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  1. High‐energy‐density storage devices play a major role in modern electronics from traditional lithium‐ion batteries to supercapacitors for a variety of applications from rechargeable devices to advanced military equipment. Despite the mass adoption of polymer capacitors, their application is limited by their low energy densities and low‐temperature tolerance. Polymer nanocomposites based on 2D nanomaterials have superior capacitive energy densities, higher thermal stabilities, and higher mechanical strength as compared to the pristine polymers and nanocomposites based on 0D or 1D nanomaterials, thus making them ideal for high‐energy‐density dielectric energy storage applications. Here, the recent advances in 2D‐nanomaterial‐based nanocomposites and their implications for energy storage applications are reviewed. Nanocomposites based on conducting 2D nanofillers such as graphene, reduced graphene oxide, MXenes, semiconducting 2D nanofillers including transition metal dichalcogenides such as MoS2, dielectric 2D nanofillers including hBN, Mica, Al2O3, TiO2, Ca2Nb3O10and MMT, and their effects on permittivity, dielectric strength, capacitive energy density, efficiency, thermal stability, and the mechanical strength, are discussed. Also, the theory and machine‐learning‐guided design of polymer 2D nanomaterial composites is learnt and the challenges and opportunities for developing ultrahigh‐capacitive‐energy‐density devices based on these nanofiller polymer composites are presented.

     
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    Recently, the developments of two-dimensional (2D) ferroelectrics and multiferroics have attracted much more attention among researchers. These materials are useful for high-density devices for multifunctional applications such as sensors, transducers, actuators, non-volatile memories, photovoltaic, and FETs. Although several theoretical works have been reported on layered ferroelectrics, experimental work is still lacking in single to few-atomic layers of 2D ferroelectric materials. In this review, we have discussed the recent theoretical as well as experimental progress of 2D ferroelectric and multiferroic materials. The emphasis is given to the development of single to few-atomic layers of 2D ferroelectric materials. In this regard, the recent developments of 2D ferroelectric polarization on vanadium oxyhalides VOX2 (X=I, Br, Cl, and F), distorted phase d1-MoTe2, In2Se3, and SnSe are discussed. d1-MoTe2 shows Curie temperature (TC) above room temperature, while few-layered In2Se3 shows in-plane ferroelectricity and interesting domain wall dynamics in a single atomic layer of SnSe. This follows the discussion of multiferroic materials based on transition metal oxyiodide MOI2 (M=Ti, V, and Cr), double perovskite bilayer, and iron-doped In2Se3. While pristine In2Se3 shows ferroelectric properties, iron-doped In2Se3 shows multiferroicity. Finally, the potential applications of 2D ferroelectrics and multiferroics have been discussed that follow the challenges and opportunities in this field, which can guide the research community to develop next-generation 2D ferroelectric and multiferroic materials with interesting properties. 
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    The synthesis of polymer-grafted nanoparticles (PGNPs) or hairy nanoparticles (HNPs) by tethering of polymer chains to the surface of nanoparticles is an important technique to obtain nanostructured hybrid materials that have been widely used in the formulation of advanced polymer nanocomposites. Ceramic-based polymer nanocomposites integrate key attributes of polymer and ceramic nanomaterial to improve the dielectric properties such as breakdown strength, energy density and dielectric loss. This review describes the ”grafting from” and ”grafting to” approaches commonly adopted to graft polymer chains on NPs pertaining to nano-dielectrics. The article also covers various surface initiated controlled radical polymerization techniques, along with templated approaches for grafting of polymer chains onto SiO2, TiO2, BaTiO3, and Al2O3 nanomaterials. As a look towards applications, an outlook on high-performance polymer nanocomposite capacitors for the design of high energy density pulsed power thin-film capacitors is also presented. 
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  6. We report intrinsic photoconductivity studies on one of the least examined layered compounds, ZrS2.Few-atomic layer ZrS2 field-effect transistors were fabricated on the Si/SiO2 substrate and photoconductivity measurements were performed using both two- and four-terminal configurations under the illumination of 532 nm laser source. We measured photocurrent as a function of the incident optical power at several source-drain (bias) voltages. We observe a significantly large photoconductivity when measured in the multiterminal (four-terminal) configuration compared to that in the two-terminal configuration. For an incident optical power of 90 nW, the estimated photosensitivity and the external quantum efficiency (EQE) measured in two-terminal configuration are 0.5 A/W and 120%, respectively, under a bias voltage of 650 mV. Under the same conditions, the four-terminal measurements result in much higher values for both the photoresponsivity (R) and EQE to 6 A/W and 1400%, respectively. This significant improvement in photoresponsivity and EQE   in the four-terminal configuration may have been influenced by the reduction of contact resistance at the metal-semiconductor interface, which greatly impacts the carrier mobility of low conducting materials. This suggests that photoconductivity measurements performed through the two-terminal configuration in previous studies on ZrS2 and other 2D materials have severely underestimated the true intrinsic properties of transition metal dichalcogenides and their remarkable potential for optoelectronic applications. 
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  7. The Metal-Insulator phase transition (MIT) is one of the most interesting phenomena to study particularly in two-dimensional transition-metal dichalcogendes (TMDCs). A few recent studies1,2 have indicated a possible MIT on MoS2 and ReS2, but the nature of the MIT is still enigmatic due to the interplay between charge carriers and disorder in 2D systems. We will present a potential MIT in few-layered MoSe2 FETs based on four-terminal conductivity measurements. Conductivities measured in multiple samples strongly demonstrate the insulating-to-metallic-like phase transition when the charge carrier density increased above a critical threshold. The nature of the phase transition will be discussed with an existing theoretical model. 1B. H. Moon et al, Nat Commun. 2018; 9: 2052. 2N. R. Pradhan et al, Nano Lett. 2015, 15, 12, 8377 *This work was performed, in part, at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. This work is also supported by NSF-DMR #1826886 and # 1900692. A portion of this work was performed at the NHMFL, which is supported by the NSF Cooperative Agreement No. DMR-1644779 and the State of Florida 
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  8. The need for high power density, flexible and light weight energy storage devices requires the use of polymer film-based dielectric capacitors. Theoretically, it has been shown that chain ends contribute adversely to electrical breakdown, resulting in low energy density in polymer capacitors. In this work, we enhanced the energy density of polymer capacitor by using well-ordered high molecular weight block copolymer (BCP), in which the chain ends are segregated to narrow zones. Cyclic homopolymers (no chain ends) and linear homopolymers having chemistry-controlled chain ends also show enhanced breakdown strength, resulting in higher energy density as compared to the linear counterparts. These novel insights into manipulating chain end distribution such as in BCPs and with molecular topology to increase the energy density of polymers will be helpful for fulfilling next-generation energy demands. 
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