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1.
J Chem Phys ; 160(14)2024 Apr 14.
Artigo em Inglês | MEDLINE | ID: mdl-38587221

RESUMO

Transition metal catalysts supported on topological insulators are predicted to show improved catalytic properties due to the presence of topological surface states, which may float up to the catalysts and provide robust electron transfer. However, experimental studies of surface structures and corresponding catalytic properties of transition metal/topological insulator heterostructures have not been demonstrated so far. Here, we report the structures, chemical states, and adsorption behaviors of two conventional transition metal catalysts, Pt and Pd, on the surface of Bi2Se3, a common topological insulator material. We reveal that Pt forms nanoparticles on the Bi2Se3 surface. Moreover, the interaction between Pt and surface Se is observed. Furthermore, thermal dosing of O2 onto the Pt/Bi2Se3 heterostructure leads to no oxygen adsorption. Detailed scanning tunneling microscopy study indicates that Pt transforms into PtSe2 after the thermal process, thus preventing O2 from adsorption. For another transition metal Pd, it exhibits approximate layer-island growth on Bi2Se3, and Pd-Se interaction is also observed. Our work provides significant insights into the behaviors of transition metals on top of a common topological insulator material and will assist in the future design of catalysts built with topological materials.

2.
Nano Lett ; 24(17): 5139-5145, 2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38639471

RESUMO

Dynamic tuning of thermal transport in solids is scientifically intriguing with wide applications for thermal transport control in electronic devices. In this work, we demonstrate a thermal transistor, a device in which heat flow can be regulated using external control, realized in a topological insulator (TI) through the topological surface states. The tuning of thermal transport is achieved by using optical gating of a thin dielectric layer deposited on the TI film. The gate-dependent thermal conductivity is measured using micro-Raman thermometry. The transistor has a large ON/OFF ratio of 2.8 at room temperature and can be continuously and repetitively switched in tens of seconds by optical gating and potentially much faster by electrical gating. Such thermal transistors with a large ON/OFF ratio and fast switching times offer the possibilities of smart thermal devices for active thermal management and control in future electronic systems.

3.
Adv Mater ; 35(36): e2301907, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37204117

RESUMO

Modification of the electronic structure of quantum matter by ad atom deposition allows for directed fundamental design of electronic and magnetic properties. This concept is utilized in the present study in order to tune the surface electronic structure of magnetic topological insulators based on MnBi2 Te4 . The topological bands of these systems are typically strongly electron-doped and hybridized with a manifold of surface states that place the salient topological states out of reach of electron transport and practical applications. In this study, micro-focused angle-resolved photoemission spectroscopy (microARPES) provides direct access to the termination-dependent dispersion of MnBi2 Te4 and MnBi4 Te7 during in situ deposition of rubidium atoms. The resulting band structure changes are found to be highly complex, encompassing coverage-dependent ambipolar doping effects, removal of surface state hybridization, and the collapse of a surface state band gap. In addition, doping-dependent band bending is found to give rise to tunable quantum well states. This wide range of observed electronic structure modifications can provide new ways to exploit the topological states and the rich surface electronic structures of manganese bismuth tellurides.

4.
Nano Lett ; 23(2): 414-421, 2023 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-36607246

RESUMO

Heterostructures composed of the intrinsic magnetic topological insulator MnBi2Te4 and its nonmagnetic counterpart Bi2Te3 host distinct surface electronic band structures depending on the stacking order and exposed termination. Here, we probe the ultrafast dynamical response of MnBi2Te4 and MnBi4Te7 following near-infrared optical excitation using time- and angle-resolved photoemission spectroscopy and disentangle surface from bulk dynamics based on density functional theory slab calculations of the surface-projected electronic structure. We gain access to the out-of-equilibrium charge carrier populations of both MnBi2Te4 and Bi2Te3 surface terminations of MnBi4Te7, revealing an instantaneous occupation of states associated with the Bi2Te3 surface layer followed by carrier extraction into the adjacent MnBi2Te4 layers with a laser fluence-tunable delay of up to 350 fs. The ensuing thermal relaxation processes are driven by phonon scattering with significantly slower relaxation times in the magnetic MnBi2Te4 septuple layers. The observed competition between interlayer charge transfer and intralayer phonon scattering demonstrates a method to control ultrafast charge transfer processes in MnBi2Te4-based van der Waals compounds.

