2D Materials in Flexible Electronics: Recent Advances and Future Prospectives.

Flexible electronics have recently gained considerable attention due to their potential to provide new and innovative solutions to a wide range of challenges in various electronic fields. These electronics require specific material properties and performance because they need to be integrated into a variety of surfaces or folded and rolled for newly formatted electronics. Two-dimensional (2D) materials have emerged as promising candidates for flexible electronics due to their unique mechanical, electrical, and optical properties, as well as their compatibility with other materials, enabling the creation of various flexible electronic devices. This article provides a comprehensive review of the progress made in developing flexible electronic devices using 2D materials. In addition, it highlights the key aspects of materials, scalable material production, and device fabrication processes for flexible applications, along with important examples of demonstrations that achieved breakthroughs in various flexible and wearable electronic applications. Finally, we discuss the opportunities, current challenges, potential solutions, and future investigative directions about this field.

Monolithic 3D integration of 2D materials-based electronics towards ultimate edge computing solutions.

Three-dimensional (3D) hetero-integration technology is poised to revolutionize the field of electronics by stacking functional layers vertically, thereby creating novel 3D circuity architectures with high integration density and unparalleled multifunctionality. However, the conventional 3D integration technique involves complex wafer processing and intricate interlayer wiring. Here we demonstrate monolithic 3D integration of two-dimensional, material-based artificial intelligence (AI)-processing hardware with ultimate integrability and multifunctionality. A total of six layers of transistor and memristor arrays were vertically integrated into a 3D nanosystem to perform AI tasks, by peeling and stacking of AI processing layers made from bottom-up synthesized two-dimensional materials. This fully monolithic-3D-integrated AI system substantially reduces processing time, voltage drops, latency and footprint due to its densely packed AI processing layers with dense interlayer connectivity. The successful demonstration of this monolithic-3D-integrated AI system will not only provide a material-level solution for hetero-integration of electronics, but also pave the way for unprecedented multifunctional computing hardware with ultimate parallelism.

Ultrathin Crystalline Silicon Nano and Micro Membranes with High Areal Density for Low-Cost Flexible Electronics.

Ultrathin crystalline silicon is widely used as an active material for high-performance, flexible, and stretchable electronics, from simple passive and active components to complex integrated circuits, due to its excellent electrical and mechanical properties. However, in contrast to conventional silicon wafer-based devices, ultrathin crystalline silicon-based electronics require an expensive and rather complicated fabrication process. Although silicon-on-insulator (SOI) wafers are commonly used to obtain a single layer of crystalline silicon, they are costly and difficult to process. Therefore, as an alternative to SOI wafers-based thin layers, here, a simple transfer method is proposed for printing ultrathin multiple crystalline silicon sheets with thicknesses between 300 nm to 13 µm and high areal density (>90%) from a single mother wafer. Theoretically, the silicon nano/micro membrane can be generated until the mother wafer is completely consumed. In addition, the electronic applications of silicon membranes are successfully demonstrated through the fabrication of a flexible solar cell and flexible NMOS transistor arrays.

Vertical Conductivity and Topography in Electrostrictive Germanium Sulfide Microribbon via Conductive Atomic Force Microscopy.

Layered group IV monochalcogenides are two-dimensional (2D) semiconducting materials with unique crystal structures and novel physical properties. Here, we report the growth of single crystalline GeS microribbons using the chemical vapor transport process. By using conductive atomic force microscopy, we demonstrated that the conductive behavior in the vertical direction was mainly affected by the Schottky barriers between GeS and both electrodes. Furthermore, we found that the topographic and current heterogeneities were significantly different with and without illumination. The topographic deformation and current enhancement were also predicted by our density functional theory (DFT)-based calculations. Their local spatial correlation between the topographic height and current was established. By virtue of 2D fast Fourier transform power spectra, we constructed the holistic spatial correlation between the topographic and current heterogeneity that indicated the diminished correlation with illumination. These findings on layered GeS microribbons provide insights into the conductive and topographic behaviors in 2D materials.

Graphene-Based Nanomaterials for Flexible and Stretchable Batteries.

