Field Effect Transistor Applications Research Articles

Magneto-transport in the monolayer MoS2 material system for high-performance field-effect transistor applications

Electronic transport in monolayer MoS2 is significantly constrained by several extrinsic factors despite showing good prospects as a transistor channel material. Our paper aims to unveil the underlying mechanisms of the electrical and magneto-transport in monolayer MoS2. In order to quantitatively interpret the magneto-transport behavior of monolayer MoS2 on different substrate materials, identify the underlying bottlenecks, and provide guidelines for subsequent improvements, we present a deep analysis of the magneto-transport properties in the diffusive limit. Our calculations are performed on suspended monolayer MoS2 and MoS2 on different substrate materials taking into account remote impurity and the intrinsic and extrinsic phonon scattering mechanisms. We calculate the crucial transport parameters such as the Hall mobility, the conductivity tensor elements, the Hall factor, and the magnetoresistance over a wide range of temperatures, carrier concentrations, and magnetic fields. The Hall factor being a key quantity for calculating the carrier concentration and drift mobility, we show that for suspended monolayer MoS2 at room temperature, the Hall factor value is around 1.43 for magnetic fields ranging from 0.001 to 1 Tesla, which deviates significantly from the usual value of unity. In contrast, the Hall factor for various substrates approaches the ideal value of unity and remains stable in response to the magnetic field and temperature. We also show that the MoS2 over an Al2O3 substrate is a good choice for the Hall effect detector. Moreover, the magnetoresistance increases with an increase in magnetic field strength for smaller magnetic fields before reaching saturation at higher magnetic fields. The presented theoretical model quantitatively captures the scaling of mobility and various magnetoresistance coefficients with temperature, carrier densities, and magnetic fields.

Performance enhancement of 2D tin-halide perovskite transistors via molecule-assisted grain boundary passivation and hole doping

Tin (Sn2+)-based halide perovskites have garnered considerable interest for potential applications in field-effect transistors, owing to their low-cost solution processing capability and favorable hole transport properties. However, the polycrystalline nature of halide perovskite films necessitates efficient grain boundary passivation for reliable and stable device operation. Additionally, as a p-type semiconductor, controllable hole-doping is desired for modulating electrical properties. In this study, we demonstrate the dual functionality of doping the small molecule tetrafluoro-tetracyanoquinodimethane (F4TCNQ) into (C6H5C2H4NH3)2SnI4 (abbreviated as (PEA)2SnI4) through a cost-effective solution process. This doping introduces F4TCNQ as both a grain boundary passivator and a charge transfer p-dopant, resulting in effective improvements in transistor performance with a 6-fold enhancement in mobility, a substantial reduction in hysteresis, an enhanced current ratio, and improved stabilities.

Logic-in-memory application of ferroelectric-based WS2-channel field-effect transistors for improved area and energy efficiency

In this study, we applied ferroelectrics to the gate stack of Field Effect Transistors (FETs) with a 2D transition-metal dichalcogenide (TMDC) channel, actively researching for sub-2nm technology node implementation. Subsequently, we analyzed the circuit characteristics of Logic-in-Memory (LiM) operation and utilized LiM features after applying ferroelectrics to achieve a single-device configuration. Based on well-calibrated simulations, we performed compact modeling in a circuit simulator to depict the temperature-dependent electrical characteristics of ferroelectric FETs with a double gate structure and 2D channel (DG 2D-FeFET) in sub-2nm dimensions. Through this, we have confirmed that the 2D FeFET-based LiM technology, designed for the 2 nm technology node, exhibits superior characteristics in terms of delay, power/energy consumption, and circuit area under all temperature conditions, compared to the conventional CMOS technology based on 2D FETs. This verification serves as proof of the future technological potential of 2D-FeFET in extremely scaled-down technology nodes.

