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1.
Nat Commun ; 15(1): 2881, 2024 Apr 03.
Article in English | MEDLINE | ID: mdl-38570519

ABSTRACT

Achieving spin-pinning at the interface of hetero-bilayer ferromagnet/antiferromagnet structures in conventional exchange bias systems can be challenging due to difficulties in interface control and the weakening of spin-pinning caused by poor interface quality. In this work, we propose an alternative approach to stabilize the exchange interaction at the interface of an uncompensated antiferromagnet by utilizing a gradient of interlayer exchange coupling. We demonstrate this exchange interaction through a designed field training protocol in the odd-layer topological antiferromagnet MnBi2Te4. Our results reveal a remarkable field-trained exchange bias of up to ~ 400 mT, which exhibits high repeatability and can be easily reset by a large training field. Notably, this field-trained exchange bias effect persists even with zero-field initialization, presenting a stark contrast to the traditional field-cooled exchange bias. The highly tunable exchange bias observed in this single antiferromagnet compound, without the need for an additional magnetic layer, provides valuable insight into the exchange interaction mechanism. These findings pave the way for the systematic design of topological antiferromagnetic spintronics.

2.
Phys Rev Lett ; 132(14): 146601, 2024 Apr 05.
Article in English | MEDLINE | ID: mdl-38640375

ABSTRACT

The layer-dependent Chern number (C) in MnBi_{2}Te_{4} is characterized by the presence of a Weyl semimetal state in the ferromagnetic coupling. However, the influence of a key factor, namely, the exchange coupling, remains unexplored. This study focuses on characterizing the C=2 state in MnBi_{2}Te_{4}, which is classified as a higher C state resulting from the anomalous n=0 Landau levels (LLs). Our findings demonstrate that the exchange coupling parameter strongly influences the formation of this Chern state, leading to a competition between the C=1 and 2 states. Moreover, the emergence of odd-even LL sequences, resulting from the breaking of LL degeneracy, provides compelling evidence for the strong exchange coupling strength. These findings highlight the significance of the exchange coupling in understanding the behavior of Chern states and LLs in magnetic quantum systems.

3.
Nat Commun ; 15(1): 3532, 2024 Apr 26.
Article in English | MEDLINE | ID: mdl-38670964

ABSTRACT

Dirac and Weyl semimetals are a central topic of contemporary condensed matter physics, and the discovery of new compounds with Dirac/Weyl electronic states is crucial to the advancement of topological materials and quantum technologies. Here we show a widely applicable strategy that uses high configuration entropy to engineer relativistic electronic states. We take the AMnSb2 (A = Ba, Sr, Ca, Eu, and Yb) Dirac material family as an example and demonstrate that mixing of Ba, Sr, Ca, Eu and Yb at the A site generates the compound (Ba0.38Sr0.14Ca0.16Eu0.16Yb0.16)MnSb2 (denoted as A5MnSb2), giving access to a polar structure with a space group that is not present in any of the parent compounds. A5MnSb2 is an entropy-stabilized phase that preserves its linear band dispersion despite considerable lattice disorder. Although both A5MnSb2 and AMnSb2 have quasi-two-dimensional crystal structures, the two-dimensional Dirac states in the pristine AMnSb2 evolve into a highly anisotropic quasi-three-dimensional Dirac state triggered by local structure distortions in the high-entropy phase, which is revealed by Shubnikov-de Haas oscillations measurements.