Recently, as flexible and wearable electronic devices have become widely popular, research on light weight and large-capacity batteries suitable for powering such devices has been actively conducted. In particular, graphene has attracted considerable attention from researchers in the battery field owing to its good mechanical properties and its applicability in various processes to fabricate electrodes for batteries. Graphene is classified into two types: flake-type, fabricated from graphite, and film-type, synthesized using chemical vapor deposition. The unique processes involved in these two types enable the fabrication of flexible and stretchable batteries with various shapes and functions. In this article, the recent progress in the development of flexible and stretchable batteries based on graphene, as well as its important technical issues are reviewed.

Extra-basal ganglia iron content and non-motor symptoms in drug-naïve, early Parkinson's disease.

BACKGROUND: Although iron dyshomeostasis is associated with Parkinson's disease (PD) pathogenesis, the relationship between iron deposition and non-motor involvement in PD is not fully understood. In this study, we investigated basal ganglia and extra-basal ganglia system iron contents and their correlation with non-motor symptoms in drug-naïve, early-stage PD patients. METHODS: We enrolled 14 drug-naïve, early-stage PD patients and 12 age/sex-matched normal controls. All participants underwent brain magnetic resonance imaging to obtain the effective transverse relaxation rate (R2*) and quantitative susceptibility mapping (QSM). Deep brain structures, including the nucleus accumbens, caudate nucleus, putamen, globus pallidus, thalamus, hippocampus, and amygdala, were delineated using the FSL-FIRST; the substantia nigra, red nucleus, and dentate nucleus were segmented manually. Inter-group differences in R2* and QSM values, as well as their association with clinical parameters of PD, were investigated. RESULTS: Substantia nigra and putamen R2* values were significantly higher in PD patients than in normal controls, despite no significant difference in QSM values. Regarding the non-motor symptom scales, PD sleep scale score negatively correlated with R2* values in the red nucleus and right amygdala, Scales for Outcomes in Parkinson's disease-Autonomic scores were positively correlated with R2* values in the right amygdala and left hippocampus, and cardiovascular sub-score of Non-Motor Symptoms Scale for PD was positively associated with the QSM value in the left hippocampus. CONCLUSION: In this study, iron content in the extra-basal ganglia system was significantly correlated with non-motor symptoms, especially sleep problems and dysautonomia, even in early-stage PD.

Dual Resonant Sum Frequency Generations from Two-Dimensional Materials.

We propose dual resonant optical sum frequency generation (SFG), where the two most singular resonances could be selected, and report for the monolayer (1L-) WSe2 when one (ω1) of two excitation pulses is resonant to A exciton and their sum frequency (ω1 + ω2) to D exciton. The dual resonant SFG confirms that, under an irradiation of ω1 and ω2 pulses with the same fluence of ∼1.4 × 1010 W/m2, its signal intensity could be enhanced about 20 times higher than the resonant SHG (i.e., 2ω1 to the D excitonic absorption). Further, the dual resonant SFG intensity of 1L-WSe2 is found to be 1 order of magnitude higher than the single resonant SFG intensity of 1L-WS2 under the same condition of two-pulse irradiation. Finally, observations of the dual resonant SFG are thoroughly examined using real-time time-dependent density functional theory (rt-TDDFT), and the relevant nonlinear optical characteristics are scrutinized using the Greenwood-Kubo formalism.

Slippery and Wear-Resistant Surfaces Enabled by Interface Engineered Graphene.

Friction and wear remain the primary cause of mechanical energy dissipation and system failure. Recent studies reveal graphene as a powerful solid lubricant to combat friction and wear. Most of these studies have focused on nanoscale tribology and have been limited to a few specific surfaces. Here, we uncover many unknown aspects of graphene's contact-sliding at micro- and macroscopic tribo-scales over a broader range of surfaces. We discover that graphene's performance reduces for surfaces with increasing roughness. To overcome this, we introduce a new type of graphene/silicon nitride (SiNx, 3 nm) bilayer overcoats that exhibit superior performance compared to native graphene sheets (mono and bilayer), that is, display the lowest microscale friction and wear on a range of tribologically poor flat surfaces. More importantly, two-layer graphene/SiNx bilayer lubricant (<4 nm in total thickness) shows the highest macroscale wear durability on tape-head (topologically variant surface) that exceeds most previous thicker (∼7-100 nm) overcoats. Detailed nanoscale characterization and atomistic simulations explain the origin of the reduced friction and wear arising from these nanoscale coatings. Overall, this study demonstrates that engineered graphene-based coatings can outperform conventional coatings in a number of technologies.

