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1.
Adv Mater ; : e2207121, 2023 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-36642840

RESUMO

Magnetic semimetals have increasingly emerged as lucrative platforms hosting spin-based topological phenomena in real- and momentum spaces. Cr1+ δ Te2 is a self-intercalated magnetic transition metal dichalcogenide (TMD), which exhibits topological magnetism, tunable electron filling, and magnetic frustration etc. While recent studies have explored real-space Berry curvature effects in this material, similar considerations of momentum-space Berry curvature have been lacking. Here, we systematically investigate the electronic structure and transport properties of epitaxial Cr1+ δ Te2 thin films over a wide range of doping, δ (0.33 - 0.71). Spectroscopic experiments reveal the presence of a characteristic semi-metallic band region near the Brillouin zone edge, which shows a rigid band like energy shift as a function of δ. Transport experiments show that the intrinsic component of the anomalous Hall effect (AHE) is sizable, and undergoes a sign flip across δ. Finally, density functional theory calculations establish a causal link between the observed doping evolution of the band structure and AHE: the AHE sign flip is shown to emerge from the sign change of the Berry curvature, as the semi-metallic band region crosses the Fermi energy. Our findings underscore the increasing relevance of momentum-space Berry curvature in magnetic TMDs and provide a unique platform for intertwining topological physics in real and momentum spaces. This article is protected by copyright. All rights reserved.

2.
Artigo em Inglês | MEDLINE | ID: mdl-35575457

RESUMO

A proximity effect facilitates the penetration of Cooper pairs that permits superconductivity in a normal metal, offering a promising approach to turn heterogeneous materials into superconductors and develop exceptional quantum phenomena. Here, we have systematically investigated proximity-induced anisotropic superconductivity in a monolayer Ni-Pb binary alloy by combining scanning tunneling microscopy/spectroscopy (STM/STS) with theoretical calculations. By means of high-temperature growth, the (33×33)R30o Ni-Pb surface alloy has been fabricated on Pb(111) and the appearance of a domain boundary as well as a structural phase transition can be deduced from a half-unit-cell lattice displacement. Given the high spatial and energy resolution, tunneling conductance (dI/dU) spectra have resolved the reduced but anisotropic superconducting gap ΔNiPb ≈ 1.0 meV, in stark contrast to the isotropic ΔPb ≈ 1.3 meV. In addition, the higher density of states at the Fermi energy (D(EF)) of the Ni-Pb surface alloy results in an enhancement of coherence peak height. According to the same Tc ≈ 7.1 K with Pb(111) from the temperature-dependent ΔNiPb and the short decay length Ld ≈ 3.55 nm from the spatially monotonic decrease of ΔNiPb, both results are supportive of a proximity-induced superconductivity. Despite a lack of a bulk counterpart, the atomically thick Ni-Pb bimetallic compound opens a pathway to engineer superconducting properties down to the two-dimensional limit, giving rise to the emergence of anisotropic superconductivity via a proximity effect.

3.
ACS Omega ; 7(18): 15760-15768, 2022 May 10.
Artigo em Inglês | MEDLINE | ID: mdl-35571781

RESUMO

Quantum spin Hall (QSH) insulators with large band gaps and dissipationless edge states are of both technological and scientific interest. Although numerous two-dimensional (2D) systems have been predicted to host the QSH phase, very few of them harbor large band gaps and retain their nontrivial band topology when they are deposited on substrates. Here, based on a first-principles analysis with hybrid functional calculations, we investigated the electronic and topological properties of inversion-asymmetric monolayer copper sulfide (Cu2S). Interestingly, we found that monolayer Cu2S possesses an intrinsic QSH phase, Rashba spin splitting, and a large band gap of 220 meV that is suitable for room-temperature applications. Most importantly, we constructed heterostructures of a Cu2S film on PtTe2, h-BN, and Cu(111) substrates and found that the topological properties remain preserved upon an interface with these substrates. Our findings suggest Cu2S as a possible platform to realize inversion-asymmetric QSH insulators with potential applications in low-dissipation electronic devices.