Illustrating the pertinacious interlayer charge compression effect in van der Waals heterointerfaces

Heterojunctions of two-dimensional (2D) van der Waals (vdW) nanomaterials often exhibit unusual, “non-textbook” bonding mechanism that involves distinct orbital coupling within the compressed vdW gap. To unravel this atypical bonding mechanism for 2D heterointerfaces, using density-functional theory calculations, we examine the compressed charge redistribution and interface dipoles for the heterostructures of ReSe2/graphene, ReSe2/h-BN, and a triply-stacked ReSe2/h-BN/graphene heterointerface. Here, we report the optimized atomic structures, electronic density-of-states, (integrated) planar-averaged electron density differences, and tip-inclusive scanning tunneling microscopy simulations for these heterostructures, while focusing on the explicit contributions of the conductive graphene and insulating h-BN substrates to the interlayer confined charges and dipoles. Using other 2D heterosystems, we also demonstrate that this charge compression effect within the vdW gap is ubiquitous and general regardless of the nature of the substrates and supports. Upon applying an external electric field, we clearly demonstrate a tunable control (in both magnitude and sign of these interface dipoles) in 2D vdW heterostructures and advance the precise engineering of pertinacious interlayer compressed charges/interface dipoles for the next-generation ambipolar field-effect (nano)transistor (FET) applications.

Robust type-III C3N/Ga2O3 van der Waals heterostructures

By combining two-dimensional (2D) materials with different band alignments at the contact interface, van der Waals heterostructures (vdWHs) can achieve multifunctional device applications. Here, through first principles methods, we constructed two C3N/Ga2O3 vdWHs named P↑ and P↓ because of the intrinsic polarization of Ga2O3 to study electronic, interfacial and optical characteristics. We find that the P↑ and P↓ both display a unique kind of band alignment known as broken-gap or type-III. This feature makes them highly suitable for tunnel field effect transistors (TFETs) applications. To the best of our knowledge, the tunnel window of the P↓ is the largest among the theoretical studies, reaching 0.993 eV. The electronic structure and band edge alignment of the C3N/Ga2O3 vdWHs show a weak dependence on strain engineering or external electric field. Normal-to-plane compressive strains effectively enhance the tunneling probability. We can acquire essential insights into this novel material system and its promise for future TFETs by analyzing the electrical characteristics of the C3N/Ga2O3 vdWHs.

A Review on the Synthetic Methods towards Benzothienobenzothiophenes.

Benzothienobenzothiophenes (BTBTs) are a class of heteroacenes for which two distinct isomers have been identified depending on the locations of the fused benzothiophene motifs. Benzothienobenzothiophenes represent a class of heteroacenes demonstrating remarkable electronic properties that make them prominent in the realm of organic semiconductors. The structure of BTBTs, incorporating two sulfur atoms, contributes to their unique electronic characteristics, including narrow bandgaps and effective charge transport pathways. These compounds have gained attention for their high charge carrier mobility, making them desirable candidates for application in organic field-effect transistors (OFETs) and other electronic devices. Researchers have explored various synthetic strategies to design and tailor the properties of BTBT derivatives, leading to advancements in the development of high-performance organic semiconductors. Various synthetic techniques for benzothienobenzothiophenes have been reported in the literature including multistep synthesis, tandem transformations, electrochemical synthesis, and annulations. This review investigates the generality of each synthetic methodology by highlighting its benefits and drawbacks, and it analyses all synthetic approaches described for the creation of the two isomers. For the advantage of the readers, we have delved upon every mechanism of the reactions that are known. Finally, we have also summarized the synthetic methodologies that are used for making benzothienobenzothiophene analogues for material applications.

Stabilizing Perovskite Pb(Mg0.33Nb0.67)O3-PbTiO3 Thin Films by Fast Deposition and Tensile Mismatched Growth Template.

Because of its low hysteresis, high dielectric constant, and strong piezoelectric response, Pb(Mg1/3Nb2/3)O3-PbTiO3 (PMN-PT) thin films have attracted considerable attention for the application in PiezoMEMS, field-effect transistors, and energy harvesting and storage devices. However, it remains a great challenge to fabricate phase-pure, pyrochlore-free PMN-PT thin films. In this study, we demonstrate that a high deposition rate, combined with a tensile mismatched template layer can stabilize the perovskite phase of PMN-PT films and prevent the nucleation of passive pyrochlore phases. We observed that an accelerated deposition rate promoted mixing of the B-site cation and facilitated relaxation of the compressively strained PMN-PT on the SrTiO3 (STO) substrate in the initial growth layer, which apparently suppressed the initial formation of pyrochlore phases. By employing La-doped-BaSnO3 (LBSO) as the tensile mismatched buffer layer, 750 nm thick phase-pure perovskite PMN-PT films were synthesized. The resulting PMN-PT films exhibited excellent crystalline quality close to that of the STO substrate.

