Optically Active Single Hole Spin in ZnSe

IF 9.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Amirehsan Alizadehherfati,Yuxi Jiang,Kelsey J. Mirrielees,Nils von den Driesch,Christine Falter,Yurii Kutovyi,Amirehsan Boreiri,Douglas L. Irving,Alexander Pawlis,Edo Waks
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Abstract

Semiconductor hole spins offer a pathway to extended coherence times by decoupling from nuclear magnetic noise, while their spin–orbit coupling enables fast all-electrical control. In ZnSe, however, realizing this potential has been limited by p-doping challenges. Here, we circumvent this limit by optically activating acceptors and demonstrate optical spin initialization. We isolate a single-hole spin bound to a shallow acceptor, confirmed by antibunching and accessed via the fast (244 ps) radiative recombination of a bound exciton. Magnetic and Raman spectroscopy reveal a spin-selective Λ system with an effective hole g-factor of 0.7 and an optical line width of 26.7 GHz. Time-resolved measurements reveal optical pumping of the hole spin with an estimated initialization fidelity of 90.7%. First-principles simulations combined with the experiment identify nitrogen as the most likely acceptor impurity. These results introduce a promising new platform for optically active spin qubits and single-photon sources in ZnSe.

Abstract Image

ZnSe中光活性单孔自旋
半导体空穴自旋通过从核磁噪声中解耦提供了延长相干时间的途径,而它们的自旋轨道耦合实现了快速的全电控制。然而,在ZnSe中,实现这一潜力受到p掺杂挑战的限制。在这里,我们通过光激活受体并演示光自旋初始化来绕过这一限制。我们分离了一个单孔自旋束缚在一个浅受体上,通过反聚束确认,并通过一个束缚激子的快速(244ps)辐射重组获得。磁谱和拉曼光谱结果表明,该系统具有自旋选择性,有效空穴g因子为0.7,光谱线宽为26.7 GHz。时间分辨的测量结果显示,光抽运的空穴自旋估计初始保真度为90.7%。第一性原理模拟与实验相结合,确定氮是最可能的受体杂质。这些结果为ZnSe的光学活性自旋量子比特和单光子源提供了一个有前途的新平台。
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来源期刊
Nano Letters
Nano Letters 工程技术-材料科学:综合
CiteScore
16.80
自引率
2.80%
发文量
1182
审稿时长
1.4 months
期刊介绍: Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.
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