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1.
Proc Natl Acad Sci U S A ; 121(23): e2401757121, 2024 Jun 04.
Article in English | MEDLINE | ID: mdl-38820004

ABSTRACT

We experimentally demonstrate the creation of defects in monolayer WSe2 via nanopillar imprinting and helium ion irradiation. Based on the first method, we realize atomically thin vertical tunneling light-emitting diodes based on WSe2 monolayers hosting quantum emitters at deterministically specified locations. We characterize these emitters by investigating the evolution of their emission spectra in external electric and magnetic fields, as well as by inducing electroluminescence at low temperatures. We identify qualitatively different types of quantum emitters and classify them according to the dominant electron-hole recombination paths, determined by the mechanisms of intervalley mixing occurring in fundamental conduction and/or valence subbands.

2.
Nat Nanotechnol ; 18(9): 1012-1019, 2023 Sep.
Article in English | MEDLINE | ID: mdl-37524907

ABSTRACT

Excitons (coupled electron-hole pairs) in semiconductors can form collective states that sometimes exhibit spectacular nonlinear properties. Here, we show experimental evidence of a collective state of short-lived excitons in a direct-bandgap, atomically thin MoS2 semiconductor whose propagation resembles that of a classical liquid as suggested by the nearly uniform photoluminescence through the MoS2 monolayer regardless of crystallographic defects and geometric constraints. The exciton fluid flows over ultralong distances (at least 60 µm) at a speed of ~1.8 × 107 m s-1 (~6% the speed of light). The collective phase emerges above a critical laser power, in the absence of free charges and below a critical temperature (usually Tc ≈ 150 K) approaching room temperature in hexagonal-boron-nitride-encapsulated devices. Our theoretical simulations suggest that momentum is conserved and local equilibrium is achieved among excitons; both these features are compatible with a fluid dynamics description of the exciton transport.

3.
Small ; 19(41): e2300144, 2023 Oct.
Article in English | MEDLINE | ID: mdl-37329196

ABSTRACT

A key advantage of utilizing van-der-Waals (vdW) materials as defect-hosting platforms for quantum applications is the controllable proximity of the defect to the surface or the substrate allowing for improved light extraction, enhanced coupling with photonic elements, or more sensitive metrology. However, this aspect results in a significant challenge for defect identification and characterization, as the defect's properties depend on the the atomic environment. This study explores how the environment can influence the properties of carbon impurity centers in hexagonal boron nitride (hBN). It compares the optical and electronic properties of such defects between bulk-like and few-layer films, showing alteration of the zero-phonon line energies and their phonon sidebands, and enhancements of inhomogeneous broadenings. To disentangle the mechanisms responsible for these changes, including the atomic structure, electronic wavefunctions, and dielectric screening, it combines ab initio calculations with a quantum-embedding approach. By studying various carbon-based defects embedded in monolayer and bulk hBN, it demonstrates that the dominant effect of the change in the environment is the screening of density-density Coulomb interactions between the defect orbitals. The comparative analysis of experimental and theoretical findings paves the way for improved identification of defects in low-dimensional materials and the development of atomic scale sensors for dielectric environments.

4.
Nat Mater ; 20(2): 181-187, 2021 Feb.
Article in English | MEDLINE | ID: mdl-33106649

ABSTRACT

Two-dimensional superconductor (2DSC) monolayers with non-centrosymmetry exhibit unconventional Ising pair superconductivity and an enhanced upper critical field beyond the Pauli paramagnetic limit, driving intense research interest. However, they are often susceptible to structural disorder and environmental oxidation, which destroy electronic coherence and provide technical challenges in the creation of artificial van der Waals heterostructures (vdWHs) for devices. Herein, we report a general and scalable synthesis of highly crystalline 2DSC monolayers via a mild electrochemical exfoliation method using flexible organic ammonium cations solvated with neutral solvent molecules as co-intercalants. Using NbSe2 as a model system, we achieved a high yield (>75%) of large-sized single-crystal monolayers up to 300 µm. The as-fabricated, twisted NbSe2 vdWHs demonstrate high stability, good interfacial properties and a critical current that is modulated by magnetic field when one flux quantum fits to an integer number of moiré cells. Additionally, formulated 2DSC inks can be exploited to fabricate wafer-scale 2D superconducting wire arrays and three-dimensional superconducting composites with desirable morphologies.

5.
J Phys Condens Matter ; 30(10): 105302, 2018 03 14.
Article in English | MEDLINE | ID: mdl-29393070

ABSTRACT

Topological insulators emerge as promising components of spintronic devices, in particular for applications where all-electrical spin control is essential. While the capability of these materials to generate spin-polarized currents is well established, only very little is known about the spin injection/extraction into/out of them. Here, we explore the switching behavior of lateral spin valves comprising the 3D topological insulator Bi2Te2Se as channel, which is separated from ferromagnetic Cobalt detector contacts by an ultrathin hexagonal boron nitride (hBN) tunnel barrier. The corresponding contact resistance displays a notable variation, which is correlated with a change of the switching characteristics of the spin valve. For contact resistances below ~5 kΩ, the hysteresis in the switching curve reverses upon reversing the applied current, as expected for spin-polarized currents carried by the helical surface states. By contrast, for higher contact resistances an opposite polarity of the hysteresis loop is observed, which is independent of the current direction, a behavior signifying negative spin detection efficiency of the multilayer hBN/Co contacts combined with bias-induced spin signal inversion. Our findings suggest the possibility to tune the spin exchange across the interface between a ferromagnetic metal and a topological insulator through the number of intervening hBN layers.

