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1.
ACS Nano ; 18(26): 16684-16691, 2024 Jul 02.
Article in English | MEDLINE | ID: mdl-38885639

ABSTRACT

Recently, there has been significant interest in topological nodal-line semimetals due to their linear energy dispersion with one-dimensional nodal lines or loops. These materials exhibit fascinating physical properties, such as drumhead surface states and 3D anisotropic nodal-line structures. Similar to Weyl semimetals, type-II nodal-line semimetals have two crossing bands that are both electron-like or hole-like along a certain direction. However, the direct observation of type-II nodal-line Fermions has been challenging due to the lack of suitable material platforms and the low density of states. Here we present experimental evidence for the coexistence of both type-I and type-II nodal-line Fermions in ZrSiSe, which was obtained through magneto-optical and angle-resolved photoemission spectroscopy (ARPES) measurements. Our density functional theory calculations predict that the type-II nodal-line structure can be developed in the Z-R line of the first Brillouin zone based on the lattice constants of the grown single crystal. Indeed, ARPES measurements reveal the type-II nodal-line band structure. The extracted type-II Landau level transitions from magneto-optical measurements exhibit good agreement with the calculated type-II energy dispersion model based on the band structure. Our experimental results demonstrate that ZrSiSe possesses two types of nodal-line Fermions, distinguishing it from other ZrSiX (X = S, Te) materials and positioning it as an ideal platform for investigating type-II nodal-line semimetals.

2.
Nano Lett ; 24(17): 5125-5131, 2024 May 01.
Article in English | MEDLINE | ID: mdl-38639405

ABSTRACT

We report a study of thickness-dependent interband and intraband magnetic breakdown by thermoelectric quantum oscillations in ZrSiSe nanoplates. Under high magnetic fields of up to 30 T, quantum oscillations arising from degenerated hole pockets were observed in thick ZrSiSe nanoplates. However, when decreasing the thickness, plentiful multifrequency quantum oscillations originating from hole and electron pockets are captured. These multiple frequencies can be explained by the emergent interband magnetic breakdown enclosing individual hole and electron pockets and intraband magnetic breakdown within spin-orbit coupling (SOC) induced saddle-shaped electron pockets, resulting in the enhanced contribution to thermal transport in thin ZrSiSe nanoplates. These experimental frequencies agree well with theoretical calculations of the intriguing tunneling processes. Our results introduce a new member of magnetic breakdown to the field and open up a dimension for modulating magnetic breakdown, which holds fundamental significance for both low-dimensional topological materials and the physics of magnetic breakdown.

3.
J Phys Condens Matter ; 36(12)2023 Dec 15.
Article in English | MEDLINE | ID: mdl-38056011

ABSTRACT

Using angle-resolved photoemission spectroscopy (ARPES) and density functional theory (DFT) calculations, we systematically studied the electronic band structure of Mn3Ge in the vicinity of the Fermi level. We observe several bands crossing the Fermi level, confirming the metallic nature of the studied system. We further observe several flat bands along various high symmetry directions, consistent with the DFT calculations. The calculated partial density of states suggests a dominant Mn 3dorbital contribution to the total valence band DOS. With the help of orbital-resolved band structure calculations, we qualitatively identify the orbital information of the experimentally obtained band dispersions. Out-of-plane electronic band dispersions are explored by measuring the ARPES data at various photon energies. Importantly, our study suggests relatively weaker electronic correlations in Mn3Ge compared to Mn3Sn.