4.
Sci Rep ; 12(1): 4582, 2022 Mar 17.
Artigo em Inglês | MEDLINE | ID: mdl-35301355

RESUMO

Topological Dirac materials are attracting a lot of attention because they offer exotic physical phenomena. An exhaustive search coupled with first-principles calculations was implemented to investigate 10 Zintl compounds with a chemical formula of CaM2X2 (M = Zn or Cd, X = N, P, As, Sb, or Bi) under three crystal structures: CaAl2Si2-, ThCr2Si2-, and BaCu2S2-type crystal phases. All of the materials were found to energetically prefer the CaAl2Si2-type structure based on total ground state energy calculations. Symmetry-based indicators are used to evaluate their topological properties. Interestingly, we found that CaM2Bi2 (M = Zn or Cd) are topological crystalline insulators. Further calculations under the hybrid functional approach and analysis using k · p model reveal that they exhibit topological Dirac semimetal (TDSM) states, where the four-fold degenerate Dirac points are located along the high symmetry line in-between Г to A points. These findings are verified through Green's function surface state calculations under HSE06. Finally, phonon spectra calculations revealed that CaCd2Bi2 is thermodynamically stable. The Zintl phase of AM2X2 compounds have not been identified in any topological material databases, thus can be a new playground in the search for new topological materials.

5.
J Phys Condens Matter ; 34(6)2021 Nov 19.
Artigo em Inglês | MEDLINE | ID: mdl-34727535

RESUMO

Cadmium oxide (CdO)-ZnO alloys (CdxZn1-xO) exhibit a transformation from the wurtzite to the rocksalt (RS) phase at a CdO composition of ∼70% with a drastic change in the band gap and electrical properties. RS-CdxZn1-xO alloys (x> 0.7) are particularly interesting for transparent conductor applications due to their wide band gap and high electron mobility. In this work, we synthesized RS-CdxZn1-xO alloys doped with different concentrations of In dopants and evaluated their electrical and optical properties. Experimental results are analyzed in terms of the amphoteric native defect model and compared directly to defect formation energies obtained by hybrid density functional theory (DFT) calculations. A saturation in electron concentration of ∼7 × 1020 cm-3accompanied by a rapid drop in electron mobility is observed for the RS-CdxZn1-xO films with 0.7 ⩽x< 1 when the In dopant concentration [In] is larger than 3%. Hybrid DFT calculations confirm that the formation energy of metal vacancy acceptor defects is significantly lower in RS-CdxZn1-xO than in CdO, and hence limits the free carrier concentration. Mobility calculations reveal that due to the strong compensation by native defects, RS-CdxZn1-xO alloys exhibit a compensation ratio of >0.7 for films withx< 0.8. As a consequence of the compensation by native defects, in heavily doped RS-CdxZn1-xO carrier-induced band filling effect is limited. Furthermore, the much lower mobility of the RS-CdxZn1-xO alloys also results in a higher resistivity and reduced transmittance in the near infra-red region (λ > 1100 nm), making the material not suitable as transparent conductors for full spectrum photovoltaics.

6.
Chem Sci ; 12(35): 11659-11667, 2021 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-34667560

RESUMO

Deciphering rich non-covalent interactions that govern many chemical and biological processes is crucial for the design of drugs and controlling molecular assemblies and their chemical transformations. However, real-space characterization of these weak interactions in complex molecular architectures at the single bond level has been a longstanding challenge. Here, we employed bond-resolved scanning probe microscopy combined with an exhaustive structural search algorithm and quantum chemistry calculations to elucidate multiple non-covalent interactions that control the cohesive molecular clustering of well-designed precursor molecules and their chemical reactions. The presence of two flexible bromo-triphenyl moieties in the precursor leads to the assembly of distinct non-planar dimer and trimer clusters by manifold non-covalent interactions, including hydrogen bonding, halogen bonding, C-H⋯π and lone pair⋯π interactions. The dynamic nature of weak interactions allows for transforming dimers into energetically more favourable trimers as molecular density increases. The formation of trimers also facilitates thermally-triggered intermolecular Ullmann coupling reactions, while the disassembly of dimers favours intramolecular cyclization, as evidenced by bond-resolved imaging of metalorganic intermediates and final products. The richness of manifold non-covalent interactions offers unprecedented opportunities for controlling the assembly of complex molecular architectures and steering on-surface synthesis of quantum nanostructures.

