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1.
Nano Lett ; 23(11): 5250-5256, 2023 Jun 14.
Article in English | MEDLINE | ID: mdl-37220075

ABSTRACT

Structural or crystal asymmetry is a necessary condition for the emergence of zero-bias photocurrent in light detectors. Structural asymmetry has been typically achieved via p-n doping, which is a technologically complex process. Here, we propose an alternative approach to achieve zero-bias photocurrent in two-dimensional (2D) material flakes exploiting the geometrical nonequivalence of source and drain contacts. As a prototypical example, we equip a square-shaped flake of PdSe2 with mutually orthogonal metal leads. Upon uniform illumination with linearly polarized light, the device demonstrates nonzero photocurrent which flips its sign upon 90° polarization rotation. The origin of zero-bias photocurrent lies in a polarization-dependent lightning-rod effect. It enhances the electromagnetic field at one contact from the orthogonal pair and selectively activates the internal photoeffect at the respective metal-PdSe2 Schottky junction. The proposed technology of contact engineering is independent of a particular light-detection mechanism and can be extended to arbitrary 2D materials.

2.
Nanotechnology ; 35(11)2023 Dec 27.
Article in English | MEDLINE | ID: mdl-38055966

ABSTRACT

Fermi-level pinning caused by the kinetic damage during metallization has been recognized as one of the major reasons for the non-ideal behavior of electrical contacts, forbidding reaching the Schottky-Mott limit. In this manuscript, we present a scalable technique wherein Indium, a low-work-function metal, is diffused to contact a few-layered MoS2flake. The technique exploits a smooth outflow of Indium over gold electrodes to make edge contacts to pre-transferred MoS2flakes. We compare the performance of three pairs of contacts made onto the same MoS2flake, the bottom-gold, top-gold, and Indium contacts, and find that the Indium contacts are superior to other contacts. The Indium contacts maintain linearI-Vcharacteristics down to cryogenic temperatures with an extracted Schottky barrier height of ∼2.1 meV. First-principle calculations show the induced in-gap states close to the Fermi level, and the damage-free contact interface could be the reason for the nearly Ohmic behavior of the Indium/MoS2interface.

3.
Sensors (Basel) ; 22(24)2022 Dec 10.
Article in English | MEDLINE | ID: mdl-36560055

ABSTRACT

Two-dimensional (2D) molybdenum disulfide (MoS2) is a promising material for constructing high-performance visible photosensor arrays because of its high mobility and scale-up process. These distinct properties enable the construction of practical optoelectrical sensor arrays. However, contact engineering for MoS2 films is not still optimized. In this work, we inserted a graphene interlayer between the MoS2 films and Au contacts (graphene/Au) via the wet-transfer method to boost the device performance. Using graphene/Au contacts, outstanding electrical properties, namely field-effect mobility of 12.06 cm2/V∙s, on/off current ratio of 1.0 × 107, and responsivity of 610 A/W under illumination at 640 nm, were achieved. These favorable results were from the Fermi-level depinning effect induced by the graphene interlayer. Our results may help to construct large-area photonic sensor arrays based on 2D materials.

4.
Nano Lett ; 20(4): 2443-2451, 2020 Apr 08.
Article in English | MEDLINE | ID: mdl-32191480

ABSTRACT

In optoelectronic devices based on two-dimensional (2D) semiconductor heterojunctions, the efficient charge transport of photogenerated carriers across the interface is a critical factor to determine the device performances. Here, we report an unexplored approach to boost the optoelectronic device performances of the WSe2-MoS2 p-n heterojunctions via the monolithic-oxidation-induced doping and resultant modulation of the interface band alignment. In the proposed device, the atomically thin WOx layer, which is directly formed by layer-by-layer oxidation of WSe2, is used as a charge transport layer for promoting hole extraction. The use of the ultrathin oxide layer significantly enhanced the photoresponsivity of the WSe2-MoS2 p-n junction devices, and the power conversion efficiency increased from 0.7 to 5.0%, maintaining the response time. The enhanced characteristics can be understood by the formation of the low Schottky barrier and favorable interface band alignment, as confirmed by band alignment analyses and first-principle calculations. Our work suggests a new route to achieve interface contact engineering in the heterostructures toward realizing high-performance 2D optoelectronics.