5.
Nano Lett ; 23(1): 25-33, 2023 Jan 11.
Artigo em Inglês | MEDLINE | ID: mdl-36383034

RESUMO

The negatively charged boron vacancy (VB-) defect in hexagonal boron nitride (hBN) with optically addressable spin states has emerged due to its potential use in quantum sensing. Remarkably, VB- preserves its spin coherence when it is implanted at nanometer-scale distances from the hBN surface, potentially enabling ultrathin quantum sensors. However, its low quantum efficiency hinders its practical applications. Studies have reported improving the overall quantum efficiency of VB- defects with plasmonics; however, the overall enhancements of up to 17 times reported to date are relatively modest. Here, we demonstrate much higher emission enhancements of VB- with low-loss nanopatch antennas (NPAs). An overall intensity enhancement of up to 250 times is observed, corresponding to an actual emission enhancement of ∼1685 times by the NPA, along with preserved optically detected magnetic resonance contrast. Our results establish NPA-coupled VB- defects as high-resolution magnetic field sensors and provide a promising approach to obtaining single VB- defects.

6.
Adv Mater ; 35(12): e2205714, 2023 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-35950446

RESUMO

Strain engineering is a promising way to tune the electrical, electrochemical, magnetic, and optical properties of 2D materials, with the potential to achieve high-performance 2D-material-based devices ultimately. This review discusses the experimental and theoretical results from recent advances in the strain engineering of 2D materials. Some novel methods to induce strain are summarized and then the tunable electrical and optical/optoelectronic properties of 2D materials via strain engineering are highlighted, including particularly the previously less-discussed strain tuning of superconducting, magnetic, and electrochemical properties. Also, future perspectives of strain engineering are given for its potential applications in functional devices. The state of the survey presents the ever-increasing advantages and popularity of strain engineering for tuning properties of 2D materials. Suggestions and insights for further research and applications in optical, electronic, and spintronic devices are provided.

7.
Nat Commun ; 13(1): 7348, 2022 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-36522317

RESUMO

Van der Waals (vdW) magnet heterostructures have emerged as new platforms to explore exotic magnetic orders and quantum phenomena. Here, we study heterostructures of layered antiferromagnets, CrI3 and CrCl3, with perpendicular and in-plane magnetic anisotropy, respectively. Using magneto-optical Kerr effect microscopy, we demonstrate out-of-plane magnetic order in the CrCl3 layer proximal to CrI3, with ferromagnetic interfacial coupling between the two. Such an interlayer exchange field leads to higher critical temperature than that of either CrI3 or CrCl3 alone. We further demonstrate significant electric-field control of the coercivity, attributed to the naturally broken structural inversion symmetry of the heterostructure allowing unprecedented direct coupling between electric field and interfacial magnetism. These findings illustrate the opportunity to explore exotic magnetic phases and engineer spintronic devices in vdW heterostructures.

8.
Nano Lett ; 22(20): 8130-8136, 2022 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-36215229

RESUMO

The search of novel topological states, such as the quantum anomalous Hall insulator and chiral Majorana fermions, has motivated different schemes to introduce magnetism into topological insulators. A promising scheme is using the magnetic proximity effect (MPE), where a ferromagnetic insulator magnetizes the topological insulator. Most of these heterostructures are synthesized by growth techniques which prevent mixing many of the available ferromagnetic and topological insulators due to difference in growth conditions. Here, we demonstrate that MPE can be obtained in heterostructures stacked via the dry transfer of flakes of van der Waals ferromagnetic and topological insulators (Cr2Ge2Te6/BiSbTeSe2), as evidenced in the observation of an anomalous Hall effect (AHE). Furthermore, devices made from these heterostructures allow modulation of the AHE when controlling the carrier density via electrostatic gating. These results show that simple mechanical transfer of magnetic van der Waals materials provides another possible avenue to magnetize topological insulators by MPE.

