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Electron. Mater., Volume 2, Issue 2 (June 2021) – 14 articles

Cover Story (view full-size image): Synthetic approaches to efficiently tune the optical, electrochemical and morphological characteristics of oligothiophene-naphthalimide assemblies are reviewed. Variables such as the planarity and the length of the semiconductor π-conjugated backbones, as well as the topology and energy levels of the frontier molecular orbitals (HOMO and LUMO) and their molecular dipole moments, are finely tuned. The tuning of these properties is connected to the microstructure properties observed by atomic force microscopy (AFM) and X-ray diffraction (XRD) in thin films, as well as to the performances of photocatalysts in the degradation of organic pollutants and of active materials in organic field-effect transistors (OFETs). View this paper
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21 pages, 3678 KiB  
Article
In-Situ Characterisation of Charge Transport in Organic Light-Emitting Diode by Impedance Spectroscopy
by Pavel Chulkin
Electron. Mater. 2021, 2(2), 253-273; https://0-doi-org.brum.beds.ac.uk/10.3390/electronicmat2020018 - 08 Jun 2021
Cited by 2 | Viewed by 3434
Abstract
The article demonstrates an original, non-destructive technique that could be used to in situ monitor charge transport in organic light-emitting diodes. Impedance spectroscopy was successfully applied to determine an OLED’s charge carrier mobility and average charge density in the hole- and electron-transport layer [...] Read more.
The article demonstrates an original, non-destructive technique that could be used to in situ monitor charge transport in organic light-emitting diodes. Impedance spectroscopy was successfully applied to determine an OLED’s charge carrier mobility and average charge density in the hole- and electron-transport layer in a range of applied voltages. The fabricated devices were composed of two commercially available materials: NPB (N,N′-di(1-naphthyl)-N,N′-diphenyl-(1,1′-biphenyl)-4,4′-diamine) and TPBi (2,2′,2″-(1,3,5-Benzinetriyl)-tris(1-phenyl-1-H-benzimidazole)) as hole- and electron-transport layers, respectively. By varying the thicknesses of the hole-transport layer (HTL) and the electron-transport layer (ETL), correlations between layer thickness and both charge carrier mobility and charge density were observed. A possibility of using the revealed dependencies to predict diode current–voltage characteristics in a wide range of applied voltage has been demonstrated. The technique based on a detailed analysis of charge carrier mobilities and densities is useful for choosing the appropriate transport layer thicknesses based on an investigation of a reference set of samples. An important feature of the work is its impact on the development of fundamental research methods that involve AC frequency response analysis by providing essential methodology on data processing. Full article
(This article belongs to the Special Issue Feature Papers of Electronic Materials)
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31 pages, 9047 KiB  
Review
Oligothiophene-Naphthalimide Hybrids Connected through Rigid and Conjugated Linkers in Organic Electronics: An Overview
by Matías J. Alonso-Navarro, Elena Gala, M. Mar Ramos, Rocío Ponce Ortiz and José L. Segura
Electron. Mater. 2021, 2(2), 222-252; https://0-doi-org.brum.beds.ac.uk/10.3390/electronicmat2020017 - 05 Jun 2021
Cited by 4 | Viewed by 3155
Abstract
In this article, we summarize the synthetic approaches developed in our research groups during the last decade to efficiently tune the optical, electrochemical and morphological characteristics of oligothiophene–naphthalimide assemblies. Different variables were tuned in these organic semiconductors, such as the planarity and the [...] Read more.
In this article, we summarize the synthetic approaches developed in our research groups during the last decade to efficiently tune the optical, electrochemical and morphological characteristics of oligothiophene–naphthalimide assemblies. Different variables were tuned in these organic semiconductors, such as the planarity and the length of their π-conjugated backbones, the topology and energy levels of the frontier molecular orbitals (HOMO and LUMO) and their molecular dipole moments. The tuning of these properties can be connected with the microstructure properties observed by atomic force microscopy (AFM) and X-ray diffraction (XRD) in thin films as well as with the performances in organic field-effect transistors (OFETs). The possibility of incorporating these donor-acceptor assemblies into macromolecular structures is also addressed, and some innovative applications for these macromolecular systems, such as the degradation of organic pollutants in aqueous media, are also presented. Full article
(This article belongs to the Special Issue Feature Papers of Electronic Materials)
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24 pages, 14412 KiB  
Article
On the Role of LiF in Organic Optoelectronics
by Ayse Turak
Electron. Mater. 2021, 2(2), 198-221; https://0-doi-org.brum.beds.ac.uk/10.3390/electronicmat2020016 - 03 Jun 2021
Cited by 21 | Viewed by 4990
Abstract
Organic optoelectronic device behaviour is heavily dependent on interfacial effects due to the device architecture and thickness. Interfaces between the inorganic electrodes and the active organic layers play a defining role in the all of the electronic and stability processes that occur in [...] Read more.
