Enhanced Photodetection Performance of an In Situ Core/Shell Perovskite-MoS2 Phototransistor.

While two-dimensional transition metal dichalcogenides (TMDCs)-based photodetectors offer prospects for high integration density and flexibility, their thinness poses a challenge regarding low light absorption, impacting photodetection sensitivity. Although the integration of TMDCs with metal halide perovskite nanocrystals (PNCs) has been known to be promising for photodetection with a high absorption coefficient of PNCs, the low charge mobility of PNCs delays efficient photocarrier injection into TMDCs. In this study, we integrated MoS2 with in situ formed core/shell PNCs with short ligands that minimize surface defects and enhance photocarrier injection. The PNCs/MoS2 heterostructure efficiently separates electrons and holes by establishing type II band alignment and consequently inducing a photogating effect. The synergistic interplay between photoconductive and photogating effects yields a high responsivity of 2.2 × 106 A/W and a specific detectivity of 9.0 × 1011 Jones. Our findings offer a promising pathway for developing low-cost, high-performance phototransistors leveraging the advantages of two-dimensional (2D) materials.

Reduced interface effect of proton beam irradiation on the electrical properties of WSe2/hBN field effect transistors.

Two-dimensional transition metal dichalcogenide (TMDC) semiconductors are emerging as strong contenders for electronic devices that can be used in highly radioactive environments such as outer space where conventional silicon-based devices exhibit nonideal characteristics for such applications. To address the radiation-induced interface effects of TMDC-based electronic devices, we studied high-energy proton beam irradiation effects on the electrical properties of field-effect transistors (FETs) made with tungsten diselenide (WSe2) channels and hexagonal boron-nitride (hBN)/SiO2gate dielectrics. The electrical characteristics of WSe2FETs were measured before and after the irradiation at various proton beam doses of 1013, 1014, and 1015cm-2. In particular, we demonstrated the dependence of proton irradiation-induced effects on hBN layer thickness in WSe2FETs. We observed that the hBN layer reduces the WSe2/dielectric interface effect which would shift the transfer curve of the FET toward the positive direction of the gate voltage. Also, this interface effect was significantly suppressed when a thicker hBN layer was used. This phenomenon can be explained by the fact that the physical separation of the WSe2channel and SiO2dielectric by the hBN interlayer prevents the interface effects originating from the irradiation-induced positive trapped charges in SiO2reaching the interface. This work will help improve our understanding of the interface effect of high-energy irradiation on TMDC-based nanoelectronic devices.

Reduced dopant-induced scattering in remote charge-transfer-doped MoS2 field-effect transistors.

Efficient doping for modulating electrical properties of two-dimensional (2D) transition metal dichalcogenide (TMDC) semiconductors is essential for meeting the versatile requirements for future electronic and optoelectronic devices. Because doping of semiconductors, including TMDCs, typically involves generation of charged dopants that hinder charge transport, tackling Coulomb scattering induced by the externally introduced dopants remains a key challenge in achieving ultrahigh mobility 2D semiconductor systems. In this study, we demonstrated remote charge transfer doping by simply inserting a hexagonal boron nitride layer between MoS2 and solution-deposited n-type dopants, benzyl viologen. A quantitative analysis of temperature-dependent charge transport in remotely doped devices supports an effective suppression of the dopant-induced scattering relative to the conventional direct doping method. Our mechanistic investigation of the remote doping method promotes the charge transfer strategy as a promising method for material-level tailoring of electrical and optoelectronic devices based on TMDCs.

Inkjet printing of two-dimensional van der Waals materials: a new route towards emerging electronic device applications.

Two-dimensional (2D) van der Waals (vdW) materials are considered one of the most promising candidates to realize emerging electrical applications. Although until recently, much effort has been dedicated to demonstrating high-performance single 2D vdW devices, associated with rapid progress in 2D vdW materials, demands for their large-scale practical applications have noticeably increased from a manufacturing perspective. Drop-on-demand inkjet printing can be the most feasible solution by exploiting the advantages of layered 2D contacts and advanced 2D vdW ink formulations. This review presents recent achievements in inkjet-printed 2D vdW material-based device applications. A brief introduction to 2D vdW materials and inkjet printing principles, followed by various ink formulation methods, is first presented. Then, the state-of-the-art inkjet-printed 2D vdW device applications and their remaining technical issues are highlighted. Finally, prospects and challenges to be overcome to demonstrate fully inkjet-printed, high-performance 2D vdW devices are also discussed.