4.
Nat Commun ; 14(1): 6210, 2023 Oct 05.
Article in English | MEDLINE | ID: mdl-37798279

ABSTRACT

Correlated electron materials (CEMs) host a rich variety of condensed matter phases. Vanadium dioxide (VO2) is a prototypical CEM with a temperature-dependent metal-to-insulator (MIT) transition with a concomitant crystal symmetry change. External control of MIT in VO2-especially without inducing structural changes-has been a long-standing challenge. In this work, we design and synthesize modulation-doped VO2-based thin film heterostructures that closely emulate a textbook example of filling control in a correlated electron insulator. Using a combination of charge transport, hard X-ray photoelectron spectroscopy, and structural characterization, we show that the insulating state can be doped to achieve carrier densities greater than 5 × 1021 cm-3 without inducing any measurable structural changes. We find that the MIT temperature (TMIT) continuously decreases with increasing carrier concentration. Remarkably, the insulating state is robust even at doping concentrations as high as ~0.2 e-/vanadium. Finally, our work reveals modulation-doping as a viable method for electronic control of phase transitions in correlated electron oxides with the potential for use in future devices based on electric-field controlled phase transitions.

5.
Nano Lett ; 23(19): 9026-9033, 2023 Oct 11.
Article in English | MEDLINE | ID: mdl-37767914

ABSTRACT

The quantum Hall effect is one of the exclusive properties displayed by Dirac Fermions in topological insulators, which propagates along the chiral edge state and gives rise to quantized electron transport. However, the quantum Hall effect formed by the nondegenerate Dirac surface states has been elusive so far. Here, we demonstrate the nondegenerate integer quantum Hall effect from the topological surface states in three-dimensional (3D) topological insulator ß-Ag2Te nanostructures. Surface-state dominant conductance renders quantum Hall conductance plateaus with a step of e2/h, along with typical thermopower behaviors of two-dimensional (2D) massless Dirac electrons. The 2D nature of the topological surface states is proven by the electrical and thermal transport responses under tilted magnetic fields. Moreover, the degeneracy of the surface states is removed by structure inversion asymmetry (SIA). The evidenced SIA-induced nondegenerate integer quantum Hall effect in low-symmetry ß-Ag2Te has implications for both fundamental study and the realization of topological magneto-electric effects.

6.
Dalton Trans ; 52(32): 11335-11348, 2023 Aug 15.
Article in English | MEDLINE | ID: mdl-37530419

ABSTRACT

A series of mononuclear manganese(III) complexes [Mn(X-sal2-323)](ReO4) (X = 5 Cl, 1; X = 5 Br, 2; X = 3,5 Cl, 3; X = 3,5 Br, 4; and X = 5 NO2, 5), containing hexadentate ligands prepared using the condensation of N,N'-bis(3-aminopropyl)ethylenediamine and 5- or 3,5-substituted salicylaldehyde, has been synthesized. Variable temperature single-crystal X-ray diffraction, magnetic, spectroscopic, electrochemical, and spectroelectrochemical analyses, and theoretical calculations have been used to explore the role of various ligand substituents in the spin-state switching behavior of the prepared manganese(III) complexes. All five complexes consist of an analogous distorted octahedral monocationic MnN4O2 surrounding offered by the flexible hexadentate ligand and ReO4- as the counter anion. However, a disordered water molecule was detected in complex 4. Complexes 1 (X = 5 Cl) and 5 (X = 5 NO2) show gradual and complete spin-state switching between the high-spin (HS) (S = 2) and the low-spin (LS) (S = 1) state with T1/2 values of 146 and 115 K respectively, while an abrupt and complete transition at 95 K was observed for complex 2 (X = 5 Br). Alternatively, complex 3 (X = 3, 5 Cl) exhibits an incomplete and sharp transition between the HS and LS states at 104 K, while complex 4 (X = 3, 5 Br) (desolvated) remains almost LS up to 300 K and then displays gradual and incomplete SCO at a higher temperature. The nature of the spin-state switch and transition temperature suggest that the structural effect (cooperativity) plays a more significant role in comparison with the electronic effect coming from various substituents (Cl, Br, and NO2), which is further supported by the detailed structural, electrochemical, and theoretical studies.