Organic optoelectronic device behaviour is heavily dependent on interfacial effects due to the device architecture and thickness. Interfaces between the inorganic electrodes and the active organic layers play a defining role in the all of the electronic and stability processes that occur in organic light emitting diodes (OLEDs) and organic solar cells (OPVs). Amongst the many interlayers introduced at these interfaces to improve charge carrier movement and stability, LiF has proven to be the most successful and it is almost ubiquitous in all organic semiconductor devices. Implemented at both top and bottom contact interfaces, doped into the charge transporting layers, and used as encapsulants, LiF has played major roles in device performance and lifetime. This review highlights the use of LiF at both top and bottom contacts in organic optoelectronics, discusses the various mechanisms proposed for the utility of LiF at each interface, and explores its impact on device lifetimes. From examples relating to charge carrier flow, interfacial electronic level modification, and interfacial stability, a comprehensive picture of the role of LiF in organic devices can be formed. This review begins with a brief overview of the role of the interface in OLEDs and OPVs, and the general properties of LiF. Then, it discusses the implementation of LiF at the top contact electrode interface, followed by the bottom substrate contact electrode, examining both performance and degradation effects in both cases. Full article
(This article belongs to the Special Issue Feature Papers of Electronic Materials)
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12 pages, 2103 KiB  
Article
Imaging the Morphological Structure of Silk Fibroin Constructs through Fluorescence Energy Transfer and Confocal Microscopy
by Alessio Bucciarelli, Alberto Quaranta and Devid Maniglio
Electron. Mater. 2021, 2(2), 186-197; https://0-doi-org.brum.beds.ac.uk/10.3390/electronicmat2020015 - 03 Jun 2021
Cited by 3 | Viewed by 2763
Abstract
Silk fibroin is a well-known biopolymer that is used in several applications in which interactions with biological tissue are required. Fibroin is extremely versatile and can be shaped to form several constructs that are useful in tissue engineering applications. Confocal imaging is usually [...] Read more.
Silk fibroin is a well-known biopolymer that is used in several applications in which interactions with biological tissue are required. Fibroin is extremely versatile and can be shaped to form several constructs that are useful in tissue engineering applications. Confocal imaging is usually performed to test cell behavior on a construct, and, in this context, the fibroin intrinsic fluorescence is regarded as a problem. In addition, the intrinsic fluorescence is not intense enough to provide useful morphological images. In fact, to study the construct’s morphology, other techniques are used (i.e., SEM and Micro-CT). In this work, we propose a method based on fluorescence energy transfer (FRET) to suppress the fibroin intrinsic fluorescence and move it to a higher wavelength that is accessible to confocal microscopy for direct imaging. This was done by creating two FRET couples by dispersing two fluorophores (2,5-diphenyloxazole (PPO) and Lumogen F Violet 570 (LV)) into the fibroin matrix and optimizing their percentages to suppress the fibroin intrinsic fluorescence. With the optimized composition, we produced an electrospun mat, and the dimensions of the fibers were accurately determined by confocal microscopy. Full article
(This article belongs to the Special Issue Feature Papers of Electronic Materials)
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12 pages, 2769 KiB  
Article
Portable Photovoltaic-Self-Powered Flexible Electrochromic Windows for Adaptive Envelopes
by Antonio Cánovas-Saura, Ramón Ruiz, Rodolfo López-Vicente, José Abad, Antonio Urbina and Javier Padilla
Electron. Mater. 2021, 2(2), 174-185; https://0-doi-org.brum.beds.ac.uk/10.3390/electronicmat2020014 - 02 Jun 2021
Viewed by 2759
Abstract
Variable transmission applications for light control or energy saving based on electrochromic materials have been successfully applied in the past in the building, sports, or automotive fields, although lower costs and ease of fabrication, installation, and maintenance are still needed for deeper market [...] Read more.
