Mesoscale interplay between phonons and crystal electric field excitations in quantum spin liquid candidate CsYbSe2

Pai, Yun-Yi; Marvinney, Claire E.; Liang, Liangbo; Xing, Jie; Scheie, Allen O.; Puretzky, Alexander; Halasz, Gabor; Li, Xun; Juneja, Rinkle; Sefat, Athena Safa; Parker, David S.; Lindsay, Lucas R.; Lawrie, Benjamin J.

doi:10.1039/d1tc05934c

Title: Mesoscale interplay between phonons and crystal electric field excitations in quantum spin liquid candidate CsYbSe₂

Journal Article · 23 February 2022 · Journal of Materials Chemistry C

DOI: https://doi.org/10.1039/d1tc05934c · OSTI ID:1855668

^[1];

^[2];

^[1];

^[2];

^[2]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Quantum Science Center, Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

In this report CsYbSe₂, a recently identified quantum spin liquid (QSL) candidate, exhibits strong crystal electric field (CEF) excitations. Here, we identify phonon and CEF modes with Raman spectroscopy and observe strong CEF-phonon coupling resulting in a vibronic bound state. Complex, mesoscale interplay between phonon modes and CEF modes is observed in real space. Additionally, an unexpected resonant Raman excitation condition is satisfied, yielding up to third-order combination modes, with a total of 17 modes identified in the spectra. This study paves the way to coherent control of possible QSL ground states with optically accessible CEF-phonon manifolds and mesoscale engineering of CEF-phonon interactions.

View Accepted Manuscript (DOE)

Cite

Export

Save

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1855668

Journal Information:: Journal of Materials Chemistry C, Journal Name: Journal of Materials Chemistry C Journal Issue: 11 Vol. 10; ISSN 2050-7526

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

References (62)