9.
Nat Mater ; 21(9): 1024-1028, 2022 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-35970964

RESUMO

Electron spins in van der Waals materials are playing a crucial role in recent advances in condensed-matter physics and spintronics. However, nuclear spins in van der Waals materials remain an unexplored quantum resource. Here we report optical polarization and coherent control of nuclear spins in a van der Waals material at room temperature. We use negatively charged boron vacancy ([Formula: see text]) spin defects in hexagonal boron nitride to polarize nearby nitrogen nuclear spins. We observe the Rabi frequency of nuclear spins at the excited-state level anti-crossing of [Formula: see text] defects to be 350 times larger than that of an isolated nucleus, and demonstrate fast coherent control of nuclear spins. Further, we detect strong electron-mediated nuclear-nuclear spin coupling that is five orders of magnitude larger than the direct nuclear-spin dipolar coupling, enabling multi-qubit operations. Our work opens new avenues for the manipulation of nuclear spins in van der Waals materials for quantum information science and technology.

10.
J Chem Theory Comput ; 17(12): 7822-7826, 2021 Dec 14.
Artigo em Inglês | MEDLINE | ID: mdl-34788039

RESUMO

Interferences emerge when multiple pathways coexist together, leading toward the same result. Here, we report a theoretical study for a reaction scheme that leads to constructive quantum interference in a photoassociation (PA) reaction of a 87Rb Bose-Einstein condensate where the reactant spin state is prepared in a coherent superposition of multiple bare spin states. This is achieved by changing the reactive scattering channel in the PA reaction. As the origin of coherent control comes from the spin part of the wavefunction, we show that it is sufficient to use radio frequency (RF) coupling to achieve the superposition state. We simulate the RF coupling on a quantum processor (IBMQ Lima), and our results show that interferences can be used as a resource for the coherent control of photochemical reactions. The approach is general and can be employed to study a wide spectrum of chemical reactions in the ultracold regime.

11.
Nano Lett ; 21(19): 8182-8189, 2021 10 13.
Artigo em Inglês | MEDLINE | ID: mdl-34606291

RESUMO

Two-dimensional hexagonal boron nitride (hBN) that hosts room-temperature single-photon emitters (SPEs) is promising for quantum information applications. An important step toward the practical application of hBN is the on-demand, position-controlled generation of SPEs. Strategies reported for deterministic creation of hBN SPEs either rely on substrate nanopatterning that is not compatible with integrated photonics or utilize radiation sources that might introduce unpredictable damage or contamination to hBN. Here, we report a radiation- and lithography-free route to deterministically activate hBN SPEs by nanoindentation with atomic force microscopy (AFM). The method applies to hBN flakes on flat silicon dioxide-silicon substrates that can be readily integrated into on-chip photonic devices. The achieved SPE yields are above 30% for multiple indent sizes, and a maximum yield of 36% is demonstrated for indents around 400 nm. Our results mark an important step toward the deterministic creation and integration of hBN SPEs with photonic and plasmonic devices.


Assuntos
Compostos de Boro , Dióxido de Silício
12.
Nano Lett ; 21(18): 7708-7714, 2021 Sep 22.
Artigo em Inglês | MEDLINE | ID: mdl-34473524

RESUMO

The recently discovered spin defects in hexagonal boron nitride (hBN), a layered van der Waals material, have great potential in quantum sensing. However, the photoluminescence and the contrast of the optically detected magnetic resonance (ODMR) of hBN spin defects are relatively low so far, which limits their sensitivity. Here we report a record-high ODMR contrast of 46% at room temperature and simultaneous enhancement of the photoluminescence of hBN spin defects by up to 17-fold by the surface plasmon of a gold film microwave waveguide. Our results are obtained with shallow boron vacancy spin defects in hBN nanosheets created by low-energy He+ ion implantation and a gold film microwave waveguide fabricated by photolithography. We also explore the effects of microwave and laser powers on the ODMR and improve the sensitivity of hBN spin defects for magnetic field detection. Our results support the promising potential of hBN spin defects for nanoscale quantum sensing.