7.
Nanoscale Adv ; 3(23): 6608-6616, 2021 Nov 24.
Artigo em Inglês | MEDLINE | ID: mdl-36132660

RESUMO

Recent studies have demonstrated the feasibility of synthesizing two-dimensional (2D) Janus materials which possess intrinsic structural asymmetry. Hence, we performed a systematic first-principles study of 2D Janus transition metal dichalcogenide (TMD) monolayers based on PtXY (X,Y = S, Se, or Te). Our calculated formation energies show that these monolayer Janus structures retain the 1T phase. Furthermore, phonon spectral calculations confirm that these Janus TMD monolayers are thermodynamically stable. We found that PtSSe, PtSTe, and PtSeTe exhibit an insulating phase with indirect band gaps of 2.108, 1.335, and 1.221 eV, respectively, from hybrid functional calculations. Due to the breaking of centrosymmetry in the crystal structure, the spin-orbit coupling (SOC)-induced anisotropic Rashba splitting is observed around the M point. The calculated Rashba strengths from M to Γ (α M-Γ R) are 1.654, 1.103, and 0.435 eV Å-1, while the calculated values from M to K (α M-K R) are 1.333, 1.244, and 0.746 eV Å-1, respectively, for PtSSe, PtSTe, and PtSeTe. Interestingly, the spin textures reveal that the spin-splitting is mainly attributed to the Rashba effect. However, a Dresselhaus-like contribution also plays a secondary role. Finally, we found that the band gaps and the strength of the Rashba effect can be further tuned through biaxial strain. Our findings indeed show that Pt-based Janus TMDs demonstrate the potential for spintronics applications.

8.
Phys Chem Chem Phys ; 23(38): 21489-21495, 2021 Oct 06.
Artigo em Inglês | MEDLINE | ID: mdl-34550130

RESUMO

Controllable fabrication of enantiospecific molecular superlattices is a matter of imminent scientific and technological interest. Herein, we demonstrate that long-range superlattice chirality in molecular self-assemblies can be tailored by tuning the interplay of weak intermolecular non-covalent interactions between hexaphenylbenzene-based enantiomers. By means of high-resolution scanning tunneling microscopy measurements, we demonstrate that the functionalization of a hexaphenylbenzene-based molecule with fluorine (F) atoms leads to the formation of molecular self-assemblies with distinct long-range chiral recognition patterns. We employed density functional theory calculations to quantify F-mediated lone pair F⋯π, C-H⋯F, and F⋯F interactions attributed to the distinct enantiospecific molecular self-organizations. Our findings underpin a viable route to fabricate long-range chiral recognition patterns in supramolecular assemblies by engineering the weak non-covalent intermolecular interactions.

9.
ACS Nano ; 14(9): 12037-12044, 2020 Sep 22.
Artigo em Inglês | MEDLINE | ID: mdl-32885948

RESUMO

The presence of two-dimensional (2D) layer-stacking heterostructures that can efficiently tune the interface properties by stacking desirable materials provides a platform to investigate some physical phenomena, such as the proximity effect and magnetic exchange coupling. Here, we report the observation of antisymmetric magnetoresistance in a van der Waals (vdW) antiferromagnetic/ferromagnetic (AFM/FM) heterostructure of MnPS3/Fe3GeTe2 when the temperature is below the Neel temperature of MnPS3. Distinguished from two resistance states in conventional giant magnetoresistance, the magnetoresistance in the MnPS3/Fe3GeTe2 heterostructure exhibits three states, of high, intermediate, and low resistance. This antisymmetric magnetoresistance spike is determined by an unsynchronized magnetic switching between the AFM/FM interface layer and the bulk of Fe3GeTe2 during magnetization reversal. Our work highlights that the artificial vdW stacking structure holds potential to explore some physical phenomena and spintronic device applications.