Thickness and Spin Dependence of Raman Modes in Magnetic Layered Fe ₃ GeTe ₂ Kong, Xiangru; Berlijn, Tom; Liang, Liangbo Advanced Electronic Materials, Vol. 7, Issue 7 https://doi.org/10.1002/aelm.202001159	journal	March 2021
Termaufspaltung in Kristallen Bethe, H. Annalen der Physik, Vol. 395, Issue 2 https://doi.org/10.1002/andp.19293950202	journal	January 1929
Resonating valence bonds: A new kind of insulator? Anderson, P. W. Materials Research Bulletin, Vol. 8, Issue 2 https://doi.org/10.1016/0025-5408(73)90167-0	journal	February 1973
Coupled quadrupole-phonon excitations: Inelastic Neutron scattering on van vleck paramagnet PrNi5 Aksenov, V. L.; Goremychkin, E. A.; Mühle, E. Physica B+C, Vol. 120, Issue 1-3 https://doi.org/10.1016/0378-4363(83)90398-4	journal	May 1983
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Crystal growth, density functional theory, and scintillation properties of Tl3LnCl6:Ce3+ and TlLn2Cl7:Ce3+ (Ln = Y, Gd) van Loef, Edgar; Shirwadkar, Urmila; Pandian, Lakshmi Soundara Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 995 https://doi.org/10.1016/j.nima.2021.165047	journal	April 2021
How the Ligand Field in Lanthanide Coordination Complexes Determines Magnetic Susceptibility Anisotropy, Paramagnetic NMR Shift, and Relaxation Behavior Parker, David; Suturina, Elizaveta A.; Kuprov, Ilya Accounts of Chemical Research, Vol. 53, Issue 8 https://doi.org/10.1021/acs.accounts.0c00275	journal	July 2020
Magnetostriction of α-RuCl ₃ Flakes in the Zigzag Phase Pai, Yun-Yi; Marvinney, Claire E.; Feldman, Matthew A. The Journal of Physical Chemistry C, Vol. 125, Issue 46 https://doi.org/10.1021/acs.jpcc.1c07472	journal	November 2021
Emergence of Interfacial Polarons from Electron–Phonon Coupling in Graphene/h-BN van der Waals Heterostructures Chen, Chaoyu; Avila, José; Wang, Shuopei Nano Letters, Vol. 18, Issue 2 https://doi.org/10.1021/acs.nanolett.7b04604	journal	January 2018
Crystal Synthesis and Frustrated Magnetism in Triangular Lattice Cs RE Se ₂ ( RE = La–Lu): Quantum Spin Liquid Candidates CsCeSe ₂ and CsYbSe ₂ Xing, Jie; Sanjeewa, Liurukara D.; Kim, Jungsoo ACS Materials Letters, Vol. 2, Issue 1 https://doi.org/10.1021/acsmaterialslett.9b00464	journal	November 2019
Interlayer Breathing and Shear Modes in Few-Trilayer MoS ₂ and WSe ₂ Zhao, Yanyuan; Luo, Xin; Li, Hai Nano Letters, Vol. 13, Issue 3 https://doi.org/10.1021/nl304169w	journal	February 2013
Strong coupling between local moments and superconducting ‘heavy’ electrons in UPd2Al3 Sato, N. K.; Aso, N.; Miyake, K. Nature, Vol. 410, Issue 6826 https://doi.org/10.1038/35066519	journal	March 2001
Evidence for a spinon Fermi surface in a triangular-lattice quantum-spin-liquid candidate Shen, Yao; Li, Yao-Dong; Wo, Hongliang Nature, Vol. 540, Issue 7634 https://doi.org/10.1038/nature20614	journal	December 2016
Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet Banerjee, A.; Bridges, C. A.; Yan, J. -Q. Nature Materials, Vol. 15, Issue 7 https://doi.org/10.1038/nmat4604	journal	April 2016
Magnon bound states versus anyonic Majorana excitations in the Kitaev honeycomb magnet α-RuCl3 Wulferding, Dirk; Choi, Youngsu; Do, Seung-Hwan Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-15370-1	journal	March 2020
Observation of the polaronic character of excitons in a two-dimensional semiconducting magnet CrI3 Jin, Wencan; Kim, Hyun Ho; Ye, Zhipeng Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-18627-x	journal	September 2020
The range of non-Kitaev terms and fractional particles in α-RuCl3 Wang, Yiping; Osterhoudt, Gavin B.; Tian, Yao npj Quantum Materials, Vol. 5, Issue 1 https://doi.org/10.1038/s41535-020-0216-6	journal	March 2020
