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Synthesis and Characterization of Constrained Magnetism in Niobates

This thesis contains the results of the extensive study into the synthesis of nickel niobate (NiNb2O6) including the formation of what was a previously unreported polymorph of the material, as well as the magnetic properties of both cobalt niobate (CoNb2O6) and nickel niobate using techniques including SQUID magnetometry, powder and single crystal x-ray scattering, powder and single crystal neutron scattering and muon spin rotation/relaxation.
In cobalt niobate we found extremely long relaxation times in the heat capacity which showed up strongly in muon spin rotation experiments but not in neutron measurements. Additionally, with field applied to the system we see the emergence of spin-wave like structures in the neutron scattering data. Within cobalt niobate the strongest interaction is ferromagnetic and along the chain. The chains themselves are laid out on a triangular fashion
and interact, although far more weakly, in an antiferromagnetic manner. This triangular patterning as well as an antiferromagnetic interaction results in interchain frustration, which protects the quasi-1D nature of the system due to the difficulty generated in creating 3D order.
In nickel niobate we found that growth conditions caused highly variable changes, and we were able to create two different polymorphs. One polymorph was in the same space group as cobalt niobate, which gave us an opportunity to explore the magnetic difference between a spin-½ and spin-1 magnetic system and in nickel niobate in the new space group we performed an ab initio characterization solving the unit cell structure, the magnetic structure with neutron scattering as well as a magnetic characterization with SQUID magnetometry and muon spin rotation, allowing us to contrast the significant crystallographic differences. For the new polymorph we were able to determine its magnetic structure, characterized by Ising-like spins arranged in frustrated tetrahedra with three of the four points lying in the same plane as the spin, and for both materials we were able to use zero-field μSR data to estimate behaviour near the critical point and determine a critical exponent near the magnetic transitions. In both polymorphs there is evidence of constrained magnetism or reduced dimensionality, although the evidence for low dimensionality is much stronger in the columbite polymorph. / Thesis / Doctor of Philosophy (PhD) / This thesis examines two different niobium-based compounds: cobalt niobate (CoNb2O6) and nickel niobate (NiNb2O6). In these systems the cobalt and nickel atoms provide interesting magnetic properties. Within a magnetic material, the magnetic atoms tend to have their spins
align in certain ways. The atoms themselves are fixed to particular sites by the way the material is assembled; an atomic framework.
In the case of cobalt niobate, the magnetic atoms are arranged in well-separated chains so that a magnetic atom interacts strongly with its magnetic neighbours within a chain, and weakly with ones that are further away. This is an example of a material that is called `low dimensional'. The chains themselves form triangular patterns, and the interactions between chains are both weaker and antialigned, which creates a frustrated competition between the chains, protecting the low dimensional state by creating conditions where it is hard for all the spins in the material to order.
For nickel niobate, the magnetic moments all want to anti-align, or be pointing in the opposite direction as its nearest neighbour. The magnetism is `frustrated' because each magnetic atom is tetrahedrally connected to three other atoms, so it cannot meet that condition. This can be visualized by drawing a triangle and trying to make each corner have an arrow pointing up
or down. The third corner of the triangle cannot satisfy this requirement for its neighbours (one up and one down arrow).
Both decreased dimensionality and frustration can lead to the emergence of novel quantum states of matter at low temperature. This thesis explores these materials with that in mind.

Identiferoai:union.ndltd.org:mcmaster.ca/oai:macsphere.mcmaster.ca:11375/21979
Date11 1900
CreatorsMunsie, Timothy John Sagan
ContributorsLuke, Graeme M., Physics and Astronomy
Source SetsMcMaster University
LanguageEnglish
Detected LanguageEnglish
TypeThesis

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