7.
J Phys Condens Matter ; 35(48)2023 Sep 06.
Article in English | MEDLINE | ID: mdl-37595610

ABSTRACT

Rashba spin-orbit coupled systems are an important class of materials noted for diverse fundamental and applied phenomena. Recently, the emergence of non-linear Hall effect under conditions of time-reversal symmetry has been discovered in materials with broken inversion symmetry. In this work, we study the second- and third-order Hall response in Rashba systems with hexagonal warping. Starting with a low-energy model, we obtain the analytic expressions and discover the unique dipole profile in Rashba systems with hexagonal warping. Furthermore, we extend the analysis using a realistic tight-binding model. Next, we predict the existence of a third-order Hall effect in these systems, and calculate the Berry connection polarizability tensor analytically. We also show how the model parameters affect the third-order conductivity. Our predictions can help in the experimental realization of Berry curvature multipole physics in Rashba materials with hexagonal warping, and provide a new platform for engineering the non-linear Hall effects.

8.
Proc Natl Acad Sci U S A ; 120(25): e2302572120, 2023 Jun 20.
Article in English | MEDLINE | ID: mdl-37307466

ABSTRACT

Non-Hermitian systems have been widely explored in platforms ranging from photonics to electric circuits. A defining feature of non-Hermitian systems is exceptional points (EPs), where both eigenvalues and eigenvectors coalesce. Tropical geometry is an emerging field of mathematics at the interface between algebraic geometry and polyhedral geometry, with diverse applications to science. Here, we introduce and develop a unified tropical geometric framework to characterize different facets of non-Hermitian systems. We illustrate the versatility of our approach using several examples and demonstrate that it can be used to select from a spectrum of higher-order EPs in gain and loss models, predict the skin effect in the non-Hermitian Su-Schrieffer-Heeger model, and extract universal properties in the presence of disorder in the Hatano-Nelson model. Our work puts forth a framework for studying non-Hermitian physics and unveils a connection of tropical geometry to this field.

9.
J Phys Condens Matter ; 35(33)2023 May 18.
Article in English | MEDLINE | ID: mdl-37130523

ABSTRACT

The synergy between non-Hermitian concepts and topological ideas have led to very fruitful activity in the recent years. Their interplay has resulted in a wide variety of new non-Hermitian topological phenomena being discovered. In this review, we present the key principles underpinning the topological features of non-Hermitian phases. Using paradigmatic models-Hatano-Nelson, non-Hermitian Su-Schrieffer-Heeger and non-Hermitian Chern insulator-we illustrate the central features of non-Hermitian topological systems, including exceptional points, complex energy gaps and non-Hermitian symmetry classification. We discuss the non-Hermitian skin effect and the notion of the generalized Brillouin zone, which allows restoring the bulk-boundary correspondence. Using concrete examples, we examine the role of disorder, describe the Floquet engineering, present the linear response framework, and analyze the Hall transport properties of non-Hermitian topological systems. We also survey the rapidly growing experimental advances in this field. Finally, we end by highlighting possible directions which, in our view, may be promising for explorations in the near future.

10.
Adv Sci (Weinh) ; 10(20): e2300413, 2023 Jul.
Article in English | MEDLINE | ID: mdl-37116118

ABSTRACT

Photodetector based on two-dimensional (2D) materials is an ongoing quest in optoelectronics. 2D photodetectors are generally efficient at low illuminating power but suffer severe recombination processes at high power, which results in the sublinear power-dependent photoresponse and lower optoelectronic efficiency. The desirable superlinear photocurrent is mostly achieved by sophisticated 2D heterostructures or device arrays, while 2D materials rarely show intrinsic superlinear photoresponse. This work reports the giant superlinear power dependence of photocurrent based on multilayer Ta2 NiS5 . While the fabricated photodetector exhibits good sensitivity (3.1 mS W-1 per □) and fast photoresponse (31 µs), the bias-, polarization-, and spatial-resolved measurements point to an intrinsic photoconductive mechanism. By increasing the incident power density from 1.5 to 200 µW µm-2 , the photocurrent power dependence varies from sublinear to superlinear. At higher illuminating conditions, prominent superlinearity is observed with a giant power exponent of γ = 1.5. The unusual photoresponse can be explained by a two-recombination-center model where density of states of the recombination centers (RC) effectively closes all recombination channels. The photodetector is integrated into camera for taking photos with enhanced contrast due to superlinearity. This work provides an effective route to enable higher optoelectronic efficiency at extreme conditions.

