TY - JOUR
T1 - Importance of dynamic lattice effects for crystal field excitations in the quantum spin ice candidate Pr2Zr2 O7
AU - Xu, Yuanyuan
AU - Man, Huiyuan
AU - Tang, Nan
AU - Baidya, Santu
AU - Zhang, Hongbing
AU - Nakatsuji, Satoru
AU - Vanderbilt, David
AU - Drichko, Natalia
N1 - Funding Information:
The authors are thankful to J. Gauget, C. Broholm, S. Bhattacharjee, T. McQueen, J.-J. Wen, and O. Tchernyshev for useful discussions. This work was supported as part of the Institute for Quantum Matter, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award No. DE-SC0019331. This work in Japan is partially supported by CREST (Grants No. JPMJCR18T3 and No. JPMJCR15Q5), by New Energy and Industrial Technology Development Organization (NEDO), by Grants-in-Aids for Scientific Research on Innovative Areas (Grants No. 15H05882 and No. 15H05883) from the Ministry of Education, Culture, Sports, Science, and Technology of Japan, and by Grants-in-Aid for Scientific Research (Grant No. 19H00650).
Publisher Copyright:
© 2021 American Physical Society.
PY - 2021/8/15
Y1 - 2021/8/15
N2 - We explore dynamic interactions between the crystal lattice and magnetic degrees of freedom in a frustrated magnetic system using the example of a pyrochlore quantum spin-ice candidate Pr2Zr2O7. Using Raman scattering spectroscopy we demonstrate that crystal electric field excitations of Pr3+, which define the magnetic properties of Pr2Zr2O7, cannot be understood within a model of a static lattice. We identify vibronic interactions with a phonon which lead to a splitting of a doublet crystal field excitation at around 55 meV. We also observe an unconventional behavior of a splitting of the non-Kramers ground state doublet of Pr3+, revealed by observing excitations to the first excited singlet state Eg0→A1g at around 10 meV. The splitting has a strong temperature dependence, where the doublet structure is most prominent between 50 and 100 K, and the weight of one of the components strongly decreases on cooling contrary to simple thermal population tendency. We suggest a static or dynamic deviation of Pr3+ from the position in the ideal crystal structure can be the origin of the effect, with the deviation strongly decreasing at low temperatures.
AB - We explore dynamic interactions between the crystal lattice and magnetic degrees of freedom in a frustrated magnetic system using the example of a pyrochlore quantum spin-ice candidate Pr2Zr2O7. Using Raman scattering spectroscopy we demonstrate that crystal electric field excitations of Pr3+, which define the magnetic properties of Pr2Zr2O7, cannot be understood within a model of a static lattice. We identify vibronic interactions with a phonon which lead to a splitting of a doublet crystal field excitation at around 55 meV. We also observe an unconventional behavior of a splitting of the non-Kramers ground state doublet of Pr3+, revealed by observing excitations to the first excited singlet state Eg0→A1g at around 10 meV. The splitting has a strong temperature dependence, where the doublet structure is most prominent between 50 and 100 K, and the weight of one of the components strongly decreases on cooling contrary to simple thermal population tendency. We suggest a static or dynamic deviation of Pr3+ from the position in the ideal crystal structure can be the origin of the effect, with the deviation strongly decreasing at low temperatures.
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U2 - 10.1103/PhysRevB.104.075125
DO - 10.1103/PhysRevB.104.075125
M3 - Article
AN - SCOPUS:85113154338
SN - 0163-1829
VL - 104
JO - Physical Review B-Condensed Matter
JF - Physical Review B-Condensed Matter
IS - 7
M1 - 075125
ER -