3D-Printed Soft Temperature Sensors Based on Thermoelectric Effects for Fast Mapping of Localized Temperature Distributions.

We propose a novel design of thermoelectric (TE) effect-based soft temperature sensors for directly monitoring localized subtle temperature stimuli. This design integrates rheology-engineered three-dimensional (3D) printing of high-performance carbon-based TE materials and polymer-based viscoelastic materials with low thermal conductivity. Rheological engineering of carbon nanotube (CNT) TE inks ensures the 3D printing of highly sensitive TE sensing units on directly written 3D soft platforms. Additionally, we pre-dope CNT inks with p- and n-type organic dopants to achieve high sensitivity and a fast response to temperature changes. The introduced 3D soft platforms with low thermal conductivity lead to an efficient thermal gradient on TE sensing units in the out-of-plane direction. Furthermore, encapsulating the temperature sensor array with the same polymer-based materials as the 3D soft platforms facilitates independent detection of localized temperature stimuli by minimizing thermal interaction between sensing units, resulting in precise temperature mapping by localized detection. Our 3D-printed soft temperature sensors exhibit high sensitivity to relatively small temperature changes, with a minimum sensing resolution of 0.1 K within tens of milliseconds. Moreover, the temperature sensor array not only detects localized temperature stimuli by imaging the temperature distribution but also demonstrates remarkable mechanical reliability against repetitive deformation with high accuracy.

Roll-to-plate 0.1-second shear-rolling process at elevated temperature for highly aligned nanopatterns.

The shear-rolling process is a promising directed self-assembly method that can produce high-quality sub-10 nm block copolymer line-space patterns cost-effectively and straightforwardly over a large area. This study presents a high temperature (280 °C) and rapid (~0.1 s) shear-rolling process that can achieve a high degree of orientation in a single process while effectively preventing film delamination, that can be applied to large-area continuous processes. By minimizing adhesion, normal forces, and ultimate shear strain of the polydimethylsiloxane pad, shearing was successfully performed without peeling up to 280 °C at which the chain mobility significantly increases. This method can be utilized for various high-χ block copolymers and surface neutralization processes. It enables the creation of block copolymer patterns with a half-pitch as small as 8 nm in a unidirectional way. Moreover, the 0.1-second rapid shear-rolling was successfully performed on long, 3-inch width polyimide flexible films to validate its potential for the roll-to-roll process.

High temporal resolution transparent thermoelectric temperature sensors for photothermal effect sensing.

We propose inkjet-printed high-speed and transparent temperature sensors based on the thermoelectric effect for direct monitoring of the photothermal effect. They consist of highly transparent organic thermoelectric materials that allow excellent biocompatibility and sub-ms temporal resolution, simultaneously. Our transparent thermoelectric temperature sensors can be used to advance various photothermal biomedical applications.

Direct patterning of colloidal quantum dots with adaptable dual-ligand surface.

Colloidal quantum dots (QDs) stand at the forefront of a variety of photonic applications given their narrow spectral bandwidth and near-unity luminescence efficiency. However, integrating luminescent QD films into photonic devices without compromising their optical or transport characteristics remains challenging. Here we devise a dual-ligand passivation system comprising photocrosslinkable ligands and dispersing ligands to enable QDs to be universally compatible with solution-based patterning techniques. The successful control over the structure of both ligands allows the direct patterning of dual-ligand QDs on various substrates using commercialized photolithography (i-line) or inkjet printing systems at a resolution up to 15,000 pixels per inch without compromising the optical properties of the QDs or the optoelectronic performance of the device. We demonstrate the capabilities of our approach for QD-LED applications. Our approach offers a versatile way of creating various structures of luminescent QDs in a cost-effective and non-destructive manner, and could be implemented in nearly all commercial photonics applications where QDs are used.

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.

Recent progress in strain-engineered elastic platforms for stretchable thin-film devices.

Strain-engineered elastic platforms that can efficiently distribute mechanical stress under deformation offer adjustable mechanical compliance for stretchable electronic systems. By fully exploiting strain-free regions that are favourable for fabricating thin-film devices and interconnecting with reliably stretchable conductors, various electronic systems can be integrated onto stretchable platforms with the assistance of strain engineering strategies. Over the last decade, applications of multifunctional stretchable thin-film devices simultaneously exhibiting superior electrical and mechanical performance have been demonstrated, shedding light on the realization of further reliable human-machine interfaces. This review highlights recent developments in enabling technologies for strain-engineered elastic platforms. In particular, representative approaches to realize strain-engineered substrates and stretchable interconnects in island-bridge configurations are introduced from the perspective of the material homogeneity and structural design of the substrate. State-of-the-art achievements in sophisticated stretchable electronic devices on strain-engineered elastic platforms are also presented, such as stretchable sensors, energy devices, thin-film transistors, and displays, and then, the challenges and outlook are 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.

Inkjet-Printing-Based Density Profile Engineering of Single-Walled Carbon Nanotube Networks for Conformable High-On/Off-Performance Thin-Film Transistors.

