Nathan J. Begue

NLOPredict: Visualization and data analysis software for nonlinear optics

A data analysis and visualization program was developed to assist in the interpretation of second‐order nonlinear optical (NLO) processes, including vibrational sum‐frequency generation and electronically resonant second harmonic generation. A novel diagrammatic approach allows concise visual representations of the resonant NLO molecular response. By mapping the predicted NLO response as a function of molecular orientation, molecular modeling results can be combined with experimental measurements for orientational analysis. A method is developed and implemented to predict the nonlinear optical properties of the amide backbones in complete proteins with known structures. NLOPredict is available for most computer operating systems from http://sda.iu.edu/nlopredict/.

Vapor detection performance of vertically aligned, ordered arrays of silicon nanowires with a porous electrode.

Vertically aligned, ordered arrays of silicon nanowires capped with a porous top electrode are used to detect gas phase ammonia and nitrogen dioxide in humidified air. The sensors had very fast response times and large signal-to-noise ratios. Calibration curves were created using both an initial slope method and a fixed-time point method. The initial-slope method had a power law dependence that correlates well with concentration, demonstrating a viable alternative for eventual quantitative vapor detection and enabling shorter sampling and regeneration times.

DNA-based polymers as chiral templates for second-order nonlinear optical materials.

The unique symmetry properties of chiral systems allow the emergence of coherent second harmonic generation in polymeric materials lacking polar order. Deoxyribonucleic acid (DNA) treated with the surfactant cetyltrimethylammonium (CTMA) was drop-cast to spontaneously form films that are active for coherent second harmonic generation (SHG). SHG images acquired as a function of incident and exigent polarization are in good agreement with theoretical predictions assuming nonpolar D(infinity) symmetry for the double-stranded DNA chains. Doping the DNA films with crystal violet substantially increases the efficiency of SHG, but does not significantly alter the polarization-dependence, suggesting that the SHG generated upon doping arises from the same chiral-specific origin, presumably templated by the DNA. These results raise the possibility of new design strategies for organic nonlinear optical materials based on soft chiral polymers that do not require polar order.

High frame-rate multichannel beam-scanning microscopy based on Lissajous trajectories

A simple beam-scanning optical design based on Lissajous trajectory imaging is described for achieving up to kHz frame-rate optical imaging on multiple simultaneous data acquisition channels. In brief, two fast-scan resonant mirrors direct the optical beam on a circuitous trajectory through the field of view, with the trajectory repeat-time given by the least common multiplier of the mirror periods. Dicing the raw time-domain data into sub-trajectories combined with model-based image reconstruction (MBIR) 3D in-painting algorithms allows for effective frame-rates much higher than the repeat time of the Lissajous trajectory. Since sub-trajectory and full-trajectory imaging are simply different methods of analyzing the same data, both high-frame rate images with relatively low resolution and low frame rate images with high resolution are simultaneously acquired. The optical hardware required to perform Lissajous imaging represents only a minor modification to established beam-scanning hardware, combined with additional control and data acquisition electronics. Preliminary studies based on laser transmittance imaging and polarization-dependent second harmonic generation microscopy support the viability of the approach both for detection of subtle changes in large signals and for trace-light detection of transient fluctuations.

Chemically selective analysis of molecular monolayers by nonlinear optical stokes ellipsometry.

The application of nonlinear optical Stokes ellipsometry (NOSE) coupled with principal component analysis (PCA) is demonstrated for the chemically selective analysis of molecular monolayers. NOSE allows for rapid polarization measurements of nonlinear optical materials and thin surface films, which in turn benefits from comparably fast data analysis approaches. PCA combined with linear curve fitting techniques greatly reduce the analysis time relative to nonlinear curve fitting. NOSE-PCA is first validated with studies of z-cut quartz, followed by analysis of four thin dye films with similar nonlinear optical properties. The high precision of NOSE measurements combined with the rapid analysis time enabled chemical discrimination between different dyes and the practical realization of NOSE microscopy.

Imaging Nonlinear Optical Stokes Ellipsometry for Thin Film and Microparticle Characterization

Nonlinear optical Stokes ellipsometry (NOSE) is shown to routinely provide precision of a few parts in 1000 in 12 ms acquisition times for determination of the χ(2) tensor elements of thin films, enabling imaging applications with detailed polarization characterization.