Tailoring the Electrical Characteristics of MoS2 FETs through Controllable Surface Charge Transfer Doping Using Selective Inkjet Printing.

Surface charge transfer doping (SCTD) has been regarded as an effective approach to tailor the electrical characteristics of atomically thin transition metal dichalcogenides (TMDs) in a nondestructive manner due to their two-dimensional nature. However, the difficulty of achieving rationally controlled SCTD on TMDs via conventional doping methods, such as solution immersion and dopant vaporization, has impeded the realization of practical optoelectronic and electronic devices. Here, we demonstrate controllable SCTD of molybdenum disulfide (MoS2) field-effect transistors using inkjet-printed benzyl viologen (BV) as an n-type dopant. By adjusting the BV concentration and the areal coverage of inkjet-printed BV dopants, controllable SCTD results in BV-doped MoS2 FETs with elaborately tailored electrical performance. Specifically, the suggested solvent system creates well-defined droplets of BV ink having a volume of ∼2 pL, which allows the high spatial selectivity of SCTD onto the MoS2 channels by depositing the BV dopant on demand. Our inkjet-printed SCTD method provides a feasible solution for achieving controllable doping to modulate the electrical and optical performances of TMD-based devices.

Channel-Length-Modulated Avalanche Multiplication in Ambipolar WSe2 Field-Effect Transistors.

Recently there has been growing interest in avalanche multiplication in two-dimensional (2D) materials and device applications such as avalanche photodetectors and transistors. Previous studies have mainly utilized unipolar semiconductors as the active material and focused on developing high-performance devices. However, fundamental analysis of the multiplication process, particularly in ambipolar materials, is required to establish high-performance electronic devices and emerging architectures. Although ambipolar 2D materials have the advantage of facile carrier-type tuning through electrostatic gating, simultaneously allowing both carrier types in a single channel poses an inherent difficulty in analyzing their individual contributions to avalanche multiplication. In ambipolar field-effect transistors (FETs), two phenomena of ambipolar transport and avalanche multiplication can occur, and both exhibit secondary rise of output current at high lateral voltage. We distinguished these two competing phenomena using the method of channel length modulation and successfully analyzed the properties of electron- and hole-initiated multiplication in ambipolar WSe2 FETs. Our study provides a simple and robust method to examine carrier multiplication in ambipolar materials and will foster the development of high-performance atomically thin electronic devices utilizing avalanche multiplication.

Proton irradiation effects on mechanochemically synthesized and flash-evaporated hybrid organic-inorganic lead halide perovskites.

A hybrid organic-inorganic halide perovskite is a promising material for developing efficient solar cell devices, with potential applications in space science. In this study, we synthesized methylammonium lead iodide (MAPbI3) perovskites via two methods: mechanochemical synthesis and flash evaporation. We irradiated these perovskites with highly energetic 10 MeV proton-beam doses of 1011, 1012, 1013, and 4 × 1013protons cm-2and examined the proton irradiation effects on the physical properties of MAPbI3perovskites. The physical properties of the mechanochemically synthesized MAPbI3perovskites were not considerably affected after proton irradiation. However, the flash-evaporated MAPbI3perovskites showed a new peak in x-ray diffraction and an increased fluorescence lifetime in time-resolved photoluminescence under high-dose conditions, indicating considerable changes in their physical properties. This difference in behavior between MAPbI3perovskites synthesized via the abovementioned two methods may be attributed to differences in radiation hardness associated with the bonding strength of the constituents, particularly Pb-I bonds. Our study will help to understand the radiation effect of proton beams on organometallic halide perovskite materials.

Role of Two-Dimensional Ising Superconductivity in the Nonequilibrium Quasiparticle Spin-to-Charge Conversion Efficiency.

Nonequilibrium studies of two-dimensional (2D) superconductors (SCs) with Ising spin-orbit coupling are prerequisite for their successful application to equilibrium spin-triplet Cooper pairs and, potentially, Majorana Fermions. By taking advantage of the recent discoveries of 2D SCs and their compatibility with any other materials, we fabricate here nonlocal magnon devices to examine how such 2D Ising superconductivity affects the conversion efficiency of magnon spin to quasiparticle charge in superconducting flakes of 2H-NbSe2 transferred onto ferrimagnetic insulating Y3Fe5O12. Comparison with a reference device based on a conventionally paired superconductor shows that the Y3Fe5O12-induced in-plane (IP) exchange spin-splitting in the NbSe2 flake is hindered by its inherent out-of-plane (OOP) spin-orbit field, which, in turn, limits the transition-state enhancement of the spin-to-charge conversion efficiency. Our out-of-equilibrium study highlights the significance of symmetry matching between underlying Cooper pairs and exchange-induced spin-splitting for the giant transition-state spin-to-charge conversion and may have implications toward proximity-engineered spin-polarized triplet pairing via tuning the relative strength of IP exchange and OOP spin-orbit fields in ferromagnetic insulator/2D Ising SC bilayers.

