Intermetallic titanium aluminides based on the ordered γ-TiAl phase fulfil many of the key requirements of lightweight high-temperature applications. In addition to a high melting point, high specific Young's modulus and strength at elevated temperatures, excellent creep properties, and a satisfactory oxidation and burn resistance, especially their low density of roughly 4 g cm À3 makes them a material of choice for challenging structural applications such as found, e.g., in environmentally friendly combustion engine options. [1][2][3][4] Capable of withstanding extreme conditions, γ-TiAl-based alloys have already entered service as low-pressure turbine blades in jet engines, such as the GEnx engine by GE Aviation, [5] the Geared Turbofan (GTF) engine by Pratt and Whitney, [6] as well as the LEAP engine by CFM International, a joint company between Safran Aircraft Engines and GE. [7,8] In these applications, γ-TiAl-based turbine blades substitute some of the blades made of twice as heavy Ni-base superalloys in a temperature range up to 750 °C. The implementation of the advanced, lightweight material, which is also attended by an adaptation of the design, entails a substantial reduction in weight, fuel consumption, and CO 2 and NO x emissions. [9] Apart from the aircraft engine industry, γ-TiAl-based alloys have also found applications in the automotive industry, e.g., as engine valves in sports and racing cars or as turbocharger turbine wheels. [1,3,[10][11][12][13][14] The past few decades have witnessed great efforts to develop intermetallic γ-TiAl-based alloy systems that are suitable for service in these demanding areas while being economically competitive at the same time. To this end, various alloy compositions and processing routes have been studied intensively. [1,[15][16][17][18][19][20][21] Recent progress has been reviewed, e.g., in the works by Appel et al., Clemens et al., and Mayer et al. [1,3,9,22] Due to the complexity of the intermetallic alloy system, which encompasses a multitude of phases and phase transformations, [23] purposeful alloy design requires the use of manifold characterization methods. Diffraction and scattering techniques, in particular, offer access to the atomic structure of the material and provide insights into a variety of microstructural parameters. [24][25][26][27] High-energy X-rays, such as available at today's synchrotron radiation sources, and recent developments in hardware technology nowadays allow to conduct so-called in situ experiments. Experiments of this kind reveal-at a high temporal resolution-the relationship between selected external