Groitl, Felix: High Resolution Spectroscopy with the Neutron Resonance Spin Echo Method. , 2013
The first part of this thesis is dedicated to explore new territory for high resolution Neutron Resonance Spin Echo (NRSE) spectroscopy beyond measuring lifetimes of elementary excitations. The data analysis of such experiments requires a detailed model for the echo amplitude as a function of correlation time. The model also offers guidance for planning NRSE experiments in terms of a sensible choice of parameters and allows predicting quantitatively the information content of NRSE spectroscopy for line shape analysis or energy level separation. Major generalizations of the existing formalism, developed in this thesis, allow for violated spin echo conditions, arbitrary local gradient components of the dispersion surface and detuned parameters of the background triple axis spectrometer (TAS) giving rise to important additional depolarizing effects, which have been neglected before. Furthermore, the formalism can now be applied to any crystal symmetry class. The model was successfully tested by experiments on phonons in a high quality single crystal of Pb and the results demonstrate the stringent necessity to consider second order depolarization effects. The formalism was subsequently extended to analyze mode doublets. As a major step forward, detuning effects for both modes are taken into account here. The model was verified by NRSE measurements on a unique tunable double dispersion setup. The results prove the potential of NRSE spectroscopy to resolve mode doublets with an energy separation smaller than the typical energy resolution of a standard TAS. The second class of NRSE experiments was dedicated to line shape analysis of temperature dependent asymmetric line broadening. Inelastic NRSE spectroscopy was performed on two systems, Cu(NO3)2·2.5D2O and Sr3Cr2O8. For this purpose high quality single crystals of Cu(NO3)2·2.5D2O were grown in the course of this thesis. As a proof of principle the results clearly show that the NRSE method can be used to detect temperature dependent asymmetric line broadening. For the first time this effect was measured with NRSE. The second major part of this thesis was the upgrade of the NRSE option of FLEXX at the BER II neutron source at HZB, Berlin. Redesigned NRSE bootstrap coils allow for a more efficient exploitation of the larger beam cross section, given due to the overall upgrade of FLEXX. Higher accessible coil tilt angles enable measurements on steeper dispersions. The newly designed spectrometer arms result in a more compact instrument, enabling direct beam calibration measurements for the entire accessible wavevector range. In combination with higher coil tilt angles the accessible Q-range in Larmor diffraction geometry is enhanced. Extensive calibration measurements were performed and the results clearly demonstrate the reliable performance of the new NRSE option, now available for the broader user community at FLEXX.