13.
J Phys Condens Matter ; 33(49)2021 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-34521077

RESUMO

Decoherence in quantum bits (qubits) is a major challenge for realizing scalable quantum computing. One of the primary causes of decoherence in qubits and quantum circuits based on superconducting Josephson junctions is the critical current fluctuation. Many efforts have been devoted to suppressing the critical current fluctuation in Josephson junctions. Nonetheless, the efforts have been hindered by the defect-induced trapping states in oxide-based tunnel barriers and the interfaces with superconductors in the traditional Josephson junctions. Motivated by this, along with the recent demonstration of 2D insulatorh-BN with exceptional crystallinity and low defect density, we fabricated a vertical NbSe2/h-BN/Nb Josephson junction consisting of a bottom NbSe2superconductor thin layer and a top Nb superconductor spaced by an atomically thinh-BN layer. We further characterized the superconducting current and voltage (I-V) relationships and Fraunhofer pattern of the NbSe2/h-BN/Nb junction. Notably, we demonstrated the critical current noise (1/fnoise power) in theh-BN-based Josephson device is at least a factor of four lower than that of the previously studied aluminum oxide-based Josephson junctions. Our work offers a strong promise ofh-BN as a novel tunnel barrier for high-quality Josephson junctions and qubit applications.

14.
Phys Chem Chem Phys ; 22(44): 25669-25674, 2020 Nov 18.
Artigo em Inglês | MEDLINE | ID: mdl-33164001

RESUMO

Entanglement is at the core of quantum information processing and may prove essential for quantum speed-up. Inspired by both theoretical and experimental studies of spin-momentum coupling in systems of ultra-cold atoms, we investigate the entanglement between the spin and momentum degrees of freedom of an optically trapped BEC of 87Rb atoms. We consider entanglement that arises due to the coupling of these degrees of freedom induced by Raman and radio-frequency fields and examine its dependence on the coupling parameters by evaluating von Neumann entropy as well as concurrence as measures of the entanglement attained. Our calculations reveal that under proper experimental conditions significant spin-momentum entanglement can be obtained, with von Neumann entropy of 80% of the maximum attainable value. Our analysis sheds some light on the prospects of using BECs for quantum information applications.

15.
Sci Rep ; 10(1): 16761, 2020 Oct 07.
Artigo em Inglês | MEDLINE | ID: mdl-33028944

RESUMO

Three-dimensional topological insulators have been demonstrated in recent years, which possess intriguing gapless, spin-polarized Dirac states with linear dispersion only on the surface. The spin polarization of the topological surface states is also locked to its momentum, which allows controlling motion of electrons using optical helicity, i.e., circularly polarized light. The electrical and thermal transport can also be significantly tuned by the helicity-control of surface state electrons. Here, we report studies of photo-thermoelectric effect of the topological surface states in Bi2Te2Se thin films with large tunability using varied gate voltages and optical helicity. The Seebeck coefficient can be altered by more than five times compared to the case without spin injection. This deep tuning is originated from the optical helicity-induced photocurrent which is shown to be enhanced, reduced, turned off, and even inverted due to the change of the accessed band structures by electrical gating. The helicity-selected topological surface state thus has a large effect on thermoelectric transport, demonstrating great opportunities for realizing helicity control of optoelectronic and thermal devices.

16.
Light Sci Appl ; 9: 126, 2020.
Artigo em Inglês | MEDLINE | ID: mdl-32704359

RESUMO

The recently proposed concept of graphene photodetectors offers remarkable properties such as unprecedented compactness, ultrabroadband detection, and an ultrafast response speed. However, owing to the low optical absorption of pristine monolayer graphene, the intrinsically low responsivity of graphene photodetectors significantly hinders the development of practical devices. To address this issue, numerous efforts have thus far been made to enhance the light-graphene interaction using plasmonic structures. These approaches, however, can be significantly advanced by leveraging the other critical aspect of graphene photoresponsivity enhancement-electrical junction control. It has been reported that the dominant photocarrier generation mechanism in graphene is the photothermoelectric (PTE) effect. Thus, the two energy conversion mechanisms involved in the graphene photodetection process are light-to-heat and heat-to-electricity conversions. In this work, we propose a meticulously designed device architecture to simultaneously enhance the two conversion efficiencies. Specifically, a gap plasmon structure is used to absorb a major portion of the incident light to induce localized heating, and a pair of split gates is used to produce a p-n junction in graphene to augment the PTE current generation. The gap plasmon structure and the split gates are designed to share common key components so that the proposed device architecture concurrently realizes both optical and electrical enhancements. We experimentally demonstrate the dominance of the PTE effect in graphene photocurrent generation and observe a 25-fold increase in the generated photocurrent compared to the un-enhanced cases. While further photocurrent enhancement can be achieved by applying a DC bias, the proposed device concept shows vast potential for practical applications.

