Raw Data for: Spin-order-dependent magneto-elastic coupling in two dimensional antiferromagnetic MnPSe3 observed through Raman spectroscopy

Layered antiferromagnetic materials have recently emerged as an intriguing subset of the two-dimensional family providing a highly accessible regime with prospects for layer-number-dependent magnetism. Furthermore, transition metal phosphorus trichalcogenides, MPX3 (M= transition metal; X= chalcogen) provide a platform on which to investigate fundamental interactions between magnetic and lattice degrees of freedom and further explore the developing fields of spintronics and magnonics. Here, we use a combination of temperature dependent Raman spectroscopy and density functional theory to explore magnetic-ordering-dependent interactions between the manganese spin degree of freedom and lattice vibrations of the non-magnetic sub-lattice via a Kramers-Anderson super-exchange pathway in both bulk, and few-layer, manganese phosphorus triselenide (MnPSe3). We observe a nonlinear temperature dependent shift of phonon modes predominantly associated with the non-magnetic sub-lattice, revealing their non-trivial spin-phonon coupling below the N'eel temperature at 74 K, allowing us to extract mode-specific spin-phonon coupling constants.

层状反铁磁材料（Layered antiferromagnetic materials）是二维材料家族中一个引人注目的新兴分支，为研究层厚依赖的磁性提供了易于探索的体系。此外，过渡金属磷三硫属化物（transition metal phosphorus trichalcogenides，MPX3，其中M为过渡金属，X为硫属元素）为研究磁自由度（magnetic degree of freedom）与晶格自由度（lattice degree of freedom）之间的基本相互作用，以及进一步探索自旋电子学（spintronics）和磁振子学（magnonics）等新兴领域提供了平台。本文结合变温拉曼光谱（temperature dependent Raman spectroscopy）和密度泛函理论（density functional theory），通过克拉默斯-安德森超交换路径（Kramers-Anderson super-exchange pathway），研究了块体及少层锰磷三硒化物（MnPSe3）中锰自旋自由度（spin degree of freedom）与非磁子晶格（non-magnetic sub-lattice）振动之间依赖于磁有序的相互作用。我们观察到主要与非磁子晶格相关的声子模式存在非线性温度依赖位移，这表明在74 K的奈尔温度（Néel temperature）以下存在显著的自旋-声子耦合（spin-phonon coupling），从而能够提取特定模式的自旋-声子耦合常数。