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1.
Nature ; 614(7946): 88-94, 2023 02.
Artigo em Inglês | MEDLINE | ID: mdl-36653458

RESUMO

Two-dimensional (2D) materials and their heterostructures show a promising path for next-generation electronics1-3. Nevertheless, 2D-based electronics have not been commercialized, owing mainly to three critical challenges: i) precise kinetic control of layer-by-layer 2D material growth, ii) maintaining a single domain during the growth, and iii) wafer-scale controllability of layer numbers and crystallinity. Here we introduce a deterministic, confined-growth technique that can tackle these three issues simultaneously, thus obtaining wafer-scale single-domain 2D monolayer arrays and their heterostructures on arbitrary substrates. We geometrically confine the growth of the first set of nuclei by defining a selective growth area via patterning SiO2 masks on two-inch substrates. Owing to substantial reduction of the growth duration at the micrometre-scale SiO2 trenches, we obtain wafer-scale single-domain monolayer WSe2 arrays on the arbitrary substrates by filling the trenches via short growth of the first set of nuclei, before the second set of nuclei is introduced, thus without requiring epitaxial seeding. Further growth of transition metal dichalcogenides with the same principle yields the formation of single-domain MoS2/WSe2 heterostructures. Our achievement will lay a strong foundation for 2D materials to fit into industrial settings.

2.
Small ; 20(25): e2307360, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38217294

RESUMO

Ion diffusion is a fundamentally important process in understanding and manipulating the optoelectronic properties of semiconductors. Most current studies on ionic diffusion have been focusing on perovskite polycrystalline thin films and nanocrystals. However, the random orientation and grain boundaries can heavily interfere with the kinetics of ion diffusion, where the experimental results only reveal the average ion exchange kinetics and the actual ion diffusion mechanisms perpendicular to the direction of individual crystal facets remain unclear. Here, the anion (Cl, I) diffusion anisotropy on (111) and (100) facets of CsPbBr3 single crystals is demonstrated. The as-grown single crystals with (111) and (100) facets exhibit anisotropic growth with different halide incorporation, which lead to different resulting optoelectronic properties. Combined experimental characterizations and theoretical calculations reveal that the (111) CsPbBr3 shows a faster anion diffusion behavior compared with that of the (100) CsPbBr3, with a lower diffusion energy barrier, a larger built-in electric field, and lower inverse defect formation energy. The work highlights the anion diffusion anisotropic mechanisms perpendicular to the direction of individual crystal facets for optimizing and designing perovskite optoelectronic devices.

3.
Angew Chem Int Ed Engl ; 63(32): e202407675, 2024 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-38770616

RESUMO

Manipulating the crystal orientation plays a crucial role in the conversion efficiency during second harmonic generation (SHG). Here, we provide a new strategy in controlling the surface-dependent anisotropic SHG with the precise design of (101) and (2 1 ‾ ${\bar 1}$ 0) MAGeI3 facets. Based on the SHG measurement, the (101) MAGeI3 single crystal exhibits larger SHG (1.3×(2 1 ‾ ${\bar 1}$ 0) MAGeI3). Kelvin probe force microscopy imaging shows a smaller work function for the (101) MAGeI3 compared with the (2 1 ‾ ${\bar 1}$ 0), which indirectly demonstrates the stronger intrinsic polarization on the (101) surface. X-ray photoelectron spectroscopy confirms the band bending within the (101) facet. Temperature-dependent steady-state and time-resolved photoluminescence spectroscopy show shorter lifetime and wider emission band in the (101) MAGeI3 single crystal, revealing the higher defect states. Additionally, powder X-ray diffraction patterns show the (101) MAGeI3 possesses larger in-plane polar units [GeI3]- density, which could directly enhance the spontaneous polarization in the (101) facet. Density functional theory (DFT) calculation further demonstrates the higher intrinsic polarization in the (101) facet compared with the (2 1 ‾ ${\bar 1}$ 0) facet, and the larger built-in electric field in the (101) facet facilitates surface vacancy defect accumulation. Our work provides a new angle in tuning and optimizing hybrid perovskite-based nonlinear optical materials.

