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Register a new userHomoepitaxial growth of SrTiO$_3$ by Pulsed Laser Deposition: energetic vs thermal growth
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Pulsed Laser Deposition (PLD) is widely used to grow epitaxial thin films of quantum materials such as complex oxides. Here, we use in-situ X-ray scattering to study homoepitaxy of SrTiO$_3$ by energetic (e-) and thermalized (th-) PLD. We find that e-PLD suppresses the lateral growth of two-dimensional islands, which suggests that energetic particles break up smaller islands. Fast interlayer transport occurs for both e-PLD and th-PLD, implying a process operating on sub-microsecond timescales that doesnt depend strongly on the kinetic energy of the incident particles.
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Control of thin film stoichiometry is of primary relevance to achieve desired functionality. Pulsed laser deposition ablating from binary-oxide targets (sequential deposition) can be applied to precisely control the film composition, offsetting the importance of growth conditions on the film stoichiometry. In this work, we demonstrate that the cation stoichiometry of SrTiO$_3$ thin films can be finely tuned by sequential deposition from SrO and TiO$_2$ targets. Homoepitaxial SrTiO$_3$ films were deposited at different substrate temperatures and Ti/Sr pulse ratios, allowing the establishment of a growth window for stoichiometric SrTiO$_3$. The growth kinetics and nucleation processes were studied by reflection high-energy electron diffraction and atomic force microscopy, providing information about the growth mode and the degree of off-stoichiometry. At the optimal (stoichiometric) growth conditions, films exhibit atomically flat surfaces, whereas off-stoichiometry is accommodated by crystal defects, 3D islands and/or surface precipitates depending on the substrate temperature and the excess cation. This technique opens the way to precisely control stoichiometry and doping of oxide thin films.
We present results on growth of large area epitaxial ReS2 thin film both on c plane sapphire substrate and MoS2 template by pulsed laser deposition (PLD). Films tend to grow with (0001) ReS2 perpendicular to (0001) Al2O3 and (0001) ReS2 perpendicular to (0001) MoS2 parallel to (0001) Al2O3 at deposition temperature below 300 deg C. Films are polycrystalline grown at temperature above 300 deg C. The smoothness and quality of the films are significantly improved when grown on MoS2 template compared to sapphire substrate. The results show that PLD is suitable to grow ReS2 epitaxial thin film over large area for practical device application.
High quality Van der Waals chalcogenides are important for phase change data storage, thermoelectrics, and spintronics. Using a combination of statistical design of experiments and density functional theory, we clarify how the out-of-equilibrium van der Waals epitaxial deposition methods can improve the crystal quality of Sb2Te3 films. We compare films grown by radio frequency sputtering and pulsed laser deposition (PLD). The growth factors that influence the crystal quality for each method are different. For PLD grown films a thin amorphous Sb2Te3 seed layer most significantly influences the crystal quality. In contrast, the crystalline quality of films grown by sputtering is rather sensitive to the deposition temperature and less affected by the presence of a seed layer. This difference is somewhat surprising as both methods are out-of-thermal-equilibrium plasma-based methods. Non-adiabatic quantum molecular dynamics simulations show that this difference originates from the density of excited atoms in the plasma. The PLD plasma is more intense and with higher energy than that used in sputtering, and this increases the electronic temperature of the deposited atoms, which concomitantly increases the adatom diffusion lengths in PLD. In contrast, the adatom diffusivity is dominated by the thermal temperature for sputter grown films. These results explain the wide range of Sb2Te3 and superlattice crystal qualities observed in the literature. These results indicate that, contrary to popular belief, plasma-based deposition methods are suitable for growing high quality crystalline chalcogenides.
To visualize the topography of thin oxide films during growth, thereby enabling to study its growth behavior quasi real-time, we have designed and integrated an atomic force microscope (AFM) in a pulsed laser deposition (PLD) vacuum setup. The AFM scanner and PLD target are integrated in a single support frame, combined with a fast sample transfer method, such that in-situ microscopy can be utilized after subsequent deposition pulses. The in-situ microscope can be operated from room temperature (RT) up to 700$^circ$C and at (process) pressures ranging from the vacuum base pressure of 10$^{-6}$ mbar up to 1 mbar, typical PLD conditions for the growth of oxide films. The performance of this instrument is demonstrated by resolving unit cell height surface steps and surface topography under typical oxide PLD growth conditions.
In many transition metal oxides (TMOs), oxygen stoichiometry is one of the most critical parameters that plays a key role in determining the structural, physical, optical, and electrochemical properties of the material. However, controlling the growth to obtain high quality single crystal films having the right oxygen stoichiometry, especially in a high vacuum environment, has been viewed as a challenge. In this work, we show that through proper control of the plume kinetic energy, stoichiometric crystalline films can be synthesized without generating oxygen defects, even in high vacuum. We use a model homoepitaxial system of SrTiO3 (STO) thin films on single crystal STO substrates. Physical property measurements indicate that oxygen vacancy generation in high vacuum is strongly influenced by the energetics of the laser plume, and it can be controlled by proper laser beam delivery. Therefore, our finding not only provides essential insight into oxygen stoichiometry control in high vacuum for understanding the fundamental properties of STO-based thin films and heterostructures, but expands the utility of pulsed laser epitaxy of other materials as well.
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