5.
Acta Crystallogr D Biol Crystallogr ; 71(Pt 10): 2040-53, 2015 Oct.
Article in English | MEDLINE | ID: mdl-26457428

ABSTRACT

The small nuclear ribonucleoproteins (snRNPs) U1, U2, U4/6 and U5 are major constituents of the pre-mRNA processing spliceosome. They contain a common RNP core that is formed by the ordered binding of Sm proteins onto the single-stranded Sm site of the snRNA. Although spontaneous in vitro, assembly of the Sm core requires assistance from the PRMT5 and SMN complexes in vivo. To gain insight into the key steps of the assembly process, the crystal structures of two assembly intermediates of U snRNPs termed the 6S and 8S complexes have recently been reported. These multimeric protein complexes could only be crystallized after the application of various rescue strategies. The developed strategy leading to the crystallization and solution of the 8S crystal structure was subsequently used to guide a combination of rational crystal-contact optimization with surface-entropy reduction of crystals of the related 6S complex. Conversely, the resulting high-resolution 6S crystal structure was used during the restrained refinement of the 8S crystal structure.


Subject(s)
Drosophila Proteins/chemistry , Drosophila melanogaster/chemistry , Ribonucleoproteins, Small Nuclear/chemistry , Spliceosomes/chemistry , Animals , Crystallization , Crystallography, X-Ray , Entropy , Models, Molecular
6.
ACS Nano ; 18(23): 15107-15113, 2024 Jun 11.
Article in English | MEDLINE | ID: mdl-38819119

ABSTRACT

Superconducting-based electronic devices have shown great potential for future quantum computing applications. One key building block device is a superconducting field-effect transistor based on a superconductor-semiconductor-superconductor Josephson-junction (JJ) with a gate-tunable semiconducting channel. However, the performance of such devices is highly dependent on the quality of the superconductor to semiconductor interface. In this study, we present an alternative method to obtain a high-quality interface by using intimate contact. We investigate the proximity-induced superconductivity in chiral crystal tellurium (Te) and fabricate a PdxTe-Te-PdxTe JJ with an ambipolar supercurrent that is gate-tunable and exhibits multiple Andreev reflections. The semiconducting two-dimensional Te single crystal is grown hydrothermally and partially converted to superconducting PdxTe by controlled annealing. Our work demonstrates a promising path for realizing controllable superconducting electronic devices with high-quality superconducting interfaces; thus, we can continue to advance the field of quantum computing and other interface-based technologies.

7.
Adv Mater ; 36(11): e2305371, 2024 Mar.
Article in English | MEDLINE | ID: mdl-37824715

ABSTRACT

The latest developments in fiber design and materials science are paving the way for fibers to evolve from parts in passive components to functional parts in active fabrics. Designing conformable, organic electrochemical transistor (OECT) structures using poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) fibers has excellent potential for low-cost wearable bioelectronics, bio-hybrid devices, and adaptive neuromorphic technologies. However, to achieve high-performance, stable devices from PEDOT:PSS fibers, approaches are required to form electrodes on fibers with small diameters and poor wettability, that leads to irregular coatings. Additionally, PEDOT:PSS-fiber fabrication needs to move away from small batch processing to roll-to-roll or continuous processing. Here, it is shown that synergistic effects from a superior electrode/organic interface, and exceptional fiber alignment from continuous processing, enable PEDOT:PSS fiber-OECTs with stable contacts, high µC* product (1570.5 F cm-1 V-1 s-1 ), and high hole mobility over 45 cm2 V-1 s-1 . Fiber-electrochemical neuromorphic organic devices (fiber-ENODes) are developed to demonstrate that the high mobility fibers are promising building blocks for future bio-hybrid technologies. The fiber-ENODes demonstrate synaptic weight update in response to dopamine, as well as a form factor closely matching the neuronal axon terminal.