Variable transmission applications for light control or energy saving based on electrochromic materials have been successfully applied in the past in the building, sports, or automotive fields, although lower costs and ease of fabrication, installation, and maintenance are still needed for deeper market integration. In this study, all-printed large area (900 cm2 active area) flexible electrochromic devices were fabricated, and an autoregulating self-power supply was implemented through the use of organic solar cells. A new perspective was applied for automotive light transmission function, where portability and mechanical flexibility added new features for successful market implementation. Special emphasis was placed in applying solution-based scalable deposition techniques and commercially available materials (PEDOT-PSS as an electrochromic material; vanadium oxide, V2O5, as a transparent ion-storage counter electrode; and organic solar modules as the power supply). A straightforward electronic control method was designed and successfully implemented allowing for easy user control. We describe a step-by-step route following the design, materials optimization, electronic control simulation, in-solution fabrication, and scaling-up of fully functional self-powered portable electrochromic devices. Full article
(This article belongs to the Special Issue Feature Papers of Electronic Materials)
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20 pages, 34459 KiB  
Article
Porous Polymer Gel Electrolytes Influence Lithium Transference Number and Cycling in Lithium-Ion Batteries
by Buket Boz, Hunter O. Ford, Alberto Salvadori and Jennifer L. Schaefer
Electron. Mater. 2021, 2(2), 154-173; https://0-doi-org.brum.beds.ac.uk/10.3390/electronicmat2020013 - 27 May 2021
Cited by 7 | Viewed by 4374
Abstract
To improve the energy density of lithium-ion batteries, the development of advanced electrolytes with enhanced transport properties is highly important. Here, we show that by confining the conventional electrolyte (1 M LiPF6 in EC-DEC) in a microporous polymer network, the cation transference [...] Read more.
To improve the energy density of lithium-ion batteries, the development of advanced electrolytes with enhanced transport properties is highly important. Here, we show that by confining the conventional electrolyte (1 M LiPF6 in EC-DEC) in a microporous polymer network, the cation transference number increases to 0.79 while maintaining an ionic conductivity on the order of 103 S cm−1. By comparison, a non-porous, condensed polymer electrolyte of the same chemistry has a lower transference number and conductivity, of 0.65 and 7.6 × 10−4 S cm−1, respectively. Within Li-metal/LiFePO4 cells, the improved transport properties of the porous polymer electrolyte enable substantial performance enhancements compared to a commercial separator in terms of rate capability, capacity retention, active material utilization, and efficiency. These results highlight the importance of polymer electrolyte structure–performance property relationships and help guide the future engineering of better materials. Full article
(This article belongs to the Special Issue Feature Papers of Electronic Materials)
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12 pages, 3516 KiB  
Article
Pyrimidine-Based Push–Pull Systems with a New Anchoring Amide Group for Dye-Sensitized Solar Cells
by Egor V. Verbitskiy, Alexander S. Steparuk, Ekaterina F. Zhilina, Viktor V. Emets, Vitaly A. Grinberg, Ekaterina V. Krivogina, Sergey A. Kozyukhin, Ekaterina V. Belova, Petr I. Lazarenko, Gennady L. Rusinov, Alexey R. Tameev, Jean Michel Nunzi and Valery N. Charushin
Electron. Mater. 2021, 2(2), 142-153; https://0-doi-org.brum.beds.ac.uk/10.3390/electronicmat2020012 - 26 May 2021
Cited by 12 | Viewed by 2819
Abstract
New donor–π–acceptor pyrimidine-based dyes comprising an amide moiety as an anchoring group have been designed. The dyes were synthesized by sequential procedures based on the microwave-assisted Suzuki cross-coupling and bromination reactions. The influence of the dye structure and length of π-linker on the [...] Read more.