10.
Nat Commun ; 11(1): 4415, 2020 Sep 04.
Artigo em Inglês | MEDLINE | ID: mdl-32887890

RESUMO

Quantum states induced by single-atomic impurities are at the frontier of physics and material science. While such states have been reported in high-temperature superconductors and dilute magnetic semiconductors, they are unexplored in topological magnets which can feature spin-orbit tunability. Here we use spin-polarized scanning tunneling microscopy/spectroscopy (STM/S) to study the engineered quantum impurity in a topological magnet Co3Sn2S2. We find that each substituted In impurity introduces a striking localized bound state. Our systematic magnetization-polarized probe reveals that this bound state is spin-down polarized, in lock with a negative orbital magnetization. Moreover, the magnetic bound states of neighboring impurities interact to form quantized orbitals, exhibiting an intriguing spin-orbit splitting, analogous to the splitting of the topological fermion line. Our work collectively demonstrates the strong spin-orbit effect of the single-atomic impurity at the quantum level, suggesting that a nonmagnetic impurity can introduce spin-orbit coupled magnetic resonance in topological magnets.

11.
Nanoscale Res Lett ; 15(1): 56, 2020 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-32140792

RESUMO

We report a new graphene allotrope named HOT graphene containing carbon hexagons, octagons, and tetragons. A corresponding series of nanotubes are also constructed by rolling up the HOT graphene sheet. Ab initio calculations are performed on geometric and electronic structures of the HOT graphene and the HOT graphene nanotubes. Dirac cone and high Fermi velocity are achieved in a non-hexagonal structure of HOT graphene, implying that the honeycomb structure is not an indispensable condition for Dirac fermions to exist. HOT graphene nanotubes show distinctive electronic structures depending on their topology. The (0,1) n (n ≥ 3) HOT graphene nanotubes reveal the characteristics of semimetals, while the other set of nanotubes (1,0) n shows continuously adjustable band gaps (0~ 0.51 eV) with tube size. A competition between the curvature effect and the zone-folding approximation determines the band gaps of the (1,0) n nanotubes. Novel conversion between semimetallicity and semiconductivity arises in ultra-small tubes (radius < 4 Å, i.e., n < 3).

12.
Small ; 16(15): e1904271, 2020 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-32196957

RESUMO

Recently, 2D transition metal dichalcogenides (TMDs) have become intriguing materials in the versatile field of photonics and optoelectronics because of their strong light-matter interaction that stems from the atomic layer thickness, broadband optical response, controllable optoelectronic properties, and high nonlinearity, as well as compatibility. Nevertheless, the low optical cross-section of 2D-TMDs inhibits the light-matter interaction, resulting in lower quantum yield. Therefore, hybridizing the 2D-TMDs with plasmonic nanomaterials has become one of the promising strategies to boost the optical absorption of thin 2D-TMDs. The appeal of plasmonics is based on their capability to localize and enhance the electromagnetic field and increase the optical path length of light by scattering and injecting hot electrons to TMDs. In this regard, recent achievements with respect to hybridization of the plasmonic effect in 2D-TMDs systems and its augmented optical and optoelectronic properties are reviewed. The phenomenon of plasmon-enhanced interaction in 2D-TMDs is briefly described and state-of-the-art hybrid device applications are comprehensively discussed. Finally, an outlook on future applications of these hybrid devices is provided.

