Monolayer 2D Materials Research Articles

Encapsulation of linear carbon chains in single-walled carbon nanotubes: Towards 1D van der Waals heterostructures for high-efficiency excitonic solar cells

One-dimensional van der Waals heterostructures (1D vdW HTs) based on single-walled carbon nanotubes (SWCNTs) encapsulating linear carbon chains (LCCs) with tunable optoelectronic properties provide a fresh ground for efficient excitonic solar cells (XSCs) alternative to those based on 2D monolayer materials. As an effort to identify for the first time 1D vdW HTs for efficient XSCs application, we perform here a systematic theoretical investigation on the energetic and structural stability, optoelectronic and photovoltaic properties of 1D vdW HTs based on SWCNTs encapsulating 50 symmetrical LCCs of different lengths, and capped with different conjugated endgroups through comprehensive first-principles calculations. We showed the fundamental role of the length and the endgroups effects in modulating the optoelectronic properties of LCCs. Through exploration of the energetic stability of the 1D vdW HTs of LCCs@SWCNTs from the universal force field (UFF) including vdW interactions, we determined the optimal SWCNTs diameters for which the resulting 1D vdW HTs are stable. Then, the band alignment in the 50 stable 1D vdW HTs of LCCs@SWCNTs is examined. Intriguingly, stable LCCs@SWCNTs are identified as type-II 1D vdW HTs complying the prerequisite of XSCs with strong optical absorption in the UV–visible-NIR spectral regions, and power conversion efficiency (PCE) reaching well over 21 %. These findings unravel the enormous potential of the 1D vdW HTs in designing next-generation XSCs devices competitive with state-of-the-art solar cells.

(Invited) Electrical, Optical, and Mechanical Properties of Two-Dimensional Materials

Atomically thin two-dimensional materials are direct bandgap semiconductors with a rich interplay of the valley and spin degrees of freedom, which offer the potential for electronics and optoelectronics. A strong Coulomb interaction leads to tightly bound electron-hole pairs or excitons and two-electron one-hole quasiparticles or trions. We solve the two-particle and three-particle problems for the wavefunctions for excitons and trions in the basis set of the model- Hamiltonian for single particles. The calculated linear absorptions, photoluminescence spectra, and polariton spectra as a function of doping and temperature explain the experimental data in 2D monolayers and predict novel spectroscopic features due to the many-body Coulomb interactions. Exciton lifetime plays a crucial role in optoelectronic applications. I will also discuss the phonon-assisted Auger non-radiative decay mechanism of excitons in doped 2D materials. Finally, I will discuss the strain engineering in monolayer 2D materials transferred on 1D and 2D patterned substrates. This material is based upon work supported by the Air Force Office of Scientific Research under award number FA9550-22-1-0312.

Spatial Control of 2D Nanomaterial Electronic Properties Using Chiral Light Beams.

Single-layer two-dimensional (2D) nanomaterials exhibit physical and chemical properties which can be dynamically modulated through out-of-plane deformations. Existing methods rely on intricate micromechanical manipulations (e.g., poking, bending, rumpling), hindering their widespread technological implementation. We address this challenge by proposing an all-optical approach that decouples strain engineering from micromechanical complexities. This method leverages the forces generated by chiral light beams carrying orbital angular momentum (OAM). The inherent sense of twist of these beams enables the exertion of controlled torques on 2D monolayer materials, inducing tailored strain. This approach offers a contactless and dynamically tunable alternative to existing methods. As a proof-of-concept, we demonstrate control over the conductivity of graphene transistors using chiral light beams, showcasing the potential of this approach for manipulating properties in future electronic devices. This optical control mechanism holds promise in enabling the reconfiguration of devices through optically patterned strain. It also allows broader utilization of strain engineering in 2D nanomaterials for advanced functionalities in next-generation optoelectronic devices and sensors.

