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2025 (English)In: Materials & design, ISSN 0264-1275, E-ISSN 1873-4197, Vol. 260Article in journal (Refereed) Published
Abstract [en]
Self-driving labs (SDLs) employing automation and machine learning (ML) offer great promise for accelerating materials discovery and optimisation. However, in thin film science, SDLs are mainly restricted to solution-based methods which are easier to automate, restricting access to the broader chemical space of inorganic materials. This work advances an SDL based on magnetron co-sputtering, addressing a key challenge: rapidly generating accurate composition maps of multi-element, compositionally graded thin films. Traditional ex-situ methods are slow and error-prone; instead, we present a fast, calibration-free, in-situ ML approach to predict the deposition rate using quartz-crystal microbalance (QCM) sensors. For each sputtering source, deposition rates are sequentially learned as a function of pressure and power via active learning with Gaussian processes (GPs). The final GPs are combined with a geometric flux model to interpolate deposition rates across the sample. Among several acquisition functions with random query as the baseline, the Bayesian active learning MacKay (BALM) approach yielded the best performance, requiring as few as 10 experiments per source. The model predictions for co-sputtering composition distributions were validated against external composition measurements. This framework significantly increases throughput in combinatorial sputtering studies and highlights the potential of ML-guided SDLs to surpass traditional Edisonian methods
Place, publisher, year, edition, pages
Elsevier, 2025
Keywords
Active learning, Bayesian optimization, Combinatorial thin films, Gaussian processes, PVD, Self-driving lab
National Category
Electrical Engineering, Electronic Engineering, Information Engineering
Identifiers
urn:nbn:se:ri:diva-79957 (URN)10.1016/j.matdes.2025.115087 (DOI)2-s2.0-105022599115 (Scopus ID)9781856174978 (ISBN)
Note
The authors thank Carl Hvarfner for helpful discussions and Corrado Comparotto and Younes Lablali for assisting with RBS measurements. This work is supported by Swedish Foundation for Strategic Research (SSF), the strategic research area STandUP for Energy, and the Wallenberg AI, Autonomous Systems and Software Program (WASP) funded by the Knut and Alice Wallenberg Foundation . The work made use of the Myfab clean-room at Uppsala University, part of a VR and KAW funded national infrastructure, and the National Academic Infrastructure for Supercomputing in Sweden (NAISS). Operation of the accelerator, used for RBS measurements, is supported by the Swedish Research Council VR-RFI (Contracts 2019_00191 & 2023_00155 ).
2025-12-112025-12-112025-12-11Bibliographically approved