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"Hong-Jun, Gao"
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Spin-polarized oxygen evolution reaction under magnetic field
The oxygen evolution reaction (OER) is the bottleneck that limits the energy efficiency of water-splitting. The process involves four electrons’ transfer and the generation of triplet state O
2
from singlet state species (OH
-
or H
2
O). Recently, explicit spin selection was described as a possible way to promote OER in alkaline conditions, but the specific spin-polarized kinetics remains unclear. Here, we report that by using ferromagnetic ordered catalysts as the spin polarizer for spin selection under a constant magnetic field, the OER can be enhanced. However, it does not applicable to non-ferromagnetic catalysts. We found that the spin polarization occurs at the first electron transfer step in OER, where coherent spin exchange happens between the ferromagnetic catalyst and the adsorbed oxygen species with fast kinetics, under the principle of spin angular momentum conservation. In the next three electron transfer steps, as the adsorbed O species adopt fixed spin direction, the OER electrons need to follow the Hund rule and Pauling exclusion principle, thus to carry out spin polarization spontaneously and finally lead to the generation of triplet state O
2
. Here, we showcase spin-polarized kinetics of oxygen evolution reaction, which gives references in the understanding and design of spin-dependent catalysts.
Here, authors demonstrate the ferromagnetic catalyst to facilitate spin polarization in water oxidation reaction. They find the ferromagnetic-exchange-like behaviour between the ferromagnetic catalyst and the adsorbed oxygen species.
Journal Article
Evidence for Majorana bound states in an iron-based superconductor
The surface of the iron-based superconductor FeTe 0.55 Se 0.45 has been identified as a potential topological superconductor and is expected to host exotic quasiparticles called the Majorana bound states (MBSs). Wang et al. looked for signatures of MBSs in this material by using scanning tunneling spectroscopy on the vortex cores formed by the application of a magnetic field. In addition to conventional states, they observed the characteristic zero-bias peaks associated with MBSs and were able to distinguish between the two, owing to the favorable ratios of energy scales in the system. Science , this issue p. 333 Scanning tunneling spectroscopy reveals signatures of Majorana bound states on the surface of FeTe 1− x Se x . The search for Majorana bound states (MBSs) has been fueled by the prospect of using their non-Abelian statistics for robust quantum computation. Two-dimensional superconducting topological materials have been predicted to host MBSs as zero-energy modes in vortex cores. By using scanning tunneling spectroscopy on the superconducting Dirac surface state of the iron-based superconductor FeTe 0.55 Se 0.45 , we observed a sharp zero-bias peak inside a vortex core that does not split when moving away from the vortex center. The evolution of the peak under varying magnetic field, temperature, and tunneling barrier is consistent with the tunneling to a nearly pure MBS, separated from nontopological bound states. This observation offers a potential platform for realizing and manipulating MBSs at a relatively high temperature.
Journal Article
Spin pinning effect to reconstructed oxyhydroxide layer on ferromagnetic oxides for enhanced water oxidation
Producing hydrogen by water electrolysis suffers from the kinetic barriers in the oxygen evolution reaction (OER) that limits the overall efficiency. With spin-dependent kinetics in OER, to manipulate the spin ordering of ferromagnetic OER catalysts (e.g., by magnetization) can reduce the kinetic barrier. However, most active OER catalysts are not ferromagnetic, which makes the spin manipulation challenging. In this work, we report a strategy with spin pinning effect to make the spins in paramagnetic oxyhydroxides more aligned for higher intrinsic OER activity. The spin pinning effect is established in oxide
FM
/oxyhydroxide interface which is realized by a controlled surface reconstruction of ferromagnetic oxides. Under spin pinning, simple magnetization further increases the spin alignment and thus the OER activity, which validates the spin effect in rate-limiting OER step. The spin polarization in OER highly relies on oxyl radicals (O∙) created by 1
st
dehydrogenation to reduce the barrier for subsequent O-O coupling.