Deviatoric stress-induced metallization, layer reconstruction and collapse of van der Waals bonded zirconium disulfide

In contrast to two-dimensional (2D) monolayer materials, van der Waals layered transition metal dichalcogenides exhibit rich polymorphism, making them promising candidates for novel superconductor, topological insulators and electrochemical catalysts. Here, we highlight the role of hydrostatic pressure on the evolution of electronic and crystal structures of layered ZrS2. Under deviatoric stress, our electrical experiments demonstrate a semiconductor-to-metal transition above 30.2 GPa, while quasi-hydrostatic compression postponed the metallization to 38.9 GPa. Both X-ray diffraction and Raman results reveal structural phase transitions different from those under hydrostatic pressure. Under deviatoric stress, ZrS2 rearranges the original ZrS6 octahedra into ZrS8 cuboids at 5.5 GPa, in which the unique cuboids coordination of Zr atoms is thermodynamically metastable. The structure collapses to a partially disordered phase at 17.4 GPa. These complex phase transitions present the importance of deviatoric stress on the highly tunable electronic properties of ZrS2 with possible implications for optoelectronic devices.

Tuning instability in suspended monolayer 2D materials

Monolayer two-dimensional (2D) materials possess excellent in-plane mechanical strength yet extremely low bending stiffness, making them particularly susceptible to instability, which is anticipated to have a substantial impact on their physical functionalities such as 2D-based Micro/Nanoelectromechanical systems (M/NEMS), nanochannels, and proton transport membrane. In this work, we achieve quantitatively tuning instability in suspended 2D materials including monolayer graphene and MoS2 by employing a push-to-shear strategy. We comprehensively examine the dynamic wrinkling-splitting-smoothing process and find that monolayer 2D materials experience stepwise instabilities along with different recovery processes. These stepwise instabilities are governed by the materials’ geometry, pretension, and the elastic nonlinearity. We attribute the different instability and recovery paths to the local stress redistribution in monolayer 2D materials. The tunable instability behavior of suspended monolayer 2D materials not only allows measuring their bending stiffness but also opens up new opportunities for programming the nanoscale instability pattern and even physical properties of atomically thin films.

Vanadium Metal Doping of Monolayer MoS2 for p-Type Transistors and Fast-Speed Phototransistors.

Modulating the electrical properties of two-dimensional (2D) materials is a fundamental prerequisite for their development to advanced electronic and optoelectronic devices. Substitutional doping has been demonstrated as an effective method for tuning the band structure in monolayer 2D materials. Here, we demonstrate a facile selective-area growth of vanadium-doped molybdenum disulfide (V-doped MoS2) flakes via pre-patterned vanadium-metal-assisted chemical vapor deposition (CVD). Optical microscopy characterization revealed the presence of flake arrays. Transmission electron microscopy, Raman spectroscopy, and X-ray photoelectron spectroscopy were employed to identify the chemical composition and crystalline structure of as-grown flakes. Electrical measurements indicated a light p-type conduction behavior in monolayer V-doped MoS2. Furthermore, the response time of phototransistors based on V-doped MoS2 monolayers exhibited a remarkable capability of 3 ms, representing approximately 3 orders of magnitude faster response than that observed in pure MoS2 phototransistors. This work hereby provides a feasible approach to doping of 2D materials, promising a scalable pathway for the integration of these materials into emerging electronic and optoelectronic devices.

Unveiling the potential of vanadium-doped CVD-grown p-type MoS2 in vertical homojunction UV–Vis photodiodes

2D materials are a popular choice for the fabrication of p-n diodes for applications in integrated optoelectronics owing to their outstanding properties such as strong light-matter interactions, high mobility, and tunable band gap. The synthesis of monolayer and few-layer 2D materials with both p-type and n-type behavior is thus essential for the design and fabrication of such devices. However, the large-scale direct synthesis of p-type 2D materials is still a challenge as most of these materials are either n-type or ambipolar. Here, we report the successful synthesis of large-area, p-type MoS2 layers doped with vanadium on SiO2/Si substrates, achieving flake sizes >100 μm. By varying the concentration of the vanadium precursor, we precisely controlled the doping level, achieving vanadium atomic percentages ranging from 0.70 % to 1.57 %. Back gate field-effect transistors (FETs) were fabricated, enabling the tuning of device characteristics to exhibit ambipolar or p-type behavior. Moreover, a vertical p-n MoS2 homojunction was fabricated for rectification and optoelectronic applications, demonstrating a high responsivity of up to 978.1 A/W and a specific detectivity (D*) of 1.06 × 1012 Jones at λ = 365 nm with varied powers of the incident light source. This work demonstrates the role of vanadium as a dopant for tunable electrical transport behavior as well as for the fabrication of a photodiode, which can be used for high-performance optoelectronic devices in the future.