4.
Nano Lett ; 22(21): 8670-8678, 2022 Nov 09.
Artigo em Inglês | MEDLINE | ID: mdl-36256439

RESUMO

Yellow-green luminescence (YGL) competes with near-bandgap emission (NBE) for carrier recombination channels, thereby reducing device efficiency; yet uncovering the origin of YGL remains a major challenge. In this paper, nearly stress-free and low dislocation density self-assembled GaN microdisks were synthesized by Na-flux method. The YGL of GaN microdisks highly depend on their polar facets. Variable accelerating voltage/power CL, variable temperature PL, and Raman spectroscopy are further performed to clarify the origin of polarity dependence of GaN microdisk YGL behavior, which indicates its independence of dislocations, surface effects, stress, crystalline quality, and gallium vacancies. It was found that the incorporation ability of carbon impurities in the polar (0001) facet is greater than that in the semipolar (101̅1) facets, producing higher content of CN or CNON defects, resulting in a more pronounced YGL in the polar (0001) facet of GaN.

5.
Nano Lett ; 21(1): 500-506, 2021 Jan 13.
Artigo em Inglês | MEDLINE | ID: mdl-33372788

RESUMO

In this work, we demonstrate enhancement-mode field-effect transistors by an atomic-layer-deposited (ALD) amorphous In2O3 channel with thickness down to 0.7 nm. Thickness is found to be critical on the materials and electron transport of In2O3. Controllable thickness of In2O3 at atomic scale enables the design of sufficient 2D carrier density in the In2O3 channel integrated with the conventional dielectric. The threshold voltage and channel carrier density are found to be considerably tuned by channel thickness. Such a phenomenon is understood by the trap neutral level (TNL) model, where the Fermi-level tends to align deeply inside the conduction band of In2O3 and can be modulated to the bandgap in atomic layer thin In2O3 due to the quantum confinement effect, which is confirmed by density function theory (DFT) calculation. The demonstration of enhancement-mode amorphous In2O3 transistors suggests In2O3 is a competitive channel material for back-end-of-line (BEOL) compatible transistors and monolithic 3D integration applications.

6.
ACS Appl Mater Interfaces ; 16(10): 13258-13266, 2024 Mar 13.
Artigo em Inglês | MEDLINE | ID: mdl-38422472

RESUMO

The high contact resistance of transition metal dichalcogenide (TMD)-based devices is receiving considerable attention due to its limitation on electronic performance. The mechanism of Fermi level (EF) pinning, which causes the high contact resistance, is not thoroughly understood to date. In this study, the metal (Ni and Ag)/Mo-TMD surfaces and interfaces are characterized by X-ray photoelectron spectroscopy, atomic force microscopy, scanning tunneling microscopy and spectroscopy, and density functional theory systematically. Ni and Ag form covalent and van der Waals (vdW) interfaces on Mo-TMDs, respectively. Imperfections are detected on Mo-TMDs, which lead to electronic and spatial variations. Gap states appear after the adsorption of single and two metal atoms on Mo-TMDs. The combination of the interface reaction type (covalent or vdW), the imperfection variability of the TMD materials, and the gap states induced by contact metals with different weights are concluded to be the origins of EF pinning.

7.
ACS Nano ; 17(20): 20353-20365, 2023 Oct 24.
Artigo em Inglês | MEDLINE | ID: mdl-37788682

RESUMO

Tungsten transition metal dichalcogenides (W-TMDs) are intriguing due to their properties and potential for application in next-generation electronic devices. However, strong Fermi level (EF) pinning manifests at the metal/W-TMD interfaces, which could tremendously restrain the carrier injection into the channel. In this work, we illustrate the origins of EF pinning for Ni and Ag contacts on W-TMDs by considering interface chemistry, band alignment, impurities, and imperfections of W-TMDs, contact metal adsorption mechanism, and the resultant electronic structure. We conclude that the origins of EF pinning at a covalent contact metal/W-TMD interface, such as Ni/W-TMDs, can be attributed to defects, impurities, and interface reaction products. In contrast, for a van der Waals contact metal/TMD system such as Ag/W-TMDs, the primary factor responsible for EF pinning is the electronic modification of the TMDs resulting from the defects and impurities with the minor impact of metal-induced gap states. The potential strategies for carefully engineering the metal deposition approach are also discussed. This work unveils the origins of EF pinning at metal/TMD interfaces experimentally and theoretically and provides guidance on further enhancing and improving the device performance.

