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1.
J Phys Chem Lett ; 15(23): 6010-6016, 2024 Jun 13.
Artigo em Inglês | MEDLINE | ID: mdl-38814350

RESUMO

This study investigates the electronic band structure of chromium sulfur bromide (CrSBr) through comprehensive photoluminescence (PL) characterization. We clearly identify low-temperature optical transitions between two closely adjacent conduction-band states and two different valence-band states. The analysis on the PL data robustly unveils energy splittings, band gaps, and excitonic transitions across different thicknesses of CrSBr, from monolayer to bulk. Temperature-dependent PL measurements elucidate the stability of the band splitting below the Néel temperature, suggesting that magnons coupled with excitons are responsible for the symmetry breaking and brightening of the transitions from the secondary conduction band minimum (CBM2) to the global valence band maximum (VBM1). Collectively, these results not only reveal splitting in both the conduction and valence bands but also highlight a significant advance in our understanding of the interplay between the optical, electronic, and magnetic properties of antiferromagnetic two-dimensional van der Waals crystals.

2.
Sci Rep ; 14(1): 5813, 2024 Mar 09.
Artigo em Inglês | MEDLINE | ID: mdl-38461196

RESUMO

Vertical stacking of different two-dimensional (2D) materials into van der Waals heterostructures exploits the properties of individual materials as well as their interlayer coupling, thereby exhibiting unique electrical and optical properties. Here, we study and investigate a system consisting entirely of different 2D materials for the implementation of electronic devices that are based on quantum mechanical band-to-band tunneling transport such as tunnel diodes and tunnel field-effect transistors. We fabricated and characterized van der Waals heterojunctions based on semiconducting layers of WSe2 and MoS2 by employing different gate configurations to analyze the transport properties of the junction. We found that the device dielectric environment is crucial for achieving tunneling transport across the heterojunction by replacing thick oxide dielectrics with thin layers of hexagonal-boronnitride. With the help of additional top gates implemented in different regions of our heterojunction device, it was seen that the tunneling properties as well as the Schottky barriers at the contact interfaces could be tuned efficiently by using layers of graphene as an intermediate contact material.

3.
Sci Adv ; 10(12): eadi2042, 2024 Mar 22.
Artigo em Inglês | MEDLINE | ID: mdl-38507479

RESUMO

The integration of heterogeneous modular units for building large-scale quantum networks requires engineering mechanisms that allow suitable transduction of quantum information. Magnon-based transducers are especially attractive due to their wide range of interactions and rich nonlinear dynamics, but most of the work to date has focused on linear magnon transduction in the traditional system composed of yttrium iron garnet and diamond, two materials with difficult integrability into wafer-scale quantum circuits. In this work, we present a different approach by using wafer-compatible materials to engineer a hybrid transducer that exploits magnon nonlinearities in a magnetic microdisc to address quantum spin defects in silicon carbide. The resulting interaction scheme points to the unique transduction behavior that can be obtained when complementing quantum systems with nonlinear magnonics.

4.
Angew Chem Int Ed Engl ; 63(20): e202320091, 2024 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-38488855

RESUMO

Conjugated coordination polymers (c-CPs) are unique organic-inorganic hybrid semiconductors with intrinsically high electrical conductivity and excellent charge carrier mobility. However, it remains a challenge in tailoring electronic structures, due to the lack of clear guidelines. Here, we develop a strategy wherein controlling the redox state of hydroquinone/benzoquinone (HQ/BQ) ligands allows for the modulation of the electronic structure of c-CPs while maintaining the structural topology. The redox-state control is achieved by reacting the ligand TTHQ (TTHQ=1,2,4,5-tetrathiolhydroquinone) with silver acetate and silver nitrate, yielding Ag4TTHQ and Ag4TTBQ (TTBQ=1,2,4,5-tetrathiolbenzoquinone), respectively. In spite of sharing the same topology consisting of a two-dimensional Ag-S network and HQ/BQ layer, they exhibit different band gaps (1.5 eV for Ag4TTHQ and 0.5 eV for Ag4TTBQ) and conductivities (0.4 S/cm for Ag4TTHQ and 10 S/cm for Ag4TTBQ). DFT calculations reveal that these differences arise from the ligand oxidation state inhibiting energy band formation near the Fermi level in Ag4TTHQ. Consequently, Ag4TTHQ displays a high Seebeck coefficient of 330 µV/K and a power factor of 10 µW/m ⋅ K2, surpassing Ag4TTBQ and the other reported silver-based c-CPs. Furthermore, terahertz spectroscopy demonstrates high charge mobilities exceeding 130 cm2/V ⋅ s in both Ag4TTHQ and Ag4TTBQ.

