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Strong manipulation of the valley splitting upon twisting and gating in MoSe2/CrI3 and WSe2/CrI3

物理 凝聚态物理 哈密顿量(控制论) 异质结 联轴节(管道) 材料科学 结晶学 化学 数学 数学优化 冶金
作者
Klaus Zollner,Paulo E. Faria,Jaroslav Fabian
出处
期刊:Physical review [American Physical Society]
卷期号:107 (3) 被引量:23
标识
DOI:10.1103/physrevb.107.035112
摘要

Van der Waals (vdW) heterostructures provide a rich playground to engineer electronic, spin, and optical properties of individual two-dimensional materials. We investigate the twist-angle and gate dependence of the proximity-induced exchange coupling in the monolayer transition-metal dichalcogenides (TMDCs) ${\mathrm{MoSe}}_{2}$ and ${\mathrm{WSe}}_{2}$ due to the vdW coupling to the ferromagnetic semiconductor ${\mathrm{CrI}}_{3}$, from first-principles calculations. A model Hamiltonian, which captures the relevant band edges at the $K/{K}^{\ensuremath{'}}$ valleys of the proximitized TMDCs, is employed to quantify the proximity-induced exchange. Upon twisting from ${0}^{\ensuremath{\circ}}$ to ${30}^{\ensuremath{\circ}}$, we find a transition of the TMDC valence band (VB) edge exchange splitting from about $\ensuremath{-}2$ to $2\phantom{\rule{4pt}{0ex}}\mathrm{meV}$, while the conduction band (CB) edge exchange splitting remains nearly unchanged at around $\ensuremath{-}3\phantom{\rule{4pt}{0ex}}\mathrm{meV}$. For the VB of ${\mathrm{WSe}}_{2}$ (${\mathrm{MoSe}}_{2}$) on ${\mathrm{CrI}}_{3}$, the exchange coupling changes sign at around ${8}^{\ensuremath{\circ}}$ (${16}^{\ensuremath{\circ}}$). We find that even at the angles with almost zero spin splittings of the VB, the real-space spin polarization profile of holes at the band edge is highly nonuniform, with alternating spin up-and spin-down orbitals. Furthermore, a giant tunability of the proximity-induced exchange coupling is provided by a transverse electric field of a few V/nm. Within our first-principles framework, we are limited to commensurate structures, and thus considered a maximum strain of 2.2% for the individual monolayers. By investigating different atomic stacking configurations of the strained supercells, we demonstrate that proximity exchange varies locally in space within experimentally realistic setups. We complement our ab initio results by calculating the excitonic valley splitting to provide experimentally verifiable optical signatures of the proximity exchange. Specifically, we predict that the valley splitting increases almost linearly as a function of the twist angle. Furthermore, the proximity exchange is highly tunable by gating, allowing to tailor the valley splitting in the range of 0 to 12 meV in ${\mathrm{WSe}}_{2}/{\mathrm{CrI}}_{3}$, which is equivalent to external magnetic fields of up to about 60 T. Our results highlight the important impact of the twist angle and gating when employing magnetic vdW heterostructures in experimental geometries.
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