Oxygen Driven Defect Engineering of Monolayer MoS2 for Tunable Electronic, Optoelectronic, and Electrochemical Devices

AbstractMolybdenum disulfide (MoS2), a two‐dimensional (2D) semiconducting material harbors intrinsic defects that can be harnessed to achieve tuneable electronic, optoelectronic, and electrochemical devices. However, achieving precise control over defect formation within monolayer MoS2, remains a notable challenge. Here, an in‐situ defect engineering approach for monolayer MoS2 using a pressure‐dependent chemical vapor deposition (CVD) process is presented. Monolayer MoS2 grown in a low pressure CVD conditions (LP‐MoS2) produces sulfur vacancy (Vs) induced defect‐rich crystals primarily attributed to the oxygen‐deficient growth conditions. Conversely, atmospheric pressure CVD‐grown MoS2 (AP‐MoS2) passivates these defects with oxygen from ambient conditions. This disparity in defect profiles profoundly impacts crucial functional properties and device performance. AP‐MoS2 shows a drastically enhanced photoluminescence, which is significantly quenched in LP‐MoS2 attributed to in‐gap electron donor states induced by the Vs defects. However, the n‐doping induced in LP‐MoS2 generates enhanced photoresponsivity and detectivity in fabricated photodetectors compared to the AP‐MoS2‐based devices. Defect‐rich LP‐MoS2 outperforms AP‐MoS2 as channel layers of field‐effect transistors (FETs), as well as electrocatalytic material for hydrogen evolution reaction (HER). This work presents a single‐step CVD approach for in situ defect engineering in monolayer MoS2 and presents a pathway to control defects in other monolayer 2D materials.

Resistive Memory Devices at the Thinnest Limit: Progress and Challenges.

The Si-based integrated circuits industry has been developing for more than half a century, by focusing on the scaling-down of transistor. However, the miniaturization of transistors will soon reach its physical limits, thereby requiring novel material and device technologies. Resistive memory is a promising candidate for in-memory computing and energy-efficient synaptic devices that can satisfy the computational demands of the future applications. However, poor cycle-to-cycle and device-to-device uniformities hinder its mass production. 2D materials, as a new type of semiconductor, is successfully employed in various micro/nanoelectronic devices and have the potential to drive future innovation in resistive memory technology. This review evaluates the potential of using the thinnest advanced materials, that is, monolayer 2D materials, for memristor or memtransistor applications, including resistive switching behavior and atomic mechanism, high-frequency device performances, and in-memory computing/neuromorphic computing applications. The scaling-down advantages of promising monolayer 2D materials including graphene, transition metal dichalcogenides, and hexagonal boron nitride are presented. Finally, the technical challenges of these atomic devices for practical applications are elaborately discussed. The study of monolayer-2D-material-based resistive memory is expected to play a positive role in the exploration of beyond-Si electronic technologies.

Tunable bandgaps, stabilities and optical properties of X3Y (X=C, Si; Y[dbnd]N, P) monolayers with and without strain

Our study explores the various properties of a novel class of two-dimensional (2D) monolayer materials, i.e., X3Y (X = C, Si; YN, P). The materials (i.e., C3N, C3P, Si3N, Si3P) exhibit dynamic and thermal stabilities through phonon and molecular dynamics calculations. Under biaxial tensile strain of approximately 11 %, the structures undergo only deformation, indicating their ideal strength. The phonon spectra remain dynamically stable under this 11 % biaxial strain, emphasizing the high mechanical stability of the three materials. The electronic structure showed band gaps of 0.39 eV, 1.56 eV, 0.0 eV, and 0.27 eV for C3N, C3P, Si3N, and Si3P, respectively, which are crucial for electronic devices. Meanwhile, we have found the transitions from metal to semiconductor (Si3N), indirect to direct band gap (Si3P), and semiconductor to metal (C3N, Si3P) by applying compressive and tensile strains to tune the bandgaps. In addition, we have investigated the optical properties excellent absorption in the visible range for C3P, Si3N. Compressive and tensile strains also have a significant effect on these four materials, with both absorption coefficient has been enhanced under strain to some extent. These findings provide potential applications in nano-electronic and opto-electronic devices.

