To improve ferroelectric properties of PZT, many studies have attempted to fabricate dense PZT films. The AD process has an advantage for forming dense ceramic films at room temperature without any additional heat treatment in low vacuum. Thick films coated by AD have a higher dielectric breakdown strength due to their higher density than those coated using conventional methods. To improve the breakdown strength, glass (SiO2-Al2O3-Y2O3, SAY) is mixed with PZT powder at various volume ratios (PZT-xSAY, x = 0, 5, 10 vol%) and coating films are produced on silicon wafers by AD method. Depending on the ratio of PZT to glass, dielectric breakdown strength and energy storage efficiency characteristics change. Mechanical impact in the AD process makes the SAY glass more viscous and fills the film densely. Compared to pure PZT film, PZT-SAY film shows an 87.5% increase in breakdown strength and a 35.3 % increase in energy storage efficiency.

Solid state grain growth (SSCG) is a method of growing large single crystals from seed single crystals by abnormal grain growth in a small-grained matrix. During grain growth, pores are often trapped in the matrix and remain in single crystals. Aerosol deposition (AD) is a method of manufacturing films with almost full density from nano grains by causing high energy collision between substrates and ceramic powders. AD and SSCG are used to grow single crystals with few pores. BaTiO3 films are coated on (100) SrTiO3 seeds by AD. To generate grain growth, BaTiO3 films are heated to 1,300 oC and held for 10 h, and entire films are grown as single crystals. The condition of grain growth driving force is ΔGmax < ΔGc ≤ ΔGseed. On the other hand, the condition of grain growth driving force in BaTiO3 AD films heat-treated at 1,100 and 1,200 oC is ΔGc < ΔGmax, and single crystals are not grown.

FDM 3D printing structures have rough surfaces and require post-treatment to improve the properties. Fumigation is a representative technique for removing surface unevenness. Surface treatment by fumigation proceeds by dissolving the surface of the protruding structure using a vaporized solvent. In this study, 3D printed PVB outputs are surface-treated with ethyl-alcohol fumigation. As the fumigation time increases, the surface flattens as ethanol dissolves the mountains on the surface of PVB and the surface valleys are filled with dissolved PVB. Through the fumigation process, the mechanical strength tends to decrease, and deformation rate increases. Ethanol vapor permeates into PVB, widening the distance between chains and resulting in weak bonding strength between chains. In order to confirm the effect of fumigation only, an annealing process is performed at 80 oC for 1, 5, 10, 30, and 50 minutes and the results of the fumigation are compared.

NKN [(Na,K)NbO3] is a candidate lead-free piezoelectric material to replace PZT [Pb(Zr,Ti)O3]. A single crystal has excellent piezoelectric-properties and its properties are dependent of the crystal orientation direction. However, it is hard to fabricate a single crystal with stoichiometrically stable composition due to volatilization of sodium during the growth process. To solve this problem, a solid solution composition is designed (Na,K)NbO3-Ba(Cu,Nb)O3 and solid state grain growth is studied for a sizable single crystal. Ceramic powders of (Na,K)NbO3-M(Cu,Nb)O3 (M = Ca, Sr, Ba) are synthesized and grain growth behavior is investigated for different temperatures and times. Average normal grain sizes of individual specimens, which are heat-treated at 1,125 oC for 10 h, are 6.9, 2.8, and 1.6 m for M = Ca, Sr, and Ba, respectively. Depending on M, the distortion of NKN structure can be altered. XRD results show that (NKN-CaCuN: shrunken orthorhombic; NKN-SrCuN: orthorhombic; NKN-BaCuN: cubic). For the sample heat-treated at 1,125 oC for 10 h, the maximum grain sizes of individual specimens are measured as 40, 5, and 4,000 m for M = Ca, Sr, and Ba, respectively. This abnormal grain size is related to the partial melting temperature (NKN-CaCuN: 960 oC; NKN-SrCuN: 971 oC; NKN-BaCuN: 945 oC).

