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1.
Nature ; 625(7993): 60-65, 2024 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-38172363

RESUMEN

Semiconducting graphene plays an important part in graphene nanoelectronics because of the lack of an intrinsic bandgap in graphene1. In the past two decades, attempts to modify the bandgap either by quantum confinement or by chemical functionalization failed to produce viable semiconducting graphene. Here we demonstrate that semiconducting epigraphene (SEG) on single-crystal silicon carbide substrates has a band gap of 0.6 eV and room temperature mobilities exceeding 5,000 cm2 V-1 s-1, which is 10 times larger than that of silicon and 20 times larger than that of the other two-dimensional semiconductors. It is well known that when silicon evaporates from silicon carbide crystal surfaces, the carbon-rich surface crystallizes to produce graphene multilayers2. The first graphitic layer to form on the silicon-terminated face of SiC is an insulating epigraphene layer that is partially covalently bonded to the SiC surface3. Spectroscopic measurements of this buffer layer4 demonstrated semiconducting signatures4, but the mobilities of this layer were limited because of disorder5. Here we demonstrate a quasi-equilibrium annealing method that produces SEG (that is, a well-ordered buffer layer) on macroscopic atomically flat terraces. The SEG lattice is aligned with the SiC substrate. It is chemically, mechanically and thermally robust and can be patterned and seamlessly connected to semimetallic epigraphene using conventional semiconductor fabrication techniques. These essential properties make SEG suitable for nanoelectronics.

2.
J Comput Chem ; 43(29): 1978-1984, 2022 Nov 05.
Artículo en Inglés | MEDLINE | ID: mdl-36125399

RESUMEN

The bonding and electronic properties of Inn - , Inn Si- , and Inn Ge- (n = 3-16) clusters have been computationally investigated. An intensive global search for the ground-state structures of these clusters were conducted using the genetic algorithm coupled with density functional theory (DFT). The ground-state structures of these clusters have been identified through the comparison between simulated photoelectron spectra (PES) of the found lowest-energy isomers and the experimentally measured ones. Doping semiconductor atom (Si or Ge) can significantly change the structures of the In clusters in most sizes, and the dopant prefers to be surrounded by In atoms. There are three structural motifs for Inn X- (X = Si, Ge, n = 3-16), and the transition occurs at sizes n = 5 and 13. All Inn Si- and Inn Ge- share the same configurations and similar electronic properties except for n = 8. Among all above studied clusters, In13 - stands out with the largest vertical detachment energy (VDE), HOMO-LUMO gap, (Eb ) and second order energy difference Δ2 E due to its closed electronic shell of (1S)2 (1P)6 (1D)10 (2S)2 (1F)14 (2P)6 . Similarly, the neutral In12 X (X = Si, Ge) clusters are also identified as superatoms but with electronic configuration of (1S)2 (1P)6 (2S)2 (1D)10 (1F)14 (2P)6 .

3.
Opt Express ; 30(9): 14651-14660, 2022 Apr 25.
Artículo en Inglés | MEDLINE | ID: mdl-35473204

RESUMEN

Subwavelength chiral metamaterials with tunable geometries and compositions are essential to advance the development of chiral biochemical samples detection. Here, we report a spatial symmetry breaking chiral terahertz (THz) metamaterial structure with stacked layers of L-shape arranged gold disks as the periodic unit cell. The chiroptical response can be adjusted on-demand by manipulating the number of stacking layers and the twisted angle of the periodic unit between adjacent array layers. We reveal that the chiroptical response originates from the optical resonances of the gold disks and the adjacent gold disks array layers via experiments and numerical simulation analysis. Furthermore, we find that this chiral metamaterial can realize label-free detection of proline in biological samples and label-free enantio-discrimination of chiral molecules. The change of the analyte concentration can also regulate the transmission circular dichroism (TCD) intensity of the chiral metamaterials. Our results not only provide new ideas into the design of functional chiral metamaterials, but also bring new strategies to develop chiroptical biosensing devices.