(Invited) Deformation of 2D Semiconductors By Interfaces with Organic Materials

2D semiconducting materials gather attention for realizing atomically thin optoelectronic devices and a platform for emerging quantum phenomena. Especially monolayer 2D materials are fascinating because of their ultrathin crystalline structure with various physicochemical characteristics such as direct-band gap and asymmetric crystalline structures. In this presentation, I will show our recent results related to the deformation of transition metal chalcogenides (TMDCs) morphology by interfaces with organic materials.The mechanical exfoliation method is a simple method to prepare TMDCs and has been widely applied in many research studies. However, the exfoliated TMDCs on substrates show a bunch of bulk flakes and very few target monolayers. In the worst case, the exfoliated monolayer is surrounded by bulk flakes and is difficult to apply for fabricating devices. We developed a method of selectively removing bulk flakes, furthermore, isolating monolayer TMDCs on substrates. The method uses ultrasonication in organic solvents with a consideration of surface chemistry. Surprisingly, bulk flakes are selectively removed, and the adjacent monolayers can be effectively isolated on substrates. [1]Monolayer TMDCs show emission properties because of their direct-band gap nature. The emission strength, e.g., photoluminescence (PL) intensity, is often low. The limitation factor includes various parameters, for example, the over-carrier concentration is one limiting factor in sulfur-based compounds (MoS2 and WS2). So far, p-type doping to reduce the electron concentration is demonstrated to enhance their PL intensity, however, the method is not applicable to selenium-based compounds, such as MoSe2 and WSe2. In addition, a universal method to enhance PL intensity for the selenium-based compounds is still few. We found a general PL enhancement method for both sulfur- and selenium-based compounds, MoS2, WS2, MoSe2, and WSe2, by applying a hydrocarbon, paraffin. The method simply uses paraffin on the surface of TMDCs. I would show the details of the results and methods in the presentation. [2]REF:[1] T. Nakamoto, et al., " Selective isolation of mono to quad layered 2D materials via sonication-based solution engineering", ChemRxiv, 2022, DOI: 10.26434/chemrxiv-2022-lgp8l[2] T. Nakahara, et al., " Spontaneous crystal fluctuation in hydrocarbon polymer–coated monolayer MoS2, MoSe2, WS2, and WSe2 with strong photoluminescence enhancement", ChemRxiv, 2023, DOI: 10.26434/chemrxiv-2023-gxzqw

Characterization of 2D Transition Metal Dichalcogenides Through Anisotropic Exciton Behaviors.

This study reports the first attempt to characterize the quality, defects, and strain of as-grown monolayer transition metal dichalcogenide (TMDC)-based 2D materials through exciton anisotropy. A standard ellipsometric parameter (Ψ) to observe anisotropic exciton behavior in monolayer 2D materials is used. According to the strong exciton effect from phonon-electron coupling processes, the change in the exciton in the Van Hove singularity is sensitive to lattice distortions such as defects and strain. In comparison with Raman spectroscopy, the variations in exciton anisotropy in Ψ are more sensitive for detecting slight changes in the quality and strain of monolayer TMDC films. Moreover, the optical power requirement for TMDC characterization through exciton anisotropy in Ψ is ≈10-5mWcm-2, which is significantly less than that of Raman spectroscopy (≈106mWcm-2). The standard deviation of the signals varies with strain (defects) in Raman spectra and exciton anisotropies in Ψ are 0.700 (0.795) and 0.033 (0.073), indicating that exciton anisotropy is more sensitive to slight changes in the quality of monolayer TMDC films.