5.
ACS Nano ; 18(4): 2898-2905, 2024 Jan 30.
Artigo em Inglês | MEDLINE | ID: mdl-38240736

RESUMO

The layered, air-stable van der Waals antiferromagnetic compound CrSBr exhibits pronounced coupling among its optical, electronic, and magnetic properties. As an example, exciton dynamics can be significantly influenced by lattice vibrations through exciton-phonon coupling. Using low-temperature photoluminescence spectroscopy, we demonstrate the effective coupling between excitons and phonons in nanometer-thick CrSBr. By careful analysis, we identify that the satellite peaks predominantly arise from the interaction between the exciton and an optical phonon with a frequency of 118 cm-1 (∼14.6 meV) due to the out-of-plane vibration of Br atoms. Power-dependent and temperature-dependent photoluminescence measurements support exciton-phonon coupling and indicate a coupling between magnetic and optical properties, suggesting the possibility of carrier localization in the material. The presence of strong coupling between the exciton and the lattice may have important implications for the design of light-matter interactions in magnetic semiconductors and provide insights into the exciton dynamics in CrSBr. This highlights the potential for exploiting exciton-phonon coupling to control the optical properties of layered antiferromagnetic materials.

6.
Phys Rev Lett ; 131(18): 186903, 2023 Nov 03.
Artigo em Inglês | MEDLINE | ID: mdl-37977608

RESUMO

We study THz-driven condensate dynamics in epitaxial thin films of MgB_{2}, a prototype two-band superconductor (SC) with weak interband coupling. The temperature and excitation density dependent dynamics follow the behavior predicted by the phenomenological bottleneck model for the single-gap SC, implying adiabatic coupling between the two condensates on the ps timescale. The amplitude of the THz-driven suppression of condensate density reveals an unexpected decrease in pair-breaking efficiency with increasing temperature-unlike in the case of optical excitation. The reduced pair-breaking efficiency of narrow-band THz pulses, displaying minimum near ≈0.7 T_{c}, is attributed to THz-driven, long-lived, nonthermal quasiparticle distribution, resulting in Eliashberg-type enhancement of superconductivity, competing with pair breaking.

7.
Nano Lett ; 23(18): 8468-8473, 2023 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-37669544

RESUMO

Layered magnetic materials are becoming a major platform for future spin-based applications. Particularly, the air-stable van der Waals compound CrSBr is attracting considerable interest due to its prominent magneto-transport and magneto-optical properties. In this work, we observe a transition from antiferromagnetic to ferromagnetic behavior in CrSBr crystals exposed to high-energy, non-magnetic ions. Already at moderate fluences, ion irradiation induces a remanent magnetization with hysteresis adapting to the easy-axis anisotropy of the pristine magnetic order up to a critical temperature of 110 K. Structure analysis of the irradiated crystals in conjunction with density functional theory calculations suggests that the displacement of constituent atoms due to collisions with ions and the formation of interstitials favors ferromagnetic order between the layers.

8.
Opt Express ; 31(16): 26451-26462, 2023 Jul 31.
Artigo em Inglês | MEDLINE | ID: mdl-37710506

RESUMO

Photonic integrated circuits require photodetectors that operate at room temperature with sensitivity at telecom wavelengths and are suitable for integration with planar complementary-metal-oxide-semiconductor (CMOS) technology. Silicon hyperdoped with deep-level impurities is a promising material for silicon infrared detectors because of its strong room-temperature photoresponse in the short-wavelength infrared region caused by the creation of an impurity band within the silicon band gap. In this work, we present the first experimental demonstration of lateral Te-hyperdoped Si PIN photodetectors operating at room temperature in the optical telecom bands. We provide a detailed description of the fabrication process, working principle, and performance of the photodiodes, including their key figure of merits. Our results are promising for the integration of active and passive photonic elements on a single Si chip, leveraging the advantages of planar CMOS technology.