4.
Nat Commun ; 14(1): 4805, 2023 Aug 09.
Article in English | MEDLINE | ID: mdl-37558682

ABSTRACT

The intrinsic magnetic topological insulator, Mn(Bi1-xSbx)2Te4, has been identified as a Weyl semimetal with a single pair of Weyl nodes in its spin-aligned strong-field configuration. A direct consequence of the Weyl state is the layer dependent Chern number, [Formula: see text]. Previous reports in MnBi2Te4 thin films have shown higher [Formula: see text] states either by increasing the film thickness or controlling the chemical potential. A clear picture of the higher Chern states is still lacking as data interpretation is further complicated by the emergence of surface-band Landau levels under magnetic fields. Here, we report a tunable layer-dependent [Formula: see text] = 1 state with Sb substitution by performing a detailed analysis of the quantization states in Mn(Bi1-xSbx)2Te4 dual-gated devices-consistent with calculations of the bulk Weyl point separation in the doped thin films. The observed Hall quantization plateaus for our thicker Mn(Bi1-xSbx)2Te4 films under strong magnetic fields can be interpreted by a theory of surface and bulk spin-polarised Landau level spectra in thin film magnetic topological insulators.

5.
ACS Nano ; 17(11): 9694-9747, 2023 Jun 13.
Article in English | MEDLINE | ID: mdl-37219929

ABSTRACT

Two-dimensional (2D) material research is rapidly evolving to broaden the spectrum of emergent 2D systems. Here, we review recent advances in the theory, synthesis, characterization, device, and quantum physics of 2D materials and their heterostructures. First, we shed insight into modeling of defects and intercalants, focusing on their formation pathways and strategic functionalities. We also review machine learning for synthesis and sensing applications of 2D materials. In addition, we highlight important development in the synthesis, processing, and characterization of various 2D materials (e.g., MXnenes, magnetic compounds, epitaxial layers, low-symmetry crystals, etc.) and discuss oxidation and strain gradient engineering in 2D materials. Next, we discuss the optical and phonon properties of 2D materials controlled by material inhomogeneity and give examples of multidimensional imaging and biosensing equipped with machine learning analysis based on 2D platforms. We then provide updates on mix-dimensional heterostructures using 2D building blocks for next-generation logic/memory devices and the quantum anomalous Hall devices of high-quality magnetic topological insulators, followed by advances in small twist-angle homojunctions and their exciting quantum transport. Finally, we provide the perspectives and future work on several topics mentioned in this review.

6.
Nat Commun ; 14(1): 364, 2023 Jan 23.
Article in English | MEDLINE | ID: mdl-36690617

ABSTRACT

Nonlinear Hall effect (NLHE) is a new type of Hall effect with wide application prospects. Practical device applications require strong NLHE at room temperature (RT). However, previously reported NLHEs are all low-temperature phenomena except for the surface NLHE of TaIrTe4. Bulk RT NLHE is highly desired due to its ability to generate large photocurrent. Here, we show the spin-valley locked Dirac state in BaMnSb2 can generate a strong bulk NLHE at RT. In the microscale devices, we observe the typical signature of an intrinsic NLHE, i.e. the transverse Hall voltage quadratically scales with the longitudinal current as the current is applied to the Berry curvature dipole direction. Furthermore, we also demonstrate our nonlinear Hall device's functionality in wireless microwave detection and frequency doubling. These findings broaden the coupled spin and valley physics from 2D systems into a 3D system and lay a foundation for exploring bulk NLHE's applications.


Subject(s)
Cold Temperature , Fruit , Temperature , Microwaves , Physics
7.
Adv Mater ; 35(11): e2208994, 2023 Mar.
Article in English | MEDLINE | ID: mdl-36566084

ABSTRACT

Thermoelectric (TE) generators enable the direct and reversible conversion between heat and electricity, providing applications in both refrigeration and power generation. In the last decade, several TE materials with relatively high figures of merit (zT) have been reported in the low- and high-temperature regimes. However, there is an urgent demand for high-performance TE materials working in the mid-temperature range (400-700 K). Herein, p-type AgSbTe2 materials stabilized with S and Se co-doping are demonstrated to exhibit an outstanding maximum figure of merit (zTmax ) of 2.3 at 673 K and an average figure of merit (zTave ) of 1.59 over the wide temperature range of 300-673 K. This exceptional performance arises from an enhanced carrier density resulting from a higher concentration of silver vacancies, a vastly improved Seebeck coefficient enabled by the flattening of the valence band maximum and the inhibited formation of n-type Ag2 Te, and ahighly improved stability beyond 673 K. The optimized material is used to fabricate a single-leg device with efficiencies up to 13.3% and a unicouple TE device reaching energy conversion efficiencies up to 12.3% at a temperature difference of 370 K. These results highlight an effective strategy to engineer high-performance TE material in the mid-temperature range.