11.
Natl Sci Rev ; 9(6): nwab117, 2022 Jun.
Article in English | MEDLINE | ID: mdl-35822066

ABSTRACT

Two-dimensional (2D) ferromagnetic materials have been discovered with tunable magnetism and orbital-driven nodal-line features. Controlling the 2D magnetism in exfoliated nanoflakes via electric/magnetic fields enables a boosted Curie temperature (T C) or phase transitions. One of the challenges, however, is the realization of high T C 2D magnets that are tunable, robust and suitable for large scale fabrication. Here, we report molecular-beam epitaxy growth of wafer-scale Fe3+XGeTe2 films with T C above room temperature. By controlling the Fe composition in Fe3+XGeTe2, a continuously modulated T C in a broad range of 185-320 K has been achieved. This widely tunable T C is attributed to the doped interlayer Fe that provides a 40% enhancement around the optimal composition X = 2. We further fabricated magnetic tunneling junction device arrays that exhibit clear tunneling signals. Our results show an effective and reliable approach, i.e. element doping, to producing robust and tunable ferromagnetism beyond room temperature in a large-scale 2D Fe3+XGeTe2 fashion.

12.
J Phys Condens Matter ; 34(38)2022 Jul 22.
Article in English | MEDLINE | ID: mdl-35820408

ABSTRACT

In the presence of time reversal symmetry, a non-linear Hall effect can occur in systems without an inversion symmetry. One of the prominent candidates for detection of such Hall signals are Weyl semimetals. In this article, we investigate the Berry curvature induced second and third order Hall effect in multi-Weyl semimetals with topological chargesn=1,2,3. We use low energy effective models to obtain general analytical expressions and discover the presence of a large Berry curvature dipole (BCD) in multi-Weyl semimetals, compared to usual (n = 1) Weyl semimetals. We also study the BCD in a realistic tight-binding lattice model and observe two different kinds of variation with increasing topological charge-these can be attributed to different underlying Berry curvature components. We provide estimates of the signatures of second harmonic of Hall signal in multi-Weyl semimetals, which can be detected experimentally. Furthermore, we predict the existence of a third order Hall signal in multi-Weyl semimetals. We derive the analytical expressions of Berry connection polarizability tensor, which is responsible for third order effects, using a low energy model and estimate the measurable conductivity. Our work can help guide experimental discovery of Berry curvature multipole physics in multi-Weyl semimetals.

13.
J Phys Condens Matter ; 33(46)2021 Sep 02.
Article in English | MEDLINE | ID: mdl-34399421

ABSTRACT

Recently discovered 2M phase of bulk WS2was observed to exhibit superconductivity with a critical temperature of 8.8 K, the highest reported among superconducting transition metal dichalcogenides. Also predicted to support protected surface states, it could be a potential topological superconductor. In the present study, we perform a detailed first-principles analysis of bulk and bilayer 2M WS2. We report a comprehensive investigation of the bulk phase, comparing structural and electronic properties obtained from different exchange correlation functionals to the experimentally reported values. By calculation of theZ2invariant and surface states, we give support for its non-trivial band nature. Based on the insights gained from the analysis of the bulk phase, we predict bilayer 2M WS2as a new two-dimensional topological material. We demonstrate its dynamical stability from first-principles phonon computations and present its electronic properties, highlighting the band inversions between the Wdand Spstates. By means ofZ2invariant computations and a calculation of the edge states, we show that bilayer 2M WS2exhibits protected, robust edge states. The broken inversion symmetry in this newly proposed bilayer also leads to the presence of Berry curvature dipole and resulting non-linear responses. We compute the Berry curvature distribution and the dipole as a function of Fermi energy. We propose that Berry curvature dipole signals, which are absent in the centrosymmetric bulk 2M WS2, can be signatures of the bilayer. We hope our predictions lead to the experimental realization of this as-yet-undiscovered two-dimensional topological material.

