Observation-dependent Bayesian active learning via input-warped Gaussian processes

Bayesian active learning relies on the precise quantification of predictive uncertainty to explore unknown function landscapes. While Gaussian process surrogates are the standard for such tasks, an underappreciated fact is that their posterior variance depends on the observed outputs only through the hyperparameters, rendering exploration largely insensitive to the actual measurements. We propose to inject observation-dependent feedback by warping the input space with a learned, monotone reparameterization. This mechanism allows the design policy to expand or compress regions of the input space in response to observed variability, thereby shaping the behavior of variance-based acquisition functions. We demonstrate that while such warps can be trained via marginal likelihood, a novel self-supervised objective yields substantially better performance. Our approach improves sample efficiency across a range of active learning benchmarks, particularly in regimes where non-stationarity challenges traditional methods.

Machine learning for in-situ composition mapping in a self-driving magnetron sputtering system

Self-driving labs (SDLs), employing automation and machine learning (ML) to accelerate experimental procedures, have enormous potential in the discovery of new materials. However, in thin film science, SDLs are mainly restricted to solution-based synthetic methods which are easier to automate but cannot access the broad chemical space of inorganic materials. This work presents an SDL based on magnetron co-sputtering. We are using combinatorial frameworks, obtaining accurate composition maps on multi-element, compositionally graded thin films. This normally requires time-consuming ex-situ analysis prone to systematic errors. We present a rapid and calibration-free in-situ, ML driven approach to produce composition maps for arbitrary source combinations and sputtering conditions. We develop a method to predict the composition distribution in a multi-element combinatorial thin film, using in-situ measurements from quartz-crystal microbalance sensors placed in a sputter chamber. For a given source, the sensor readings are learned as a function of the sputtering pressure and magnetron power, through active learning using Gaussian processes (GPs). The final GPs are combined with a geometric model of the deposition flux distribution in the chamber, which allows interpolation of the deposition rates from each source, at any position across the sample. We investigate several acquisition functions for the ML procedure. A fully Bayesian GP - BALM (Bayesian active learning MacKay) - achieved the best performance, learning the deposition rates for a single source in 10 experiments. Prediction accuracy for co-sputtering composition distributions was verified experimentally. Our framework dramatically increases throughput by avoiding the need for extensive characterisation or calibration, thus demonstrating the potential of ML-guided SDLs to accelerate materials exploration.