8.
Adv Mater ; 34(49): e2202841, 2022 Dec.
Article in English | MEDLINE | ID: mdl-36189841

ABSTRACT

Magnetism in topological materials creates phases exhibiting quantized transport phenomena with potential technological applications. The emergence of such phases relies on strong interaction between localized spins and the topological bands, and the consequent formation of an exchange gap. However, this remains experimentally unquantified in intrinsic magnetic topological materials. Here, this interaction is quantified in MnBi2 Te4 , a topological insulator with intrinsic antiferromagnetism. This is achieved by optically exciting Bi-Te p states comprising the bulk topological bands and interrogating the consequent Mn 3d spin dynamics, using a multimodal ultrafast approach. Ultrafast electron scattering and magneto-optic measurements show that the p states demagnetize via electron-phonon scattering at picosecond timescales. Despite being energetically decoupled from the optical excitation, the Mn 3d spins, probed by resonant X-ray scattering, are observed to disorder concurrently with the p spins. Together with atomistic simulations, this reveals that the exchange coupling between localized spins and the topological bands is at least 100 times larger than the superexchange interaction, implying an optimal exchange gap of at least 25 meV in the surface states. By quantifying this exchange coupling, this study validates the materials-by-design strategy of utilizing localized magnetic order to manipulate topological phases, spanning static to ultrafast timescales.

9.
Sci Adv ; 8(43): eadd6169, 2022 Oct 28.
Article in English | MEDLINE | ID: mdl-36288317

ABSTRACT

Metals are canonical plasmonic media at infrared and optical wavelengths, allowing one to guide and manipulate light at the nanoscale. A special form of optical waveguiding is afforded by highly anisotropic crystals revealing the opposite signs of the dielectric functions along orthogonal directions. These media are classified as hyperbolic and include crystalline insulators, semiconductors, and artificial metamaterials. Layered anisotropic metals are also anticipated to support hyperbolic waveguiding. However, this behavior remains elusive, primarily because interband losses arrest the propagation of infrared modes. Here, we report on the observation of propagating hyperbolic waves in a prototypical layered nodal-line semimetal ZrSiSe. The observed waveguiding originates from polaritonic hybridization between near-infrared light and nodal-line plasmons. Unique nodal electronic structures simultaneously suppress interband loss and boost the plasmonic response, ultimately enabling the propagation of infrared modes through the bulk of the crystal.

10.
Nat Commun ; 13(1): 1929, 2022 Apr 08.
Article in English | MEDLINE | ID: mdl-35396393

ABSTRACT

The emergence of magnetism in quantum materials creates a platform to realize spin-based applications in spintronics, magnetic memory, and quantum information science. A key to unlocking new functionalities in these materials is the discovery of tunable coupling between spins and other microscopic degrees of freedom. We present evidence for interlayer magnetophononic coupling in the layered magnetic topological insulator MnBi2Te4. Employing magneto-Raman spectroscopy, we observe anomalies in phonon scattering intensities across magnetic field-driven phase transitions, despite the absence of discernible static structural changes. This behavior is a consequence of a magnetophononic wave-mixing process that allows for the excitation of zone-boundary phonons that are otherwise 'forbidden' by momentum conservation. Our microscopic model based on density functional theory calculations reveals that this phenomenon can be attributed to phonons modulating the interlayer exchange coupling. Moreover, signatures of magnetophononic coupling are also observed in the time domain through the ultrafast excitation and detection of coherent phonons across magnetic transitions. In light of the intimate connection between magnetism and topology in MnBi2Te4, the magnetophononic coupling represents an important step towards coherent on-demand manipulation of magnetic topological phases.

