On the interplay of spin dynamics and chemical kinetics in the nuclear spin hyperpolarization technique signal amplification by reversible exchange (SABRE) : a simulation and experimental NMR study Abstract: In this thesis The nuclear hyperpolarization technique Signal Amplification By Reversible Exchange (SABRE) is studied. SABRE utilizes externally supplied parahydrogen (pH2) to generate hyperpolarized molecules in a transient SABRE active organometallic complex which can result in several orders of magnitude enhanced NMR signals of the target molecules. The main focus of this work is the interplay of chemical kinetics and spin dynamics in these complexes and their effect on the SABRE hyperpolarization process at high magnetic fields. For this purpose a theoretical model was developed and implemented which is presented in chapter 4. In contrast to previous approaches this model explicitly takes into account both spin dynamics and chemical exchange. Subsequently the model was used to analyze several aspects of SABRE hyperpolarization. In chapter 5 the dependence of the ’classical’ SABRE scheme generating hyperpolarization at low magnetic fields on coherent and incoherent parameters of the spin system (e.g. J couplings and relaxation rates) as well as exchange rates is analyzed. Chapter 6 presents a study of the evolution of spin state of freely dissolved parahydrogen in the SABRE system. This study revealed that pH2 suffers an unexpected loss of coherence. Upon further investigation it was found that two low concentrated intermediate catalytic complexes exist in the SABRE system studied here which are the source of the coherence loss. This hypothesis was substantiated by theoretical modelling of the obtained data and by experiments where these intermediates wereselectively isolated and studied. In Chapter 7 the previously unexplained phenomena of spontaneous formation of hyperpolarized molecules at high magnetic fields (here meaning > 1 Tesla) is analyzed and a pathway for the formation proposed which is supported by experiments and theoretical calculations. The last two chapters of this work are dedicated to the analysis of high field hyperpolarization transfer schemes for SABRE. In chapter 8 a previously proposed scheme based on continuous radio frequency irradiation (RF) is studied with regards to the influence of ongoing exchange and loss of coherences of freely dissolved pH2. Several modifications were proposed and experimentally tested as a result of this analysis. These modifications yield an improvement of this scheme by more than one order of magnitude. In the last chapter of this thesis the SABRE INEPT sequence a NMR pu ...