Observation of two types of fractional excitation in the Kitaev honeycomb magnet Janša, Nejc; Zorko, Andrej; Gomilšek, Matjaž Nature Physics, Vol. 14, Issue 8 https://doi.org/10.1038/s41567-018-0129-5	journal	May 2018
Field-tunable quantum disordered ground state in the triangular-lattice antiferromagnet NaYbO2 Bordelon, Mitchell M.; Kenney, Eric; Liu, Chunxiao Nature Physics, Vol. 15, Issue 10 https://doi.org/10.1038/s41567-019-0594-5	journal	July 2019
Majorana quantization and half-integer thermal quantum Hall effect in a Kitaev spin liquid Kasahara, Y.; Ohnishi, T.; Mizukami, Y. Nature, Vol. 559, Issue 7713 https://doi.org/10.1038/s41586-018-0274-0	journal	July 2018
Electronic Raman Spectra. I. Raman Transitions of Trivalent Ytterbium, Europium, and Neodymium in Yttrium Gallium Garnet Koningstein, J. A. The Journal of Chemical Physics, Vol. 46, Issue 7 https://doi.org/10.1063/1.1841119	journal	April 1967
Synthesis and anisotropic magnetism in quantum spin liquid candidates A YbSe ₂ ( A = K and Rb) Xing, Jie; Sanjeewa, Liurukara D.; May, Andrew F. APL Materials, Vol. 9, Issue 11 https://doi.org/10.1063/5.0071161	journal	November 2021
Magnetoelastic hybrid excitations in CeAuAl ₃ Čermák, Petr; Schneidewind, Astrid; Liu, Benqiong Proceedings of the National Academy of Sciences, Vol. 116, Issue 14 https://doi.org/10.1073/pnas.1819664116	journal	March 2019
Quantum spin liquids: a review Savary, Lucile; Balents, Leon Reports on Progress in Physics, Vol. 80, Issue 1 https://doi.org/10.1088/0034-4885/80/1/016502	journal	November 2016
Rare-Earth Chalcogenides: A Large Family of Triangular Lattice Spin Liquid Candidates Liu, Weiwei; Zhang, Zheng; Ji, Jianting Chinese Physics Letters, Vol. 35, Issue 11 https://doi.org/10.1088/0256-307X/35/11/117501	journal	October 2018
Theory of the Variations in Paramagnetic Anisotropy Among Different Salts of the Iron Group Van Vleck, J. H. Physical Review, Vol. 41, Issue 2 https://doi.org/10.1103/PhysRev.41.208	journal	July 1932
Gapless spin-liquid state in the structurally disorder-free triangular antiferromagnet NaYbO 2 Ding, Lei; Manuel, Pascal; Bachus, Sebastian Physical Review B, Vol. 100, Issue 14 https://doi.org/10.1103/PhysRevB.100.144432	journal	October 2019
Field-induced magnetic transition and spin fluctuations in the quantum spin-liquid candidate CsYbSe 2 Xing, Jie; Sanjeewa, Liurukara D.; Kim, Jungsoo Physical Review B, Vol. 100, Issue 22 https://doi.org/10.1103/PhysRevB.100.220407	journal	December 2019
Anisotropic field-induced ordering in the triangular-lattice quantum spin liquid NaYbSe 2 Ranjith, K. M.; Luther, S.; Reimann, T. Physical Review B, Vol. 100, Issue 22 https://doi.org/10.1103/PhysRevB.100.224417	journal	December 2019
Quantum spin liquid ground state in the disorder free triangular lattice NaYbS 2 Sarkar, R.; Schlender, Ph.; Grinenko, V. Physical Review B, Vol. 100, Issue 24 https://doi.org/10.1103/PhysRevB.100.241116	journal	December 2019
High-field quantum disordered state in α − RuCl 3 : Spin flips, bound states, and multiparticle continuum Sahasrabudhe, A.; Kaib, D. A. S.; Reschke, S. Physical Review B, Vol. 101, Issue 14 https://doi.org/10.1103/PhysRevB.101.140410	journal	April 2020
Crystalline electric field excitations in the quantum spin liquid candidate NaYbSe 2 Zhang, Zheng; Ma, Xiaoli; Li, Jianshu Physical Review B, Vol. 103, Issue 3 https://doi.org/10.1103/PhysRevB.103.035144	journal	January 2021
Temperature evolution of the phonon dynamics in the Kitaev spin liquid Feng, Kexin; Ye, Mengxing; Perkins, Natalia B. Physical Review B, Vol. 103, Issue 21 https://doi.org/10.1103/PhysRevB.103.214416	journal	June 2021