Chemical Bonding and Activity of Atomically Dispersed Silicon in Two- and Three-Dimensional Materials.

On the basis of the especially tunable electronic property of Si, several kinds of nanomaterials with atomically dispersed Si were constructed and characterized by extensive first-principles calculations and ab initio molecular dynamics (AIMD) simulations. The new-type Si(X≡Y)n wide-bandgap semiconductors featuring through-space d-π* hyperconjugation exhibit unique properties in photoelectric conversion, photoconductivity, structural mechanics, etc. The SiC8 siligraphene with the planar tetracoordinate Si (ptSi) has a high lithium-storage capacity and comparably facile surface migration behaviors of both Li and Li+, making it a promising anode material for high-performance Li-ion batteries. The atomically dispersed Si sites of 2D monolayer materials, such as ptSi and three- and four-coordinated Si atoms, generally exhibit remarkable catalytic activity toward CO2 activation with different electron mechanisms, resulting in different scaling relations between the activity and the p-band center. The computational findings enrich the understanding of structural and chemical properties of silicon and open up avenues for developing Si-based functional materials.

Theoretical prediction of stable WB4 monolayer as a high-capacity anode material for alkali-metal ion batteries

As a rapidly evolving 2D monolayer material, tungsten tetraboride MBene exhibits innate advantages in electrochemical applications because of its unique graphene-like structure and metallic properties. In this study, we utilized first-principles calculations to identify the potential applications of WB4 as an anode material in rechargeable alkali-metal-ion batteries. The findings imply that the Li, Na, and K adsorption on the WB4 surface results in exceptionally high conductivity, and the WB4 monolayer can effectively adsorb these ions with significant adsorption energies of −2.516 eV, −2.356 eV, and −2.941 eV for Li, Na, and K ions, respectively. The results indicate that WB4 exhibits excellent stability during lithiation, sodiation, and potassiation. Notably, we propose high storage capacities for LIBs (708mAh/g), SIBs (472mAh/g), and KIBs (177 mAh/g), with maintained structural stability for the adsorption of these metal ions. The measured average open circuit voltages for WB4 were found to be 0.77 V (Li), 0.73 V (Na), and 0.80 V (K), and metallicity remain good maintained within the entire adsorption process. The calculated migration energy barriers for Li, Na, and K were 0.47 eV,0.21 eV and 0.13 eV respectively. The notable properties of WB4 make it an advantageous electrode material for alkali-metal ion batteries.

Negative Poisson’s Ratios of Layered Materials by First-Principles High-Throughput Calculations

Auxetic two-dimensional (2D) materials, known from their negative Poisson’s ratios (NPRs), exhibit the unique property of expanding (contracting) longitudinally while being laterally stretched (compressed), contrary to typical materials. These materials offer improved mechanical characteristics and hold great potential for applications in nanoscale devices such as sensors, electronic skins, and tissue engineering. Despite their promising attributes, the availability of 2D materials with NPRs is limited, as most 2D layered materials possess positive Poisson’s ratios. In this study, we employ first-principles high-throughput calculations to systematically explore Poisson’s ratios of 40 commonly used 2D monolayer materials, along with various bilayer structures. Our investigation reveals that BP, GeS and GeSe exhibit out-of-plane NPRs due to their hinge-like puckered structures. For 1T-type transition metal dichalcogenides such as MX 2 (M = Mo, W; X = S, Se, Te) and transition metal selenides/halides the auxetic behavior stems from a combination of geometric and electronic structural factors. Notably, our findings unveil V2O5 as a novel material with out-of-plane NPR. This behavior arises primarily from the outward movement of the outermost oxygen atoms triggered by the relaxation of strain energy under uniaxial tensile strain along one of the in-plane directions. Furthermore, our computations demonstrate that Poisson’s ratio can be tuned by varying the bilayer structure with distinct stacking modes attributed to interlayer coupling disparities. These results not only furnish valuable insights into designing 2D materials with a controllable NPR but also introduce V2O5 as an exciting addition to the realm of auxetic 2D materials, holding promise for diverse nanoscale applications.