8.
ACS Appl Mater Interfaces ; 16(9): 12095-12105, 2024 Mar 06.
Article in English | MEDLINE | ID: mdl-38384197

ABSTRACT

Two-dimensional transition metal dichalcogenides (2D TMDCs) are considered promising alternatives to Si as channel materials because of the possibility of retaining their superior electronic transport properties even at atomic body thicknesses. However, the realization of high-performance 2D TMDC field-effect transistors remains a challenge owing to Fermi-level pinning (FLP) caused by gap states and the inherent high Schottky barrier height (SBH) within the metal contact and channel layer. This study demonstrates that high-quality van der Waals (vdW) heterojunction-based contacts can be formed by depositing semimetallic TiS2 onto monolayer (ML) MoS2. After confirming the successful formation of a TiS2/ML MoS2 heterojunction, the contact properties of vdW semimetal TiS2 were thoroughly investigated. With clean interfaces of the TiS2/ML MoS2 heterojunctions, atomic-layer-deposited TiS2 can induce gap-state saturation and suppress FLP. Consequently, compared with conventional evaporated metal electrodes, the TiS2/ML MoS2 heterojunctions exhibit a lower SBH of 8.54 meV and better contact properties. This, in turn, substantially improves the overall performance of the device, including its on-current, subthreshold swing, and threshold voltage. Furthermore, we believe that our proposed strategy for vdW-based contact formation will contribute to the development of 2D materials used in next-generation electronics.

9.
ACS Nano ; 18(5): 4180-4188, 2024 Feb 06.
Article in English | MEDLINE | ID: mdl-38271989

ABSTRACT

Recent advancements in ferroelectric field-effect transistors (FeFETs) using two-dimensional (2D) semiconductor channels and ferroelectric Al0.68Sc0.32N (AlScN) allow high-performance nonvolatile devices with exceptional ON-state currents, large ON/OFF current ratios, and large memory windows (MW). However, previous studies have solely focused on n-type FeFETs, leaving a crucial gap in the development of p-type and ambipolar FeFETs, which are essential for expanding their applicability to a wide range of circuit-level applications. Here, we present a comprehensive demonstration of n-type, p-type, and ambipolar FeFETs on an array scale using AlScN and multilayer/monolayer WSe2. The dominant injected carrier type is modulated through contact engineering at the metal-semiconductor junction, resulting in the realization of all three types of FeFETs. The effect of contact engineering on the carrier injection is further investigated through technology-computer-aided design simulations. Moreover, our 2D WSe2/AlScN FeFETs achieve high electron and hole current densities of ∼20 and ∼10 µA/µm, respectively, with a high ON/OFF ratio surpassing ∼107 and a large MW of >6 V (0.14 V/nm).

10.
Nanomaterials (Basel) ; 14(5)2024 Mar 06.
Article in English | MEDLINE | ID: mdl-38470809

ABSTRACT

Tungsten diselenide (WSe2) has emerged as a promising ambipolar semiconductor material for field-effect transistors (FETs) due to its unique electronic properties, including a sizeable band gap, high carrier mobility, and remarkable on-off ratio. However, engineering the contacts to WSe2 remains an issue, and high contact barriers prevent the utilization of the full performance in electronic applications. Furthermore, it could be possible to tune the contacts to WSe2 for effective electron or hole injection and consequently pin the threshold voltage to either conduction or valence band. This would be the way to achieve complementary metal-oxide-semiconductor devices without doping of the channel material.This study investigates the behaviour of two-dimensional WSe2 field-effect transistors with multi-layer palladium diselenide (PdSe2) as a contact material. We demonstrate that PdSe2 contacts favour hole injection while preserving the ambipolar nature of the channel material. This consequently yields high-performance p-type WSe2 devices with PdSe2 van der Waals contacts. Further, we explore the tunability of the contact interface by selective laser alteration of the WSe2 under the contacts, enabling pinning of the threshold voltage to the valence band of WSe2, yielding pure p-type operation of the devices.