Tailoring Contacts for High-Performance 1D Ta2Pt3S8 Field-Effect Transistors.

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.

Coexisting Phases in Transition Metal Dichalcogenides: Overview, Synthesis, Applications, and Prospects.

Over the past decade, significant advancements have been made in phase engineering of two-dimensional transition metal dichalcogenides (TMDCs), thereby allowing controlled synthesis of various phases of TMDCs and facile conversion between them. Recently, there has been emerging interest in TMDC coexisting phases, which contain multiple phases within one nanostructured TMDC. By taking advantage of the merits from the component phases, the coexisting phases offer enhanced performance in many aspects compared with single-phase TMDCs. Herein, this review article thoroughly expounds the latest progress and ongoing efforts on the syntheses, properties, and applications of TMDC coexisting phases. The introduction section overviews the main phases of TMDCs (2H, 3R, 1T, 1T', 1Td), along with the advantages of phase coexistence. The subsequent section focuses on the synthesis methods for coexisting phases of TMDCs, with particular attention to local patterning and random formations. Furthermore, on the basis of the versatile properties of TMDC coexisting phases, their applications in magnetism, valleytronics, field-effect transistors, memristors, and catalysis are discussed. Lastly, a perspective is presented on the future development, challenges, and potential opportunities of TMDC coexisting phases. This review aims to provide insights into the phase engineering of 2D materials for both scientific and engineering communities and contribute to further advancements in this emerging field.

Acetylene-extended triarylamines for solution-processable p-channel OFETs

New acetylene-extended molecules were developed as a semiconducting layer for application in solution-processable organic field-effect transistors through coupling reactions using substituted triphenylamines as wings and diacetylene as spacer units. The influence of donor ability and spacer strength on the electrical properties was explored by developing different acetylene-extended triarylamines with D–π and D–π–π–D architectures and their structure–properties analysis. Their optical studies revealed narrow Stoke's shift and optical bandgap values, especially for highly electron-rich systems. Encouraging results supported by their electrochemical studies that revealed high HOMO energy levels ranging from –5.1 to –5.3 eV suggested a low energy barrier and good hole-transporting ability, hence, their applicability as p-channel OFETs. Furthermore, the extended conjugation in D–π–π–D based molecules relative to their corresponding D–π system caused enhanced molecular orbital overlap along the triphenylamine and facilitated good charge transport characteristics. Upon fabrication as the semiconducting channel in top-gate/bottom-contact OFET devices, the acetylene-extended D–π–π–D system showed good p-channel properties with hole mobilities up to 1.2 cm2/Vs and the highest on/off ratio of 107.

Future prospects of MXenes: synthesis, functionalization, properties, and application in field effect transistors.

MXenes are a family of two-dimensional (2D) materials that have drawn a lot of interest recently because of their distinctive characteristics and possible uses in a variety of industries. This review emphasizes the bright future prospects of MXene materials in the realm of FETs. Their remarkable properties, coupled with their tunability and compatibility, position MXenes as promising candidates for the development of high-performance electronic devices. As research in this field continues to evolve, the potential of MXenes to drive innovation in electronics becomes increasingly evident, fostering excitement for their role in shaping the future of electronic technology. This paper presents a comprehensive overview of MXene materials, focusing on their synthesis methods, functionalization strategies, intrinsic properties, and their promising application in Field Effect Transistors (FETs).

