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Abstract Although metal–organic (MO) precursors are widely used in technologically relevant deposition techniques, reports on their temperature-dependent evaporation and decomposition behaviors are scarce. Here, MO precursors of the metals Ti, V, Al, Hf, Zr, Ge, Ta, and Pt were subjected to thermogravimetric analysis to experimentally determine their vapor pressure curves and to gain insight into their temperature-dependent decomposition kinetics. Benzoic acid was used as a calibration standard and vapor pressure curves were extracted from thermogravimetric measurements using the Langmuir equation. The obtained data is used to discuss the suitability of these MO precursors in chemical vapor deposition-based thin film growth approaches in general, and hybrid molecular beam epitaxy in particular. All MOs, except for Ta- and one Ti-based MOs, were deemed suitable for gas inlet systems. The Ta-based MO demonstrated suitability for an effusion cell, while all MOs showed compatibility with cracker usage. Graphical Abstract 

Abstract BaTiO₃is a technologically relevant material in the perovskite oxide class with above‐room‐temperature ferroelectricity and a very large electro‐optical coefficient, making it highly suitable for emerging electronic and photonic devices. An easy, robust, straightforward, and scalable growth method is required to synthesize epitaxial BaTiO₃thin films with sufficient control over the film's stoichiometry to achieve reproducible thin film properties. Here the growth of BaTiO₃thin films by hybrid molecular beam epitaxy is reported. A self‐regulated growth window is identified using complementary information obtained from reflection high energy electron diffraction, the intrinsic film lattice parameter, film surface morphology, and scanning transmission electron microscopy. Subsequent optical characterization of the BaTiO₃films by spectroscopic ellipsometry revealed refractive index and extinction coefficient values closely resembling those of stoichiometric bulk BaTiO₃crystals for films grown inside the growth window. Even in the absence of a lattice parameter change of BaTiO₃thin films, degradation of optical properties is observed, accompanied by the appearance of a wide optical absorption peak in the IR spectrum, attributed to optical transitions involving defect states present. Therefore, the optical properties of BaTiO₃can be utilized as a much finer and more straightforward probe to determine the stoichiometry level present in BaTiO₃films.