Vibronic collapse of ordered quadrupolar ice in the pyrochore magnet Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$

Fuente: arXiv
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Auteurs principaux: Alexanian, Yann, Robert, Julien, Simonet, Virginie, Langérôme, Benjamin, Brubach, Jean-Blaise, Roy, Pascale, Decorse, Claudia, Lhotel, Elsa, Constable, Evan, Ballou, Rafik, De Brion, Sophie
Format: Preprint
Publié: 2022
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author Alexanian, Yann
Robert, Julien
Simonet, Virginie
Langérôme, Benjamin
Brubach, Jean-Blaise
Roy, Pascale
Decorse, Claudia
Lhotel, Elsa
Constable, Evan
Ballou, Rafik
De Brion, Sophie
author_facet Alexanian, Yann
Robert, Julien
Simonet, Virginie
Langérôme, Benjamin
Brubach, Jean-Blaise
Roy, Pascale
Decorse, Claudia
Lhotel, Elsa
Constable, Evan
Ballou, Rafik
De Brion, Sophie
contents While the spin liquid state in the frustrated pyrochlore Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ has been studied both experimentally and theoretically for more than two decades, no definite description of this unconventional state has been achieved. Using synchrotron based THz spectroscopy in combination with quantum numerical simulations, we highlight a significant link between two previously unrelated features: the existence of a quadrupolar order following an ice rule and the presence of strong magneto-elastic coupling in the form of hybridized Tb$^{3+}$ crystal-field and phonon modes. The magnitude of this so-called vibronic process, which involves quadrupolar degrees of freedom, is significantly dependent on small off-stoichiometry $x$ and favors all-in all-out like correlations between quadrupoles. This mechanism competes with the long range ordered quadrupolar ice, and for slightly different stoichiometry, is able to destabilize it.
format Preprint
id arxiv_https___arxiv_org_abs_2207_10036
institution arXiv
publishDate 2022
record_format arxiv
spellingShingle Vibronic collapse of ordered quadrupolar ice in the pyrochore magnet Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$
Alexanian, Yann
Robert, Julien
Simonet, Virginie
Langérôme, Benjamin
Brubach, Jean-Blaise
Roy, Pascale
Decorse, Claudia
Lhotel, Elsa
Constable, Evan
Ballou, Rafik
De Brion, Sophie
Strongly Correlated Electrons
While the spin liquid state in the frustrated pyrochlore Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ has been studied both experimentally and theoretically for more than two decades, no definite description of this unconventional state has been achieved. Using synchrotron based THz spectroscopy in combination with quantum numerical simulations, we highlight a significant link between two previously unrelated features: the existence of a quadrupolar order following an ice rule and the presence of strong magneto-elastic coupling in the form of hybridized Tb$^{3+}$ crystal-field and phonon modes. The magnitude of this so-called vibronic process, which involves quadrupolar degrees of freedom, is significantly dependent on small off-stoichiometry $x$ and favors all-in all-out like correlations between quadrupoles. This mechanism competes with the long range ordered quadrupolar ice, and for slightly different stoichiometry, is able to destabilize it.
title Vibronic collapse of ordered quadrupolar ice in the pyrochore magnet Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$
topic Strongly Correlated Electrons
url https://arxiv.org/abs/2207.10036