8.
ACS Appl Mater Interfaces ; 14(22): 25670-25679, 2022 Jun 08.
Artigo em Inglês | MEDLINE | ID: mdl-35609177

RESUMO

The development of high-performance p-type oxides with wide band gap and high hole mobility is critical for the application of oxide semiconductors in back-end-of-line (BEOL) complementary metal-oxide-semiconductor (CMOS) devices. SnO has been intensively studied as a high-mobility p-type oxide due to its low effective hole mass resulting from the hybridized O-2p/Sn-5s orbital character at the valence band edge. However, SnO has a very small band gap (∼0.7 eV) for practical p-type oxide devices. In this work, we report an engineering method to enhance the band gap and hole mobility in SnO. It is found that both the band gap and the hole mobility of a layer-structured SnO increase with the interlayer stacking spacing change. By exploiting this unique electronic structure feature, we propose expanding the interlayer spacing by interlayer intercalation to engineer the band gap and p-type mobility in SnO. Small molecules like NH3 and CH4 are shown to be capable of expanding the interlayer spacing and of increasing the band gap and hole mobility in SnO and thus could potentially serve as the interlayer intercalants. The results provide a viable way for the experimental realization of wide-band-gap and high hole-mobility p-type SnO for BEOL vertical CMOS device applications.

9.
Nat Commun ; 13(1): 7501, 2022 Dec 06.
Artigo em Inglês | MEDLINE | ID: mdl-36473851

RESUMO

Solid state quantum defects are promising candidates for scalable quantum information systems which can be seamlessly integrated with the conventional semiconductor electronic devices within the 3D monolithically integrated hybrid classical-quantum devices. Diamond nitrogen-vacancy (NV) center defects are the representative examples, but the controlled positioning of an NV center within bulk diamond is an outstanding challenge. Furthermore, quantum defect properties may not be easily tuned for bulk crystalline quantum defects. In comparison, 2D semiconductors, such as transition metal dichalcogenides (TMDs), are promising solid platform to host a quantum defect with tunable properties and a possibility of position control. Here, we computationally discover a promising defect family for spin qubit realization in 2D TMDs. The defects consist of transition metal atoms substituted at chalcogen sites with desirable spin-triplet ground state, zero-field splitting in the tens of GHz, and strong zero-phonon coupling to optical transitions in the highly desirable telecom band.

10.
ACS Nano ; 16(12): 21536-21545, 2022 Dec 27.
Artigo em Inglês | MEDLINE | ID: mdl-36446079

RESUMO

High drive current is a critical performance parameter in semiconductor devices for high-speed, low-power logic applications or high-efficiency, high-power, high-speed radio frequency (RF) analogue applications. In this work, we demonstrate an In2O3 transistor grown by atomic layer deposition (ALD) at back-end-of-line (BEOL) compatible temperatures with a record high drain current in planar FET, exceeding 10 A/mm, the performance of which is 2-3 times better than all known transistors with semiconductor channels. A high transconductance reaches 4 S/mm, recorded among all transistors with a planar structure. Planar FETs working ballistically or quasi-ballistically are exploited as one of the simplest platforms to investigate the intrinsic transport properties. It is found experimentally and theoretically that a high carrier density and high electron velocity both contribute to this high on-state performance in ALD In2O3 transistors, which is made possible by the high-quality oxide/oxide interface, the metal-like charge-neutrality-level (CNL) alignment, and the high band velocities induced by the low density-of-state (DOS). Experimental Hall, I-V, and split C-V measurements at room temperature confirm a high carrier density of up to 6-7 × 1013 /cm2 and a high velocity of about 107 cm/s, well-supported by density functional theory (DFT) calculations. The simultaneous demonstration of such high carrier concentration and average band velocity is enabled by the exploitation of the ultrafast pulse scheme and heat dissipation engineering.

11.
Nanomaterials (Basel) ; 12(23)2022 Dec 06.
Artigo em Inglês | MEDLINE | ID: mdl-36500970

RESUMO

In this work, an AlGaN-based Deep-Ultraviolet Light-Emitting Diode structure has been designed and simulated for the zincblende and wurtzite approaches, where the polarization effect is included. DFT analysis was performed to determine the band gap direct-to-indirect cross-point limit, AlN carrier mobility, and activation energies for p-type dopants. The multiple quantum wells analysis describes the emission in the deep-ultraviolet range without exceeding the direct-to-indirect bandgap cross-point limit of around 77% of Al content. Moreover, the quantum-confined Stark effect on wavefunctions overlapping has been studied, where Al-graded quantum wells reduce it. Both zincblende and wurtzite have improved electrical and optical characteristics by including a thin AlGaN with low Al content. Mg and Be acceptor activation energies have been calculated at 260 meV and 380 meV for Be and Mg acceptor energy, respectively. The device series resistance has been decreased by using Be instead of Mg as the p-type dopant from 3 kΩ to 0.7 kΩ.