13.
Angew Chem Int Ed Engl ; 59(21): 8270-8276, 2020 May 18.
Artigo em Inglês | MEDLINE | ID: mdl-32003098

RESUMO

Ligand-induced surface restructuring with heteroatomic doping is used to precisely modify the surface of a prototypical [Au25 (SR1 )18 ]- cluster (1) while maintaining its icosahedral Au13 core for the synthesis of a new bimetallic [Au19 Cd3 (SR2 )18 ]- cluster (2). Single-crystal X-ray diffraction studies reveal that six bidentate Au2 (SR1 )3 motifs (L2) attached to the Au13 core of 1 were replaced by three quadridentate Au2 Cd(SR2 )6 motifs (L4) to create a bimetallic cluster 2. Experimental and theoretical results demonstrate a stronger electronic interaction between the surface motifs (Au2 Cd(SR2 )6 ) and the Au13 core, attributed to a more compact cluster structure and a larger energy gap of 2 compared to that of 1. These factors dramatically enhance the photoluminescence quantum efficiency and lifetime of crystal of the cluster 2. This work provides a new route for the design of a wide range of bimetallic/alloy metal nanoclusters with superior optoelectronic properties and functionality.

14.
Phys Rev Lett ; 124(3): 036402, 2020 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-32031832

RESUMO

Platinum ditelluride (PtTe_{2}), a type-II Dirac semimetal, remains semimetallic in ultrathin films down to just two triatomic layers (TLs) with a negative gap of -0.36 eV. Further reduction of the film thickness to a single TL induces a Lifshitz electronic transition to a semiconductor with a large positive gap of +0.79 eV. This transition is evidenced by experimental band structure mapping of films prepared by layer-resolved molecular beam epitaxy, and by comparing the data to first-principles calculations using a hybrid functional. The results demonstrate a novel electronic transition at the two-dimensional limit through film thickness control.

15.
Phys Rev Lett ; 123(21): 217004, 2019 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-31809171

RESUMO

The interplay between unconventional Cooper pairing and quantum states associated with atomic scale defects is a frontier of research with many open questions. So far, only a few of the high-temperature superconductors allow this intricate physics to be studied in a widely tunable way. We use scanning tunneling microscopy to image the electronic impact of Co atoms on the ground state of the LiFe_{1-x}Co_{x}As system. We observe that impurities progressively suppress the global superconducting gap and introduce low energy states near the gap edge, with the superconductivity remaining in the strong-coupling limit. Unexpectedly, the fully opened gap evolves into a nodal state before the Cooper pair coherence is fully destroyed. Our systematic theoretical analysis shows that these new observations can be quantitatively understood by the nonmagnetic Born-limit scattering effect in an s±-wave superconductor, unveiling the driving force of the superconductor to metal quantum phase transition.

16.
ACS Appl Mater Interfaces ; 11(36): 33012-33021, 2019 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-31414595

RESUMO

Spinel oxides (AB2O4) with unique crystal structures have been widely explored as promising alternative catalysts for efficient oxygen evolution reactions; however, developing novel methods to fabricate robust, cost-effective, and high-performance spinel oxide based electrocatalysts is still a great challenge. Here, utilizing a complementary experimental and theoretical approach, pentavalent vanadium doping in the spinel oxides (i.e., Co3O4 and NiFe2O4) has been thoroughly investigated to engineer their surface structures for the enhanced electrocatalytic oxygen evolution reaction. Specifically, when the optimal concentration of vanadium (ca. 7.7 at. %) is incorporated into Co3O4, the required overpotential to reach a certain jGEOM and jECSA decreases dramatically for oxygen evolution reactions in alkaline media. Even after 30 h of chronopotentiometry, the required potential for V-doped Co3O4 just increases by 16.3 mV, being much lower than that of the undoped one. It is observed that the pentavalent vanadium doping introduces lattice distortions and defects on the surface, which in turn exposes more active sites for reactions. DFT calculations further reveal the rate-determining step changing from the step of *-O to *-OOH to the step of *-OH to *-O, while the corresponding energy barriers decrease from 1.73 to 1.57 eV accordingly after high-valent V doping. Moreover, the oxygen intermediate probing method using methanol as a probing reagent also demonstrates a stronger OH* adsorption on the surface after V doping. When vanadium doping is performed in the inverse spinel matrix of NiFe2O4, impressive performance enhancement in the oxygen evolution reaction is as well witnessed. All these results clearly illustrate that the V doping process can not only efficiently improve the electrochemical properties of spinel transition metal oxides but also provide new insights into the design of high-performance water oxidation electrocatalysts.

