Masterarbeit, 2018
118 Seiten, Note: 1,0
1 Introduction and Motivation
2 Theoretical Background
2.1 Low-Temperature Dynamics in Glasses
2.1.1 Glass Formation and Thermal Properties
2.1.2 Structure of Amorphous Materials
2.1.3 Energy States in a Double Well Potential
2.1.4 The Standard Tunnelling Model
2.1.5 Frequency Response of Amorphous Samples
2.2 Nuclear Quadrupole Moments
2.2.1 Nuclear Quadrupole Resonance
2.2.2 Resonant Susceptibility
2.2.3 Relaxation Mechanisms
3 Experimental Methods
3.1 Working at Low Temperatures
3.1.1 Cooling Methods
3.1.2 Thermometry
3.2 Polymer Glass FR-122P
3.2.1 Chemical Structure
3.2.2 Sample Production
3.2.3 Material Choice
3.3 Acoustic Measurements
3.3.1 Double Paddle Oscillator
3.3.2 Measurement Strategy
3.3.3 Probing the Nuclear Bath
3.4 Dielectric Measurements
4 Results and Analysis
4.1 Preparatory Measurements
4.1.1 High Temperatures
4.1.2 Background
4.1.3 Voltage Scaling
4.1.4 Thermalisation
4.2 Complex Acoustic and Dielectric Susceptibilities
4.2.1 Temperature Overview
4.2.2 Acoustic Measurements
4.2.3 Dielectric Measurements
4.3 Numerical Calculations
4.3.1 Standard Tunnelling Model
4.3.2 Resonant Susceptibility
4.3.3 Additional Relaxation Rate
4.4 Impact of RF Bias
5 Discussion
5.1 Validity of Data
5.2 Conclusion
5.2.1 Interpretation of Results
5.2.2 Comparison to Related Work
5.3 Outlook
6 Summary
This thesis investigates the impact of nuclear quadrupole moments (NQM) on the low-frequency elastic and dielectric properties of the polymer glass FR-122P at temperatures ranging from 7 mK to 600 mK. The research aims to determine whether observed deviations from the Standard Tunnelling Model (STM) arise primarily from an additional relaxation mechanism between NQM and atomic tunnelling systems or from modifications to the tunnelling system distribution function.
1. Introduction and Motivation
Glasses have since long attracted special interest among humans thanks to some of their interesting and useful properties, for instance their transparency which enabled their usage as window panes along with traces of metallic admixtures providing colour. This fact is also what gave glass its name which is derived from the Germanic word glasa meaning "shimmering" or "shining". The existence of glass precedes human history, though, for early glass samples on Earth originate from volcanic eruptions. Upon sufficiently fast cooling below the glass transition temperature hot lava forms an amorphous solid, or in other words a glass, called obsidian. Another possibility for natural glass production are volcanic lightnings caused by friction between ash particles which melt in the course of a flash. Under certain cooling conditions they can form glass spheres that allow scientists to study eruption parameters at a safe distance [Ber17].
While the variety of glasses is as wide as their application spectrum, ranging from storing liquids over glass fibres to optical devices, the common and defining trait is their amorphous structure in contrast to crystals. The latter are characterised by a well defined crystal lattice that determines order and symmetry of the crystal by setting the position of every atom of the solid once a single atomic position is fixed. The former do not exhibit such a long range order. Rather, in glasses both the distances and bonding angles between neighbouring atoms are not discrete but show a distribution resulting in structural disorder.
1 Introduction and Motivation: Summarizes the history of glass research and identifies the research gap regarding the impact of nuclear quadrupole moments on the low-temperature physics of amorphous systems.
2 Theoretical Background: Provides the theoretical foundation, detailing the Standard Tunnelling Model and the theory of nuclear quadrupole moments and their interactions.
3 Experimental Methods: Describes the cooling techniques, the fabrication of the FR-122P samples, the acoustic measurements using a double paddle oscillator, and the design of the novel RF bias module.
4 Results and Analysis: Presents the experimental findings for acoustic and dielectric measurements and compares them to numerical simulations of the STM and its proposed extensions.
5 Discussion: Evaluates the validity of the obtained data, interprets the results within the context of previous research, and offers an outlook on future investigations.
6 Summary: Concludes the thesis by summarizing the experimental approach and the core findings regarding the role of NQM in the relaxation processes of polymer glasses.
Polymer glass, FR-122P, low-temperature physics, nuclear quadrupole moments, NQM, Standard Tunnelling Model, STM, elastic susceptibility, dielectric susceptibility, atomic tunnelling systems, relaxation mechanisms, double paddle oscillator, acoustic measurements, cryogenics.
The thesis focuses on examining how nuclear quadrupole moments (NQM) affect the low-frequency elastic and dielectric properties of the polymer glass FR-122P at temperatures below 1 Kelvin.
The work covers the structural properties of glasses, the Standard Tunnelling Model, the theoretical physics of nuclear quadrupole moments, and advanced low-temperature measurement techniques.
The research investigates whether the observed anomalies in the dielectric and acoustic properties of NQM-containing glasses are caused by an additional relaxation pathway between NQM and tunnelling systems or by structural changes (a pseudogap) in the tunnelling system distribution.
The research used low-frequency acoustic measurements via a custom-fabricated double paddle oscillator (DPO) and dielectric susceptibility measurements in a capacitance bridge, both conducted in a 3He/4He dilution cryostat.
The main part encompasses the theoretical derivation of tunnelling interactions, the experimental characterization of the FR-122P polymer, the fabrication of the DPO, and the development of an RF bias module for nuclear quadrupole transition driving.
Key terms include Polymer glass, FR-122P, nuclear quadrupole moments (NQM), Standard Tunnelling Model (STM), and low-temperature acoustics.
FR-122P contains bromine atoms with a large, well-defined nuclear quadrupole moment. Furthermore, the bromine atoms are covalently bonded to carbon, providing a uniform chemical and electrical environment, which simplifies the interpretation of the quadrupole splitting.
While the module allowed for RF excitation, it was determined that the observed changes in susceptibility were predominantly due to thermal heating caused by eddy currents in the gold-coated surface of the DPO, setting an upper limit on the method's sensitivity for detecting NQM transitions.
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