12.
J Phys Condens Matter ; 33(35)2021 Jul 05.
Artigo em Inglês | MEDLINE | ID: mdl-34139679

RESUMO

Exploiting two-dimensional (2D) materials with natural band gaps and anisotropic quasi-one-dimensional (quasi-1D) carrier transport character is essential in high-performance nanoscale transistors and photodetectors. Herein, the stabilities, electronic structures and carrier mobilities of 2D monolayer ternary metal iodides MLaI5(M = Mg, Ca, Sr, Ba) have been explored by utilizing first-principles calculations combined with numerical calculations. It is found that exfoliating MLaI5monolayers are feasible owing to low cleavage energy of 0.19-0.21 J m-2and MLaI5monolayers are thermodynamically stable based on phonon spectra. MLaI5monolayers are semiconductors with band gaps ranging from 2.08 eV for MgLaI5to 2.51 eV for BaLaI5. The carrier mobility is reasonably examined considering both acoustic deformation potential scattering and polar optical phonon scattering mechanisms. All MLaI5monolayers demonstrate superior anisotropic and quasi-1D carrier transport character due to the striped structures. In particular, the anisotropic ratios of electron and hole mobilities along different directions reach hundreds and tens for MLaI5monolayers, respectively. Thus, the effective electron-hole spatial separation could be actually achieved. Moreover, the absolute locations of band edges of MLaI5monolayers have been aligned. These results would provide fundamental insights for MLaI5monolayers applying in nano-electronic and optoelectronic devices.

13.
Sci Rep ; 10(1): 16858, 2020 Oct 08.
Artigo em Inglês | MEDLINE | ID: mdl-33033291

RESUMO

We have studied the Mg doping of cubic GaN grown by plasma-assisted Molecular Beam Epitaxy (PA-MBE) over GaAs (001) substrates. In particular, we concentrated on conditions to obtain heavy p-type doping to achieve low resistance films which can be used in bipolar devices. We simulated the Mg-doped GaN transport properties by density functional theory (DFT) to compare with the experimental data. Mg-doped GaN cubic epitaxial layers grown under optimized conditions show a free hole carrier concentration with a maximum value of 6 × 1019 cm-3 and mobility of 3 cm2/Vs. Deep level transient spectroscopy shows the presence of a trap with an activation energy of 114 meV presumably associated with nitrogen vacancies, which could be the cause for the observed self-compensation behavior in heavily Mg-doped GaN involving Mg-VN complexes. Furthermore, valence band analysis by X-ray photoelectron spectroscopy and photoluminescence spectroscopy revealed an Mg ionization energy of about 100 meV, which agrees quite well with the value of 99.6 meV obtained by DFT. Our results show that the cubic phase is a suitable alternative to generate a high free hole carrier concentration for GaN.

15.
ACS Appl Mater Interfaces ; 8(11): 7595-600, 2016 Mar 23.
Artigo em Inglês | MEDLINE | ID: mdl-26939534

RESUMO

Indium (In) out-diffusion through high-k oxides severely undermines the thermal reliability of the next generation device of III-V/high-k based metal oxide semiconductor (MOS). To date, the microscopic mechanism of In diffusion is not yet fully understood. Here, we utilize angle resolved X-ray photoelectron spectroscopy (ARXPS) and density functional theory (DFT) to explore In diffusion in high-k oxide HfO2. Our ARXPS results confirm the In diffusion through as-prepared and annealed HfO2 grown on InP substrate. The theoretical results show that the In diffusion barrier is reduced to ∼0.88 eV in the presence of oxygen vacancies (VO), whereas this barrier is as high as ∼4.78 eV in pristine HfO2. Fundamentally, we found that the high feasibility of In diffusion is owing to In nonbonding with its neighboring atoms. These findings can be extended to understand the In diffusion in other materials in addition to HfO2.

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