6.
Nat Commun ; 9(1): 331, 2018 01 23.
Article in English | MEDLINE | ID: mdl-29362413

ABSTRACT

Three-dimensional topological insulators are a class of Dirac materials, wherein strong spin-orbit coupling leads to two-dimensional surface states. The latter feature spin-momentum locking, i.e., each momentum vector is associated with a spin locked perpendicularly to it in the surface plane. While the principal spin generation capability of topological insulators is well established, comparatively little is known about the interaction of the spins with external stimuli like polarized light. We observe a helical, bias-dependent photoconductance at the lateral edges of topological Bi2Te2Se platelets for perpendicular incidence of light. The same edges exhibit also a finite bias-dependent Kerr angle, indicative of spin accumulation induced by a transversal spin Hall effect in the bulk states of the Bi2Te2Se platelets. A symmetry analysis shows that the helical photoconductance is distinct to common longitudinal photoconductance and photocurrent phenomena, but consistent with optically injected spins being transported in the side facets of the platelets.

7.
Nano Lett ; 17(2): 973-979, 2017 02 08.
Article in English | MEDLINE | ID: mdl-28081604

ABSTRACT

Topological insulators constitute a fascinating class of quantum materials with nontrivial, gapless states on the surface and insulating bulk states. By revealing the optoelectronic dynamics in the whole range from femto- to microseconds, we demonstrate that the long surface lifetime of Bi2Te2Se nanowires allows us to access the surface states by a pulsed photoconduction scheme and that there is a prevailing bolometric response of the surface states. The interplay of the surface and bulk states dynamics on the different time scales gives rise to a surprising physical property of Bi2Te2Se nanowires: their pulsed photoconductance changes polarity as a function of laser power. Moreover, we show that single Bi2Te2Se nanowires can be used as THz generators for on-chip high-frequency circuits at room temperature. Our results open the avenue for single Bi2Te2Se nanowires as active modules in optoelectronic high-frequency and THz circuits.

8.
Adv Mater ; 28(30): 6436-41, 2016 Aug.
Article in English | MEDLINE | ID: mdl-27167512

ABSTRACT

Dilute isovalent sulfur doping simultaneously increases electrical conductivity and Seebeck coefficient in Bi2 Te2 Se nanoplates, and bulk pellets made from them. This unusual trend at high electron concentrations is underpinned by multifold increases in electron effective mass attributable to sulfur-induced band topology effects, providing a new way for accessing a high thermoelectric figure-of-merit in topological-insulator-based nanomaterials through doping.

9.
Nano Lett ; 16(4): 2595-602, 2016 Apr 13.
Article in English | MEDLINE | ID: mdl-26982565

ABSTRACT

Further development of the field of all-electric spintronics requires the successful integration of spin transport channels with spin injector/generator elements. While with the advent of graphene and related 2D materials high performance spin channel materials are available, the use of nanostructured spin generators remains a major challenge. Especially promising for the latter purpose are 3D topological insulators, whose 2D surface states host massless Dirac Fermions with spin-momentum locking. Here, we demonstrate injection of spin-polarized current from a topological insulator into graphene, enabled by its intimate coupling to an ultrathin Bi2Te2Se nanoplatelet within a van der Waals epitaxial heterostructure. The spin switching signal, whose magnitude scales inversely with temperature, is detectable up to ∼15 K. Our findings establish topological insulators as prospective future components of spintronic devices wherein spin manipulation is achieved by purely electrical means.

10.
Sci Rep ; 5: 11691, 2015 Jun 29.
Article in English | MEDLINE | ID: mdl-26118383

ABSTRACT

Three-dimensional topological insulators comprise topologically protected surface states displaying massless, Dirac-like linear dispersion with spin-momentum locking. Electrical conduction through such surface states has been documented to manifest itself in a two-dimensional character of the angle-dependent magnetotransport behavior. Here, we explore the size-dependent electronic properties of nanostructures made of the lead-containing mineral Aleksite, a naturally occurring topological insulator. Compared to its sister compound Kawazulite, a member of the well-studied Tetradymite crystal class, the crystal structure of Aleksite is distinguished by its lack of any counterpart within the group of synthetic topological insulators. Low temperature Hall measurements on thin Aleksite nanosheets reveal a significant carrier mobility on the order of 1000 cm(2)/(Vs), and a high carrier density of n = 3.9 × 10(25) m(-3). Importantly, for Aleksite nanoribbons with a width below 150 nm, a 1D weak antilocalization effect along with 1D universal conductance fluctuations emerges, which transforms into 2D behavior for larger ribbon widths.

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