Yb delafossites: Unique exchange frustration of 4 f spin- 1 2 moments on a perfect triangular lattice Schmidt, B.; Sichelschmidt, J.; Ranjith, K. M. Physical Review B, Vol. 103, Issue 21 https://doi.org/10.1103/PhysRevB.103.214445	journal	June 2021
Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y. Physical Review B, Vol. 57, Issue 3, p. 1505-1509 https://doi.org/10.1103/PhysRevB.57.1505	journal	January 1998
Spin-order-dependent Raman scattering in RuSr 2 GdCu 2 O 8 Fainstein, A.; Etchegoin, P.; Trodahl, H. J. Physical Review B, Vol. 61, Issue 22 https://doi.org/10.1103/PhysRevB.61.15468	journal	June 2000
Superconductivity and heavy fermion behavior in PrOs 4 Sb 12 Bauer, E. D.; Frederick, N. A.; Ho, P. -C. Physical Review B, Vol. 65, Issue 10 https://doi.org/10.1103/PhysRevB.65.100506	journal	February 2002
Inelastic neutron scattering from UPd 2 Al 3 under high magnetic fields Blackburn, E.; Hiess, A.; Bernhoeft, N. Physical Review B, Vol. 74, Issue 2 https://doi.org/10.1103/PhysRevB.74.024406	journal	July 2006
Spectroscopy of Yb 3 + : CaF 2 : From isolated centers to clusters Petit, V.; Camy, P.; Doualan, J-L. Physical Review B, Vol. 78, Issue 8 https://doi.org/10.1103/PhysRevB.78.085131	journal	August 2008
First-principles calculations of the ferroelastic transition between rutile-type and CaCl 2 -type SiO 2 at high pressures Togo, Atsushi; Oba, Fumiyasu; Tanaka, Isao Physical Review B, Vol. 78, Issue 13 https://doi.org/10.1103/PhysRevB.78.134106	journal	October 2008
Electronic hybridization effect on 4 f electron crystal field states of PrOs 4 P 12 Iwasa, Kazuaki; Saito, Kotaro; Murakami, Youichi Physical Review B, Vol. 79, Issue 23 https://doi.org/10.1103/PhysRevB.79.235113	journal	June 2009
Magnetoelastically induced vibronic bound state in the spin-ice pyrochlore Ho 2 Ti 2 O 7 Gaudet, J.; Hallas, A. M.; Buhariwalla, C. R. C. Physical Review B, Vol. 98, Issue 1 https://doi.org/10.1103/PhysRevB.98.014419	journal	July 2018
Lattice dynamics and coupled quadrupole-phonon excitations in CeAuAl 3 Liu, B. -Q.; Čermák, P.; Franz, C. Physical Review B, Vol. 98, Issue 17 https://doi.org/10.1103/PhysRevB.98.174306	journal	November 2018
NaYbS 2 : A planar spin- 1 2 triangular-lattice magnet and putative spin liquid Baenitz, M.; Schlender, Ph.; Sichelschmidt, J. Physical Review B, Vol. 98, Issue 22 https://doi.org/10.1103/PhysRevB.98.220409	journal	December 2018
Field-induced instability of the quantum spin liquid ground state in the J eff = 1 2 triangular-lattice compound NaYbO 2 Ranjith, K. M.; Dmytriieva, D.; Khim, S. Physical Review B, Vol. 99, Issue 18 https://doi.org/10.1103/PhysRevB.99.180401	journal	May 2019
Vibron Quasibound State in the Noncentrosymmetric Tetragonal Heavy-Fermion Compound CeCuAl 3 Adroja, D. T.; del Moral, A.; de la Fuente, C. Physical Review Letters, Vol. 108, Issue 21 https://doi.org/10.1103/PhysRevLett.108.216402	journal	May 2012
Scattering Continuum and Possible Fractionalized Excitations in α − RuCl 3 Sandilands, Luke J.; Tian, Yao; Plumb, Kemp W. Physical Review Letters, Vol. 114, Issue 14 https://doi.org/10.1103/PhysRevLett.114.147201	journal	April 2015
Evidence for a Field-Induced Quantum Spin Liquid in α - RuCl 3 Baek, S. -H.; Do, S. -H.; Choi, K. -Y. Physical Review Letters, Vol. 119, Issue 3 https://doi.org/10.1103/PhysRevLett.119.037201	journal	July 2017
Emergent Vibronic Excitations in the Magnetodielectric Regime of Ce 2 O 3 Sethi, A.; Slimak, J. E.; Kolodiazhnyi, T. Physical Review Letters, Vol. 122, Issue 17 https://doi.org/10.1103/PhysRevLett.122.177601	journal	April 2019