Water oxidation to triplet oxygen requires a spin polarization process for faster kinetics. Here, the authors show an interface spin pinning effect between ferromagnetic oxides and reconstructed oxyhydroxide surface layer, where the spin ordering in paramagnetic oxyhydroxide catalyst layer can be tuned to improve the intrinsic activity.
Journal Article
Anomalous thickness dependence of Curie temperature in air-stable two-dimensional ferromagnetic 1T-CrTe2 grown by chemical vapor deposition
The discovery of ferromagnetic two-dimensional van der Waals materials has opened up opportunities to explore intriguing physics and to develop innovative spintronic devices. However, controllable synthesis of these 2D ferromagnets and enhancing their stability under ambient conditions remain challenging. Here, we report chemical vapor deposition growth of air-stable 2D metallic 1T-CrTe
2
ultrathin crystals with controlled thickness. Their long-range ferromagnetic ordering is confirmed by a robust anomalous Hall effect, which has seldom been observed in other layered 2D materials grown by chemical vapor deposition. With reducing the thickness of 1T-CrTe
2
from tens of nanometers to several nanometers, the easy axis changes from in-plane to out-of-plane. Monotonic increase of Curie temperature with the thickness decreasing from ~130.0 to ~7.6 nm is observed. Theoretical calculations indicate that the weakening of the Coulomb screening in the two-dimensional limit plays a crucial role in the change of magnetic properties.
Here, the authors report chemical vapor deposition growth of metallic 1T-CrTe
2
ultrathin crystals with controlled thickness and long-range ferromagnetic ordering, and observe a monotonic increase of the Curie temperature with decreasing thickness.
Journal Article
Atomically sharp interface enabled ultrahigh-speed non-volatile memory devices
The development of high-performance memory devices has played a key role in the innovation of modern electronics. Non-volatile memory devices have manifested high capacity and mechanical reliability as a mainstream technology; however, their performance has been hampered by low extinction ratio and slow operational speed. Despite substantial efforts to improve these characteristics, typical write times of hundreds of micro- or milliseconds remain a few orders of magnitude longer than that of their volatile counterparts. Here we demonstrate non-volatile, floating-gate memory devices based on van der Waals heterostructures with atomically sharp interfaces between different functional elements, achieving ultrahigh-speed programming/erasing operations in the range of nanoseconds with extinction ratio up to 10
10
. This enhanced performance enables new device capabilities such as multi-bit storage, thus opening up applications in the realm of modern nanoelectronics and offering future fabrication guidelines for device scale up.
Atomically sharp interfaces in van der Waals heterostructures enable the realization of ultrafast non-volatile memory devices.
Journal Article
A new Majorana platform in an Fe-As bilayer superconductor
Iron-chalcogenide superconductors have emerged as a promising Majorana platform for topological quantum computation. By combining topological band and superconductivity in a single material, they provide significant advantage to realize isolated Majorana zero modes. However, iron-chalcogenide superconductors, especially Fe(Te,Se), suffer from strong inhomogeneity which may hamper their practical application. In addition, some iron-pnictide superconductors have been demonstrated to have topological surface states, yet no Majorana zero mode has been observed inside their vortices, raising a question of universality about this new Majorana platform. In this work, through angle-resolved photoemission spectroscopy and scanning tunneling microscopy/spectroscopy measurement, we identify Dirac surface states and Majorana zero modes, respectively, for the first time in an iron-pnictide superconductor, CaKFe
4
As
4
. More strikingly, the multiple vortex bound states with integer-quantization sequences can be accurately reproduced by our model calculation, firmly establishing Majorana nature of the zero mode.
Iron-pnictide superconductors share similar topological band structure with iron-chalcogenide superconductors, but no Majorana modes have been observed in the former. Here, the authors observe both the superconducting Dirac surface states and Majorana zero modes inside its vortex cores in CaKFe
4
As
4
.
