Solution-processed organo-lead halide perovskite solar cells with deep pinholes in the perovskite layer lead to shunt-current leakage in devices. Herein, we report a facile method for improving the performance of perovskite solar cells by inserting a solution-processed polymer layer between the perovskite layer and the hole-transporting layer. The photovoltaic conversion efficiency of the perovskite solar cell increased to 18.1% and the stability decreased by only about 5% during 20 days of exposure in moisture ambient conditions through the incorporation of a poly­(methyl methacrylate) (PMMA) polymer layer. The improved photovoltaic performance of devices with a PMMA layer is attributed to the reduction of carrier recombination loss from pinholes, boundaries, and surface states of perovskite layer. The significant gain generated by this simple procedure supports the use of this strategy in further applications of thin-film optoelectronic devices.

Conducting polymer thin films containing inherent structural disorder exhibit complicated electronic, transport, and thermoelectric properties. The unconventional power-law relation between the Seebeck coefficient (S) and the electrical conductivity (σ) is one of the typical consequences of this disorder, where no maximum of the thermoelectric power factor (P = S2σ) has been observed upon doping, unlike conventional systems. Here, it is demonstrated that a thiophene-based semicrystalline polymer exhibits a clear maximum of P through wide-range carrier doping by the electrolyte gating technique. The maximum value appears around the macroscopic insulator-to-metal transition upon doping, which is firmly confirmed by the temperature dependence of σ and magnetoresistance measurements. The effect of disorder on charge transport is suppressed in the metallic state, resulting in the conventional S-σ relation described by the Mott equation. The present results provide a physical background for controlling the performance of conducting polymers toward the application to thermoelectric devices.

The rapid development of the concept of the “Internet of Things (IoT)” requires wearable devices with maintenance‐free batteries, and thermoelectric energy conversion based on large‐area flexible materials has attracted much attention. Among large‐area flexible materials, 2D materials, such as graphene and related materials, are promising for thermoelectric applications due to their excellent transport properties and large power factors. In this Review, both single‐crystalline and polycrystalline 2D materials are surveyed using the experimental reports on thermoelectric devices of graphene, black phosphorus, transition metal dichalcogenides, and other 2D materials. In particular, their carrier‐density dependent thermoelectric properties and power factors maximized by Fermi level tuning techniques are focused. The comparison of the relevant performances between 2D materials and commonly used thermoelectric materials reveals the significantly enhanced power factors in 2D materials. Moreover, the current progress in thermoelectric module applications using large‐area 2D material thin films is summarized, which consequently offers great potential for the use of 2D materials in large‐area flexible thermoelectric device applications. Finally, important remaining issues and future perspectives, such as preparation methods, thermal transports, device designs, and promising effects in 2D materials, are discussed.

The carrier-density-dependent conductance and thermoelectric properties of large-area MoS 2 and WSe 2 monolayers are simultaneously investigated using the electrolyte gating method. The sign of the thermoelectric power changes across the transistor off-state in the ambipolar WSe 2 transistor as the majority carrier density switches from electron to hole. The thermopower and thermoelectric power factor of monolayer samples are one order of magnitude larger than that of bulk materials, and their carrier-density dependences exhibit a quantitative agreement with the semiclassical Mott relation based on the two-dimensional energy band structure, concluding the thermoelectric properties are enhanced by the low-dimensional effect.

Thermoelectric detection of a multi-subband density of states in semiconducting and metallic single-walled carbon nanotubes is demonstrated by scanning the Fermi energy from electron-doped to hole-doped regions. The Fermi energy is systematically controlled by utilizing the strong electric field induced in electric-double-layer transistor configurations, resulting in the optimization of the thermoelectric power factor.

This study reports on the thermoelectric properties of large-area graphene films grown by chemical vapor deposition (CVD) methods. Using the electric double layer gating technique, both the continuous doping of hole or electron carriers and modulation of the Fermi energy are achieved, leading to wide-range control of the Seebeck coefficient and electrical conductivity. Consequently, the maximum power factors of the CVD-grown large-area graphene films are 6.93 and 3.29 mW m-1 K-2 for p-and n-type carrier doping, respectively. These results are the best values among large-scale flexible materials, such as organic conducting polymers and carbon nanotubes, suggesting that CVD-grown large-area graphene films have potential for thermoelectric applications.

Triethylene glycol (TEG), a common side chain, has been attached to two different dye moieties, diketopyrrolopyrrole (DPP) and isoindigo (II), and their bromo derivative monomers were copolymerized, respectively, with common bisstannyl alkylated bithiophene via Stille Coupling. The resulting donor-acceptor low-band-gap copolymers, namely, PTDPP-DT and PTII-DT are rationally deigned and synthesized conjugated polymeric systems suitable for doping. Both polymers were successfully investigated as singlecomponent and composite-system based electrochemical transistors (ECT) and light-emitting electrochemical cells (LEC) respectively. The PTDPP-DT thin film exhibits relatively high This article is protected by copyright. All rights reserved. electrical conductivity of up to 80 S cm -1 in the electrochemically doped state whereas PTII-DT thin film prevents the macroscopic charge transport due to a large-scale crystalline disorientation. Upon evaluating both polymers as an active conjugated material in the lightemitting electrochemical cells, they both exhibit emission under efficient electron/hole doping conditions.

Large-area graphene films have substantial potential for use as next-generation electrodes because of their good chemical stability, high flexibility, excellent carrier mobility, and lightweight structure. However, various issues remain unsolved. In particular, highdensity carrier doping within a short time by a simple method, and air stability of doped graphene films, are highly desirable. Here, we demonstrate a solution-based high-density (>10 14 cm −2) hole doping approach that promises to push the performance limit of graphene films. The reaction of graphene films with a tetrakis(pentafluorophenyl)borate salt, containing a two-coordinate boron cation, achieves doping within an extremely short time (4 s), and the doped graphene films are air stable for at least 31 days. X-ray photoelectron spectroscopy reveals that the graphene films are covered by the chemically stable anions, resulting in an improved stability in air. Moreover, the doping reduces the transmittance by only 0.44 ± 0.23%. The simplicity of the doping process offers a viable route to the large-scale production of functional graphene electrodes.