Molecular Dopant-Dependent Charge Transport in Surface-Charge-Transfer-Doped Tungsten Diselenide Field Effect Transistors.

The controllability of carrier density and major carrier type of transition metal dichalcogenides(TMDCs) is critical for electronic and optoelectronic device applications. To utilize doping in TMDC devices, it is important to understand the role of dopants in charge transport properties of TMDCs. Here, the effects of molecular doping on the charge transport properties of tungsten diselenide (WSe2 ) are investigated using three p-type molecular dopants, 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4 -TCNQ), tris(4-bromophenyl)ammoniumyl hexachloroantimonate (magic blue), and molybdenum tris(1,2-bis(trifluoromethyl)ethane-1,2-dithiolene) (Mo(tfd-COCF3 )3 ). The temperature-dependent transport measurements show that the dopant counterions on WSe2 surface can induce Coulomb scattering in WSe2 channel and the degree of scattering is significantly dependent on the dopant. Furthermore, the quantitative analysis revealed that the amount of charge transfer between WSe2 and dopants is related to not only doping density, but also the contribution of each dopant ion toward Coulomb scattering. The first-principles density functional theory calculations show that the amount of charge transfer is mainly determined by intrinsic properties of the dopant molecules such as relative frontier orbital positions and their spin configurations. The authors' systematic investigation of the charge transport of doped TMDCs will be directly relevant for pursuing molecular routes for efficient and controllable doping in TMDC nanoelectronic devices.

Long-range supercurrents through a chiral non-collinear antiferromagnet in lateral Josephson junctions.

The proximity-coupling of a chiral non-collinear antiferromagnet (AFM)1-5 with a singlet superconductor allows spin-unpolarized singlet Cooper pairs to be converted into spin-polarized triplet pairs6-8, thereby enabling non-dissipative, long-range spin correlations9-14. The mechanism of this conversion derives from fictitious magnetic fields that are created by a non-zero Berry phase15 in AFMs with non-collinear atomic-scale spin arrangements1-5. Here we report long-ranged lateral Josephson supercurrents through an epitaxial thin film of the triangular chiral AFM Mn3Ge (refs. 3-5). The Josephson supercurrents in this chiral AFM decay by approximately one to two orders of magnitude slower than would be expected for singlet pair correlations9-14 and their response to an external magnetic field reflects a clear spatial quantum interference. Given the long-range supercurrents present in both single- and mixed-phase Mn3Ge, but absent in a collinear AFM IrMn16, our results pave a way for the topological generation of spin-polarized triplet pairs6-8 via Berry phase engineering15 of the chiral AFMs.

Ultrasensitive Photodetection in MoS2 Avalanche Phototransistors.

Recently, there have been numerous studies on utilizing surface treatments or photosensitizing layers to improve photodetectors based on 2D materials. Meanwhile, avalanche breakdown phenomenon has provided an ultimate high-gain route toward photodetection in the form of single-photon detectors. Here, the authors report ultrasensitive avalanche phototransistors based on monolayer MoS2 synthesized by chemical vapor deposition. A lower critical field for the electrical breakdown under illumination shows strong evidence for avalanche breakdown initiated by photogenerated carriers in MoS2 channel. By utilizing the photo-initiated carrier multiplication, their avalanche photodetectors exhibit the maximum responsivity of ≈3.4 × 107 A W-1 and the detectivity of ≈4.3 × 1016 Jones under a low dark current, which are a few orders of magnitudes higher than the highest values reported previously, despite the absence of any additional chemical treatments or photosensitizing layers. The realization of both the ultrahigh photoresponsivity and detectivity is attributed to the interplay between the carrier multiplication by avalanche breakdown and carrier injection across a Schottky barrier between the channel and metal electrodes. This work presents a simple and powerful method to enhance the performance of photodetectors based on carrier multiplication phenomena in 2D materials and provides the underlying physics of atomically thin avalanche photodetectors.