17.
Sci Adv ; 5(7): eaav7717, 2019 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-31360763

RESUMO

The zigzag-edged triangular graphene molecules (ZTGMs) have been predicted to host ferromagnetically coupled edge states with the net spin scaling with the molecular size, which affords large spin tunability crucial for next-generation molecular spintronics. However, the scalable synthesis of large ZTGMs and the direct observation of their edge states have been long-standing challenges because of the molecules' high chemical instability. Here, we report the bottom-up synthesis of π-extended [5]triangulene with atomic precision via surface-assisted cyclodehydrogenation of a rationally designed molecular precursor on metallic surfaces. Atomic force microscopy measurements unambiguously resolve its ZTGM-like skeleton consisting of 15 fused benzene rings, while scanning tunneling spectroscopy measurements reveal edge-localized electronic states. Bolstered by density functional theory calculations, our results show that [5]triangulenes synthesized on Au(111) retain the open-shell π-conjugated character with magnetic ground states.

18.
Sci Rep ; 9(1): 756, 2019 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-30679630

RESUMO

Synchrotron radiation core-level photoemission spectroscopy, scanning tunneling microscopy (STM), and first-principles calculations have been utilized to explore the growth processes and the atomic structure of the resulting films during the two-step molecular beam epitaxy (MBE) of In and Bi on the Si(111) surface. Deposition of 1.0-ML Bi on the In/Si(111)-(4 × 1) surface at room temperature results in Bi-terminated BiIn-(4 × 3) structures, which are stable up to ~300 °C annealing. By contrast, deposition of In on the ß-Bi/Si(111)-(√3 × âˆš3) surface at room temperature results in three dimensional (3D) In islands. In both cases, annealing at 460 °C results in the same In-terminated In0.75Bi/Si(111)-(2 × 2) surface. Our DFT calculations confirm that the surface energy of In-terminated In0.75Bi/Si(111)-(2 × 2) system is lower than that of Bi-terminated Bi0.75In/Si(111)-(2 × 2). These findings provide means for the control of the polarity of the MBE In-Bi atomically thick films.

19.
Nanoscale ; 11(3): 878-881, 2019 Jan 17.
Artigo em Inglês | MEDLINE | ID: mdl-30604812

RESUMO

We employ an on-surface assembly protocol to synthesize a single layer of a two-dimensional conjugated network (Ni3(HITP)2) on a Au(111) surface. The electronic coupling between the π orbital of the diimine ligand and the d orbital of the metal ion renders efficient π-conjugation. Density-functional theory calculations provide evidence of a non-trivial topological gap in the surface-adsorbed single layer. This work demonstrates that single-layer 2D metal-organic frameworks adsorbed on surfaces are a new class of 2D materials that host quantum phases.

20.
Small ; 14(19): e1800032, 2018 May.
Artigo em Inglês | MEDLINE | ID: mdl-29635730

RESUMO

The formation of PtSe2 -layered films is reported in a large area by the direct plasma-assisted selenization of Pt films at a low temperature, where temperatures, as low as 100 °C at the applied plasma power of 400 W can be achieved. As the thickness of the Pt film exceeds 5 nm, the PtSe2 -layered film (five monolayers) exhibits a metallic behavior. A clear p-type semiconducting behavior of the PtSe2 -layered film (≈trilayers) is observed with the average field effective mobility of 0.7 cm2 V-1 s-1 from back-gated transistor measurements as the thickness of the Pt film reaches below 2.5 nm. A full PtSe2 field effect transistor is demonstrated where the thinner PtSe2 , exhibiting a semiconducting behavior, is used as the channel material, and the thicker PtSe2 , exhibiting a metallic behavior, is used as an electrode, yielding an ohmic contact. Furthermore, photodetectors using a few PtSe2 -layered films as an adsorption layer synthesized at the low temperature on a flexible substrate exhibit a wide range of absorption and photoresponse with the highest photocurrent of 9 µA under the laser wavelength of 408 nm. In addition, the device can maintain a high photoresponse under a large bending stress and 1000 bending cycles.

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