Asunto(s)
Oro , Dicroismo Circular , Simulación por Computador , Estereoisomerismo
4.
Phys Chem Chem Phys ; 24(30): 18321-18330, 2022 Aug 03.
Artículo en Inglés | MEDLINE | ID: mdl-35880636

RESUMEN

We investigated the structural evolution and electronic properties of medium-sized silicon cluster anions doped with two transition metal atoms, TM2Sin- (TM = V, Cr; n = 14-20), by using mass-selective anion photoelectron spectroscopy combined with density functional theory (DFT) calculations. Putative ground state structures of these clusters were obtained by using a genetic algorithm coupled with the DFT calculations. It was found that the two TM atoms tend to form a TM-TM bond, which - except for V2Si19- - is shorter than the nearest neighbour distance in the crystalline state of the respective metals. The V2Sin- clusters with n = 14 to 17 exhibit structures based on a silicon hexagonal antiprism, while the larger ones exhibit more fullerene-like cage structures. Cr2Sin- clusters follow the same trend, although with a silicon hexagonal prism structure for n = 14 and 15, and the transition to fullerene-like structures occurring at n = 17. Among these clusters, TM2Si18- have the largest average binding energy and second order differences in energy, therefore the highest relative stability. All of the clusters possess total magnetic moment of 1 µB, but with very different contributions from the doped TM atoms. Especially in the Cr doped clusters there is a tendency towards an anitiferromagnetic arrangement of the magnetic moments of the two Cr atoms.

5.
Phys Chem Chem Phys ; 24(15): 8839-8845, 2022 Apr 13.
Artículo en Inglés | MEDLINE | ID: mdl-35355038

RESUMEN

We present a systematic study of the structures and electronic properties of vanadium-doped silicon cluster anions, VSin- (n = 14-20), by combining photoelectron spectroscopy (PES) measurements and density functional theory (DFT) based theoretical calculations. High resolution PES of low temperature (10 K) clusters are acquired at a photon wavelength of 248 nm. Low-lying structures of VSi14-20- are obtained by a genetic algorithm based global minimum search code combined with DFT calculations. Excellent agreement is found between the measured PES and the simulated electron density of states of the putative ground-state structures. We conclude that clusters with sizes n = 14 and n = 15 prefer cage-like structures, with the encapsulated vanadium atom bonding with all silicon atoms, while a fullerene-like motif is more favorable for n ≥ 16. For the sizes n = 16 to 19, the structures consist of a V@Si14 with two, three, four, and five Si atoms on the surface of the cage. For n = 20 the structure consists of a V@Si15 with five Si atoms on the surface of the cage. VSi14- has the highest stability and stands out as a simultaneous closing of electronic and geometrical shells.

6.
J Phys Chem A ; 126(8): 1329-1335, 2022 Mar 03.
Artículo en Inglés | MEDLINE | ID: mdl-35175756

RESUMEN

CrSin- (n = 14-18) cluster anions have been investigated by a combination of photoelectron spectroscopy (PES) and first-principles calculations. The lowest-lying structures of the clusters have been determined by a global minimum search based on the genetic algorithm, combined with density functional theory (DFT) calculations. The simulated PES spectra of the lowest-energy isomers are in agreement with the experimental results, which gives strong evidence that the correct structures have been found. While sizes n = 14 and n = 15 prefer cage-like structures based on multi-center bonding within the cage, the larger sizes adopt structures based on fullerene-type cages around the Cr atom, with the additional atoms attached to the cage surface. A Hirshfeld analysis shows that the Cr atoms act as electron donors in all clusters, thus enhancing the electron count in the cage. It also reveals that the magnetic moment of 1µB shown by all clusters is mainly contributed by the Cr atom. One interesting exception is size 17, where the Cr atom contributes a small moment antiparallel to that of the silicon cage.

