Abstract
ABSTRACT
Chemical short‐range order (CSRO) in Multi‐Principal Element Alloys (MPEAs) arises from non‐random atomic arrangements within local coordination shells and plays a critical role in governing mechanical properties, diffusion kinetics, and phase stability. Capturing CSRO requires synergistic computational and experimental strategies. Advanced first‐principles methods evaluate mixing enthalpies and local distortions, while atomistic simulations enable large‐scale configurational sampling. Analytical frameworks, such as the Cluster Variation Method, predict temperature‐dependent ordering trends. Concurrent experimental approaches, including pair distribution function analysis, in situ synchrotron diffraction, atom probe tomography, and resistivity measurements, provide indirect yet complementary insights into local ordering. However, the field lacks a unified framework linking the thermodynamic origin, kinetic evolution, and experimental observability of CSRO, limiting the ability to systematically interpret and compare different approaches. This perspective examines computational and experimental methods in the context of CSRO formation, evolution, and measurement, emphasizes the importance of modeling–experiment cross‐validation pathways for integrating these complementary approaches, and provides a critical assessment of their capabilities, limitations, and roles in advancing the understanding and design of MPEAs.