Giant enhancement of second harmonic generation from monolayer 2D materials placed on photonic moiré superlattice

Abstract We numerically investigate second harmonic generation (SHG) from a monolayer of 2D-material placed on photonic moiré superlattice fabricated by dielectric materials. The greatly enhanced local field at the resonance modes of moiré superlattice can dramatically boost the SHG response in 2D materials. Considering a typical 2D-material MoS2 monolayer placed on a photonic moiré superlattice of a twist angle 9.43°, the maximum SHG conversion efficiency reaches up to 10−1 at a relatively low intensity of fundamental light 1 kW/cm2, which is around 14 orders of magnitude larger than that from the monolayer placed on a flat dielectric slab without moiré superlattices. The SHG conversion efficiency from the monolayer can be further enhanced with the decrease of the twist angles of moiré superlattice due to the even more confinement of local field. The flat bands in the moiré superlattices formed by the small twist angles can particularly ensure the efficiency even under wide-angle illuminations. The results indicate that photonic moiré superlattice which can tightly confine light is a promising platform for efficient nonlinear optics.

Two-Dimensional Ferroelectric C2N/In2Se3 Heterobilayer with Tunable Electronic Property and Photovoltaic Effect.

Two-dimensional ferroelectric monolayer materials with reversible spontaneous polarization provide more regulatory dimensions for their relevant van der Waals heterostructures. Using first-principles calculations, we construct the C2N/In2Se3 bilayer heterostructure and study its physical properties as well as the effects of E-field and strain. The results indicate that the intrinsic polarization of the component In2Se3 monoalyer can significantly adjust the electronic properties of the C2N/In2Se3 heterobilayer. When the polarization of the In2Se3 monolayer points to the interface (up-In2Se3), the C2N/In2Se3 bilayer behaves as the type-I indirect band gap heterostructure, while it transforms to the type-II direct band gap heterostructure after reversing the polarization of the In2Se3 monolayer (dp-In2Se3). Furthermore, the two C2N/In2Se3 heterostructures both have enhanced optical absorption in the visible region than the isolated In2Se3 and C2N monolayers. More importantly, the external electric field and strain can easily regulate the electronic properties of the C2N/In2Se3 heterostructures. The power conversion efficiency (PCE) of the type-II C2N/dp-In2Se3 heterostructure is 8.16%, and the electric field of 0.1 V/Å and the strain of -2% can transform the C2N/up-In2Se3 heterostructure into type-II one, conducive to the high PCE up to 24.03 and 24%, respectively. Our proposed C2N/In2Se3 heterostructure is promising in future luminescent and photovoltaic fields, and our findings also provide a strategy for functionalizing 2D monolayer materials by the intrinsic polarization property of ferroelectric materials.

Dielectric breakdown and sub-wavelength patterning of monolayer hexagonal boron nitride using femtosecond pulses

Hexagonal boron nitride (hBN) has emerged as a promising two-dimensional (2D) material for many applications in electronics and photonics. Although its linear and nonlinear optical properties have been extensively studied, the interaction of hBN with high-intensity laser pulses, which is important for realizing high-harmonic generation, creating deterministic defects as quantum emitters, and resist-free patterning in this material, has not been investigated. Here we report the first systematic study of dielectric breakdown in chemical vapor deposition (CVD)-grown hBN monolayers induced by single femtosecond laser pulses. We report a breakdown fluence of 0.7 J cm−2, which is at least 7× higher than that of other monolayer 2D materials. A clean removal of hBN without leaving traces behind or causing lateral damage is demonstrated. The ablation features exhibit excellent fidelity with very small edge roughness, which we attribute to its ultrahigh fracture toughness due to its heterogeneous nature with three-fold symmetry. Moreover, even though defects are known to be abundant in CVD-grown hBN, we show experimentally and theoretically that its nonlinear optical breakdown is nearly intrinsic as defects only marginally lower the breakdown threshold. On top of this, we observe that hBN monolayers have a 4–5× lower breakdown threshold than their bulk equivalent. The last two observations can be understood if the carrier generation in monolayers is intrinsically enhanced due to its 2D nature. Finally, we demonstrate laser patterning of array of holes and lines in hBN with sub-wavelength feature sizes. Our work advances the fundamental knowledge of light-hBN interaction in the strong field regime and firmly establishes femtosecond lasers as novel and promising tools for resist-free patterning of hBN monolayers with high fidelity.