Controllable P- and N-Type Conversion of MoTe2 via Oxide Interfacial Layer for Logic Circuits.

To realize basic electronic units such as complementary metal-oxide-semiconductor (CMOS) inverters and other logic circuits, the selective and controllable fabrication of p- and n-type transistors with a low Schottky barrier height is highly desirable. Herein, an efficient and nondestructive technique of electron-charge transfer doping by depositing a thin Al2 O3 layer on chemical vapor deposition (CVD)-grown 2H-MoTe2 is utilized to tune the doping from p- to n-type. Moreover, a type-controllable MoTe2 transistor with a low Schottky barrier height is prepared. The selectively converted n-type MoTe2 transistor from the p-channel exhibits a maximum on-state current of 10 µA, with a higher electron mobility of 8.9 cm2 V-1 s-1 at a drain voltage (Vds ) of 1 V with a low Schottky barrier height of 28.4 meV. To validate the aforementioned approach, a prototype homogeneous CMOS inverter is fabricated on a CVD-grown 2H-MoTe2 single crystal. The proposed inverter exhibits a high DC voltage gain of 9.2 with good dynamic behavior up to a modulation frequency of 1 kHz. The proposed approach may have potential for realizing future 2D transition metal dichalcogenide-based efficient and ultrafast electronic units with high-density circuit components under a low-dimensional regime.

Epidural Electrotherapy for Epilepsy.

Penetrating electronics have been used for treating epilepsy, yet their therapeutic effects are debated largely due to the lack of a large-scale, real-time, and safe recording/stimulation. Here, the proposed technology integrates ultrathin epidural electronics into an electrocorticography array, therein simultaneously sampling brain signals in a large area for diagnostic purposes and delivering electrical pulses for treatment. The system is empirically tested to record the ictal-like activities of the thalamocortical network in vitro and in vivo using the epidural electronics. Also, it is newly demonstrated that the electronics selectively diminish epileptiform activities, but not normal signal transduction, in live animals. It is proposed that this technology heralds a new generation of diagnostic and therapeutic brain-machine interfaces. Such an electronic system can be applicable for several brain diseases such as tinnitus, Parkinson's disease, Huntington's disease, depression, and schizophrenia.

Thickness-Dependent Phonon Renormalization and Enhanced Raman Scattering in Ultrathin Silicon Nanomembranes.

We report on the thickness-dependent Raman spectroscopy of ultrathin silicon (Si) nanomembranes (NMs), whose thicknesses range from 2 to 18 nm, using several excitation energies. We observe that the Raman intensity depends on the thickness and the excitation energy due to the combined effects of interference and resonance from the band-structure modulation. Furthermore, confined acoustic phonon modes in the ultrathin Si NMs were observed in ultralow-frequency Raman spectra, and strong thickness dependence was observed near the quantum limit, which was explained by calculations based on a photoelastic model. Our results provide a reliable method with which to accurately determine the thickness of Si NMs with thicknesses of less than a few nanometers.

Epitaxial Growth of Thin Ferroelectric Polymer Films on Graphene Layer for Fully Transparent and Flexible Nonvolatile Memory.