Single crystals, which have complexed composition, are fabricated by solid state grain growth. However, it is hard to achieve stable properties in a single crystal due to trapped pores. Aerosol deposition (AD) is suitable for fabrication of single crystals with stable properties because this process can make a high density coating layer. Because of their unique features (nano sized grains, stress inner site), it is hard to fabricate single crystals, and so studies of grain growth behavior of AD film are essential. In this study, a BaTiO3 coating layer with ~ 9 μm thickness is fabricated using an aerosol deposition method on (100) and (110) cut SrTiO3 single crystal substrates, which are adopted as seeds for grain growth. Each specimen is heat-treated at various conditions (900, 1,100, and 1,300℃ for 5 h). BaTiO3 layer shows different growth behavior and X-ray diffraction depending on cutting direction of SrTiO3 seed. Rectangular pillars at SrTiO3 (100) and laminating thin plates at SrTiO3 (110), respectively, are observed.

Pb(Zr,Ti)O3 (PZT) is used for the various piezoelectric devices owing to its high piezoelectric properties. However, lead (Pb), which is contained in PZT, causes various environment contaminations. (K,Na)NbO3 (NKN) is the most well-known candidate for a lead-free composition to replace PZT. A single crystal has excellent piezoelectric-properties and its properties can be changed by changing the orientation direction. It is hard to fabricate a NKN single crystal due to the sodium and potassium. Thus, (Na,K)NbO3-Ba(Cu,Nb)O3 (NKN-BCuN) is chosen to fabricate the single crystal with relative ease. NKNBCuN pellets consist of two parts, yellow single crystals and gray poly-crystals that contain copper. The area that has a large amount of copper particles may melt at low temperature but not the other areas. The liquid phase may be responsible for the abnormal grain growth in NKN-BCuN ceramics. The dielectric constant and tan δ are measured to be 684 and 0.036 at 1 kHz in NKN-BCuN, respectively. The coercive field and remnant polarization are 14 kV/cm and 20 μC/cm2.

This study examines paraelectric Bi1.5Zn1.0Nb1.5O7 (BZN), which has no hysteresis and high dielectric strength, for energy density capacitor applications. To increase the breakdown dielectric strength of the BZN film further, poly(vinylidene fluoride) BZN-PVDF composite film is fabricated by aerosol deposition. The volume ratio of each composition is calculated using dielectric constant of each composition, and we find that it was 12:88 vol% (BZN:PVDF). To modulate the structure and dielectric properties of the ferroelectric polymer PVDF, the composite film is heat-treated at 200 oC for 5 and 30 minutes following quenching. The amount of α-phase in the PVDF increases with an increasing annealing time, which in turn decreases the dielectric constant and dielectric loss. The breakdown dielectric strength of the BZN film increases by mixing PVDF. However, the breakdown field decreases with an increasing annealing time. The BZN-PVDF composite film has the energy density of 4.9 J/cm3, which is larger than that of the pure BZN film of 3.6 J/cm3.

Lead free (Ba0.7Ca0.3) TiO3 thick films with nano-sized grains are prepared using an aerosol deposition (AD) method at room temperature. The crystallinity of the AD thick films is enhanced by a post annealing process. Contrary to the sharp phase transition of bulk ceramics that has been reported, AD films show broad phase transition behaviors due to the nanosized grains. The polarization-electric hysteresis loop of annealed AD film shows ferroelectric behaviors. With an increase in annealing temperature, the saturation polarization increases because of an increase in crystallinity. However, the remnant polarization and cohesive field are not affected by the annealing temperature. BCT AD thick films annealed at 700 ℃/2h have an energy density of 1.84 J/cm3 and a charge-discharge efficiency of 69.9%, which is much higher than those of bulk ceramic with the same composition. The higher energy storage properties are likely due to the increase in the breakdown field from a large number of grain boundaries of nano-sized grains.