Characterisation of Rb and Cs spin-exchange optical pumping for application to hyperpolarised 129Xe functional lung MRI

Abstract

When performing nuclear magnetic resonance (NMR) it is desirable to maximise the available polarisation of the spin system in order to achieve optimal signal-to-noise ratios. One method of achieving this is via the process of spin-exchange optical pumping (SEOP). SEOP can be used to produce hyperpolarised (HP) noble gases, which possess numerous applications in the fields of science and medicine, ranging from spectroscopic imaging of porous media to Magnetic Resonance Imaging (MRI) of the human lungs. The SEOP process involves transfer of angular momentum from circularly polarised laser photons to the electrons of an alkali metal vapour. Noble gas nuclei can then be polarised via collisions with the alkali metal vapour. Ultra-low frequency Raman Spectroscopy may be used to perform rotational temperature measurements of a nitrogen buffer gas in these SEOP experiments in real-time, in an attempt to understand the poorly understood and highly complex system dynamics and energy transport processes. The work contained in this thesis aims to investigate the co-dependence of these dynamics, in order to characterise the SEOP process in greater detail for a variety of gas mixtures, temperatures and alkali metal targets. With this, it is hoped that HP noble gases may be produced with greater efficiency, achieving faster build-up rates and higher net magnetisation. In addition to in situ Raman spectroscopy, additional diagnostic techniques were implemented in order to illustrate the co-dependence of variables during the thermal exchange processes present in SEOP. Low-field NMR spectroscopy was utilised to determine the 129Xe net spin polarisation (P_Xe) as a function of time and position within the SEOP vessel, whilst near-infra-red (NIR) optical absorption spectroscopy allowed an estimate of the alkali metal polarisation and global pump laser power absorption to be determined. Additionally, initial studies into the use of optical absorption spectroscopy at various wavelengths for determination of the alkali metal number density are discussed. A chronology of experiments conducted using an `in-line', optically filtered Raman probe arrangement will be presented, culminating in the development of a fully automated, single-axis translational stage to perform rapid measurement of the rotational nitrogen temperature (T_N2) within the optical pumping cell with a high degree of temporal and spatial precision. The automated nature of the system facilitates a >3-fold improvement in the rate of thermal data acquisition, with greater ease and reliability than the previous manual method. In addition to pure rubidium, rotational temperature determination via Raman spectroscopy is demonstrated in a variety of rubidium/caesium hybrid alloy mixtures. In this way it may be possible to more efficiently utilise the greater spin exchange rate of caesium with 129Xe to achieve hybrid Rb/Cs cross-polarisation. The result of this is the first observation of 129Xe polarisation in a hybrid Rb/Cs system exceeding that of an equivalent pure Rb system under otherwise identical experimental conditions