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DEVELOPMENT OF INSTRUMENTATION AND ALGORITHMS FOR CHEMICAL STRUCTURE AND KINETICS ANALYSIS IN CHEMICAL IMAGING 

thesis
posted on 2023-06-20, 15:34 authored by Jiayue RongJiayue Rong

    

Development on instrumentation and algorithms for chemical structure and chemical kinetics are discussed in this thesis. In Chapter 2 and 3, a consensus equilibrium formalism is introduced for the integration of multiple quantum chemical calculations of molecular and electronic structure. In multi-agent consensus equilibrium (MACE), iterative updates in structure optimization are intertwined with the net output, representing an equilibrium balance between multiple computational agents. MACE structure calculations from the integration of multiple low-level electronic structure calculations were compared favorably for small molecules, with results evaluated through comparison with higher level structure (CCSD). Notably, MACE results differed substantially from the average of the independent computational agent outputs, with MACE yielding improved agreement with higher-level CCSD calculations. The primary focus is on the development of the mathematical framework for implementing MACE for molecular and electronic structure determination, these initial preliminary results suggest potential promise for the use of MACE to improve the accuracy of low-level electronic structure calculations through the integration of multiple parallel methods. In Chapter 4 and 5, Fourier- transform fluorescence recovery after photobleaching (FT-FRAP) coupled with periodically comb pattern was demonstrated to monitor the controlled-release mechanisms of microparticles. By monitoring the time-lapse recovery patterns, spatial mobility were decoded in FT domain. Due to the nature of mobility encoded in FT domain, substantial improvements were demonstrated in terms of enhanced signal-to-noise, simplified mathematics, low requirements of sampling, and multiphoton compatibility to probe inside samples. FT-FRAP was able to discriminate and quantify the internal diffusion and exchange to higher mobility in fitting the recovery kinetics within microparticles. Theoretical modeling of exchange and diffusion- controlled release revealed that both RS and RL microparticles exhibited similar exchange decay, with RL having a much higher diffusion decay. The microscopically higher diffusion of RL microparticles is consistent with the dissolution performance of RL microparticles macroscopically. The distinction of controlled release mechanisms provided by FT-FRAP is important to understand and further optimize the design of controlled release systems for GI tract. 

History

Degree Type

  • Doctor of Philosophy

Department

  • Chemistry

Campus location

  • West Lafayette

Advisor/Supervisor/Committee Chair

Garth J Simpson

Additional Committee Member 2

Graham Cooks

Additional Committee Member 3

Chi Zhang

Additional Committee Member 4

Lyudmila Slipchenko