Journal Article
Majorana zero modes in impurity-assisted vortex of LiFeAs superconductor
The iron-based superconductor is emerging as a promising platform for Majorana zero mode, which can be used to implement topological quantum computation. One of the most significant advances of this platform is the appearance of large vortex level spacing that strongly protects Majorana zero mode from other low-lying quasiparticles. Despite the advantages in the context of physics research, the inhomogeneity of various aspects hampers the practical construction of topological qubits in the compounds studied so far. Here we show that the stoichiometric superconductor LiFeAs is a good candidate to overcome this obstacle. By using scanning tunneling microscopy, we discover that the Majorana zero modes, which are absent on the natural clean surface, can appear in vortices influenced by native impurities. Our detailed analysis reveals a new mechanism for the emergence of those Majorana zero modes, i.e. native tuning of bulk Dirac fermions. The discovery of Majorana zero modes in this homogeneous material, with a promise of tunability, offers an ideal material platform for manipulating and braiding Majorana zero modes, pushing one step forward towards topological quantum computation.
Despite the discovery of Majorana zero modes (MZM) in iron-based superconductors, sample inhomogeneity may destroy MZMs during braiding. Here, authors observe MZM in impurity-assisted vortices due to tuning of the bulk Dirac fermions in a homogeneous superconductor LiFeAs.
Journal Article
The origin of magnetization-caused increment in water oxidation
Magnetization promoted activity of magnetic catalysts towards the oxygen evolution reaction (OER) has attracted great attention, but remains a puzzle where the increment comes from. Magnetization of a ferromagnetic material only changes its magnetic domain structure. It does not directly change the spin orientation of unpaired electrons in the material. The confusion is that each magnetic domain is a small magnet and theoretically the spin-polarization promoted OER already occurs on these magnetic domains, and thus the enhancement should have been achieved without magnetization. Here, we demonstrate that the enhancement comes from the disappeared domain wall upon magnetization. Magnetization leads to the evolution of the magnetic domain structure, from a multi-domain one to a single domain one, in which the domain wall disappears. The surface occupied by the domain wall is reformatted into one by a single domain, on which the OER follows the spin-facilitated pathways and thus the overall increment on the electrode occurs. This study fills the missing gap for understanding the spin-polarized OER and it further explains the type of ferromagnetic catalysts which can give increment by magnetization.
Magnetic field has been observed to promote oxygen evolution at some circumstance, however the reason for the enhancement remains unclear. Here, the authors show that enhancement is due to the disappearance of magnetic domain walls.
Journal Article
Localized spin-orbit polaron in magnetic Weyl semimetal Co3Sn2S2
The kagome lattice Co
3
Sn
2
S
2
exhibits the quintessential topological phenomena of a magnetic Weyl semimetal such as the chiral anomaly and Fermi-arc surface states. Probing its magnetic properties is crucial for understanding this correlated topological state. Here, using spin-polarized scanning tunneling microscopy/spectroscopy (STM/S) and non-contact atomic force microscopy (nc-AFM) combined with first-principle calculations, we report the discovery of localized spin-orbit polarons (SOPs) with three-fold rotation symmetry nucleated around single S-vacancies in Co
3
Sn
2
S
2.
The SOPs carry a magnetic moment and a large diamagnetic orbital magnetization of a possible topological origin associated relating to the diamagnetic circulating current around the S-vacancy. Appreciable magneto-elastic coupling of the SOP is detected by nc-AFM and STM. Our findings suggest that the SOPs can enhance magnetism and more robust time-reversal-symmetry-breaking topological phenomena. Controlled engineering of the SOPs may pave the way toward practical applications in functional quantum devices.
Kagome lattice material Co
3
Sn
2
S
2
is identified as a magnetic Weyl semimetal and its magnetic properties are less studied. Here, the authors observe localized spin-orbit polarons nucleated around single S-vacancies carrying a large diamagnetic orbital magnetism in Co
3
Sn
2
S
2
.
Journal Article