11.
ACS Appl Mater Interfaces ; 16(6): 7593-7603, 2024 Feb 14.
Article in English | MEDLINE | ID: mdl-38315799

ABSTRACT

Materials with van der Waals (vdW) unit structures rely on weak interunit vdW forces, facilitating physical separation and advancing nanomaterial research with remarkable electrical properties. Recently, there has been growing interest in one-dimensional (1D) vdW materials, celebrated for their advantageous properties, characterized by reduced dimensionality and the absence of dangling bonds. In this context, we synthesize Ta2Pt3S8, a 1D vdW material, and assess its suitability for field-effect transistor (FET) applications. Spectroscopic analysis and electrical characterization confirmed that the band gap and work function of Ta2Pt3S8 are 1.18 and 4.77 eV, respectively. Leveraging various electrode materials, we fabricated n-type FETs based on Ta2Pt3S8 and identified Cr as the optimal electrode, exhibiting a high mobility of 57 cm2 V-1 s-1. In addition, we analyzed the electron transport mechanism in n-type FETs by investigating Schottky barrier height, Schottky barrier tunneling width, and contact resistance. Furthermore, we successfully fabricated p-type operating Ta2Pt3S8 FETs using a molybdenum trioxide (MoO3) layer as a high work function contact electrode. Finally, we achieved Ta2Pt3S8 nanowire rectifying diodes by creating a p-n junction with asymmetric contact electrodes of Cr and MoO3, demonstrating an ideality factor of 1.06. These findings highlight the electronic properties of Ta2Pt3S8, positioning it as a promising 1D vdW material for future nanoelectronics and functional vdW-based device applications.

12.
Adv Mater ; 34(18): e2108616, 2022 May.
Article in English | MEDLINE | ID: mdl-34995372

ABSTRACT

Contact engineering is a prerequisite for achieving desirable functionality and performance of semiconductor electronics, which is particularly critical for organic-inorganic hybrid halide perovskites due to their ionic nature and highly reactive interfaces. Although the interfaces between perovskites and charge-transporting layers have attracted lots of attention due to the photovoltaic and light-emitting diode applications, achieving reliable perovskite/electrode contacts for electronic devices, such as transistors and memories, remains as a bottleneck. Herein, a critical review on the elusive nature of perovskite/electrode interfaces with a focus on the interfacial electrochemistry effects is presented. The basic guidelines of electrode selection are given for establishing non-polarized interfaces and optimal energy level alignment for perovskite materials. Furthermore, state-of-the-art strategies on interface-related electrode engineering are reviewed and discussed, which aim at achieving ohmic transport and eliminating hysteresis in perovskite devices. The role and multiple functionalities of self-assembled monolayers that offer a unique approach toward improving perovskite/electrode contacts are also discussed. The insights on electrode engineering pave the way to advancing stable and reliable perovskite devices in diverse electronic applications.

13.
ACS Nano ; 16(6): 8827-8836, 2022 Jun 28.
Article in English | MEDLINE | ID: mdl-35435652

ABSTRACT

A rapid surge in global energy consumption has led to a greater demand for renewable energy to overcome energy resource limitations and environmental problems. Recently, a number of van der Waals materials have been highlighted as efficient absorbers for very thin and highly efficient photovoltaic (PV) devices. Despite the predicted potential, achieving power conversion efficiencies (PCEs) above 5% in PV devices based on van der Waals materials has been challenging. Here, we demonstrate a vertical WSe2 PV device with a high PCE of 5.44% under one-sun AM1.5G illumination. We reveal the multifunctional nature of a tungsten oxide layer, which promotes a stronger internal electric field by overcoming limitations imposed by the Fermi-level pinning at WSe2 interfaces and acts as an electron-selective contact in combination with monolayer graphene. Together with the developed bottom contact scheme, this simple yet effective contact engineering method improves the PCE by more than five times.

