Engineering Commons^™

Instrumentation For Dynamic Nuclear Polarization And Application Of Electron Decoupling For Electron Relaxation Measurement, Nicholas Howard Alaniva

Arts & Sciences Electronic Theses and Dissertations

Dynamic nuclear polarization nuclear magnetic resonance (DNP NMR) exploits internal electron spin and nuclear spin interactions to increase sensitivity and uncover valuable information regarding structure and dynamics of a system. To manipulate these interactions, instrumentation is developed to combine high-power microwave and radiofrequency irradiation with the ability to spin samples at the magic angle (MAS) at temperatures from 90 K to 4.2 K. Electron decoupling uses frequency-modulated microwaves to mitigate the electron-nuclear dipolar interaction, improving signal intensity and resolution in DNP NMR experiments. Electron decoupling is combined with short DNP periods to encode electron spin information in polarized nuclear signal. …

Self-Assembly Of Conducting Polymer Nano- And Microstructures For Energy Storage, Luciano Matteo Santino

Arts & Sciences Electronic Theses and Dissertations

Plastics are materials composed of many long chains of molecules with repeating subunits; strong interactions between neighboring molecules lead to the material used throughout the world. Plastics are commonly thought to be insulating, in stark contrast to the conductivity of metals. However, certain polymer structures were discovered to exhibit semiconducting properties, the subject of the Nobel Prize in Chemistry in 2000. Conducting polymers have a unique molecular structure with an electronically conjugated backbone, allowing electrons to freely travel both across the chain and in between chains. This work focuses on controlling the kinetics of the reaction between the vapors of …

Wave Function Engineering In Cdse/Pbs Core/Shell Nanocrystal Heterostructures, Brian Matthew Wieliczka

Arts & Sciences Electronic Theses and Dissertations

Colloidal semiconducting nanocrystals hold significant potential for third generation photovoltaics as solution processable materials that can surpass the Shockley-Queisser limit through multiexciton generation. In pursuit of this goal, the synthesis and optical characterization of CdSe/PbS core/shell quantum dots is reported. The spectroscopic behavior of these particles demonstrates their potential for use in optoelectronic devices, taking advantage of wave function engineering of the electron and hole. The rock salt PbS shell grows on all sides of the underlying zinc blende CdSe quantum dot, creating a core/shell structure. With increasing shell thickness, the band edge absorption and photoluminescence transitions decrease in energy …

Magic Angle Spinning Spheres And Improved Microwave Coupling For Magnetic Resonance, Pin-Hui Chen

Arts & Sciences Electronic Theses and Dissertations

Nuclear magnetic resonance (NMR) is a nondestructive technique used to characterize molecular structure and dynamics with atomic resolution. In solid-state NMR, magic angle spinning (MAS) is commonly implemented to improve spectral resolution by partially averaging anisotropic interactions. To further improve NMR sensitivity, dynamic nuclear polarization (DNP) is utilized to transfer the polarization from electron spins to nuclei of interest using microwaves. Advanced MAS DNP NMR instrumentation, such as spherical rotors for stable and fast spinning, dielectric lenses to effectively couple the microwaves into the sample, and the separation of receiving and transmitting circuits to decrease measurement noise, are developed to …

Erratum: "Imaging The Three‐Dimensional Orientation And Rotational Mobility Of Fluorescent Emitters Using The Tri‐Spot Point Spread Function", Oumeng Zhang, Jin Lu, Tianben Ding, Matthew D. Lew

Electrical & Systems Engineering Publications and Presentations

In the original paper, a calibration error exists in the image-formation model used to analyze experimental images taken by our microscope, causing a bias in the orientation measurements in Figs. 2 and 3. The updated measurements are shown in Fig. E1. We have also updated the supplementary material for the original article to discuss the revised PSF model and estimation algorithms (supplementary material 2) and show the revised model and measurements (Figs. S1, S3, S7, S8, and S10–S13).

Defect Chemistry And Ion Intercalation During The Growth And Solid-State Transformation Of Metal Halide Nanocrystals, Bo Yin

McKelvey School of Engineering Theses & Dissertations

Abstract of the Dissertation

Defect Chemistry and Ion Intercalation During the Growth and Solid-State Transformation of Metal Halide Nanocrystals

Semiconductor metal halides as light-sensitive materials have applications in multiple areas, such as photographic film, antibacterial agents and photocatalysts. One focus of this dissertation is to achieve novel morphologies of ternary silver bromoiodide (AgBr1-xIx, 0

For the silver halide system, we demonstrate that the anion composition of AgBr1-xIx nanocrystals determines their shape through the introduction of twin defects as the nanocrystals are made more iodide-rich. AgBr1-xIx nanocrystals grow as single-phase, solid solutions with the rock salt crystal structure for anions compositions …

Isotopically-Resolved Neutron Cross Sections As Probe Of The Nuclear Optical Potential, Cole Davis Pruitt

Arts & Sciences Electronic Theses and Dissertations

Neutron scattering experiments provide direct access to the forces experienced by nucleons in the nuclear environment. Due to the experimental difficulty of cross section measurements with neutrons, isotopically-resolved neutron scattering cross sections are sorely needed as inputs for many nuclear models. This dissertation presents the results from a campaign of isotope-specific neutron total cross section measurements on 16,18O, 58,64Ni, 112,124Sn, and 103Rh from 3-450 MeV and elastic scattering differential cross section measurements on 112,nat,124Sn at 11 and 17 MeV. Equipped with these new data and with computational improvements to the Dispersive Optical Model (DOM), we present DOM treatments of 16,18O, …

Fundamental Limits Of Measuring Single-Molecule Rotational Mobility, Oumeng Zhang, Matthew D. Lew

Electrical & Systems Engineering Publications and Presentations

Various methods exist for measuring molecular orientation, thereby providing insight into biochemical activities at nanoscale. Since fluorescence intensity and not electric field is detected, these methods are limited to measuring even-order moments of molecular orientation. However, any measurement noise, for example photon shot noise, will result in nonzero measurements of any of these even-order moments, thereby causing rotationally-free molecules to appear to be partially constrained. Here, we build a model to quantify measurement errors in rotational mobility. Our theoretical framework enables scientists to choose the optimal single-molecule orientation measurement technique for any desired measurement accuracy and photon budget.