Enhancing the device performance of organic memory devices while providing high optical transparency and mechanical flexibility requires an optimized combination of functional materials and smart device architecture design. However, it remains a great challenge to realize fully functional transparent and mechanically durable nonvolatile memory because of the limitations of conventional rigid, opaque metal electrodes. Here, we demonstrate ferroelectric nonvolatile memory devices that use graphene electrodes as the epitaxial growth substrate for crystalline poly(vinylidene fluoride-trifluoroethylene) (PVDF-TrFE) polymer. The strong crystallographic interaction between PVDF-TrFE and graphene results in the orientation of the crystals with distinct symmetry, which is favorable for polarization switching upon the electric field. The epitaxial growth of PVDF-TrFE on a graphene layer thus provides excellent ferroelectric performance with high remnant polarization in metal/ferroelectric polymer/metal devices. Furthermore, a fully transparent and flexible array of ferroelectric field effect transistors was successfully realized by adopting transparent poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] semiconducting polymer.

Highly Flexible Hybrid CMOS Inverter Based on Si Nanomembrane and Molybdenum Disulfide.

2D semiconductor materials are being considered for next generation electronic device application such as thin-film transistors and complementary metal-oxide-semiconductor (CMOS) circuit due to their unique structural and superior electronics properties. Various approaches have already been taken to fabricate 2D complementary logics circuits. However, those CMOS devices mostly demonstrated based on exfoliated 2D materials show the performance of a single device. In this work, the design and fabrication of a complementary inverter is experimentally reported, based on a chemical vapor deposition MoS2 n-type transistor and a Si nanomembrane p-type transistor on the same substrate. The advantages offered by such CMOS configuration allow to fabricate large area wafer scale integration of high performance Si technology with transition-metal dichalcogenide materials. The fabricated hetero-CMOS inverters which are composed of two isolated transistors exhibit a novel high performance air-stable voltage transfer characteristic with different supply voltages, with a maximum voltage gain of ≈16, and sub-nano watt power consumption. Moreover, the logic gates have been integrated on a plastic substrate and displayed reliable electrical properties paving a realistic path for the fabrication of flexible/transparent CMOS circuits in 2D electronics.

Stretchable Si Logic Devices with Graphene Interconnects.

Stretchable integrated circuits consisting of ultrathin Si transistors connected by multilayer graphene are demonstrated. Graphene interconnects act as an effective countervailing component to maintain the electrical performance of Si integrated circuits against external strain. Concentration of the applied strain on the graphene interconnect parts can stably protect the Si active devices against applied strains over 10%.

Flexible graphene based microwave attenuators.

We demonstrate flexible 3 dB and 6 dB microwave attenuators using multilayer graphene grown by the chemical vapor deposition method. On the basis of the characterized results of multilayer graphene and graphene-Au ohmic contacts, the graphene attenuators are designed and measured. The flexible graphene-based attenuators have 3 dB and 6 dB attenuation with a return loss of less than -15 dB at higher than 5 GHz. The devices have shown durability in a bending cycling test of 100 times. The circuit model of the attenuator based on the characterized results matches the experimental results well.

Large-scale pattern growth of graphene films for stretchable transparent electrodes.

Problems associated with large-scale pattern growth of graphene constitute one of the main obstacles to using this material in device applications. Recently, macroscopic-scale graphene films were prepared by two-dimensional assembly of graphene sheets chemically derived from graphite crystals and graphene oxides. However, the sheet resistance of these films was found to be much larger than theoretically expected values. Here we report the direct synthesis of large-scale graphene films using chemical vapour deposition on thin nickel layers, and present two different methods of patterning the films and transferring them to arbitrary substrates. The transferred graphene films show very low sheet resistance of approximately 280 Omega per square, with approximately 80 per cent optical transparency. At low temperatures, the monolayers transferred to silicon dioxide substrates show electron mobility greater than 3,700 cm(2) V(-1) s(-1) and exhibit the half-integer quantum Hall effect, implying that the quality of graphene grown by chemical vapour deposition is as high as mechanically cleaved graphene. Employing the outstanding mechanical properties of graphene, we also demonstrate the macroscopic use of these highly conducting and transparent electrodes in flexible, stretchable, foldable electronics.

Observation of the inverse giant piezoresistance effect in silicon nanomembranes probed by ultrafast terahertz spectroscopy.

