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1.
Small ; : e2402217, 2024 Jun 25.
Article in English | MEDLINE | ID: mdl-38924273

ABSTRACT

As demand for higher integration density and smaller devices grows, silicon-based complementary metal-oxide-semiconductor (CMOS) devices will soon reach their ultimate limits. 2D transition metal dichalcogenides (TMDs) semiconductors, known for excellent electrical performance and stable atomic structure, are seen as promising materials for future integrated circuits. However, controlled and reliable doping of 2D TMDs, a key step for creating homogeneous CMOS logic components, remains a challenge. In this study, a continuous electrical polarity modulation of monolayer WS2 from intrinsic n-type to ambipolar, then to p-type, and ultimately to a quasi-metallic state is achieved simply by introducing controllable amounts of vanadium (V) atoms into the WS2 lattice as p-type dopants during chemical vapor deposition (CVD). The achievement of purely p-type field-effect transistors (FETs) is particularly noteworthy based on the 4.7 at% V-doped monolayer WS2, demonstrating a remarkable on/off current ratio of 105. Expanding on this triumph, the first initial prototype of ultrathin homogeneous CMOS inverters based on monolayer WS2 is being constructed. These outcomes validate the feasibility of constructing homogeneous CMOS devices through the atomic doping process of 2D materials, marking a significant milestone for the future development of integrated circuits.

2.
Nat Commun ; 15(1): 4440, 2024 May 24.
Article in English | MEDLINE | ID: mdl-38789422

ABSTRACT

Inorganic semiconductors typically have limited p-type behavior due to the scarcity of holes and the localized valence band maximum, hindering the progress of complementary devices and circuits. In this work, we propose an inorganic blending strategy to activate the hole-transporting character in an inorganic semiconductor compound, namely tellurium-selenium-oxygen (TeSeO). By rationally combining intrinsic p-type semimetal, semiconductor, and wide-bandgap semiconductor into a single compound, the TeSeO system displays tunable bandgaps ranging from 0.7 to 2.2 eV. Wafer-scale ultrathin TeSeO films, which can be deposited at room temperature, display high hole field-effect mobility of 48.5 cm2/(Vs) and robust hole transport properties, facilitated by Te-Te (Se) portions and O-Te-O portions, respectively. The nanosphere lithography process is employed to create nanopatterned honeycomb TeSeO broadband photodetectors, demonstrating a high responsibility of 603 A/W, an ultrafast response of 5 µs, and superior mechanical flexibility. The p-type TeSeO system is highly adaptable, scalable, and reliable, which can address emerging technological needs that current semiconductor solutions may not fulfill.

3.
Nat Commun ; 15(1): 728, 2024 Jan 25.
Article in English | MEDLINE | ID: mdl-38272917

ABSTRACT

High synthesis temperatures and specific growth substrates are typically required to obtain crystalline or oriented inorganic functional thin films, posing a significant challenge for their utilization in large-scale, low-cost (opto-)electronic applications on conventional flexible substrates. Here, we explore a pulse irradiation synthesis (PIS) to prepare thermoelectric metal chalcogenide (e.g., Bi2Se3, SnSe2, and Bi2Te3) films on multiple polymeric substrates. The self-propagating combustion process enables PIS to achieve a synthesis temperature as low as 150 °C, with an ultrafast reaction completed within one second. Beyond the photothermoelectric (PTE) property, the thermal coupling between polymeric substrates and bismuth selenide films is also examined to enhance the PTE performance, resulting in a responsivity of 71.9 V/W and a response time of less than 50 ms at 1550 nm, surpassing most of its counterparts. This PIS platform offers a promising route for realizing flexible PTE or thermoelectric devices in an energy-, time-, and cost-efficient manner.

