Spin-phonon relaxation from a universal ab initio density-matrix approach
Spin-phonon relaxation from a universal ab initio density-matrix approach
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DOI：
10.1038/s41467-020-16063-5
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发表时间：
2020-06
影响因子：
16.6
通讯作者：
Junqing Xu;A. Habib;Sushant Kumar;Feng Wu;R. Sundararaman;Y. Ping
中科院分区：
文献类型：
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作者：
Junqing Xu;A. Habib;Sushant Kumar;Feng Wu;R. Sundararaman;Y. Ping
设计具有长寿命电子自旋态的新量子材料迫切需要一种通用的理论形式和计算技术来可靠地预测本征自旋弛豫时间。基于密度矩阵的Lindbladian动力学，我们提出了一种新的、精确的、普适的第一原理方法来计算具有任意自旋混合和晶体对称性的固体的自旋-声子弛豫时间。该方法描述了Elliott-Yafet(EY)和D‘yakonov-Perel’(DP)机制对具有和不具有反转对称体系的自旋驰豫的贡献。结果表明，内禀自旋和动量弛豫时间都随着温度的升高而减小；而对于DP机制，自旋驰豫时间与外在散射时间成反比。我们预测了过渡金属二卤化物的自旋寿命具有很大的各向异性。与广泛材料实验的良好一致性突显了我们方法对量子信息科学至关重要的性质的预测能力。
Designing new quantum materials with long-lived electron spin states urgently requires a general theoretical formalism and computational technique to reliably predict intrinsic spin relaxation times. We present a new, accurate and universal first-principles methodology based on Lindbladian dynamics of density matrices to calculate spin-phonon relaxation time () of solids with arbitrary spin mixing and crystal symmetry. This method describes contributions of Elliott-Yafet (EY) and D'yakonov-Perel' (DP) mechanisms to spin relaxation for systems with and without inversion symmetry on an equal footing. We show that intrinsic spin and momentum relaxation times both decrease with increasing temperature; however, for the DP mechanism, spin relaxation time varies inversely with extrinsic scattering time. We predict large anisotropy of spin lifetime in transition metal dichalcogenides. The excellent agreement with experiments for a broad range of materials underscores the predictive capability of our method for properties critical to quantum information science.