14.
ACS Appl Mater Interfaces ; 14(11): 13560-13571, 2022 Mar 23.
Article in English | MEDLINE | ID: mdl-35258275

ABSTRACT

Efficient charge injection/extraction from/to contact electrodes is essential to realize organic electronic and optoelectronic devices with optimum characteristics for many applications. Herein, we studied a versatile reductive interlayer based on sodium borohydride (NaBH4) to control the contact properties of the staggered organic field-effect transistors (OFETs) either by doping and/or by regulating the contribution of charge carriers. The versatile functionalities of the NaBH4 layer are mainly determined by the alignment of frontier molecular orbitals of donor-acceptor (D-A) type copolymer semiconductors and the work function of the contact electrode. After incorporating the NaBH4 layer, the work function of the bottom-contact gold electrode can be decreased significantly by 1.0 eV, which makes it favorable to efficient electron injection. An Ohmic contact is achieved by the spontaneous injection of electrons to the n-type organic semiconductors with high electron affinity while converting the OFET operation mode to n-type characteristics by blocking the counter-charge carriers for the other types of ambipolar and p-type semiconductors. The solution-processed reducing agent can be a valuable approach to develop high-performance printed and flexible electronic devices through careful engineering to obtain proper contributions of charge carriers either as electrons or holes in various D-A copolymer semiconductors.

15.
ACS Nano ; 16(11): 17778-17801, 2022 11 22.
Article in English | MEDLINE | ID: mdl-36355033

ABSTRACT

Microelectromechanical-system (MEMS)-based semiconductor gas sensors are considered one of the fastest-growing, interdisciplinary high technologies during the post-Moore era. Modern advancements within this arena include wearable electronics, Internet of Things, and artificial brain-inspired intelligence, among other modalities, thus bringing opportunities to drive MEMS-based gas sensors with higher performance, lower costs, and wider applicability. However, the high demand for miniature and micropower sensors with unified processes on a single chip imposes great challenges. This review focuses on recent developments and pitfalls in MEMS-based micro- and nanoscale gas sensors and details future trends. We also cover the background of the topic, seminal efforts, current applications and challenges, and opportunities for next-generation systems.


Subject(s)
Micro-Electrical-Mechanical Systems , Smell , Electronics , Semiconductors
16.
Micromachines (Basel) ; 12(12)2021 Dec 16.
Article in English | MEDLINE | ID: mdl-34945416

ABSTRACT

Physical mechanisms underlying the multilevel resistive tuning over seven orders of magnitude in structures based on TiO2/Al2O3 bilayers, sandwiched between platinum electrodes, are responsible for the nonlinear dependence of the conductivity of intermediate resistance states on the writing voltage. To improve the linearity of the electric-field resistance tuning, we apply a contact engineering approach. For this purpose, platinum top electrodes were replaced with aluminum and copper ones to induce the oxygen-related electrochemical reactions at the interface with the Al2O3 switching layer of the structures. Based on experimental results, it was found that electrode material substitution provokes modification of the physical mechanism behind the resistive switching in TiO2/Al2O3 bilayers. In the case of aluminum electrodes, a memory window has been narrowed down to three orders of magnitude, while the linearity of resistance tuning was improved. For copper electrodes, a combination of effects related to metal ion diffusion with oxygen vacancies driven resistive switching was responsible for a rapid relaxation of intermediate resistance states in TiO2/Al2O3 bilayers.

17.
ACS Appl Mater Interfaces ; 13(45): 54246-54257, 2021 Nov 17.
Article in English | MEDLINE | ID: mdl-34726368

ABSTRACT

2D materials exhibit intriguing electrical and optical properties, making them promising candidates for next-generation nanoelectronic devices. However, the high contact resistance of 2D materials to electrode material often limits the ultimate performance and potential of 2D materials and devices. In this work, we demonstrate a localized femtosecond (fs) laser irradiation process to substantially minimize the resistance of MoS2-metal contacts. A reduction of the contact resistance exceeding three orders of magnitude is achieved for mechanically exfoliated MoS2, which remarkably improves the overall FET performance. The underlying mechanisms of resistance reduction are the removal of organic contamination induced by the transfer process, as well as the lowering of Schottky barrier resistance (RSB) attributed to interface Fermi level pinning (FLP) by Au diffusion, and the lowering of interlayer resistance (Rint) due to interlayer coupling enhancement by Au intercalation under fs laser irradiation. By taking advantage of the improved MoS2-metal contact behavior, a high-performance MoS2 photodetector was developed with a photoresponsivity of 68.8 A W-1 at quite a low Vds of 0.5 V, which is ∼80 times higher than the pristine multilayer photodetector. This contamination-free, site-specific, and universal photonic fabrication technique provides an effective tool for the integration of complex 2D devices, and the mechanism of MoS2-metal interface modification reveals a new pathway to engineer the 2D material-metal interface.