4.
ACS Nano ; 18(1): 1204-1213, 2024 Jan 09.
Article in English | MEDLINE | ID: mdl-38127724

ABSTRACT

Enzyme-mimicking confined catalysis has attracted great interest in heterogeneous catalytic systems that can regulate the geometric or electronic structure of the active site and improve its performance. Herein, a liquid-assisted chemical vapor deposition (LCVD) strategy is proposed to simultaneously confine the single-atom Ru sites onto sidewalls and Janus Ni/NiO nanoparticles (NPs) at the apical nanocavities to thoroughly energize the N-doped carbon nanotube arrays (denoted as Ni/NiO@Ru-NC). The bifunctional Ni/NiO@Ru-NC electrocatalyst exhibits overpotentials of 88 and 261 mV for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) at 100 mA cm-2 in alkaline solution, respectively, all ranking the top tier among the carbon-supported metal-based electrocatalysts. Moreover, once integrated into an anion-exchange membrane water electrolysis (AEMWE) system, Ni/NiO@Ru-NC can act as an efficient and robust bifunctional electrocatalyst to operate stably for 50 h under 500 mA cm-2. Theoretical calculations and experimental exploration demonstrate that the confinement of Ru single atoms and Janus Ni/NiO NPs can regulate the electron distribution with strong orbital couplings to activate the NC nanotube from sidewall to top, thus boosting overall water splitting.

5.
Nano Lett ; 23(11): 5264-5271, 2023 Jun 14.
Article in English | MEDLINE | ID: mdl-37229610

ABSTRACT

Optically readable organic synaptic devices have great potential in both artificial intelligence and photonic neuromorphic computing. Herein, a novel optically readable organic electrochemical synaptic transistor (OR-OEST) strategy is first proposed. The electrochemical doping mechanism of the device was systematically investigated, and the basic biological synaptic behaviors that can be read by optical means are successfully achieved. Furthermore, the flexible OR-OESTs are capable of electrically switching the transparency of semiconductor channel materials in a nonvolatile manner, and thus the multilevel memory can be achieved through optical readout. Finally, the OR-OESTs are developed for the preprocessing of photonic images, such as contrast enhancement and denoising, and feeding the processed images into an artificial neural network, achieving a recognition rate of over 90%. Overall, this work provides a new strategy for the implementation of photonic neuromorphic systems.

6.
Small Methods ; 7(7): e2201567, 2023 Jul.
Article in English | MEDLINE | ID: mdl-37029706

ABSTRACT

The operation stability of halide perovskite devices is the critical issue that impedes their commercialization. The main reasons are that the ambient H2 O molecules can easily deteriorate the perovskites, while the metal electrodes react in different degrees with the perovskites. Herein, one kind of new electrode, the metalloids, is reported, which are much more stable than the conventional noble metals as electrical contacts for halide perovskites. The degradation mechanism of halide perovskites with noble metal electrodes is carefully studied and compared with the metalloid electrodes. It is found that the iodide ions can easily halogenate Cu and Ag in halide perovskites. Although Au is almost not halogenated, it can also decompose the perovskite film. On the contrary, after long-term storage, the metalloid electrodes remain intact on the perovskite film without any degradation. In addition, the long-time operation stability of the perovskite devices with metalloid electrodes is much higher than that of noble metals. First-principles calculations confirm the exceptional stability of the metalloid electrodes.This work explores the ultra-stable electrodes for halide perovskites, paving the way to the large-scale deployment of perovskite-based electronic devices.

7.
Nat Commun ; 14(1): 2431, 2023 Apr 27.
Article in English | MEDLINE | ID: mdl-37105992

ABSTRACT

Chemical bonds, including covalent and ionic bonds, endow semiconductors with stable electronic configurations but also impose constraints on their synthesis and lattice-mismatched heteroepitaxy. Here, the unique multi-scale van der Waals (vdWs) interactions are explored in one-dimensional tellurium (Te) systems to overcome these restrictions, enabled by the vdWs bonds between Te atomic chains and the spontaneous misfit relaxation at quasi-vdWs interfaces. Wafer-scale Te vdWs nanomeshes composed of self-welding Te nanowires are laterally vapor grown on arbitrary surfaces at a low temperature of 100 °C, bringing greater integration freedoms for enhanced device functionality and broad applicability. The prepared Te vdWs nanomeshes can be patterned at the microscale and exhibit high field-effect hole mobility of 145 cm2/Vs, ultrafast photoresponse below 3 µs in paper-based infrared photodetectors, as well as controllable electronic structure in mixed-dimensional heterojunctions. All these device metrics of Te vdWs nanomesh electronics are promising to meet emerging technological demands.

