Universität zu Köln

Amelin, K., Alexanian, Y., Nagel, U., Room, T., Robert, J., Debray, J., Simonet, V, Decorse, C., Wang, Z., Ballou, R., Constable, E. and de Brion, S. (2020). Terahertz magneto-optical investigation of quadrupolar spin-lattice effects in magnetically frustrated Tb2Ti2O7. Phys. Rev. B, 102 (13). COLLEGE PK: AMER PHYSICAL SOC. ISSN 2469-9969

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Abstract

Condensed matter magneto-optical investigations can be a powerful probe of a material's microscopic magnetoelectric properties. This is because subtle interactions between electric and magnetic multipoles on a crystal lattice show up in predictable and testable ways in a material's optical response tensor, which dictates the polarization state and absorption spectrum of propagating electromagnetic waves. Magneto-optical techniques are therefore strong complements to probes such as neutron scattering, particularly when spin-lattice coupling effects are present. Here we perform a magneto-optical investigation of vibronic spin-lattice coupling in the magnetically frustrated pyrochlore Tb2Ti2O7. Coupling of this nature involving quadrupolar mixing between the Tb3+ electronic levels and phonons in Tb2Ti2O7 has been a topic of debate for some time. This is particularly due to its implication for describing the exotic spin-liquid phase diagram of this highly debated system. A manifestation of this vibronic effect is observed as splitting of the ground and first excited crystal field doublets of the Tb3+ electronic levels, providing a fine structure to the absorption spectra in the terahertz (THz) frequency range. In this investigation, we apply a static magnetic field along the cubic [111] direction while probing with linearly polarized THz radiation. Through the Zeeman effect, the magnetic field enhances the splitting within the low-energy crystal field transitions revealing new details in our THz spectra. Complementary magneto-optical quantum calculations including quadrupolar terms show that indeed vibronic effects are required to describe our observations at 3 K. A further prediction of our theoretical model is the presence of a novel magneto-optical birefringence as a result of this vibronic process. Essentially, spin-lattice coupling within Tb2Ti2O7 may break the optical isotropy of the cubic system, supporting two different electromagnetic wave propagations within the crystal. Together our results reveal the significance of considering quadrupolar spin-lattice effects when describing the spin-liquid ground state of Tb2Ti2O7. They also highlight the potential for future magneto-optical investigations to probe complex materials where spin-lattice coupling is present and reveal new magneto-optical activity in the THz range.

Item Type:	Journal Article
Creators:	Creators Email ORCID ORCID Put Code Amelin, K. UNSPECIFIED UNSPECIFIED UNSPECIFIED Alexanian, Y. UNSPECIFIED UNSPECIFIED UNSPECIFIED Nagel, U. UNSPECIFIED UNSPECIFIED UNSPECIFIED Room, T. UNSPECIFIED UNSPECIFIED UNSPECIFIED Robert, J. UNSPECIFIED UNSPECIFIED UNSPECIFIED Debray, J. UNSPECIFIED UNSPECIFIED UNSPECIFIED Simonet, V UNSPECIFIED UNSPECIFIED UNSPECIFIED Decorse, C. UNSPECIFIED UNSPECIFIED UNSPECIFIED Wang, Z. UNSPECIFIED UNSPECIFIED UNSPECIFIED Ballou, R. UNSPECIFIED UNSPECIFIED UNSPECIFIED Constable, E. UNSPECIFIED UNSPECIFIED UNSPECIFIED de Brion, S. UNSPECIFIED UNSPECIFIED UNSPECIFIED
URN:	urn:nbn:de:hbz:38-314615
DOI:	10.1103/PhysRevB.102.134428
Journal or Publication Title:	Phys. Rev. B
Volume:	102
Number:	13
Date:	2020
Publisher:	AMER PHYSICAL SOC
Place of Publication:	COLLEGE PK
ISSN:	2469-9969
Language:	English
Faculty:	Unspecified
Divisions:	Unspecified
Subjects:	no entry
Uncontrolled Keywords:	Keywords Language CRYSTAL Multiple languages Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed Matter Multiple languages
URI:	http://kups.ub.uni-koeln.de/id/eprint/31461