9.
Nat Commun ; 14(1): 5089, 2023 Aug 22.
Artigo em Inglês | MEDLINE | ID: mdl-37607945

RESUMO

Negatively-charged boron vacancy centers ([Formula: see text]) in hexagonal Boron Nitride (hBN) are attracting increasing interest since they represent optically-addressable qubits in a van der Waals material. In particular, these spin defects have shown promise as sensors for temperature, pressure, and static magnetic fields. However, their short spin coherence time limits their scope for quantum technology. Here, we apply dynamical decoupling techniques to suppress magnetic noise and extend the spin coherence time by two orders of magnitude, approaching the fundamental T1 relaxation limit. Based on this improvement, we demonstrate advanced spin control and a set of quantum sensing protocols to detect radiofrequency signals with sub-Hz resolution. The corresponding sensitivity is benchmarked against that of state-of-the-art NV-diamond quantum sensors. This work lays the foundation for nanoscale sensing using spin defects in an exfoliable material and opens a promising path to quantum sensors and quantum networks integrated into ultra-thin structures.

10.
ACS Appl Mater Interfaces ; 15(25): 30517-30523, 2023 Jun 28.
Artigo em Inglês | MEDLINE | ID: mdl-37327253

RESUMO

B20-CoSi is a newly discovered Weyl semimetal that crystallizes into a noncentrosymmetric crystal structure. However, the investigation of B20-CoSi has so far been focused on bulk materials, whereas the growth of thin films on technology-relevant substrates is a prerequisite for most practical applications. In this study, we have used millisecond-range flash-lamp annealing, a nonequilibrium solid-state reaction, to grow B20-CoSi thin films. By optimizing the annealing parameters, we were able to obtain thin films with a pure B20-CoSi phase. The magnetic and transport measurements indicate the appearance of the charge density wave and chiral anomaly. Our work presents a promising method for preparing thin films of most binary B20 transition-metal silicides, which are candidates for topological Weyl semimetals.

11.
Nanoscale Adv ; 5(2): 443-449, 2023 Jan 18.
Artigo em Inglês | MEDLINE | ID: mdl-36756265

RESUMO

Layered van der Waals crystals exhibit unique properties making them attractive for applications in nanoelectronics, optoelectronics, and sensing. The integration of two-dimensional materials with complementary metal-oxide-semiconductor (CMOS) technology requires controllable n- and p-type doping. In this work, we demonstrate the fabrication of vertical p-n heterojunctions made of p-type tin monoselenide (SnSe) and n-type tin diselenide (SnSe2). The p-n heterojunction is created in a single flake by the NH3-plasma-assisted phase transformation from SnSe2 to SnSe. We show that the transformation rate and crystal quality strongly depend on plasma parameters like plasma power, temperature, partial pressure, NH3 flow, and duration of plasma treatment. With optimal plasma parameters, the full transformation of SnSe2 flakes into SnSe is achieved within a few seconds. The crystal quality and the topography of the fabricated SnSe-SnSe2 heterostructures are investigated using micro-Raman spectroscopy and cross-sectional transmission electron microscopy. The formation of a p-n junction is verified by current-voltage measurements.

12.
J Am Chem Soc ; 145(4): 2430-2438, 2023 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-36661343

RESUMO

Electrically conductive coordination polymers and metal-organic frameworks are attractive emerging electroactive materials for (opto-)electronics. However, developing semiconducting coordination polymers with high charge carrier mobility for devices remains a major challenge, urgently requiring the rational design of ligands and topological networks with desired electronic structures. Herein, we demonstrate a strategy for synthesizing high-mobility semiconducting conjugated coordination polymers (c-CPs) utilizing novel conjugated ligands with D2h symmetry, namely, "4 + 2" phenyl ligands. Compared with the conventional phenyl ligands with C6h symmetry, the reduced symmetry of the "4 + 2" ligands leads to anisotropic coordination in the formation of c-CPs. Consequently, we successfully achieve a single-crystalline three-dimensional (3D) c-CP Cu4DHTTB (DHTTB = 2,5-dihydroxy-1,3,4,6-tetrathiolbenzene), containing orthogonal ribbon-like π-d conjugated chains rather than 2D conjugated layers. DFT calculation suggests that the resulting Cu4DHTTB exhibits a small band gap (∼0.2 eV), strongly dispersive energy bands near the Fermi level with a low electron-hole reduced effective mass (∼0.2m0*). Furthermore, the four-probe method reveals a semiconducting behavior with a decent conductivity of 0.2 S/cm. Thermopower measurement suggests that it is a p-type semiconductor. Ultrafast terahertz photoconductivity measurements confirm Cu4DHTTB's semiconducting nature and demonstrate the Drude-type transport with high charge carrier mobilities up to 88 ± 15 cm2 V-1 s-1, outperforming the conductive 3D coordination polymers reported till date. This molecular design strategy for constructing high-mobility semiconducting c-CPs lays the foundation for achieving high-performance c-CP-based (opto-)electronics.