17.
Adv Biosyst ; 4(7): e2000040, 2020 07.
Artigo em Inglês | MEDLINE | ID: mdl-32462817

RESUMO

Genetically encoded photoelectric silk that can convert photons to electrons (light to electricity) over a wide visible range in a self-power mode is reported. As silk is a versatile host material with electrical conductivity, biocompatibility, and processability, a photoelectric protein is genetically fused with silk by silkworm transgenesis. Specifically, mKate2, which is conventionally known as a far-red fluorescent protein, is used as a photoelectric protein. Characterization of the electrochemical and optical properties of mKate2 silk allows designing a photoelectric measurement system. A series of in situ photocurrent experiments support the sensitive and stable performance of photoelectric conversion. In addition, as a plasmonic nanomaterial with a broad spectral resonance, titanium nitride (TiN) nanoparticles are biologically hybridized into the silk glands, taking full advantage of the silkworms' open circulatory system as well as the absorption band of mKate2 silk. This biological hybridization via direct feeding of TiN nanoparticles further enhances the overall photoelectric conversion ability of mKate2 silk. It is envisioned that the biologically derived photoelectric protein, its ecofriendly scalable production by transgenic silkworms, and the bioassisted plasmonic hybridization can potentially broaden the biomaterial choices for developing next-generation biosensing, retina prosthesis, and neurostimulation applications.


Assuntos
Animais Geneticamente Modificados , Bombyx/química , Proteínas Luminescentes/química , Nanopartículas/química , Seda/química , Titânio/química , Animais , Bombyx/genética , Bombyx/metabolismo , Proteínas Luminescentes/biossíntese , Proteínas Luminescentes/genética , Seda/biossíntese , Seda/genética , Proteína Vermelha Fluorescente
18.
Phys Rev B ; 102(23): 235304, 2020 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-34485786

RESUMO

Quantum Boltzmann formalism is employed to study the transport properties of strongly-coupled double layer systems that enable the formation of interlayer excitons and exciton condensation. The importance of exciton formation, dissociation, and condensation is highlighted in the context of thermoelectric power generation, and this mathematical inquiry provides an alternative methodology to calculate the thermoelectric efficiency given the conditions of exciton formation. The Onsager relation for the Coulomb drag resistivity is shown to be valid even when exciton condensation is present. In addition, it is found that the traditional thermoelectric figure of merit is no longer sufficient to predict the efficiency of thermoelectric power generation in the presented situations. This inquiry offers insights for designing double layer systems, including their interlayer interactions, with enhanced thermoelectric energy conversion efficiency.

19.
Phys Rev Lett ; 123(20): 207701, 2019 Nov 15.
Artigo em Inglês | MEDLINE | ID: mdl-31809081

RESUMO

A pair of Dirac points (analogous to a vortex-antivortex pair) associated with opposite topological numbers (with ±π Berry phases) can be merged together through parameter tuning and annihilated to gap the Dirac spectrum, offering a canonical example of a topological phase transition. Here, we report transport studies on thin films of BiSbTeSe_{2}, which is a 3D topological insulator that hosts spin-helical gapless (semimetallic) Dirac fermion surface states for sufficiently thick samples, with an observed resistivity close to h/4e^{2} at the charge neutral point. When the sample thickness is reduced to below ∼10 nm thick, we observe a transition from metallic to insulating behavior, consistent with the expectation that the Dirac cones from the top and bottom surfaces hybridize (analogous to a "merging" in the real space) to give a trivial gapped insulator. Furthermore, we observe that an in-plane magnetic field can drive the system again towards a metallic behavior, with a prominent negative magnetoresistance (up to ∼-95%) and a temperature-insensitive resistivity close to h/2e^{2} at the charge neutral point. The observation is consistent with a predicted effect of an in-plane magnetic field to reduce the hybridization gap (which, if small enough, may be smeared by disorder and give rise to a metallic behavior). A sufficiently strong magnetic field is predicted to restore and split again the Dirac points in the momentum space, inducing a distinct 2D topological semimetal phase with two single-fold Dirac cones of opposite spin-momentum windings.

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