Can a deep-learning model make fast predictions of vacancy formation in diverse materials?

The presence of point defects, such as vacancies, plays an important role in materials design. Here, we explore the extrapolative power of a graph neural network (GNN) to predict vacancy formation energies. We show that a model trained only on perfect materials can also be used to predict vacancy formation energies (Evac) of defect structures without the need for additional training data. Such GNN-based predictions are considerably faster than density functional theory (DFT) calculations and show potential as a quick pre-screening tool for defect systems. To test this strategy, we developed a DFT dataset of 530 Evac consisting of 3D elemental solids, alloys, oxides, semiconductors, and 2D monolayer materials. We analyzed and discussed the applicability of such direct and fast predictions. We applied the model to predict 192 494 Evac for 55 723 materials in the JARVIS-DFT database. Our work demonstrates how a GNN-model performs on unseen data.

Solution-Processed 2D Transition Metal Dichalcogenides: Materials to CMOS Electronics

ConspectusTwo-dimensional (2D) semiconducting transition metal dichalcogenides (TMDs) have demonstrated exceptional potential as materials for future complementary metal-oxide-semiconductor (CMOS) technology. This is primarily because of their atomic thickness and excellent electrical and mechanical properties. With advancements in fabrication technology, electronic devices based on 2D TMD materials have rapidly progressed from isolated units for scientific experimentation to integrated circuits with practical applications. Among the different production methods, the solution-processing of 2D TMD nanomaterial dispersions offers the distinct advantages of low-temperature processing and cost-effective manufacturing for large-scale flexible and wearable electronics. A wide range of 2D nanoflake inks with versatile electronic properties can be assembled into atomic-thick thin films with dangling-bond-free van der Waals interfaces between adjacent nanoflakes. Furthermore, direct printing techniques can easily integrate multifunctional devices, such as n-type and p-type transistors, into CMOS devices and more complex integrated circuits. Despite these benefits and previous accomplishments, the field of solution-processed CMOS electronics using 2D TMD semiconducting materials is in its early stages of development and requires further research. One of the current challenges is the production of scalable and high-purity 2D semiconductor mono- and few layers with large lateral sizes and narrow thickness distribution. The field-effect mobility of solution-processed 2D TMD transistors remains lower than that of the transistors manufactured using mechanical exfoliation and chemical vapor deposition methods. In particular, limited research has been conducted on solution-processed p-type 2D TMD transistors. As a result, solution-processed CMOS devices using n-type and p-type 2D TMD transistors are scarce. In this Account, we provide an overview of the recent progress in the field of solution-processed CMOS electronics employing 2D TMD materials. First, we introduce the basic liquid exfoliation methods, such as sonication-assisted exfoliation and molecular intercalation methods, that are commonly utilized to prepare 2D TMD dispersions. In addition, we discuss the production of monolayer 2D materials, which serve as the building blocks for fabricating atomic-thick thin films. Subsequently, we review the typical techniques for depositing 2D inks, including spin coating, drop casting, and inkjet printing. Furthermore, we outline the thin-film patterning process for each technique, which is crucial for integrating multifunctional materials in CMOS devices. Subsequently, we focus on the recent advancements in solution-processed 2D TMD transistors. Furthermore, we explore the various factors that can improve the performance of the devices with regard to charge transport and charge traps. Afterward, we highlight notable applications of solution-processed CMOS technology, such as logic circuits and ring oscillators. Finally, we provide an overview of the challenges and opportunities in the development of solution-processed 2D materials and the integration of multifunctional devices for the advancement of CMOS electronics. This Account aims to provide a comprehensive guide for readers, offering both a broad overview and an in-depth insight into solution-processed 2D material-based electronics, covering a wide range of topics from the preparation of 2D TMD ink to device fabrication and CMOS applications. Therefore, this Account is expected to drive further progress and advancements in this field and promote the realization of practical applications.