Date of Award

1-1-2015

Document Type

Dissertation

Degree Name

Ph.D.

Organizational Unit

Chemistry and Biochemistry

First Advisor

Susan Sadler

Second Advisor

Sandra Eaton

Third Advisor

Bryan Cowen

Fourth Advisor

Brian J. Majestic

Fifth Advisor

Brian Michel

Keywords

Arbitrary waveform generator, Digital electron paramagnetic resonance, Digital saturation recovery, Field-stepped direct detection, Rapid scan, Tooth dosimetry

Abstract

Rapid scan electron paramagnetic resonance (EPR) was developed in the Eaton laboratory at the University of Denver. Applications of rapid scan to wider spectra, such as for immobilized nitroxides, spin-labeled proteins, irradiated tooth and fingernail samples were demonstrated in this dissertation. The scan width has been increased from 55 G to 160 G. The signal to noise (S/N) improvement for slowly tumbling spin-labeled protein samples that is provided by rapid scan EPR will be highly advantageous for biophysical studies. With substantial improvement in S/N by rapid scan, the dose estimation for irradiated tooth enamels became more reliable than the traditional continuous wave (CW) EPR.

An alternate approach of rapid scan, called field-stepped direct detection EPR, was developed to reconstruct wider EPR signals. A Mn2+ containing crystal was measured by field-stepped direct detection EPR, which had a spectrum more than 6000 G wide. Since the field-stepped direct detection extends the advantages of rapid scan to much wider scan ranges, this methodology has a great potential to replace the traditional CW EPR.

With recent advances in digital electronics, a digital rapid scan spectrometer was built based on an arbitrary waveform generator (AWG), which can excite spins and detect EPR signals with a fully digital system. A near-baseband detection method was used to acquire the in-phase and quadrature signals in one physical channel. The signal was analyzed digitally to generate ideally orthogonal quadrature signals.

A multiharmonic algorithm was developed that employed harmonics of the modulation frequencies acquired in the spectrometer transient mode. It was applied for signals with complicated lineshapes, and can simplify the selection of modulation amplitude.

A digital saturation recovery system based on an AWG was built at X-band (9.6 GHz). To demonstrate performance of the system, the spin-lattice relaxation time of a fused quartz rod was measured at room temperature with fully digital excitation and detection.

Publication Statement

Copyright is held by the author. User is responsible for all copyright compliance.

Rights Holder

Zhelin Yu

Provenance

Received from ProQuest

File Format

application/pdf

Language

en

File Size

184 p.

Discipline

Chemistry, Physical Chemistry

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