MoTe2超导异质结及约瑟夫森结的低温输运性质研究

MoTe₂是一种第二类拓扑外尔半金属，在温度小于100 mK时，可转变为超导体。然而，MoTe₂的超导能隙尚未在输运测量中被直接观测到。MoTe₂存在边界态超导现象，但是该边界态是否为高阶拓扑物态的一维拓扑铰链态，又或者其是否在超导相变温度之上依然存在，还有待进一步的研究。此外，MoTe₂还具有很强的自旋轨道耦合，且其晶格不具有中心反演对称性，因此非常有望基于MoTe₂超导约瑟夫森结实现显著的超导二极管效应。本文利用微纳结构加工技术制备了Nb-MoTe₂超导异质结以及Nb-MoTe₂-Nb约瑟夫森结，在低温及不同磁场条件下系统深入地研究了这些器件的量子输运性质，取得的主要研究成果如下：

在Nb-MoTe₂超导异质结中，通过超导邻近效应在MoTe₂中诱导产生了两个超导能隙 Δ_s和Δ_b  ，且能隙 Δ_s 的临界温度明显大于能隙Δ_b 。随着MoTe₂厚度的增加，能隙 Δ_s 减小得更快。此外，能隙Δ_b  的面内临界磁场与面外临界磁场的比值高达45，显示出强烈的各向异性。以上结果表明能隙 Δ_s和Δ_b 应分别来自MoTe₂的表面态和体态，而非之前μ子自旋弛豫和扫描隧道显微镜等工作所认为的s_+-双能隙超导。能隙 Δ_s的强各向异性及其随磁场的非单调变化还可能意味着非常规超导的出现。

在Nb-MoTe₂-Nb约瑟夫森结上发现仅在垂直磁场条件下即可实现非对称约瑟夫森效应，且其大小和符号可被外磁场有效的调节。通过对中心反演对称性破缺的MoTe₂点群的分析，我们发现随着MoTe₂样品厚度的增加，MoTe₂的点群会从C_1v变成C_2v。由于非对称约瑟夫森效应仅在MoTe₂较薄的样品上被观测到，可以将其归因于Edelstein效应。我们还基于Nb-MoTe₂-Nb约瑟夫森结进一步演示了对约瑟夫森超流的整流特性，也即超流的单向流动性，实现了高达50.4%的整流效率。

制备了超导电极覆盖MoTe₂薄片边缘的约瑟夫森结，并通过Dynes-Fulton方法分析了其超流的空间分布，发现约瑟夫森超流主要通过MoTe₂薄片的边缘传输。我们还在同一块MoTe₂薄片上进一步制备了超导电极接触和未接触样品边缘的两类约瑟夫森结器件，发现在同样的测量条件下，仅能在超导电极接触样品边缘的这一类器件上观测到约瑟夫森超流。这不仅直接证实了边缘态超流的存在，还排除了边缘态来自于费米弧表面态的可能性。我们认为其很大可能为理论预测的一维拓扑铰链态，从而为证明MoTe₂为二阶三维拓扑半金属提供了初步的实验证据。

总而言之，本论文的研究揭示了超导与拓扑半金属的耦合给第二类外尔半金属MoTe₂所带来的一系列新奇量子输运现象，找到了MoTe₂中存在一维铰链态的实验证据，还实现了极高整流效率的约瑟夫森超导二极管效应。不仅加深了人们对高阶拓扑物态量子输运性质的了解，并进一步展示了其在超导电子学方面的潜在应用。

Fu Liang and Kane has discovered that when an s-wave superconductor is in proximity to the surface state of a strong topological insulator, the composite structure can induce Majorana bound states at vortices. MoTe₂, as a type-II Weyl semimetal, has attracted broad interest in condensed matter physics, especially for its superconductivity below 100 mK. Experiments such as muon spin relaxation and scanning tunneling microscopy have suggested that superconducting MoTe₂ may exhibit s₊₋ pairing similar to that found in MgB₂ or iron-based superconductors. But up to now, the superconducting gap in MoTe₂ has not been directly observed in transport measurements. The edge state supercurrent has drawn widespread attention due to its potential relation to topological superconductivity or Majorana fermions. The Little-Parks experiment has revealed the existence of edge superconductivity in MoTe₂, but whether these edge states are one-dimensional topological hinge states or if they persist above the superconducting transition temperature remains to be clarified. Superconducting diode effect has become a hot topic in condensed matter physics and materials science. The strong spin-orbit coupling and the lack of inversion symmetry in MoTe₂ make it a prime candidate for realizing the superconducting diode effect, and exploring its mechanism is equally important. Addressing these issues, we have specially prepared Nb-MoTe₂ superconducting heterostructures and Nb-MoTe₂-Nb Josephson junctions using micro-nano fabrication techniques and systematically investigated the quantum transport properties of these devices at low temperatures and under various magnetic field conditions. The main outcomes are as follows:

In Nb-MoTe₂ heterostructures, two superconducting gaps Δ_s & Δ_b have been induced in MoTe₂ via the superconducting proximity effect. The gap Δ_s has a much higher critical temperature than Δ_b . As the thickness of the MoTe₂ flake increases, the gap Δ_b shrinks obviously. Besides, the ratio of the upper out-of-plane critical field to the in-plane one of Δ_s reaches up to 45, exhibiting very strong field anisotropy. All these lead us to believe that Δ_s & Δ_b arise from the surface and bulk states of MoTe₂, instead of the s₊₋ two-gap superconductivity reported previously. The strong anisotropy of Δ_s and its non-monotonic field dependence further suggest the emergence of unconventional superconductivity in the surface states of MoTe₂.

Asymmetric Josephson effect (AJE) is observed in perpendicular fields in Nb-MoTe₂-Nb Josephson junctions, with highly field-tunable magnitude and sign of the asymmetry. By careful examination of the structural symmetry of MoTe₂, it’s revealed that the point group will change from C_1v to C_2v as the flake thickness increases. Since the AJE is only observed in Josephson junctions with thin MoTe₂ flakes, it can be considered very likely that the Edelstein effect gives rise to the observed AJE. Based on this field-tunable AJE, we further demonstrate the efficient rectification of supercurrent in Nb-MoTe₂-Nb Josephson junctions, i.e, the supercurrent only flows in one direction, thus realizing the Josephson diode with the giant rectification efficiency of 50.4%.

We have prepared Josephson junctions with the superconducting electrodes covering the edges of the MoTe₂ flake. By analyzing the spatial distribution of the Josephson supercurrent with the Dynes-Fulton method, it’s found that the supercurrent mainly flows via the edges of the flake. We have also performed a comparative study of the edge-touched and -untouched Josephson junctions on the same MoTe₂ flake. Under the same measurement conditions, only the edge-touched device exhibits the Josephson supercurrent. This not only directly proves the existence of edge supercurrent in MoTe₂, but also rules out the possible contribution from the side surface states of MoTe₂. The one-dimensional hinge states are believed to be the most plausible source of the observed edge state, thus providing initial transport evidence for the 2^nd-order topological insulator phase in MoTe₂.

In summary, our study has revealed a series of exotic quantum transport phenomena due to the interplay between superconductivity and topology in MoTe_2. It not only deepens our understanding of the physical properties of higher-order topological materials, but also demonstrates the great application potential in superconducting electronics.

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