New donor–π–acceptor pyrimidine-based dyes comprising an amide moiety as an anchoring group have been designed. The dyes were synthesized by sequential procedures based on the microwave-assisted Suzuki cross-coupling and bromination reactions. The influence of the dye structure and length of π-linker on the photophysical and electrochemical properties and on the photovoltaic effectiveness of dye-sensitized solar cells was investigated. An increase in efficiency with a decrease in the length of π-linker was revealed. The D1 dye with only one 2,5-thienylene-linker provided the highest power conversion efficiency among the fabricated dye sensitized solar cells. Full article
(This article belongs to the Special Issue Feature Papers of Electronic Materials)
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17 pages, 477 KiB  
Article
A Model for Bias Potential Effects on the Effective Langmuir Adsorption–Desorption Processes
by Luiz Roberto Evangelista, Giovanni Barbero and Anca Luiza Alexe-Ionescu
Electron. Mater. 2021, 2(2), 125-141; https://0-doi-org.brum.beds.ac.uk/10.3390/electronicmat2020011 - 17 May 2021
Cited by 1 | Viewed by 1857
Abstract
We discuss the foundations of a model based on an extension of the Langmuir approximation for the adsorption–desorption phenomena, in which the phenomenological coefficients depend on the bias potential, in addition to their dependence on the adsorption energy. The theoretical analysis focuses on [...] Read more.
We discuss the foundations of a model based on an extension of the Langmuir approximation for the adsorption–desorption phenomena, in which the phenomenological coefficients depend on the bias potential, in addition to their dependence on the adsorption energy. The theoretical analysis focuses on the effect of these effective coefficients on the electrical response of an electrolytic cell to an external electric field, as predicted by the Poisson–Nernst–Planck model. Kinetic balance equations govern the current densities on the electrodes when the adsorption phenomenon occurs in the presence of an electric bias. The influence of the phenomenological parameters entering the model, as well as of the symmetry of the cell on the cyclic voltammetry, is investigated. Full article
(This article belongs to the Special Issue Feature Papers of Electronic Materials)
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9 pages, 5414 KiB  
Article
Photochemical Micro-/Nano-Swelling of Silicone Rubber Induced by Long Pulse-Repetition Interval of an ArF Excimer Laser
by Masayuki Okoshi
Electron. Mater. 2021, 2(2), 116-124; https://0-doi-org.brum.beds.ac.uk/10.3390/electronicmat2020010 - 06 May 2021
Cited by 1 | Viewed by 1806
Abstract
Long pulse-repetition intervals of 100 to 500 ms of a 193 nm ArF excimer laser successfully increased the height of the photochemical micro-/nano-swelling of silicone rubber, observed with a scanning electron microscope. The effect of the interval was seen despite the heating of [...] Read more.
Long pulse-repetition intervals of 100 to 500 ms of a 193 nm ArF excimer laser successfully increased the height of the photochemical micro-/nano-swelling of silicone rubber, observed with a scanning electron microscope. The effect of the interval was seen despite the heating of the silicone rubber to 80 °C during laser irradiation. The height of the micro-/nano-swelling was saturated when the laser pulse number was 300 or greater, although each of the saturated heights of the micro-/nano-swelling formed by several pulse-repetition intervals was different. Thus, a second ArF excimer laser irradiated the growing micro-/nano-swelling before the saturation; the saturated height of the growing micro-/nano-swelling could be controlled by the pulse-repetition interval of the second ArF excimer laser. To examine the process of micro-/nano-swelling, an early stage of the growth was observed using an atomic force microscope; a dent structure of the micro-/nano-swelling was clearly recognized. In addition, a needle-like structure of the micro-/nano-swelling could be formed when silica glass microspheres were sparsely aligned. Full article
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11 pages, 2114 KiB  
Article
Towards Sustainable Crossbar Artificial Synapses with Zinc-Tin Oxide
by Carlos Silva, Jorge Martins, Jonas Deuermeier, Maria Elias Pereira, Ana Rovisco, Pedro Barquinha, João Goes, Rodrigo Martins, Elvira Fortunato and Asal Kiazadeh
Electron. Mater. 2021, 2(2), 105-115; https://0-doi-org.brum.beds.ac.uk/10.3390/electronicmat2020009 - 16 Apr 2021
Cited by 6 | Viewed by 3277
Abstract
In this article, characterization of fully patterned zinc-tin oxide (ZTO)-based memristive devices with feature sizes as small as 25 µm2 is presented. The devices are patterned via lift-off with a platinum bottom contact and a gold-titanium top contact. An on/off ratio of [...] Read more.
