A Mechanistic Study of Nanoscale Structure Development, Phase Transition, Morphology Evolution, and Growth of Ultrathin

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erials play an important role in sensor and actuator development because of their remarkable electromechanical performance.[1–3] The most experimentally and theoretically investigated ferroelectric material is barium titanate (BaTiO3; BTO) which is used extensively in the capacitor industry, particularly in form of multilayer ceramic capacitors (MLCCs).[4,5] Recently, nanoscale ferroelectric materials have received considerable attention due to their potential applications in microelectronics and integrated optics technologies.[6–8] BTO with perovskite structure has been of practical interest for more than 60 years due to its attractive properties.[9] The significance of this material is mainly ROUHOLAH ASHIRI, formerly Graduated with Department of Materials Science and Engineering, Sharif University of Technology, Tehran, Iran, is now PhD Student with the Department of Materials Science and Engineering, Isfahan University of Technology, Isfahan, Iran, and also Lecturer with Department of Materials Science and Engineering, Dezful Branch, Islamic Azad University, P.O. Box 313, Dezful, Iran, Contact e-mail: [email protected] Manuscript submitted January 25, 2014. Article published online May 22, 2014 4138—VOLUME 45A, AUGUST 2014

due to the wide variety of applications for which it is used. Previous researches into BTO thin films have mainly been focused on the MLCC applications, because BTO thin films exhibit high dielectric constant and low dielectric loss at ambient conditions.[10,11] Recently, much attention has also been paid to BTO thin films in integrated optical and opto-electronic device applications as they have prominent properties such as high visible transmission and relatively low optical losses.[1,12] BTO is the most common ferroelectric material.[13] Due to its pyroelectricity, ferroelectricity, excellent dielectrical performance, desired chemical stability, low toxicity, and large electro-optic coefficients, BTO thin films are of interest in the construction of devices such as pyroelectric detectors, nonvolatile memories with high density [such as ferroelectric random access memories (FRAMs) and dynamic random access memories (DRAMs)], parametric amplifiers, photovoltaic devices,[14] temperature, humidity, and gas sensors,[15] ferroelectric tunnel junctions (FTJs), layered multiferroics[16] electro-optic switches, optical waveguides,[17] frequency doublers, infrared sensors, tunable oscillators, piezoelectric actuators, transducers, electroluminescent panels, positive temperature coefficient resistors (PTCRs),[18] controllers, METALLURGICAL AND MATERIALS TRANSACTIONS A

and optical second harmonic generators.[1,19] Furthermore, with the increasing demands for complex functionality and device miniaturization, BTO-based thin films are potential candidates for embedded capacitors in circuit boards.[20] Demands to miniaturize and/or upgrade capacitors in integrated circuits necessitate fabrication of layered microstructures. Due to the miniaturization of such components and devices, the related industries have bee