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Jonathan J. S. Scragg

Publications and source records attributed to Jonathan J. S. Scragg.

2 recordsLinked to original sources

Correcting Boundary Bias and Observation Independence in Bayesian Experimental Design

In many experimental settings, active learning can improve sample efficiency by sequentially selecting where to measure, which is particularly valuable when experiments are expensive. Gaussian processes with variance-based acquisition criteria are widely used for this purpose, but have two limitations. First, they are observation-independent: their posterior variance depends only on where samples are acquired, not on what is measured, impairing their sensitivity to the structure of the acquired data. Second, they inflate the variance near boundaries, leading to excessive sampling at the edges of the space compared to the interior. These limitations undermine the gains in sampling efficiency expected from sequential acquisition. We address both limitations. We derive a reconstruction-driven design density and use the posterior mean to build a training-free warp that places more measurements where the target function varies rapidly. A geometric equalizer separately corrects boundary bias. Across sixteen synthetic and two real-data benchmarks, the geometric equalizer consistently improves function reconstruction by correcting boundary bias, while the reconstruction warp provides further gains by concentrating measurements where the posterior mean varies rapidly.

cs.LG↗

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.

cs.LG↗