7.
Sensors (Basel) ; 20(6)2020 Mar 23.
Artículo en Inglés | MEDLINE | ID: mdl-32210206

RESUMEN

High sensitivity biosensors based on the coupling of surface plasmon polaritons on titanium nitride (TiN) and a planar waveguide mode were built; they were proved by sensing three different media: air, water and dried egg white; sensors described here could be useful for sensing materials with a refractive index between 1.0 and 1.6; in particular, materials of biological interest with a refractive index in the range 1.3-1.6, like those containing biotin and/or streptavidin. They were built by depositing Nb2O5/SiO2/TiN multilayer structures on the flat surface of D-shaped sapphire prisms by using the dc magnetron sputtering technique. Attenuated total reflection (ATR) experiments in the Kretschmann configuration were accomplished for the air/TiN/Prism and S/Nb2O5/SiO2/TiN/Prism structures, S being the sample or sensing medium. ATR spectra for plasmons at the TiN/air interface showed a broad absorption band for angles of incidence between 36 and 85°, with full width at half maximum (FWHM) of approximately 40°. For the S/Nb2O5/SiO2/TiN/Prism structures, ATR spectra showed a sharp reflectivity peak, within the broad plasmonic absorption band, which was associated with Fano resonances. The angular position and FWHM of the Fano resonances strongly depend on the refractive index of the sensing medium. ATR spectra were fitted by using the transfer-matrix method. Additionally, we found that angular sensitivity and figure of merit increase with increasing the refractive index of the sensing medium.


Asunto(s)
Técnicas Biosensibles , Titanio/química , Modelos Teóricos , Niobio/química , Óxidos/química , Refractometría , Difracción de Rayos X
8.
Phys Rev Lett ; 113(15): 157203, 2014 Oct 10.
Artículo en Inglés | MEDLINE | ID: mdl-25375737

RESUMEN

Simultaneous magnetic and electric deflection measurements of rhodium clusters (Rh(N), 6 ≤ N ≤ 40) reveal ferromagnetism and ferroelectricity at low temperatures, while neither property exists in the bulk metal. Temperature-independent magnetic moments (up to 1 µ(B) per atom) are observed, and superparamagnetic blocking temperatures up to 20 K. Ferroelectric dipole moments on the order of 1D with transition temperatures up to 30 K are observed. Ferromagnetism and ferroelectricity coexist in rhodium clusters in the measured size range, with size-dependent variations in the transition temperatures that tend to be anticorrelated in the range n = 6-25. Both effects diminish with size and essentially vanish at N = 40. The ferroelectric properties suggest a Jahn-Teller ground state. These experiments represent the first example of multiferroic behavior in pure metal clusters.

9.
Toxicon ; 235: 107325, 2023 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-37838004

RESUMEN

The consumption of Ipomoea carnea produces a neurological syndrome in animals. The toxic principles of I. carnea are the alkaloids swainsonine (SW) and calystegines B1, B2, B3 and C1. In this study, we investigated the cytotoxicity of an alkaloid extract of Ipomoea carnea (AEE) and natural swainsonine (SW) isolated from Astragalus lentiginosus (25-1000 µM of SW) for 48 h in a glioma cell line. Although the natural SW did not induce any changes in cell viability, the AEE exhibited a dose dependent cytotoxic effect and release of lactate dehydrogenase (LDH) indicative of cytolysis. In order to evaluate the morphological changes involved, cells were examined using phase contrast and fluorescence microscopy with acridine orange-ethidium bromide staining. The AEE caused a cell death compatible with necrosis, whereas exposure to 1000 µM of SW resulted in cytoplasmic vacuolation. Immunocytochemical studies revealed that astrocytes treated with 150 µM of AEE from I. carnea or 1000 µM of SW exhibited morphological characteristics of cell activation. These findings suggest that swainsonine would not be the only component present in the AEE of I. carnea responsible for in vitro cytotoxicity. Calystegines might also play a role in acting synergistically and triggering cell death through necrosis.