8.
Adv Mater ; 35(12): e2210854, 2023 Mar.
Article in English | MEDLINE | ID: mdl-36621966

ABSTRACT

Atomically 2D layered ferroelectric semiconductors, in which the polarization switching process occurs within the channel material itself, offer a new material platform that can drive electronic components toward structural simplification and high-density integration. Here, a room-temperature 2D layered ferroelectric semiconductor, bismuth oxychalcogenides (Bi2 O2 Se), is investigated with a thickness down to 7.3 nm (≈12 layers) and piezoelectric coefficient (d33 ) of 4.4 ± 0.1 pm V-1 . The random orientations and electrically dependent polarization of the dipoles in Bi2 O2 Se are separately uncovered owing to the structural symmetry-breaking at room temperature. Specifically, the interplay between ferroelectricity and semiconducting characteristics of Bi2 O2 Se is explored on device-level operation, revealing the hysteresis behavior and memory window (MW) formation. Leveraging the ferroelectric polarization originating from Bi2 O2 Se, the fabricated device exhibits "smart" photoresponse tunability and excellent electronic characteristics, e.g., a high on/off current ratio > 104 and a large MW to the sweeping range of 47% at VGS  = ±5 V. These results demonstrate the synergistic combination of ferroelectricity with semiconducting characteristics in Bi2 O2 Se, laying the foundation for integrating sensing, logic, and memory functions into a single material system that can overcome the bottlenecks in von Neumann architecture.

9.
Nano Lett ; 23(3): 812-819, 2023 Feb 08.
Article in English | MEDLINE | ID: mdl-36579841

ABSTRACT

Converting vapor precursors to solid nanostructures via a liquid noble-metal seed is a common vapor deposition principle. However, such a noble-metal-seeded process is excluded from the crystalline halide perovskite synthesis, mainly hindered by the growth mechanism shortness. Herein, powered by a spontaneous exothermic nucleation process (ΔH < 0), the Au-seeded CsPbI3 nanowires (NWs) growth is realized based on a vapor-liquid-solid (VLS) growth mode. It is energetically favored that the Au seeds are reacted with a Pb vapor precursor to form molten Au-Pb droplets at temperatures down to 212 °C, further triggering the low-temperature VLS growth of CsPbI3 NWs. More importantly, this Au-seeded process reduces in-bandgap trap states and consequently avoids Shockley-Read-Hall recombination, contributing to outstanding photodetector performances. Our work extends the powerful Au-seeded VLS growth mode to the emerging halide perovskites, which will facilitate their nanostructures with tailored material properties.

10.
ACS Nano ; 16(7): 11036-11048, 2022 Jul 26.
Article in English | MEDLINE | ID: mdl-35758898

ABSTRACT

The incapability of modulating the photoresponse of assembled heterostructure devices has remained a challenge for the development of optoelectronics with multifunctionality. Here, a gate-tunable and anti-ambipolar phototransistor is reported based on 1D GaAsSb nanowire/2D MoS2 nanoflake mixed-dimensional van der Waals heterojunctions. The resulting heterojunction shows apparently asymmetric control over the anti-ambipolar transfer characteristics, possessing potential to implement electronic functions in logic circuits. Meanwhile, such an anti-ambipolar device allows the synchronous adjustment of band slope and depletion regions by gating in both components, thereby giving rise to the gate-tunability of the photoresponse. Coupled with the synergistic effect of the materials in different dimensionality, the hybrid heterojunction can be readily modulated by the external gate to achieve a high-performance photodetector exhibiting a large on/off current ratio of 4 × 104, fast response of 50 µs, and high detectivity of 1.64 × 1011 Jones. Due to the formation of type-II band alignment and strong interfacial coupling, a prominent photovoltaic response is explored in the heterojunction as well. Finally, a visible image sensor based on this hybrid device is demonstrated with good imaging capability, suggesting the promising application prospect in future optoelectronic systems.

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