In the present work, BaTiO3 nanoparticles of four different size ranges were prepared by sol-gel method. The optical band gap of these particles at some size ranges has come down to 2.53 eV from 3.2 eV, resulting in substantial increase in optical absorption by these ferroelectric nanoparticles making them potential candidates for light energy harvesting. XRD results show the presence of higher compressive strain in 23 nm and 54 nm size particles, they exhibit a higher band gap narrowing, whereas tensile strain is observed in 31 nm and 34 nm particles, and they do not show the marginal band gap narrowing. The 23 nm and 54 nm particles also show a coupling of free carriers to phonons by increasing the intensity of LO phonon mode at 715 cm−1. The higher surface charge density is expected in case of enhanced surface optical Raman modes (638 cm−1) contained in 31 and 34 nm size particles. In addition to this, the red shift in an LO mode Raman spectral line at 305 cm−1 with decrease in particle size depicts the presence of phonon confinement in it. The enhanced optical absorption in 23 nm and 54 nm size particles with a narrowed band gap of 3 eV and 2.53 eV is due to exchange correlation interactions between the carriers present in these particles. In 31 nm and 34 nm range particles, the absorption got bleached exhibiting increased band gaps of 3.08 eV and 3.2 eV, respectively. It is due to filling up of conduction band resulting from weakening of exchange correlation interactions between the charge carriers. Hence, it is concluded that the band gap narrowing in the nanoparticles of average size 23 nm/54 nm is a consequence of multiple effects like strain, electron-phonon interaction, and exchange correlation interactions between the carriers which is subdued in some other size ranges like 31 nm/34 nm.
In our earlier studies the BaTiO3 samples were processed at higher temperatures like 1000oC and explained the observed magnetism in it. It is found that the charge transfer effects are playing crucial role in explaining the observed ferromagnetism in it. In the present work the samples were processed at lower temperatures like 650oC-800oC. The carrier densities in these particles were estimated to be ∼ 1019-1020/cm3 range. The band gap is in the range of 2.53eV to 3.2eV. It is observed that magnetization increased with band gap narrowing. The higher band gap narrowed particles exhibited increased magnetization with a higher carrier density of 1.23×1020/cm3 near to the Mott critical density. This hint the exchange interactions between the carriers play a dominant role in deciding the magnetic properties of these particles. The increase in charge carrier density in this undoped BaTiO3 is because of oxygen defects only. The oxygen vacancy will introduce electrons in the system and hence more charge carriers means more oxygen defects in the system and increases the exchange interactions between Ti3+, Ti4+, hence high magnetic moment. The coercivity is increased from 23 nm to 31 nm and then decreased again for higher particle size of 54 nm. These particles do not show photoluminescence property and hence it hints the absence of uniformly distributed distorted [TiO5]-[TiO6] clusters formation and charge transfer between them. Whereas these charge transfer effects are vital in explaining the observed magnetism in high temperature processed samples. Thus the variation of magnetic properties like magnetization, coercivity with band gap narrowing, particle size and charge carrier density reveals the super paramagnetic nature of BaTiO3 nanoparticles. The nonlinear optical coefficients extracted from Z-scan studies suggest that these are potential candidates for optical imaging and signal processing applications.
This article demonstrates a method to fabricate crystalline Ba0.5Sr0.5TiO3 (BST) thin films at a lower temperature of ≈300 °C using an excimer laser by an alternating depositing and annealing process. Firstly, a BST thin film with a thickness of ≈120 nm is deposited at 300 °C (laser energy of ≈2 J cm−2) and subsequently laser annealed (66 mJ cm−2) at 300 °C. This process is repeated five times to obtain thicker device quality films. XRD patterns, TEM, Raman, and UV–Vis–NIR spectroscopy confirm that phase formation of BST thin films has taken place. The band edge value for BST thin films is observed to decrease systematically from 4.65 eV (amorphous, 300 °C) to 3.56 eV (5‐layers, crystalline, 300 °C). A varactor device with a Circular Patch Capacitor (CPC) structure is patterned on the five‐stage laser annealed BST thin films processed at 300 °C, which shows a microwave tunability of 34% at 1 GHz compared to conventionally deposited BST films (prepared at 700 °C). This study provides a way for fabricating ferroelectric thin film based tunable devices at low temperatures, making the process compatible with low melting substrates in flexible electronics and other situations where there is a temperature constraint.
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