Crystallinity-dependent device characteristics of polycrystalline 2D n = 4 Ruddlesden-Popper perovskite photodetectors.

Ruddlesden-Popper (RP) perovskites have attracted a lot of attention as the active layer for optoelectronic devices due to their excellent photophysical properties and environmental stability. Especially, local structural properties of RP perovskites have shown to play important roles in determining the performance of optoelectronic devices. Here, we report the photodetector performance variation depending on the crystallinity of n = 4 two-dimensional (2D) RP perovskite polycrystalline films. Through controlling the solvent evaporation rate, 2D RP perovskite films could be tuned between highly- and randomly-orientated phases. We investigated how different factors related to the film crystallinity are reflected in the variation of photodetector performances by considering grain boundary and low energy edge state effects in n = 4 RP perovskites. Better understanding the interplay between these factors that govern the photophysical properties of the devices would be beneficial for designing high-performance RP perovskite-based optoelectronic devices.

Effect of Facile p-Doping on Electrical and Optoelectronic Characteristics of Ambipolar WSe2 Field-Effect Transistors.

We investigated the electrical and optoelectronic characteristics of ambipolar WSe2 field-effect transistors (FETs) via facile p-doping process during the thermal annealing in ambient. Through this annealing, the oxygen molecules were successfully doped into the WSe2 surface, which ensured higher p-type conductivity and the shift of the transfer curve to the positive gate voltage direction. Besides, considerably improved photoswitching response characteristics of ambipolar WSe2 FETs were achieved by the annealing in ambient. To explore the origin of the changes in electrical and optoelectronic properties, the analyses via X-ray photoelectron, Raman, and photoluminescence spectroscopies were performed. From these analyses, it turned out that WO3 layers formed by the annealing in ambient introduced p-doping to ambipolar WSe2 FETs, and disorders originated from the WO3/WSe2 interfaces acted as non-radiative recombination sites, leading to significantly improved photoswitching response time characteristics.

Recent Advances in Interface Engineering of Transition-Metal Dichalcogenides with Organic Molecules and Polymers.

The interface engineering of two-dimensional (2D) transition-metal dichalcogenides (TMDs) has been regarded as a promising strategy to modulate their outstanding electrical and optoelectronic properties because of their inherent 2D nature and large surface-to-volume ratio. In particular, introducing organic molecules and polymers directly onto the surface of TMDs has been explored to passivate the surface defects or achieve better interfacial properties with neighboring surfaces efficiently, thus leading to great opportunities for the realization of high-performance TMD-based applications. This review provides recent progress in the interface engineering of TMDs with organic molecules and polymers corresponding to the modulation of their electrical and optoelectronic characteristics. Depending on the interfaces between the surface of TMDs and dielectric, conductive contacts or the ambient environment, we present various strategies to introduce an organic interlayer from materials to processing. In addition, the role of native defects on the surface of TMDs, such as adatoms or vacancies, in determining their electrical characteristics is also discussed in detail. Finally, the future challenges and opportunities associated with the interface engineering are highlighted.

Intrinsic Optoelectronic Characteristics of MoS2 Phototransistors via a Fully Transparent van der Waals Heterostructure.

In the past decade, intensive studies on monolayer MoS2-based phototransistors have been carried out to achieve further enhanced optoelectronic characteristics. However, the intrinsic optoelectronic characteristics of monolayer MoS2 have still not been explored until now because of unintended interferences, such as multiple reflections of incident light originating from commonly used opaque substrates. This leads to overestimated photoresponsive characteristics inevitably due to the enhanced photogating and photoconductive effects. Here, we reveal the intrinsic photoresponsive characteristics of monolayer MoS2, including its internal responsivity and quantum efficiency, in fully transparent monolayer MoS2 phototransistors employing a van der Waals heterostructure. Interestingly, as opposed to the previous reports, the internal photoresponsive characteristics do not significantly depend on the wavelength of the incident light as long as the electron-hole pairs are generated in the same k-space. This study provides a deeper understanding of the photoresponsive characteristics of MoS2 and lays the foundation for two-dimensional materials-based transparent phototransistors.

Dose-dependent effect of proton irradiation on electrical properties of WSe2 ambipolar field effect transistors.