Asunto(s)
Alcaloides , Antineoplásicos , Ipomoea , Animales , Swainsonina/toxicidad , Alcaloides/farmacología , Neuroglía , Extractos Vegetales/toxicidad , Necrosis
10.
Rev Sci Instrum ; 94(6)2023 Jun 01.
Artículo en Inglés | MEDLINE | ID: mdl-37862520

RESUMEN

Ultra-fast high-voltage switches (UFHVSs) are a core component of time-of-flight mass spectrometers for realizing high accuracy ion acceleration, deceleration, and temporal focusing. The desirable features of high performance UFHVSs include a large range of adjustability of pulse width, a high maximum output amplitude, and minute rising and falling times. Besides the simplicity of the driver circuit, the total cost of the whole device is also critical to its practical applications. In this work, we present a low-cost and easy-fabrication 5000 V bipolar solid-state UFHVS for a high-resolution mass spectrometer. A double-pulse transformer isolates the circuit's high- and low-voltage sides and synchronously drives series-connected cascode SiC FETs to form its push-pull topology. This scheme allows transmitting drive signals with long widths but without the magnetic saturation of the transformer. Testing results show that output pulses reach a maximum voltage of 5000 V and a width of 150 µs, with rising and falling times of 8.5 and 18.3 ns, respectively. More importantly, they have nearly no voltage decay.

11.
Rev Sci Instrum ; 93(11): 113310, 2022 Nov 01.
Artículo en Inglés | MEDLINE | ID: mdl-36461426

RESUMEN

A cryogenic beam apparatus for studying neutral clusters has been built and tested. The lowest beam temperature reaches less than 9 K at a repetition rate of 20 Hz. Mechanical decoupling from the refrigerator avoids misalignment during temperature ramping. Adopting a permanent magnet based magnetic deflector eliminates the hysteresis and electric noise of the traditional electromagnet and offers excellent reproducibility of the applied magnetic field. The mass spectrometer can operate in either Mass Spectroscopy Time-Of-Flight mode or Position-Sensitive Time-Of-Flight mode with spatial resolution better than 7 µm. Its performance is demonstrated with niobium and cobalt clusters.

12.
Phys Rev Lett ; 107(5): 057203, 2011 Jul 29.
Artículo en Inglés | MEDLINE | ID: mdl-21867094

RESUMEN

Homonuclear cobalt and iron clusters Co(N) and Fe(N) measured in a cryogenic molecular beam exist in two states with distinct magnetic moments (µ), polarizabilities, and ionization potentials, indicating distinct valences. The µ is approximately quantized: µ(N)∼2Nµ(B) in the ground states and µ(N)(*)∼Nµ(B) in the excited states for Co; µ(N)∼3Nµ(B) and µ(N)(*)∼Nµ(B) for Fe. At a large size, the average µ of the two states converges to the bulk value with diminishing ionization potential differences. The experiments suggest localized ferromagnetism in the two states and that itinerant ferromagnetism emerges from their superposition.

13.
Rev Sci Instrum ; 92(2): 024701, 2021 Feb 01.
Artículo en Inglés | MEDLINE | ID: mdl-33648091

RESUMEN

Pulse delay generators are ubiquitous in laboratories to coordinate and control the timing between different devices in applications that include lasers, mass spectrometers, and other scientific instruments. The most important required characteristics are precision, to control time exactly, and low-jitter, to minimize uncertainty in experiments. Here, we introduce a new design of a high precision and low-jitter digital delay generator based on a Field Programmable Gate Array (FPGA). The final delay is composed of steps of 4.2 ns (coarse delay) with fine steps of 16 ps (fine delay). The coarse delay is generated by a 240 MHz pulse sequence from the FPGA with a 50 MHz clock. An embedded time-to-digital conversion unit is used to measure the interval between the external trigger and the clock signal, which, together with an integrated delay generator, is used to realize the fine delay. Jitter compensation is achieved through a measurement-and-feedback module. A computer interface is designed to control the system through a Nios II processor. Measurements confirm a time resolution of 16 ± 2 ps with jitter below 450 ± 20 ps (at 24 °C) with a maximum delay of 1 s. The whole system is simple in structure and low in cost.

