We present a first-principles investigation of spin-phonon relaxation in a molecular crystal of Co(II) single-ion magnets. Our study combines electronic structure calculations with machine-learning force fields and unravels the nature of both the Orbach and the Raman relaxation channels in terms of atomistic processes. We find that although both mechanisms are mediated by the excited spin states, the low temperature spin dynamics is dominated by phonons in the THz energy range, which partially suppress the benefit of having a large magnetic anisotropy. This study also determines the importance of intra-molecular motions for both the relaxation mechanisms and paves the way to the rational design of a new generation of single-ion magnets with tailored spin-phonon coupling.
Zeeman split Kramers doublets in spin-supersolid candidate Na$_{2}$BaCo(PO$_{4}$)$_{2}$
School of Physics and Astronomy, University of Edinburgh（爱丁堡大学物理与天文学院）；ISIS Pulsed Neutron and Muon Source, STFC Rutherford Appleton Laboratory（STFC卢瑟福阿普尔顿实验室ISIS脉冲中子与缪子源）；NIST Center for Neutron Research（美国国家标准与技术研究院中子研究中心）；Department of Chemistry, Princeton University（普林斯顿大学化学系）
Field-Induced Up-Up-Down State and Frustrated Magnetism in a Non-Kramers Triangular Antiferromagnet
Shenzhen Institute for Quantum Science and Engineering, Southern University of Science and Technology（南方科技大学量子科学和工程研究院）；International Quantum Academy（国际量子学院）；Tsung-Dao Lee Institute, Shanghai Jiao Tong University（上海交通大学李政道研究所）；School of Physics and Astronomy, Shanghai Jiao Tong University（上海交通大学物理与天文学院）；School of Physics and Electronics, Henan University（河南大学物理与电子学院）
Ln2(SeO3)2(SO4)(H2O)2 (Ln = Sm, Dy, Yb): A Mixed-Ligand Pathway to New Lathanide (III) Multifunctional Materials Featuring Nonlinear Optical and Magnetic Anisotropy Properties
Loss of altermagnetic order and smooth restoration of Kramers' spin degeneracy with increasing temperature in CrSb and MnTe
H.H. Wills Physics Laboratory, University of Bristol（布里斯托大学 H.H. 威尔斯物理实验室）；Department of Physics, University of Warwick（华威大学物理系）；Institute for Theoretical Physics, Johannes Keppler University Linz（林茨约翰内斯·开普勒大学理论物理研究所）；Donostia International Physics Center（圣塞巴斯蒂安国际物理中心）；Max-Planck-Institut für Mikrostrukturphysik（马克斯·普朗克微结构物理研究所）
Magnetic field-tuned size and dual annihilation pathways of chiral magnetic bobbers
School of Materials and Physics, China University of Mining and Technology（中国矿业大学材料科学与工程学院）；Key Laboratory of Magnetism and Magnetic Functional Materials of MoE, Lanzhou University（兰州大学磁性及磁功能材料教育部重点实验室）
A fluctuation-free pathway for a topological magnetic phase transition
Helmholtz-Zentrum Berlin für Materialien und Energie GmbH（柏林赫尔姆霍兹材料与能源中心有限公司）；Experimental Physics V, Center for Electronic Correlations and Magnetism, University of Augsburg（奥格斯堡大学实验物理学第五系、电子相关与磁学中心）；Institute for Molecules and Materials, Radboud University（拉波德大学分子与材料研究所）；Institut für Ionenstrahlphysik und Materialforschung, Helmholtz-Zentrum Dresden - Rossendorf（德累斯顿-罗斯多夫赫尔姆霍兹中心离子束物理与材料研究所）；Laboratoire Albert Fert CNRS, Thales, Université Paris-Saclay（阿尔伯特·费尔特实验室（CNRS）、泰雷兹集团、巴黎萨克雷大学）；Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy（马克斯·玻恩非线性光学与短脉冲光谱研究所）