Advancements in conjugated polymer research: applications in organic photovoltaics and field effect transistors

This review provides a comprehensive overview of the development and applications of conjugated polymer semiconductors. The review summarizes the current state of research in this field, including the synthesis and characterization of these materials, their properties, and potential applications. The scope covers a wide range of topics, including organic photovoltaics, organic field-effect transistors, and conjugated polymer nanoparticles. The main findings highlight the significant progress that has been made in this field, with conjugated polymers exhibiting favorable electronic and optical properties, as well as high charge mobility. These materials have shown great potential for use in various applications, including solar cells, light-emitting diodes, and field-effect transistors. The applications are far-reaching, with the potential to revolutionize the electronics industry by providing low-cost, flexible, and environmentally friendly alternatives to traditional inorganic materials. One of the key challenges facing this field is the need to improve the efficiency and stability of conjugated polymer-based devices. While significant progress has been made in this area, there is still much work to be done to develop materials and device architectures that can achieve high performance over extended periods of time. Another challenge is the need to develop scalable manufacturing processes that can produce large quantities of high-quality conjugated polymers at a reasonable cost. The continued advancement of this field holds great promise for the development of new technologies that can improve our lives and help to address some of the world’s most pressing challenges.

A high-performance organic lithium salt-doped OFET with the optical radical effect for photoelectric pulse synaptic simulation and neuromorphic memory learning.

Simulation of synaptic characteristics is essential for the application of organic field effect transistors (OFETs) in neural morphology. Although excellent performance, including bias stability and mobility, as well as photoelectric pulse synaptic simulation, has been achieved in SiO2-gated OFETs with PDVT-10 as an organic channel, there are relatively few studies on photoelectric pulse synaptic simulation of electrolyte-gated OFETs based on environmentally friendly and low-voltage operation. Herein, synaptic transistors based on organic semiconductors are reported to simulate the photoelectric pulse response by developing solution-based organic semiconductor PDVT-10, and polyvinyl alcohol (PVA) with an electric double layer (EDL) effect to act as a channel and gate dielectric layer, respectively, and organic lithium salt-doped PVA is used to enhance the EDL effect. The presence of electrical pulses in doped devices not only achieves basic electrical synaptic characteristics, but also significantly realizes the long-term characteristics, pain perception, memory and sensitization applications. Furthermore, the introduction of photoinitiator molecules into the channel layer leads to improved photosynaptic performances by using light-induced free radicals, and the photoelectric synergistic effect has been actualized by introducing heterojunction architecture. This work provides promising prospects for achieving photoelectric pulse modulation based on organic synaptic devices, which shows great potential for the development of artificial intelligence.

Ideal two-dimensional quantum spin Hall insulators MgA2Te4 (A = Ga, In) with Rashba spin splitting and tunable properties.

For decades, topological insulators have played a pivotal role in fundamental condensed-matter physics owing to their distinctive edge states and electronic properties. Here, based on in-depth first-principles calculations, we investigate the MgA2Te4 (A = Ga, In) structures belonging to the MA2Z4 2D material family. Among them, the topological insulator MgGaInTe4 exhibits band inversion and a sizeable bandgap of up to 60.8 meV which satisfies the requirement for room-temperature realization. Under the spin-orbit coupling effect, MgGaInTe4 with inversion asymmetry undergoes Rashba spin splitting. The Rashba-like and Dirac-type edge states emerge from different terminals along (010) for MgGaInTe4. The external vertical electric field is verified to modulate the inverted bandgap and topological state of MgGaInTe4 by converting a nontrivial state to a trivial state and MgIn2Te4 with the original trivial state to a nontrivial one. Accordingly, MgGaInTe4 and MgIn2Te4 have significant potential for application in topological quantum field-effect transistors. Our research identifies that the MgA2Te4 (A = Ga, In) structures have huge potential to be candidate 2D materials for spintronics and topological quantum devices.

Retracted: Investigation on V2O5 Thin Films for Field Effect Transistor Applications

Retracted: Investigation on V₂O₅ Thin Films for Field Effect Transistor Applications

(Invited) Atomic Imaging and Device Characterization of Molecularly Thin 2D Hybrid Perovskites