14.
J Phys Condens Matter ; 33(37)2021 Jul 15.
Article in English | MEDLINE | ID: mdl-34186528

ABSTRACT

Multifold fermion systems feature free fermionic excitations, which have no counterparts in high-energy physics, and exhibit several unconventional properties. Using first-principles calculations, we predict that strain engineering can be used to control the distribution of topological charges in transition metal silicide candidate CoSi, hosting multifold fermions. We demonstrate that breaking the rotational symmetry of the system, by choosing a suitable strain, destroys the multifold fermions, and at the same time results in the creation of Weyl points. We introduce a low energy effective model to complement the results obtained from density functional calculations. Our findings suggest that strain-engineering is a useful approach to tune topological properties of multifold fermions.

15.
J Phys Condens Matter ; 33(22)2021 May 05.
Article in English | MEDLINE | ID: mdl-33601357

ABSTRACT

Recently, many novel and exotic phases have been proposed by considering the role of topology in non-Hermitian systems, and their emergent properties are of wide current interest. In this work we propose the non-Hermitian generalization of semi-Dirac semimetals, which feature a linear dispersion along one momentum direction and a quadratic one along the other. We study the topological phase transitions in such two-dimensional semi-Dirac semimetals in the presence of a particle gain-and-loss term. We show that such a non-Hermitian term creates exceptional points (EPs) originating out of each semi-Dirac point. We map out the topological phase diagram of our model, using winding number and vorticity as topological invariants of the system. By means of numerical and analytical calculations, we examine the nature of edge states for different types of semi-Dirac models and establish bulk-boundary correspondence and absence of the non-Hermitian skin effect, in one class. On the other hand, for other classes of semi-Dirac models with asymmetric hopping, we restore the non-Hermitian skin effect, an anomalous feature usually present in non-Hermitian topological systems.

16.
Natl Sci Rev ; 7(9): 1468-1475, 2020 Sep.
Article in English | MEDLINE | ID: mdl-34691543

ABSTRACT

WTe2, as a type-II Weyl semimetal, has 2D Fermi arcs on the (001) surface in the bulk and 1D helical edge states in its monolayer. These features have recently attracted wide attention in condensed matter physics. However, in the intermediate regime between the bulk and monolayer, the edge states have not been resolved owing to its closed band gap which makes the bulk states dominant. Here, we report the signatures of the edge superconductivity by superconducting quantum interference measurements in multilayer WTe2 Josephson junctions and we directly map the localized supercurrent. In thick WTe2 ([Formula: see text], the supercurrent is uniformly distributed by bulk states with symmetric Josephson effect ([Formula: see text]). In thin WTe2 (10 nm), however, the supercurrent becomes confined to the edge and its width reaches up to [Formula: see text]and exhibits non-symmetric behavior [Formula: see text]. The ability to tune the edge domination by changing thickness and the edge superconductivity establishes WTe2 as a promising topological system with exotic quantum phases and a rich physics.

17.
J Phys Condens Matter ; 32(12): 125501, 2020 Mar 20.
Article in English | MEDLINE | ID: mdl-31751959

ABSTRACT

We systematically investigate the effect of strain and doping on the polar metal phase in lithium osmate, LiOsO3, using first-principles calculations. We demonstrate that the polar metal phase in LiOsO3 can be controlled by biaxial strain. Based on density functional calculations, we show that a compressive biaxial strain enhances the stability of the polar R3c phase. On the other hand, a tensile biaxial strain favors the centrosymmetric [Formula: see text] structure. Thus, strain emerges as a promising control parameter over polar metallicity in this material. We uncover a strain-driven quantum phase transition under tensile strain, and highlight intriguing properties that could emerge in the vicinity of this polar to non-polar metal transition. We examine the effect of charge doping on the polar metal phase. By means of electrostatic doping as well as supercell calculations, we find that screening from additional charge carriers, expected to suppress the polar distortions, have only a small effect on them. Rather remarkably, and in contrast to conventional ferroelectrics, the polar metal phase in LiOsO3 remains robust against charge doping up to large doping values.