13.
Nat Commun ; 13(1): 7683, 2022 Dec 12.
Artigo em Inglês | MEDLINE | ID: mdl-36509736

RESUMO

A highly promising route to scale millions of qubits is to use quantum photonic integrated circuits (PICs), where deterministic photon sources, reconfigurable optical elements, and single-photon detectors are monolithically integrated on the same silicon chip. The isolation of single-photon emitters, such as the G centers and W centers, in the optical telecommunication O-band, has recently been realized in silicon. In all previous cases, however, single-photon emitters were created uncontrollably in random locations, preventing their scalability. Here, we report the controllable fabrication of single G and W centers in silicon wafers using focused ion beams (FIB) with high probability. We also implement a scalable, broad-beam implantation protocol compatible with the complementary-metal-oxide-semiconductor (CMOS) technology to fabricate single telecom emitters at desired positions on the nanoscale. Our findings unlock a clear and easily exploitable pathway for industrial-scale photonic quantum processors with technology nodes below 100 nm.

14.
Sci Rep ; 12(1): 16388, 2022 Sep 30.
Artigo em Inglês | MEDLINE | ID: mdl-36180461

RESUMO

B20-type MnSi is the prototype magnetic skyrmion material. Thin films of MnSi show a higher Curie temperature than their bulk counterpart. However, it is not yet clear what mechanism leads to the increase of the Curie temperature. In this work, we grow MnSi films on Si(100) and Si(111) substrates with a broad variation in their structures. By controlling the Mn thickness and annealing parameters, the pure MnSi phase of polycrystalline and textured nature as well as the mixed phase of MnSi and MnSi1.7 are obtained. Surprisingly, all these MnSi films show an increased Curie temperature of up to around 43 K. The Curie temperature is likely independent of the structural parameters within our accessibility including the film thickness above a threshold, strain, cell volume and the mixture with MnSi1.7. However, a pronounced phonon softening is observed for all samples, which can tentatively be attributed to slight Mn excess from stoichiometry, leading to the increased Curie temperature.

15.
ACS Appl Mater Interfaces ; 14(26): 30000-30006, 2022 Jul 06.
Artigo em Inglês | MEDLINE | ID: mdl-35666627

RESUMO

Delta doping (δ-doping) can find a wide range of applications in advanced metal oxide semiconductor field effect transistors, deep UV photodetectors, quantum devices, and others. In this work, we formed a δ-doping layer in silicon by employing flash lamp annealing to treat the PCl3 monolayers grafted on silicon surfaces. The δ-doping layer is atomically thin (<1 nm). Low-temperature Hall measurements show that the δ-doping layer is in a metallic state and exhibits a weak localization phenomenon, implying that a two-dimensional electron gas is formed. When we form such an n-type δ-doping layer on a highly doped p-type Si substrate, a highly sensitive solar-blind UV photodetector is created, which traditionally was only possible by using wide band gap semiconductors such as gallium nitride (GaN) or silicon carbide (SiC).

16.
Nano Lett ; 22(13): 5137-5142, 2022 Jul 13.
Artigo em Inglês | MEDLINE | ID: mdl-35758596

RESUMO

Negatively charged boron vacancies (VB-) in hexagonal boron nitride (hBN) exhibit a broad emission spectrum due to strong electron-phonon coupling and Jahn-Teller mixing of electronic states. As such, the direct measurement of the zero-phonon line (ZPL) of VB- has remained elusive. Here, we measure the room-temperature ZPL wavelength to be 773 ± 2 nm by coupling the hBN layer to the high-Q nanobeam cavity. As the wavelength of cavity mode is tuned, we observe a pronounced intensity resonance, indicating the coupling to VB-. Our observations are consistent with the spatial redistribution of VB- emission. Spatially resolved measurements show a clear Purcell effect maximum at the midpoint of the nanobeam, in accord with the optical field distribution of the cavity mode. Our results are in good agreement with theoretical calculations, opening the way to using VB- as cavity spin-photon interfaces.