2D Organic-Inorganic Hybrid perovskites (OIHPs) possess alternating layers of organic molecules and inorganic quantum wells. By tuning the interaction between organic and inorganic layers, very interesting properties can be introduced. The successful isolation of hybrid perovskite monolayers with clean and flat surfaces are particularly suitable for atomic structure characterization and optoelectronic device fabrication. In this talk, I will present recent results on the excitonic properties and atomic structure of molecularly thin OIHPs1,2. We found that a reversible shift in excitonic energies can be induced upon laser irradiation in large-sized 2D hybrid perovskite monolayers which is attributed to the reversible structural reorientation of the surface BA cations in the easily deformable lattice3. The photodetection performance of monolayer, bilayer and thicker OIHPs were compared. The internal quantum efficiency was measured to be 34% for a monolayer (BA)2(MA)3Pb4I13 and 19% for the bulk crystal. In addition, 2D heterostructures of molecularly thin OIHPs/graphene were constructed which exhibited a lower barrier than gold for carrier injection, enabling applications in field effect transistors (FETs)4. Electron tunneling occurs across the interface of organic molecular layers on 2D perovskite and graphene, while photoinduced charge transfer occurs at femtosecond timescale (~50 fs).Resolving the atomic structure of 2D hybrid perovskite is a challenging task because it is easily damaged by electron beam. Here we use scanning tunneling microscopy (STM) & Qplus AFM to directly visualize surface octahedral tilt in freshly exfoliated 2D Ruddlesden-Popper perovskites (RPPs)5. The experimentally determined octahedral tilts from n = 1 to n = 4 RPPs from STM images are found to agree very well with out-of-plane surface octahedral tilts predicted by density functional theory calculations. The surface-enhanced octahedral tilt is correlated to excitonic redshift observed in photoluminescence (PL) and promotes Rashba spin splitting for n > 1. Our studies demonstrate a protocol to investigate structure-property correlations in low dimensional 2D OIHPs, which will pave the way to better material design and device performance.References Leng, W. Fu, Y. Liu, M. Chhowalla & KP Loh* “From Bulk to Molecularly Thin Hybrid Perovskites” Nature Reviews Materials , 5, 482-500 (2020).Zhao, KP Loh, K. Leng* “Organic-inorganic hybrid perovskites and their heterostructures” Matter , 5, 4153-4169 (2022).Leng, I. Abdelwaha, I. Verzhbitskiy, M. Telychko, L. Chu, W. Fu, X. Chi, N. Guo, Z. Chen, Z. Chen, C. Zhang, Q. Xu, J. Lu, M. Chhowalla, G. Eda, KP Loh* “Molecularly thin two-dimensional hybrid perovskites with tunable optoelectronic properties due to reversible surface relaxation” Nature Materials , 17, 908-914 (2018).Leng, L. Wang, Y. Shao, I. Abdelwahab, G. Grinblat, I. Verzhbitskiy, Y. Cai, X. Chi, W. Fu, P. Song, G. Eda, S. A. Maier & KP Loh* “Electron Tunneling at the Molecularly Thin 2D Perovskite and Graphene Van der Waals Interface” Nature Communications , 11, 5483 (2020).Y Shao, W. Gao, H. Yan, R. Li, I. Abdelwahab, L. Zhuang, W. Fu, SP Lau, SF YU, Y. Cai, KP Loh, K. Leng* “Unlocking Surface Octahedral Tilt in Two-dimensional Ruddlesden-Popper Perovskites” Nature Communications , 13, 138 (2022). AcknowledgementK.L. would like to acknowledge the Research Grants Council of the Hong Kong Special Administrative Region, China (Project No. PolyU15305221 for GRF project funded in 2021/22 Exercise and Project No. PolyU25305222 for ECS project funded in 2022/23 Exercise).

The effects of MS2 (M = Mo or W) substrates on electronic properties under electric fields in germanene-based field-effect transistors

Germanene has attracted significant attention due to its novel electronic properties and strong spin-coupling effect. However, the tiny band gap of the germanene dramatically limits its application in field-effect transistors (FETs). Inspired by the utilization of the substrates and electric fields to adjust the band gaps of two-dimensional materials, we investigated the fundamental mechanism of electric fields on the atomic structures and electronic properties of germanene supported by MS2 (M = Mo or W) substrates through first-principles calculation. The results show that the substrates can induce a symmetry breaking in the germanene sublattice via van der Waals interaction, leading to a sizable band gap at the Dirac point. In addition, the band gaps of the germanene/MS2 heterostructures can be effectively modulated by applying an external electric field. Under suitable electric fields, the considerable band gap values of CMo germanene/MoS2 and TGeL-W germanene/WS2 configurations can open the maximum band gaps with 263 and 247 meV, which satisfy the requirements of FETs at room temperature. Meanwhile, the evolutions of charge transfers under electric fields were explored to illustrate how electric fields and substrates promote the electronic properties of germanene. More interestingly, a Schottky–Ohmic transition can occur when a specific electric field is imposed on the germanene/MS2 heterostructures. Note that the hole and electron carrier mobilities of germanene/MS2 heterostructures are still significantly preserved, showing some superior electronic performances than some heterostructures. The results provide a critical theoretical guide for improving the electronic properties of germanene, and demonstrate the designed germanene/MS2 heterostructures with the tunable band gaps and higher carrier mobilities as germanene-based FETs.