18.
ACS Nano ; 15(3): 3674-3708, 2021 Mar 23.
Article in English | MEDLINE | ID: mdl-33656860

ABSTRACT

Graphene nanoribbons (GNRs) have recently emerged as promising candidates for channel materials in future nanoelectronic devices due to their exceptional electronic, thermal, and mechanical properties and chemical inertness. However, the adoption of GNRs in commercial technologies is currently hampered by materials science and integration challenges pertaining to synthesis and devices. In this Review, we present an overview of the current status of challenges, recent breakthroughs toward overcoming these challenges, and possible future directions for the field of GNR electronics. We motivate the need for exploration of scalable synthetic techniques that yield atomically precise, placed, registered, and oriented GNRs on CMOS-compatible substrates and stimulate ideas for contact and dielectric engineering to realize experimental performance close to theoretically predicted metrics. We also briefly discuss unconventional device architectures that could be experimentally investigated to harness the maximum potential of GNRs in future spintronic and quantum information technologies.

19.
Biotechnol J ; 15(11): e2000010, 2020 Nov.
Article in English | MEDLINE | ID: mdl-32302461

ABSTRACT

Technical crystallization is an attractive method to purify recombinant proteins. However, it is rarely applied due to the limited crystallizability of many proteins. To overcome this limitation, single amino acid exchanges are rationally introduced to enhance intermolecular interactions at the crystal contacts of the industrially relevant biocatalyst Lactobacillus brevis alcohol dehydrogenase (LbADH). The wildtype (WT) and the best crystallizing and enzymatically active LbADH mutants K32A, D54F, Q126H, and T102E are produced with Escherichia coli and subsequently crystallized from cell lysate in stirred mL-crystallizers. Notwithstanding the high host cell protein (HCP) concentrations in the lysate, all mutants crystallize significantly faster than the WT. Combinations of mutations result in double mutants with faster crystallization kinetics than the respective single mutants, demonstrating a synergetic effect. The almost entire depletion of the soluble LbADH fraction at crystallization equilibrium is observed, proving high yields. The HCP concentration is reduced to below 0.5% after crystal dissolution and recrystallization, and thus a 100-fold HCP reduction is achieved after two successive crystallization steps. The combination of fast kinetics, high yields, and high target protein purity highlights the potential of crystal contact engineering to transform technical crystallization into an efficient protein capture and purification step in biotechnological downstream processes.


Subject(s)
Biotechnology , Oxidoreductases , Alcohol Dehydrogenase/genetics , Crystallization , Crystallography, X-Ray , Recombinant Proteins/genetics
20.
Adv Sci (Weinh) ; 7(11): 1903044, 2020 Jun.
Article in English | MEDLINE | ID: mdl-32537396

ABSTRACT

Recent research shows that the interface state in perovskite solar cells is the main factor which affects the stability and performance of the device, and interface engineering including strain engineering is an effective method to solve this issue. In this work, a CsBr buffer layer is inserted between NiO x hole transport layer and perovskite layer to relieve the lattice mismatch induced interface stress and induce more ordered crystal growth. The experimental and theoretical results show that the addition of the CsBr buffer layer optimizes the interface between the perovskite absorber layer and the NiO x hole transport layer, reduces interface defects and traps, and enhances the hole extraction/transfer. The experimental results show that the power conversion efficiency of optimal device reaches up to 19.7% which is significantly higher than the efficiency of the device without the CsBr buffer layer. Meanwhile, the device stability is also improved. This work provides a deep understanding of the NiO x /perovskite interface and provides a new strategy for interface optimization.

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