The irradiation effect of high energy proton beams on tungsten diselenide (WSe2) ambipolar field-effect transistors was investigated. We measured the electrical characteristics of the fabricated WSe2 FETs before and after the 10 MeV proton beam irradiation with different doses of 1012, 1013, 1014, and 1015 cm-2. For low dose conditions (1012, 1013, and 1014 cm-2), the threshold voltages shifted to the negative gate voltage direction, and the current in the hole and electron accumulation regimes decreased and increased, respectively. However, the trends were opposite for the high dose condition (1015 cm-2); the threshold voltages shifted to the positive gate voltage direction, and the current in the hole and electron accumulation regimes increased and decreased, respectively. These phenomena can be explained by the combined effect of proton irradiation-induced traps and the applied gate bias condition. Specifically, irradiation-induced positive oxide traps in SiO2 dielectrics play a role in enhancing electron accumulation and reducing hole accumulation in the WSe2 channel, whereas the irradiation-induced holes near the WSe2/SiO2 interface act as electron trapping sites, with enhancing hole accumulation and reducing electron accumulation in the WSe2 channel. This work will help improve the understanding of the effect of high energy irradiation on WSe2-based and other ambipolar nanoelectronic devices. In addition, this work shows the possibility of tuning the electrical properties of WSe2-based devices.

Recent Progress in Inkjet-Printed Thin-Film Transistors.

Drop-on-demand inkjet printing is one of the most attractive techniques from a manufacturing perspective due to the possibility of fabrication from a digital layout at ambient conditions, thus leading to great opportunities for the realization of low-cost and flexible thin-film devices. Over the past decades, a variety of inkjet-printed applications including thin-film transistors (TFTs), radio-frequency identification devices, sensors, and displays have been explored. In particular, many research groups have made great efforts to realize high-performance TFTs, for application as potential driving components of ubiquitous wearable electronics. Although there are still challenges to enable the commercialization of printed TFTs beyond laboratory-scale applications, the field of printed TFTs still attracts significant attention, with remarkable developments in soluble materials and printing methodology. Here, recent progress in printing-based TFTs is presented from materials to applications. Significant efforts to improve the electrical performance and device-yield of printed TFTs to match those of counterparts fabricated using conventional deposition or photolithography methods are highlighted. Moreover, emerging low-dimension printable semiconductors, including carbon nanotubes and transition metal dichalcogenides as well as mature semiconductors, and new-concept printed switching devices, are also discussed.

Enhanced Charge Injection Properties of Organic Field-Effect Transistor by Molecular Implantation Doping.

Organic semiconductors (OSCs) have been widely studied due to their merits such as mechanical flexibility, solution processability, and large-area fabrication. However, OSC devices still have to overcome contact resistance issues for better performances. Because of the Schottky contact at the metal-OSC interfaces, a non-ideal transfer curve feature often appears in the low-drain voltage region. To improve the contact properties of OSCs, there have been several methods reported, including interface treatment by self-assembled monolayers and introducing charge injection layers. Here, a selective contact doping of 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4 -TCNQ) by solid-state diffusion in poly(2,5-bis(3-hexadecylthiophen-2-yl)thieno[3,2-b]thiophene) (PBTTT) to enhance carrier injection in bottom-gate PBTTT organic field-effect transistors (OFETs) is demonstrated. Furthermore, the effect of post-doping treatment on diffusion of F4 -TCNQ molecules in order to improve the device stability is investigated. In addition, the application of the doping technique to the low-voltage operation of PBTTT OFETs with high-k gate dielectrics demonstrated a potential for designing scalable and low-power organic devices by utilizing doping of conjugated polymers.

Two-Dimensional Thickness-Dependent Avalanche Breakdown Phenomena in MoS2 Field-Effect Transistors under High Electric Fields.

As two-dimensional (2D) transition metal dichalcogenides electronic devices are scaled down to the sub-micrometer regime, the active layers of these materials are exposed to high lateral electric fields, resulting in electrical breakdown. In this regard, understanding the intrinsic nature in layer-stacked 2D semiconducting materials under high lateral electric fields is necessary for the reliable applications of their field-effect transistors. Here, we explore the electrical breakdown phenomena originating from avalanche multiplication in MoS2 field-effect transistors with different layer thicknesses and channel lengths. Modulating the band structure and bandgap energy in MoS2 allows the avalanche multiplication to be controlled by adjusting the number of stacking layers. This phenomenon could be observed in transition metal dichalcogenide semiconducting systems due to its quantum confinement effect on the band structure. The relationship between the critical electric field for avalanche breakdown and bandgap energy is well fitted to a power law curve in both monolayer and multilayer MoS2.