In this article, characterization of fully patterned zinc-tin oxide (ZTO)-based memristive devices with feature sizes as small as 25 µm2 is presented. The devices are patterned via lift-off with a platinum bottom contact and a gold-titanium top contact. An on/off ratio of more than two orders of magnitude is obtained without the need for electroforming processes. Set operation is a current controlled process, whereas the reset is voltage dependent. The temperature dependency of the electrical characteristics reveals a bulk-dominated conduction mechanism for high resistance states. However, the charge transport at low resistance state is consistent with Schottky emission. Synaptic properties such as potentiation and depression cycles, with progressive increases and decreases in the conductance value under 50 successive pulses, are shown. This validates the potential use of ZTO memristive devices for a sustainable and energy-efficient brain-inspired deep neural network computation. Full article
(This article belongs to the Special Issue Feature Papers of Electronic Materials)
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23 pages, 5024 KiB  
Article
Trapping of Electrons around Nanoscale Metallic Wires Embedded in a Semiconductor Medium
by Chi Cuong Huynh, Roger Evrard and Ngoc Duy Nguyen
Electron. Mater. 2021, 2(2), 82-104; https://0-doi-org.brum.beds.ac.uk/10.3390/electronicmat2020008 - 14 Apr 2021
Viewed by 2129
Abstract
We predict that conduction electrons in a semiconductor film containing a centered square array of metal nanowires normal to its plane are bound in quantum states around the central wires, if a positive bias voltage is applied between the wires at the square [...] Read more.
We predict that conduction electrons in a semiconductor film containing a centered square array of metal nanowires normal to its plane are bound in quantum states around the central wires, if a positive bias voltage is applied between the wires at the square vertices and the latter. We obtain and discuss the eigenenergies and eigenfunctions of two models with different dimensions. The results show that the eigenstates can be grouped into different shells. The energy differences between the shells is typically a few tens of meV, which corresponds to frequencies of emitted or absorbed photons in a range of 3THz to 20THz approximately. These energy differences strongly depend on the bias voltage. We calculate the linear response of individual electrons on the ground level of our models to large-wavelength electromagnetic waves whose electric field is in the plane of the semiconductor film. The computed oscillator strengths are dominated by the transitions to the states in each shell whose wave function has a single radial node line normal to the wave electric field. We include the effect of the image charge induced on the central metal wires and show that it modifies the oscillator strengths so that their sum deviates from the value given by the Thomas-Reiche-Kuhn rule. We report the linear response, or polarizability, versus photon energy, of the studied models and their absorption spectra. The latter show well-defined peaks as expected from the study of the oscillator strengths. We show that the position of these absorption peaks is strongly dependent on the bias voltage so that the frequency of photon absorption or emission in the systems described here is easily tunable. This makes them good candidates for the development of novel infrared devices. Full article
(This article belongs to the Special Issue Feature Papers of Electronic Materials)
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10 pages, 3361 KiB  
Article
High-Throughput Nanoparticle Chemisorption Printing of Chemical Sensors with High-Wiring-Density Electrodes
by Jun’ya Tsutsumi
Electron. Mater. 2021, 2(2), 72-81; https://0-doi-org.brum.beds.ac.uk/10.3390/electronicmat2020007 - 08 Apr 2021
Viewed by 1948
Abstract
We report on the high-throughput non-lithographic microprinting of a high-wiring-density interdigitated array electrode (line and space = 5 µm/5 µm), based on a facile wet/dewet patterning of silver nanoparticle ink. The trade-off between high-density wiring and pattern collapse in the wet/dewet patterning is [...] Read more.
