Low-temperature nuclear magnetic resonance investigation of systems frustrated by competing exchange interactions

Roy, Beas
Major Professor
Yuji Furukawa
Committee Member
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Physics and Astronomy
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Physics and Astronomy

This doctoral thesis emphasizes on the study of frustrated systems which form a very interesting class of compounds in physics. The technique used for the investigation of the magnetic properties of the frustrated materials is Nuclear Magnetic Resonance (NMR). NMR is a very novel tool for the microscopic study of the spin systems. NMR enables us to investigate the local magnetic properties of any system exclusively. The NMR experiments on the different systems yield us knowledge of the static as well as the dynamic behavior of the electronic spins. Frustrated systems bear great possibilities of revelation of new physics through the new ground states they exhibit.

The vandates AA'VO(PO4)2 [AA' ≡ Zn2 and BaCd] are great prototypes of the J1-J2 model which consists of magnetic ions sitting on the corners of a square lattice. Frustration is caused by the competing nearest-neighbor (NN) and next-nearest neighbor (NNN) exchange interactions. The NMR investigation concludes a columnar antiferromagnetic (AFM) state for both the compounds from the sharp peak of the nuclear spin-lattice relaxation rate (1/T1) and a sudden broadening of the 31P-NMR spectrum. The important conclusion from our study is the establishment of the first H-P-T phase diagram of BaCdVO(PO4)2. Application of high pressure reduces the saturation field (HS) in BaCdVO(PO4)2 and decreases the ratio J2/J1, pushing the system more towards a questionable boundary (a disordered ground state) between the columnar AFM and a ferromagnetic ground state. A pressure up to 2.4 GPa will completely suppress HS.

The Fe ions in the `122' iron-arsenide superconductors also sit on a square lattice thus closely resembling the J1-J2 model. The 75As-NMR and Nuclear Quadrupole Resonance (NQR) experiments are conducted in the compound CaFe2As2 prepared by two different heat treatment methods (`as-grown' and `annealed'). Interestingly the two samples show two different ground states. While the ground state of the `as-grown' sample shows a non-magnetic collapsed tetragonal phase (with no magnetic fluctuations), the ground state of the `annealed' sample shows a magnetically long-range ordered orthorhombic phase. The temperature dependence of 1/T1 and that of Knight shift showed that the electron correlations completely disappear in the nonsuperconducting collapsed tetragonal phase in `as-grown' sample of CaFe2As2 indicating quenching of Fe moments.

The insulating A-site spinel compound CoAl2O4 exhibits frustration due to competing NN and NNN exchange interactions. This compound has been studied for a long time yet there has been a contradiction as to what the ground state of this compound is. The origin of this ambiguity was pointed out to be microstructure effects such as site-inversion between Co and Al. Thus depending on the value of degree of site inversion x [(Co{1-x}Alx)[Al{2-x}Cox]O4], the ground states differ. A very high quality sample was prepared (x ≈ 0.06) and 27Al and 59Co NMR were performed to study the ground state of this compound. Together with the results from heat capacity, magnetic measurements and neutron diffraction measurements we conclude that the ground state is collinear AFM. We settled a long debated problem for the ground state of CoAl2O4.

The compound BiMn2PO6 is a magnetically frustrated system with three-dimensional magnetic ordering. Frustration in this compound is caused by the comparable values of the exchange interactions along the chain, along the rung and in between the ladders. Thus the magnetic structure of this compound is quite complex with the temperature dependence of magnetic susceptibility exhibiting peak at 30 K, a jump at 43 K and a change of slope at 10 K. 31P-NMR study was done on this system to investigate the nature of transitions (if any) at these temperatures. NMR study suggested a long-range AFM transition at 30 K with a sharp peak in 1/T1. No signature of transition at 43 K suggested its origin is extrinsic. Between 10 K and 30 K the NMR spectra proved the existence of a commensurate magnetic order while below 10 K, the shape of the NMR spectrum changes either due to an incommensurate magnetic order or due to spin reorientation.

In summary the work presented in this thesis focusses on the NMR investigation of the magnetic properties of various compounds frustrated by the competing exchange interactions.


[1] A. Yogi, N. Ahmad, R. Nath, A. A. Tsirlin, J. Sichelschmidt, B. Roy and Y. Furukawa, arXiv:1409.3076 (submitted to Phys. Rev. B).

[2] Beas Roy, Yuji Furukawa, Ramesh Nath, David C. Johnston, J. Phys.: Conf. Ser. 320, 012048 (2011).

[3] Beas Roy, Yuji Furukawa, David Johnston, Ramesh Nath, Yasuhiro Komaki, Hideto Fukazawa, and Yoh Kohori, ``Magnetic phase diagram of the two-dimensional frustrated square lattice compound BaCdVO(PO4)2 from high-pressure and low-temperature 31P-NMR study'', Paper to be submitted.

[4] S. Ran, S. L. Bud'ko, D. K. Pratt, A. Kreyssig, M. G. Kim, M. J. Kramer, D. H. Ryan, W. N. Rowan-Weetaluktuk, Y. Furukawa, B. Roy, A. I. Goldman, and P. C. Canfield, Phys. Rev. B 83, 144517 (2011).

[5] Y. Furukawa, B. Roy, S. Ran, S. L. Bud'ko and P. C. Canfield, Phys. Rev. B 89, 121109 (R) (2014).

[6] B. Roy, Abhishek Pandey, Q. Zhang, T. W. Heitmann, D. Vaknin, D. C. Johnston, and Y. Furukawa, Phys. Rev. B 88, 174415 (2013).

[7] R. Nath, K. M. Ranjith, B. Roy, D. C. Johnston, Y. Furukawa, and A. A. Tsirlin, Phys. Rev. B 90, 024431 (2014).