18.
Nat Mater ; 18(5): 482-488, 2019 05.
Article in English | MEDLINE | ID: mdl-30886399

ABSTRACT

In two-dimensional (2D) systems, high mobility is typically achieved in low-carrier-density semiconductors and semimetals. Here, we discover that the nanobelts of Weyl semimetal NbAs maintain a high mobility even in the presence of a high sheet carrier density. We develop a growth scheme to synthesize single crystalline NbAs nanobelts with tunable Fermi levels. Owing to a large surface-to-bulk ratio, we argue that a 2D surface state gives rise to the high sheet carrier density, even though the bulk Fermi level is located near the Weyl nodes. A surface sheet conductance up to 5-100 S per □ is realized, exceeding that of conventional 2D electron gases, quasi-2D metal films, and topological insulator surface states. Corroborated by theory, we attribute the origin of the ultrahigh conductance to the disorder-tolerant Fermi arcs. The evidenced low-dissipation property of Fermi arcs has implications for both fundamental study and potential electronic applications.

19.
Nat Mater ; 18(3): 223-228, 2019 03.
Article in English | MEDLINE | ID: mdl-30598537

ABSTRACT

The zero-temperature limit of a continuous phase transition is marked by a quantum critical point, which can generate physical effects that extend to elevated temperatures. Magnetic quantum criticality is now well established, and has been explored in systems ranging from heavy fermion metals to quantum Ising materials. Ferroelectric quantum critical behaviour has also been recently demonstrated, motivating a flurry of research investigating its consequences. Here, we introduce the concept of multiferroic quantum criticality, in which both magnetic and ferroelectric quantum criticality occur in the same system. We develop the phenomenology of multiferroic quantum criticality and describe the associated experimental signatures, such as phase stability and modified scaling relations of observables. We propose several material systems that could be tuned to multiferroic quantum criticality utilizing alloying and strain as control parameters. We hope that these results stimulate exploration of the interplay between different kinds of quantum critical behaviours.

20.
Nature ; 565(7739): 331-336, 2019 01.
Article in English | MEDLINE | ID: mdl-30559378

ABSTRACT

Discovered decades ago, the quantum Hall effect remains one of the most studied phenomena in condensed matter physics and is relevant for research areas such as topological phases, strong electron correlations and quantum computing1-5. The quantized electron transport that is characteristic of the quantum Hall effect typically originates from chiral edge states-ballistic conducting channels that emerge when two-dimensional electron systems are subjected to large magnetic fields2. However, whether the quantum Hall effect can be extended to higher dimensions without simply stacking two-dimensional systems is unknown. Here we report evidence of a new type of quantum Hall effect, based on Weyl orbits in nanostructures of the three-dimensional topological semimetal Cd3As2. The Weyl orbits consist of Fermi arcs (open arc-like surface states) on opposite surfaces of the sample connected by one-dimensional chiral Landau levels along the magnetic field through the bulk6,7. This transport through the bulk results in an additional contribution (compared to stacked two-dimensional systems and which depends on the sample thickness) to the quantum phase of the Weyl orbit. Consequently, chiral states can emerge even in the bulk. To measure these quantum phase shifts and search for the associated chiral modes in the bulk, we conduct transport experiments using wedge-shaped Cd3As2 nanostructures with variable thickness. We find that the quantum Hall transport is strongly modulated by the sample thickness. The dependence of the Landau levels on the magnitude and direction of the magnetic field and on the sample thickness agrees with theoretical predictions based on the modified Lifshitz-Onsager relation for the Weyl orbits. Nanostructures of topological semimetals thus provide a way of exploring quantum Hall physics in three-dimensional materials with enhanced tunability.

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