Magnetoelastically induced vibronic bound state in the spin-ice pyrochlore Ho2Ti2O7

Gaudet, J; Hallas, A. M.; Buhariwalla, C. R. C.; Sala, Gabriele; Stone, Matthew B.; Tachibana, Makoto; Baroudi, K; Cava, R. J.; Gaulin, Bruce D.

doi:10.1103/PhysRevB.98.014419

Title: Magnetoelastically induced vibronic bound state in the spin-ice pyrochlore ${Ho}_{2} {Ti}_{2} O_{7}$

Journal Article · Thu Jul 19 00:00:00 EDT 2018 · Physical Review B

DOI:https://doi.org/10.1103/PhysRevB.98.014419· OSTI ID:1470882

Gaudet, J ^[1]; Hallas, A. M. ^[1]; Buhariwalla, C. R. C. ^[1];

^[2];

^[3]; Tachibana, Makoto ^[4]; Baroudi, K ^[5]; Cava, R. J. ^[6]; Gaulin, Bruce D. ^[7]

McMaster Univ., Hamilton, ON (Canada). Dept. of Physics and Astronomy
McMaster Univ., Hamilton, ON (Canada). Dept. of Physics and Astronomy; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
National Inst. for Materials Science (NIMS), Tsukuba (Japan)
Princeton Univ., NJ (United States). Dept. of Chemistry
Princeton Univ., NJ (United States). Dept. of Chemistry; Princeton Univ., NJ (United States). Princeton Materials Inst.
McMaster Univ., Hamilton, ON (Canada). Dept. of Physics and Astronomy; Canadian Inst. for Advanced Research, Toronto (Canada); Brockhouse Inst. for Materials Research, Hamilton, ON (Canada)

The single-ion physics of Ho₂Ti₂O₇ is well understood to produce strong Ising anisotropy, which is an essential ingredient to its low-temperature spin-ice state. We present inelastic neutron scattering measurements on Ho₂Ti₂O₇ that reveal a clear inconsistency with its established single-ion Hamiltonian. Specifically, we show that a crystal-field doublet near 60 meV is split by approximately 3 meV. Furthermore, this crystal-field splitting is not isolated to Ho₂Ti₂O₇ but can also be found in its chemical pressure analogs Ho₂Ge₂O₇ and Ho₂Sn₂O₇. We demonstrate that the origin of this effect is a vibronic bound state, resulting from the entanglement of a phonon and crystal-field excitation. In conclusion, we derive the microscopic Hamiltonian that describes the magnetoelastic coupling and provides a quantitative description of the inelastic neutron spectra.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; FG02-98ER46544

OSTI ID:: 1470882

Alternate ID(s):: OSTI ID: 1460908

Journal Information:: Physical Review B, Vol. 98, Issue 1; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 17 works

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