17.
Nanoscale ; 14(7): 2826-2836, 2022 Feb 17.
Artigo em Inglês | MEDLINE | ID: mdl-35133384

RESUMO

Plasmonic sensing in the infrared region employs the direct interaction of the vibrational fingerprints of molecules with the plasmonic resonances, creating surface-enhanced sensing platforms that are superior to traditional spectroscopy. However, the standard noble metals used for plasmonic resonances suffer from high radiative losses as well as fabrication challenges, such as tuning the spectral resonance positions into mid- to far-infrared regions, and the compatibility issue with the existing complementary metal-oxide-semiconductor (CMOS) manufacturing platform. Here, we demonstrate the occurrence of mid-infrared localized surface plasmon resonances (LSPR) in thin Si films hyperdoped with the known deep-level impurity tellurium. We show that the mid-infrared LSPR can be further enhanced and spectrally extended to the far-infrared range by fabricating two-dimensional arrays of micrometer-sized antennas in a Te-hyperdoped Si chip. Since Te-hyperdoped Si can also work as an infrared photodetector, we believe that our results will unlock the route toward the direct integration of plasmonic sensors with the on-chip CMOS platform, greatly advancing the possibility of mass manufacturing of high-performance plasmonic sensing systems.

18.
ACS Appl Mater Interfaces ; 14(9): 11927-11936, 2022 Mar 09.
Artigo em Inglês | MEDLINE | ID: mdl-35191687

RESUMO

Two-dimensional (2D) van der Waals materials with broadband optical absorption are promising candidates for next-generation UV-vis-NIR photodetectors. FePS3, one of the emerging antiferromagnetic van der Waals materials with a wide bandgap and p-type conductivity, has been reported as an excellent candidate for UV optoelectronics. However, a high sensitivity photodetector with a self-driven mode based on FePS3 has not yet been realized. Here, we report a high-performance and self-powered photodetector based on a multilayer MoSe2/FePS3 type-II n-p heterojunction with a working range from 350 to 900 nm. The presented photodetector operates at zero bias and at room temperature under ambient conditions. It exhibits a maximum responsivity (Rmax) of 52 mA W-1 and an external quantum efficiency (EQEmax) of 12% at 522 nm, which are better than the characteristics of its individual constituents and many other photodetectors made of 2D heterostructures. The high performance of MoSe2/FePS3 is attributed to the built-in electric field in the MoSe2/FePS3 n-p junction. Our approach provides a promising platform for broadband self-driven photodetector applications.

19.
Nat Commun ; 12(1): 6642, 2021 Nov 17.
Artigo em Inglês | MEDLINE | ID: mdl-34789741

RESUMO

Transistor concepts based on semiconductor nanowires promise high performance, lower energy consumption and better integrability in various platforms in nanoscale dimensions. Concerning the intrinsic transport properties of electrons in nanowires, relatively high mobility values that approach those in bulk crystals have been obtained only in core/shell heterostructures, where electrons are spatially confined inside the core. Here, it is demonstrated that the strain in lattice-mismatched core/shell nanowires can affect the effective mass of electrons in a way that boosts their mobility to distinct levels. Specifically, electrons inside the hydrostatically tensile-strained gallium arsenide core of nanowires with a thick indium aluminium arsenide shell exhibit mobility values 30-50 % higher than in equivalent unstrained nanowires or bulk crystals, as measured at room temperature. With such an enhancement of electron mobility, strained gallium arsenide nanowires emerge as a unique means for the advancement of transistor technology.

20.
Nanomaterials (Basel) ; 11(11)2021 Oct 30.
Artigo em Inglês | MEDLINE | ID: mdl-34835681

RESUMO

The fabrication of individual nanowire-based devices and their comprehensive electrical characterization remains a major challenge. Here, we present a symmetric Hall bar configuration for highly p-type germanium nanowires (GeNWs), fabricated by a top-down approach using electron beam lithography and inductively coupled plasma reactive ion etching. The configuration allows two equivalent measurement sets to check the homogeneity of GeNWs in terms of resistivity and the Hall coefficient. The highest Hall mobility and carrier concentration of GeNWs at 5 K were in the order of 100 cm2/(Vs) and 4×1019cm-3, respectively. With a decreasing nanowire width, the resistivity increases and the carrier concentration decreases, which is attributed to carrier scattering in the region near the surface. By comparing the measured data with simulations, one can conclude the existence of a depletion region, which decreases the effective cross-section of GeNWs. Moreover, the resistivity of thin GeNWs is strongly influenced by the cross-sectional shape.

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