Towards ultralow-power and high-speed electronics: Tunnel transistor based on single-chain Tellurium

The application of tunnel field-effect transistors (TFETs) in the sub-5.1 nm range meets the challenges of low on-state current (Ion), elevated leakage current (Ileak) and a limited bias range with sub-thermionic subthreshold swing (SS) characteristics. Here, by the design of gate-all-around (GAA) single-chain Te (1Te) TFETs, the sub-thermionic SS characteristics span nearly six orders of magnitude of drain current, overcoming the above challenges. While there usually exists trade-offs between maximizing Ion and minimizing Ileak, our optimized 5.1 nm GAA 1Te TFET defies this convention. Its steep turn-on characteristics result in an ultra-low Ileak of 7.9 × 10−10 μA/μm coupled with a high Ion of 1352 μA/μm, surpassing other low-dimensional materials-based FETs. These exceptional performances are attributed to the desirable properties from ultra-thin 1Te, including its moderate bandgap, anisotropic effective mass, and reduced screening length. Crucially, this device demonstrates key figure of merits for digital electronics that fulfill both the requirements of high-performance and low-power device specified by the International Technology Roadmap for Semiconductors, indicating the potential as energy-efficient and high-speed electronic switch. Our findings are expected to stimulate further research into sub-5.1 nm quasi-1D materials-based TFETs and provide valuable insights for optimizing their performance.

Experimental Realization of Monolayer α-Tellurene.

2D materials emerge as a versatile platform for developing next-generation devices. The experimental realization of novel artificial 2D atomic crystals, which does not have bulk counterparts in nature, is still challenging and always requires new physical or chemical processes. Monolayer α-tellurene is predicted to be a stable 2D allotrope of tellurium (Te), which has great potential for applications in high-performance field-effect transistors. However, the synthesis of monolayer α-tellurene remains elusive because of its complex lattice configuration, in which the Te atoms are stacked in tri-layers in an octahedral fashion. Here, a self-assemble approach, using three atom-long Te chains derived from the dynamic non-equilibrium growth of an a-Si:Te alloy as building blocks, is reported for the epitaxial growth of monolayer α-tellurene on a Sb2 Te3 substrate. By combining scanning tunneling microscopy/spectroscopy with density functional theory calculations, the surface morphology and electronic structure of monolayer α-tellurene are revealed and the underlying growth mechanism is determined. The successful synthesis of monolayer α-tellurene opens up the possibility for the application of this new single-element 2D material in advanced electronic devices.

Enhanced visible-light-driven photocatalytic activity in SiPGaS/arsenene-based van der Waals heterostructures

Van der Waals heterostructures (vdWHs) showcase robust and tunable light-matter interactions, establishing an intriguing realm for investigating atomic-scale photocatalytic properties. Here, we employ ab initio methods to study the photocatalytic and optical properties of semiconducting SiPGaS/arsenene-based vdWHs with a type-II band alignment. Across the heterointerfaces, there exists significant built-in electric fields and large potential drop, in turn facilitating the spatial separation of photo-generated electron-hole pairs. These vdWHs further possess high carrier mobility in the order of 102 cm2V⁻1S⁻1, which combining with appropriate band edge positions, endow the vdWHs an absorption coefficient of ∼10⁵ cm⁻1 to harvest a maximal portion of the solar spectrum for visible-light-driven photocatalytic applications. Our findings also reveal transition of the type-II band alignment in a type-III configuration via compressive strain for tunneling field-effect transistor application. Furthermore, both types of vdWHs exhibit enhanced suitability for photocatalysis under conditions with a pH of 2.