Abstract
A low-temperature (≤450 °C) crystallization path for the solution-derived lead zirconium titanate (PZT) thin-film, the first choice for high-density ferroelectric/piezoelectric nanodevices, has been sought for long but with limited success. In this work, we report on a facile route enabling the crystallization of PZT thin-films at 300–450 °C by using a novel solution-combustion-synthetic (SCS) approach. The SCS precursor solution consists of metal nitrates and organic fuels (tricine and/or urea) as oxidizing and reducing agents, respectively. The essential aspect of this route is that the single and intense exothermic combustion reaction between the oxidizer and fuels occurring at 234 °C provides high self-localized thermal energy, which allows for the efficient conversion of the amorphous metal-oxide gel framework into final crystallized oxides even at very low externally applied temperature. Effects of annealing conditions such as temperature and time are systematically investigated. At optimized conditions, high-quality PZT thin-films are achieved with pure perovskite phase, large remanent polarization (∼37 µC/cm2), and small leakage current (∼0.1 µA/cm2 at 600 kV/cm). Furthermore, an application of the developed low-temperature PZT film for the ferroelectric-gate memory transistor is demonstrated. The potential integration of low-temperature processed PZT layers with other active components may redefine the design concept of classical nano-microelectronic devices.
Highlights
Ferroelectric materials find applications in a variety of electronic and electromechanical devices
As a key parameter determining the efficiency of SCS reaction, the impact of the metal to fuel to oxidizer ratio on the thermal behavior of SCS solution was investigated by thermogravimetry (TG)-differential thermal analysis (DTA) (Fig. S3)
A facile route enabling the crystallization of PZT thin-films at 300–450 ○C was established by using a novel SCS approach
Summary
Ferroelectric materials find applications in a variety of electronic and electromechanical devices. Lead zirconate titanate (PZT) is the first choice for high-density ferroelectric/piezoelectric nanodevices because of its excellent properties and relatively low processing temperatures compared to the other two major options,[1] strontium bismuth tantalate (≥700 ○C) and bismuth lanthanum titanate (≥650 ○C).[2,3] the current processing temperatures of PZT, usually 600–700 ○C, are still too high, and the usual silicon-based CMOS circuits are severely damaged upon integrating with PZT elements. Compared to vacuum-based deposition methods (e.g., sputtering, pulse laser deposition, and metal-organic chemical vapor deposition), the chemical-solution-deposition (CSD) ones offer advantages, such as simplicity, low cost, large area deposition, and direct printability, making it more preferable for future practical applications
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