near-field microscopy, and the coupled dipoles model explaining the origin of the chemical contrast present in near-field infrared imaging was discussed. Simultaneous topographic and chemical contrast images were collected at different wavelengths for the block copolymer thin film, polystyrene-b-poly(methyl ethacrylate) (PS-b-PMMA) and for amyloid fibrils synthesized from the #21-31 peptide of β2-microglobulin. In both cases it was observed that the experimental scattered field spectrum correlates strongly with that calculated using the far-field absorption spectrum, and using near-field microscopy, nanoscale structural and/or compositional variations were observed, which would not have been possible using ensemble FTIR measurements. Lastly, tip-enhanced Raman spectra of the #21-31 and #16-22 peptide fragments from the β2-microglobulin and Aβ(1-40) peptide were collected, examined, and an outline of the optimization conditions described.

Thesis (Ph. D.)--University of Texas at Austin, 2007. / Vita. Includes bibliographical references.

Thesis (Ph. D.)--Duke University, 2007. / Includes bibliographical references.

Thesis (M.S. in Combat Systems Science and Technology)--Naval Postgraduate School, December 2008. / Thesis Advisor(s): Haegel, Nancy M. ; Luscombe, James. "December 2008." Description based on title screen as viewed on January 29, 2009. Sponsoring/Monitoring Agency Report Number: "DMR-0526330." Includes bibliographical references (p. 59-61). Also available in print.

Thesis (Ph. D.)--University of Texas at Austin, 2000. / Vita. Includes bibliographical references (leaves 177-184). Available also in a digital version from Dissertation Abstracts.

abstract: In this work, atomic force microscopy (AFM) and time resolved confocal fluorescence microscopy are combined to create a microscopy technique which allows for nanometer resolution topographic and fluorescence imaging. This technique can be applied to any sample which can be immobilized on a surface and which can be observed by fluorescence microscopy. Biological problems include small molecular systems, such as membrane receptor clusters, where very high optical resolutions need to be achieved. In materials science, fluorescent nanoparticles or other optically active nanostructures can be investigated using this technique. In the past decades, multiple techniques have been developed that yield high resolution optical images. Multiple far-field techniques have overcome the diffraction limit and allow fluorescence imaging with resolutions of few tens of nanometers. On the other hand, near-field microscopy, that makes use of optically active structures much smaller than the diffraction limit can give resolutions around ten nanometers with the possibility to collect topographic information from flat samples. The technique presented in this work reaches resolutions in the nanometer range along with topographic information from the sample. DNA origami with fluorophores attached to it was used to show this high resolution. The fluorophores with 21 nm distance could be resolved and their position on the origami determined within 10 nm. Not only did this work reach a new record in optical resolution in near-field microscopy (5 nm resolution in air and in water), it also gave an insight into the physics that happens between a fluorescent molecule and a dielectric nanostructure, which the AFM tip is. The experiments with silicon tips made a detailed comparison with models possible on the single molecule level, highly resolved in space and time. On the other hand, using silicon nitride and quartz as tip materials showed that effects beyond the established models play a role when the molecule is directly under the AFM tip, where quenching of up to 5 times more efficient than predicted by the model was found. / Dissertation/Thesis / Ph.D. Physics 2012