The anomalous piezoresistance (a-PZR) effects, including giant PZR (GPZR) with large magnitude and inverse PZR of opposite, have exciting technological potentials for their integration into novel nanoelectromechanical systems. However, the nature of a-PZR effect and the associated kinetics have not been clearly determined yet. Even further, there are intense research debates whether the a-PZR effect actually exists or not; although numerous investigations have been conducted, the origin of the effect has not been clearly understood. This paper shows the existence of a-PZR and provides direct experimental evidence through the performance of well-established electrical measurements and terahertz spectroscopy on silicon nanomembranes (Si NMs). The clear inverse PZR behavior was observed in the Si NMs when the thickness was less than 40 nm and the magnitude of the PZR response linearly increased with the decreasing thickness. Observations combined with electrical and optical measurements strongly corroborate that the a-PZR effect originates from the carrier concentration changes via charge carrier trapping into strain-induced defect states.

Organic solar cells using CVD-grown graphene electrodes.

We report on the development of flexible organic solar cells (OSCs) incorporating graphene sheets synthesized by chemical vapor deposition (CVD) as transparent conducting electrodes on polyethylene terephthalate (PET) substrates. A key barrier that must be overcome for the successful fabrication of OSCs with graphene electrodes is the poor-film properties of water-based poly(3,4-ethylenedioxythiphene):poly(styrenesulfonate) (PEDOT:PSS) when coated onto hydrophobic graphene surfaces. To form a uniform PEDOT:PSS film on a graphene surface, we added perfluorinated ionomers (PFI) to pristine PEDOT:PSS to create 'GraHEL', which we then successfully spin coated onto the graphene surface. We systematically investigated the effect of number of layers in layer-by-layer stacked graphene anode of an OSC on the performance parameters including the open-circuit voltage (Voc), short-circuit current (Jsc), and fill factor (FF). As the number of graphene layers increased, the FF tended to increase owing to lower sheet resistance, while Jsc tended to decrease owing to the lower light absorption. In light of this trade-off between sheet resistance and transmittance, we determined that three-layer graphene (3LG) represents the best configuration for obtaining the optimal power conversion efficiency (PCE) in OSC anodes, even at suboptimal sheet resistances. We finally developed efficient, flexible OSCs with a PCE of 4.33%, which is the highest efficiency attained so far by an OSC with CVD-grown graphene electrodes to the best of our knowledge.

Photo-patternable ion gel-gated graphene transistors and inverters on plastic.

We demonstrate photo-patternable ion gel-gated graphene transistors and inverters on plastic substrates. The photo-patternable ion gel can be used as a negative photoresist for the patterning of underlying graphene as well as gate dielectrics. As a result, an extra graphene-patterning step is not required, which simplifies the device fabrication and avoids a side effect arising from the photoresist residue. The high capacitance of ion gel gate dielectrics yielded a low voltage operation (~2 V) of the graphene transistor and inverter. The graphene transistors on plastic showed an on/off-current ratio of ~11.5, along with hole and electron mobilities of 852 ± 124 and 452 ± 98 cm(2) V(-1) s(-1), respectively. In addition, the flexible graphene inverter was successfully fabricated on plastic through the potential superposition effect from the drain bias. These devices show excellent mechanical flexibility and fatigue stability.

Quantum confinement effects in transferrable silicon nanomembranes and their applications on unusual substrates.

Two dimensional (2D) semiconductors have attracted attention for a range of electronic applications, such as transparent, flexible field effect transistors and sensors owing to their good optical transparency and mechanical flexibility. Efforts to exploit 2D semiconductors in electronics are hampered, however, by the lack of efficient methods for their synthesis at levels of quality, uniformity, and reliability needed for practical applications. Here, as an alternative 2D semiconductor, we study single crystal Si nanomembranes (NMs), formed in large area sheets with precisely defined thicknesses ranging from 1.4 to 10 nm. These Si NMs exhibit electronic properties of two-dimensional quantum wells and offer exceptionally high optical transparency and low flexural rigidity. Deterministic assembly techniques allow integration of these materials into unusual device architectures, including field effect transistors with total thicknesses of less than 12 nm, for potential use in transparent, flexible, and stretchable forms of electronics.