11.
Rev Sci Instrum ; 92(11): 113907, 2021 Nov 01.
Article in English | MEDLINE | ID: mdl-34852521

ABSTRACT

We present the development of a multi-resolution photoemission spectroscopy (MRPES) setup, which probes quantum materials in energy, momentum, space, and time. This versatile setup integrates three light sources in one photoemission setup and can conveniently switch between traditional angle-resolved photoemission spectroscopy (ARPES), time-resolved ARPES (trARPES), and micrometer-scale spatially resolved ARPES. It provides a first-time all-in-one solution to achieve an energy resolution of <4 meV, a time resolution of <35 fs, and a spatial resolution of ∼10 µm in photoemission spectroscopy. Remarkably, we obtain the shortest time resolution among the trARPES setups using solid-state nonlinear crystals for frequency upconversion. Furthermore, this MRPES setup is integrated with a shadow-mask assisted molecular beam epitaxy system, which transforms the traditional photoemission spectroscopy into a quantum device characterization instrument. We demonstrate the functionalities of this novel quantum material testbed using FeSe/SrTiO3 thin films and MnBi4Te7 magnetic topological insulators.

12.
Nat Commun ; 11(1): 3056, 2020 Jun 16.
Article in English | MEDLINE | ID: mdl-32546839

ABSTRACT

A state of matter with a multi-component order parameter can give rise to vestigial order. In the vestigial phase, the primary order is only partially melted, leaving a remaining symmetry breaking behind, an effect driven by strong classical or quantum fluctuations. Vestigial states due to primary spin and charge-density-wave order have been discussed in iron-based and cuprate materials. Here we present the observation of a partially melted superconductivity in which pairing fluctuations condense at a separate phase transition and form a nematic state with broken Z3, i.e., three-state Potts-model symmetry. Thermal expansion, specific heat and magnetization measurements of the doped topological insulators NbxBi2Se3 and CuxBi2Se3 reveal that this symmetry breaking occurs at [Formula: see text] above [Formula: see text], along with an onset of superconducting fluctuations. Thus, before Cooper pairs establish long-range coherence at Tc, they fluctuate in a way that breaks the rotational invariance at Tnem and induces a crystalline distortion.

13.
Inorg Chem ; 55(5): 2114-22, 2016 Mar 07.
Article in English | MEDLINE | ID: mdl-26890202

ABSTRACT

A new ternary compound with composition Cu5Sn2Te7 has been synthesized using the stoichiometric reaction of Cu, Sn, and Te. The compound crystallizes in C2 space group with unit cell parameters of a = 13.549(2) Å, b = 6.0521(11) Å, c = 9.568(2) Å, and ß = 98.121(2)°. Cu5Sn2Te7 is a superstructure of sphalerite and exhibits tetrahedral coordination of Cu, Sn, and Te atoms, containing a unique adamantane-like arrangement. The compound is formally mixed valent with a high electrical conductivity of 9.8 × 10(5) S m(-1) at 300 K and exhibits metallic behavior having p-type charge carriers as indicated from the positive Seebeck coefficient. Hall effect measurements further confirm holes as charge carriers with a carrier density of 1.39 × 10(21) cm(-3) and Hall mobility of 4.5 cm(2) V(-1) s(-1) at 300 K. The electronic band structure calculations indicate the presence of a finite density of states around the Fermi level and agree well with the p-type metallic conductivity. Band structure analysis suggests that the effective mass of the hole state is small and could be responsible for high electronic conductivity and Hall mobility. The high thermal conductivity of 15.1 W m(-1) K(-1) at 300 K coupled with the low Seebeck coefficient results in a poor thermoelectric figure of merit (ZT) for this compound. Theoretical calculations indicate that if Cu5Sn2Te7 is turned into a valence precise compound by substituting one Cu by a Zn, a semiconducting material, Cu4ZnSn2Te7, with a direct band gap of ∼ 0.5 eV can be obtained.

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