Random networks of single-walled carbon nanotubes (SWCNTs) offer new-form-factor electronics such as transparent, flexible, and intrinsically stretchable devices. However, the long-standing trade-off between carrier mobility and on/off ratio due to the coexistence of metallic and semiconducting nanotubes has limited the performance of SWCNT-random-network-based thin-film transistors (SWCNT TFTs), hindering their practical circuit-level applications. Methods for high-purity separation between metallic and semiconducting nanotubes have been proposed, but they require high cost and energy and are vulnerable to contamination and nanotube shortening, leading to performance degradation. Alternatively, additional structures have been proposed to reduce the off-state current, but they still compromise carrier mobility and suffer from inevitable expansion in device dimensions. Here, we propose a density-modulated SWCNT network using an inkjet-printing method as a facile approach that can achieve superior carrier mobility and a high on/off ratio simultaneously. By exploiting picoliter-scale drops on demand, we form a low-density channel network near the source and drain junctions and a high-density network at the middle of the channel. The modulated density profile forms a large band gap near the source and drain junctions that efficiently blocks electron injection under the reverse bias and a narrow band gap at the high-density area that facilitates the hole transport under the on-state bias. As a result, the density-modulated SWCNT TFTs show both high carrier mobility (27.02 cm2 V-1 s-1) and a high on/off ratio (>106). We also demonstrate all-inkjet-printed flexible inverter circuits whose gain is doubled by the density-modulated SWCNT TFTs, highlighting the feasibility of our approach for realizing high-performance flexible and conformable electronics.

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.

High-performance compliant thermoelectric generators with magnetically self-assembled soft heat conductors for self-powered wearable electronics.

Softening of thermoelectric generators facilitates conformal contact with arbitrary-shaped heat sources, which offers an opportunity to realize self-powered wearable applications. However, existing wearable thermoelectric devices inevitably exhibit reduced thermoelectric conversion efficiency due to the parasitic heat loss in high-thermal-impedance polymer substrates and poor thermal contact arising from rigid interconnects. Here, we propose compliant thermoelectric generators with intrinsically stretchable interconnects and soft heat conductors that achieve high thermoelectric performance and unprecedented conformability simultaneously. The silver-nanowire-based soft electrodes interconnect bismuth-telluride-based thermoelectric legs, effectively absorbing strain energy, which allows our thermoelectric generators to conform perfectly to curved surfaces. Metal particles magnetically self-assembled in elastomeric substrates form soft heat conductors that significantly enhance the heat transfer to the thermoelectric legs, thereby maximizing energy conversion efficiency on three-dimensional heat sources. Moreover, automated additive manufacturing paves the way for realizing self-powered wearable applications comprising hundreds of thermoelectric legs with high customizability under ambient conditions.

Highly Stable Contact Doping in Organic Field Effect Transistors by Dopant-Blockade Method.

In organic device applications, a high contact resistance between metal electrodes and organic semiconductors prevents an efficient charge injection and extraction, which fundamentally limits the device performance. Recently, various contact doping methods have been reported as an effective way to resolve the contact resistance problem. However, the contact doping has not been explored extensively in organic field effect transistors (OFETs) due to dopant diffusion problem, which significantly degrades the device stability by damaging the ON/OFF switching performance. Here, the stability of a contact doping method is improved by incorporating "dopant-blockade molecules" in the poly(2,5-bis(3-hexadecylthiophen-2-yl)thieno[3,2-b]thiophene) (PBTTT) film in order to suppress the diffusion of the dopant molecules. By carefully selecting the dopant-blockade molecules for effectively blocking the dopant diffusion paths, the ON/OFF ratio of PBTTT OFETs can be maintained over 2 months. This work will maximize the potential of OFETs by employing the contact doping method as a promising route toward resolving the contact resistance problem.

Enhanced Output Performance of All-Solution-Processed Organic Thermoelectrics: Spray Printing and Interface Engineering.

We report two organocompatible strategies to enhance the output performance of all-solution-processed poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) thermoelectric generators (TEGs): introducing an additive spray printing process and functionalized polymer interlayers to reduce the module resistance. The spray printing enabled the deposition of 1-µm-thick PEDOT:PSS layers with a high degree of design freedom, resulting in a significantly reduced sheet resistance of 16 Ω sq-1 that is closely related to the thermoelectric output performance. Also, by inserting an ultrathin silane-terminated polystyrene (PS) interlayer between the PEDOT:PSS thermoelectric layers and inkjet-printed Ag interconnects selectively, the contact resistivity extracted by the transmission line method was reduced from 6.02 × 10-2 to 2.77 × 10-2 Ω cm2. We found that the PS interlayers behaved as a thin tunneling layer, which facilitated the carrier injection from the inkjet-printed Ag electrodes into the PEDOT:PSS films by field emission with an effectively lowered energy barrier. The activation energy was also extracted using the Richardson equation, resulting in a reduction of 2.59 ± 0.04 meV after the PS treatment. Scalable plastic-compatible processability and selective interface engineering enabled to demonstrate the flexible 74-leg PEDOT:PSS TEGs exhibiting the open-circuit voltage of 9.21 mV and the output power of 2.23 nW at a temperature difference of 10 K.

Transparent ZnO Thin-Film Deposition by Spray Pyrolysis for High-Performance Metal-Oxide Field-Effect Transistors.

Solution-based metal oxide semiconductors (MOSs) have emerged, with their potential for low-cost and low-temperature processability preserving their intrinsic properties of high optical transparency and high carrier mobility. In particular, MOS field-effect transistors (FETs) using the spray pyrolysis technique have drawn huge attention with the electrical performances compatible with those of vacuum-based FETs. However, further intensive investigations are still desirable, associated with the processing optimization and operational instabilities when compared to other methodologies for depositing thin-film semiconductors. Here, we demonstrate high-performing transparent ZnO FETs using the spray pyrolysis technique, exhibiting a field-effect mobility of ~14.7 cm2 V-1 s-1, an on/off ratio of ~109, and an SS of ~0.49 V/decade. We examine the optical and electrical characteristics of the prepared ZnO films formed by spray pyrolysis via various analysis techniques. The influence of spray process conditions was also studied for realizing high quality ZnO films. Furthermore, we measure and analyze time dependence of the threshold voltage (Vth) shifts and their recovery behaviors under prolonged positive and negative gate bias, which were expected to be attributed to defect creation and charge trapping at or near the interface between channel and insulator, respectively.

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 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.