Dynamic Jahn-Teller Effect in a Rare-Earth Compound: Ce Al 2 Loewenhaupt, M.; Rainford, B. D.; Steglich, F. Physical Review Letters, Vol. 42, Issue 25 https://doi.org/10.1103/PhysRevLett.42.1709	journal	June 1979
Effect of Configuration Crossover on the Electronic Raman Scattering by 4 f Multiplets Güntherodt, G.; Jayaraman, A.; Anastassakis, E. Physical Review Letters, Vol. 46, Issue 13 https://doi.org/10.1103/PhysRevLett.46.855	journal	March 1981
Bound State between a Crystal-Field Excitation and a Phonon in Ce Al 2 Thalmeier, Peter; Fulde, Peter Physical Review Letters, Vol. 49, Issue 21 https://doi.org/10.1103/PhysRevLett.49.1588	journal	November 1982
Raman Scattering from Coupled Phonon and Electronic Crystal-Field Excitations in Ce Al 2 Güntherodt, G.; Jayaraman, A.; Batlogg, G. Physical Review Letters, Vol. 51, Issue 25 https://doi.org/10.1103/PhysRevLett.51.2330	journal	December 1983
Coupling of phonons to crystal-field excitations in NdBa 2 Cu 3 O 7 − δ Heyen, E. T.; Wegerer, R.; Cardona, M. Physical Review Letters, Vol. 67, Issue 1 https://doi.org/10.1103/PhysRevLett.67.144	journal	July 1991
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Phonon dynamics in the Kitaev spin liquid Ye, Mengxing; Fernandes, Rafael M.; Perkins, Natalia B. Physical Review Research, Vol. 2, Issue 3 https://doi.org/10.1103/PhysRevResearch.2.033180	journal	August 2020
Systematic extraction of crystal electric-field effects and quantum magnetic model parameters in triangular rare-earth magnets Pocs, Christopher A.; Siegfried, Peter E.; Xing, Jie Physical Review Research, Vol. 3, Issue 4 https://doi.org/10.1103/PhysRevResearch.3.043202	journal	December 2021
PyCrystalField : software for calculation, analysis and fitting of crystal electric field Hamiltonians Scheie, A. Journal of Applied Crystallography, Vol. 54, Issue 1 https://doi.org/10.1107/S160057672001554X	journal	February 2021
Neutron scattering in the proximate quantum spin liquid α-RuCl ₃ Banerjee, Arnab; Yan, Jiaqiang; Knolle, Johannes Science, Vol. 356, Issue 6342 https://doi.org/10.1126/science.aah6015	journal	June 2017
Gapped magnetic ground state in quantum spin liquid candidate κ-(BEDT-TTF) ₂ Cu ₂ (CN) ₃ Miksch, Björn; Pustogow, Andrej; Rahim, Mojtaba Javaheri Science, Vol. 372, Issue 6539 https://doi.org/10.1126/science.abc6363	journal	April 2021
A Field Guide to Spin Liquids Knolle, J.; Moessner, R. Annual Review of Condensed Matter Physics, Vol. 10, Issue 1 https://doi.org/10.1146/annurev-conmatphys-031218-013401	journal	March 2019
Probabilistic programming in Python using PyMC3 Salvatier, John; Wiecki, Thomas V.; Fonnesbeck, Christopher PeerJ Computer Science, Vol. 2 https://doi.org/10.7717/peerj-cs.55	journal	January 2016

Similar Records

Direct Observation of Symmetry-Dependent Electron–Phonon Coupling in Black Phosphorus

Journal Article · 2019 · Journal of the American Chemical Society · OSTI ID:1607235

Mao, Nannan; Wang, Xingzhi; Lin, Yuxuan; +10 more

Separation of crystal-field levels and phonons in Pr dideuteride using polarized neutrons

Conference · 1985 · OSTI ID:6954474

Arons, R R; Cable, J W; Nicklow, R M

Importance of dynamic lattice effects for crystal field excitations in the quantum spin ice candidate Pr₂Zr₂O₇

Journal Article · 2021 · Physical Review B · OSTI ID:1813342

Xu, Yuanyuan; Man, Huiyuan; Tang, Nan; +5 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Title: Mesoscale interplay between phonons and crystal electric field excitations in quantum spin liquid candidate CsYbSe2

Citation Formats

References (62)

Similar Records

Related Subjects

Title: Mesoscale interplay between phonons and crystal electric field excitations in quantum spin liquid candidate CsYbSe₂