14.
ACS Omega ; 4(10): 14179-14187, 2019 Sep 03.
Artículo en Inglés | MEDLINE | ID: mdl-31508539

RESUMEN

Nitrogen dioxide (NO2) is one of the most dangerous air pollutants that can affect human health even at the ppb (part per billion) level. Thus, the superior sensing performance of nitrogen dioxide gas sensors is an imperative for real-time environmental monitoring. Traditional solid-state sensors based on metal-oxide transistors have the drawbacks of high power consumption, high operating temperature, poor selectivity, and difficult integration with other electronics. In that respect, graphene-based gas sensors have been extensively studied as potential replacements. However, their advantages of high sensing efficiency, low power consumption, and simple electronic integration have been countered by their slow response and poor repeatability. Here, we report the fabrication of high-performance ultraviolet (UV)-assisted room temperature NO2 sensors based on chemical vapor deposition-grown graphene. UV irradiation improves the response of the sensor sevenfold with respect to the dark condition attaining 26% change in resistance at 100 ppm NO2 concentration with a practical detection limit below 1 ppm (42.18 ppb). In addition, the recovery time was shortened fivefold to a few minutes and the excellent repeatability. This work may provide a promising and practical method to mass produce room-temperature NO2 gas sensors for real-time environment monitoring due to its simple fabrication process, low cost, and practicality.

15.
Phys Rev Lett ; 98(11): 113401, 2007 Mar 16.
Artículo en Inglés | MEDLINE | ID: mdl-17501052

RESUMEN

Magnetic moments of Co(N)Mn(M) and Co(N)V(M) clusters (N < or = 60; M < or = N/3) are measured in molecular beams using the Stern-Gerlach deflection method. Surprisingly, the per atom average moments of Co(N)Mn(M) clusters are found to increase with Mn concentration, in contrast to bulk CoMn. The enhancement with Mn doping is found to be independent of cluster size and composition in the size range studied. Meanwhile, Co(N)V(M) clusters show reduction of average moments with increasing V doping, consistent with what is expected in bulk CoV. The results are discussed within the virtual bound states model.

16.
J Chem Phys ; 124(14): 146102, 2006 Apr 14.
Artículo en Inglés | MEDLINE | ID: mdl-16626254

RESUMEN

Water clusters (H(2)O)(n), n

17.
Phys Rev Lett ; 97(12): 123401, 2006 Sep 22.
Artículo en Inglés | MEDLINE | ID: mdl-17025964

RESUMEN

The response of (H2O)(n=3-18) clusters to an electric field is studied by beam deflection. All clusters deflect uniformly, behaving as polarizable particles. The effective polarizabilities exceed the electronic component and increase as the clusters are cooled, revealing a large permanent dipole contribution. The results resolve a discrepancy concerning the polarity of water clusters and show that all species access conformations with moments exceeding 1 D. The data show no evidence for a freezing transition down to approximately 120 K, but suggest a shift in the conformer arrangement at n=8-9.

19.
Phys Rev Lett ; 95(23): 237209, 2005 Dec 02.
Artículo en Inglés | MEDLINE | ID: mdl-16384341

RESUMEN

Magnetizations and magnetic moments of free cobalt clusters Co(N) (12 < N < 200) in a cryogenic (25 K < or = T < or = 100 K) molecular beam were determined from Stern-Gerlach deflections. All clusters preferentially deflect in the direction of the increasing field and the average magnetization resembles the Langevin function for all cluster sizes even at low temperatures. We demonstrate in the avoided crossing model that the average magnetization may result from adiabatic processes of rotating and vibrating clusters in the magnetic field and that spin relaxation is not involved. This resolves a long-standing problem in the interpretation of cluster beam deflection experiments with implications for nanomagnetic systems in general.

20.
Phys Rev Lett ; 93(8): 086803, 2004 Aug 20.
Artículo en Inglés | MEDLINE | ID: mdl-15447214

RESUMEN

Molecular beam Stern-Gerlach deflection measurements on Nb clusters (Nb(N), N<100) show that at very low temperatures the odd-N clusters deflect due to a single unpaired spin that is uncoupled from the cluster. At higher temperatures the spin is coupled and no deflections are observed. Spin uncoupling occurs concurrently with the transition to the recently found ferroelectric state, which has superconductor characteristics [Science 300, 1265 (2003)]]. Spin uncoupling (also seen in V, Ta, and Al clusters) is analogous to the reduction of spin-relaxation rates observed in bulk superconductors below T(c).

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