We report on the high-throughput non-lithographic microprinting of a high-wiring-density interdigitated array electrode (line and space = 5 µm/5 µm), based on a facile wet/dewet patterning of silver nanoparticle ink. The trade-off between high-density wiring and pattern collapse in the wet/dewet patterning is overcome by employing a new herringbone design of interdigitated array electrode. We demonstrate electrochemical sensing of p-benzoquinone by the fabricated interdigitated array electrode, showing a typical steady-state IV characteristics with superior signal amplification benefiting from the redox cycling effect. Our findings provide a new technical solution for the scalable manufacture of advanced chemical sensors, with an economy of scale that cannot be realized by other techniques. Full article
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12 pages, 1497 KiB  
Article
Solution-Processed Organic and ZnO Field-Effect Transistors in Complementary Circuits
by John Barron, Alec Pickett, James Glaser and Suchismita Guha
Electron. Mater. 2021, 2(2), 60-71; https://0-doi-org.brum.beds.ac.uk/10.3390/electronicmat2020006 - 30 Mar 2021
Cited by 4 | Viewed by 2899
Abstract
The use of high κ dielectrics lowers the operating voltage in organic field-effect transistors (FETs). Polymer ferroelectrics open the path not just for high κ values but allow processing of the dielectric films via electrical poling. Poled ferroelectric dielectrics in p-type organic FETs [...] Read more.
The use of high κ dielectrics lowers the operating voltage in organic field-effect transistors (FETs). Polymer ferroelectrics open the path not just for high κ values but allow processing of the dielectric films via electrical poling. Poled ferroelectric dielectrics in p-type organic FETs was seen to improve carrier mobility and reduce leakage current when compared to unpoled devices using the same dielectric. For n-type FETs, solution-processed ZnO films provide a viable low-cost option. UV–ozone-treated ZnO films was seen to improve the FET performance due to the filling of oxygen vacancies. P-type FETs were fabricated using the ferroelectric polymer poly(vinylidene fluoride-trifluoroethylene) (PVDF-TrFE) as the dielectric along with a donor–acceptor polymer based on diketopyrrolopyrrole (DPP-DTT) as the semiconductor layer. The DPP-DTT FETs yield carrier mobilities upwards of 0.4 cm2/Vs and high on/off ratios when the PVDF-TrFE layer is electrically poled. For n-type FETs, UV–ozone-treated sol–gel ZnO films on SiO2 yield carrier mobilities of 10−2 cm2/Vs. DPP-DTT-based p- and ZnO-based n-type FETs were used in a complementary voltage inverter circuit, showing promising characteristic gain. A basic inverter model was used to simulate the inverter characteristics, using parameters from the individual FET characteristics. Full article
(This article belongs to the Special Issue Feature Papers of Electronic Materials)
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11 pages, 1652 KiB  
Article
Structural Changes Induced by Heating in Sputtered NiO and Cr2O3 Thin Films as p-Type Transparent Conductive Electrodes
by Cecilia Guillén and José Herrero
Electron. Mater. 2021, 2(2), 49-59; https://0-doi-org.brum.beds.ac.uk/10.3390/electronicmat2020005 - 29 Mar 2021
Cited by 7 | Viewed by 2512
Abstract
NiO and Cr2O3 are transition metal oxides with a partially filled d electron band that supports p-type conduction. Both are transparent to the visible light due to optical absorption beginning at wavelengths below 0.4 μm and the creation of holes [...] Read more.
NiO and Cr2O3 are transition metal oxides with a partially filled d electron band that supports p-type conduction. Both are transparent to the visible light due to optical absorption beginning at wavelengths below 0.4 μm and the creation of holes by metal vacancy defects. The defect and strain effects on the electronic characteristics of these materials need to be established. For this purpose, NiO and Cr2O3 thin films were deposited on unheated glass substrates by reactive DC sputtering from metallic targets. Their structural, morphological, optical and electrical properties were analyzed comparatively in the as-grown conditions (25 °C) and after heating in air at 300 °C or 500 °C. The cubic NiO structure was identified with some tensile strain in the as-grown conditions and compressive strain after heating. Otherwise, the chromium oxide layers were amorphous as grown at 25 °C and crystallized into hexagonal Cr2O3 at 300 °C or above also with compressive strain after heating. Both materials achieved the highest visible transmittance (72%) and analogous electrical conductivity (~10−4 S/cm) by annealing at 500 °C. The as-grown NiO films showed a higher conductivity (2.5 × 10−2 S/cm) but lower transmittance (34%), which were related to more defects causing tensile strain in these samples. Full article
(This article belongs to the Special Issue Feature Papers of Electronic Materials)
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