arXiv subjects

Armi Tiihonen

Publications and source records attributed to Armi Tiihonen.

10 recordsLinked to original sources

arXiv2026

Charting the thermodynamic stability of hybrid perovskite alloys with machine learning

Alloy-based perovskite solar cells offer tunable properties and improved stability, but their complexity has impeded accurate modeling, hindering development. We present a machine-learning (ML) accelerated atomistic modeling approach for the phase stability of (Cs/FA)Pb(Br/I)3 and (Cs/FA)Sn(Br/I)3 perovskites, with FA being formamidinium. To make such quaternary alloys tractable, we adopt a two-level ML strategy, combining 1) graph neural network interatomic potentials trained on density functional theory data for efficient structure relaxations with 2) secondary ML models for direct energy prediction from unrelaxed structures. These models enable computations of free energy landscapes across compositions and phases, capturing alloy disorder and FA molecular orientations. Our results reveal narrower stable composition regions for the Sn-based system compared to its Pb-based counterpart, limiting options for compositional engineering. Maximum stability occurs at high I content, and no stabilization is observed near the center of the composition space. Our results guide the design of stable perovskites.

cond-mat.mtrl-sci↗

arXiv2025

Multi-Variable Batch Bayesian Optimization in Materials Research: Synthetic Data Analysis of Noise Sensitivity and Problem Landscape Effects

Bayesian Optimization (BO) machine learning method is increasingly used to guide experimental optimization tasks in materials science. To emulate the large number of input variables and noise-containing results in experimental materials research, we perform batch BO simulation of six design variables with a range of noise levels. Two test cases relevant for materials science problems are examined: a needle-in-a-haystack case (Ackley function) that may be encountered in, e.g., molecule optimizations, and a smooth landscape with a local optimum in addition to the global optimum (Hartmann function) that may be encountered in, e.g., material composition optimization. We show learning curves, performance metrics, and visualization to effectively track the optimization progression and evaluate how the optimization outcomes are affected by noise, batch-picking method, choice of acquisition function, and exploration hyperparameter values. We find that the effects of noise depend on the problem landscape: noise degrades the optimization results of a needle-in-a-haystack search (Ackley) dramatically more. However, with increasing noise, we observe an increasing probability of landing on the local optimum in Hartmann. Therefore, prior knowledge of the problem domain structure and noise level is essential when designing BO for materials research experiments. Synthetic data studies -- with known ground truth and controlled noise levels -- enable us to isolate and evaluate the impact of different batch BO components, {\it e.g.}, acquisition policy, objective metrics, and hyperparameter values, before transitioning to the inherent uncertainties of real experimental systems. The results and methodology of this study will facilitate a greater utilization of BO in guiding experimental materials research, specifically in settings with a large number of design variables to optimize.

stat.ML↗

arXiv2025

Multi-objective Bayesian Optimization with Human-in-the-Loop for Flexible Neuromorphic Electronics Fabrication

Neuromorphic computing hardware enables edge computing and can be implemented in flexible electronics for novel applications. Metal oxide materials are promising candidates for fabricating flexible neuromorphic electronics, but suffer from processing constraints due to the incompatibilities between oxides and polymer substrates. In this work, we use photonic curing to fabricate flexible metal-insulator-metal capacitors with solution-processible aluminum oxide dielectric tailored for neuromorphic applications. Because photonic curing outcomes depend on many input parameters, identifying an optimal processing condition through a traditional grid-search approach is unfeasible. Here, we apply multi-objective Bayesian optimization (MOBO) to determine photonic curing conditions that optimize the trade-off between desired electrical properties of large capacitance-frequency dispersion and low leakage current. Furthermore, we develop a human-in-the-loop (HITL) framework for incorporating failed experiments into the MOBO machine learning workflow, demonstrating that this framework accelerates optimization by reducing the number of experimental rounds required. Once optimization is concluded, we analyze different Pareto-optimal conditions to tune the dielectrics properties and provide insight into the importance of different inputs through Shapley Additive exPlanations analysis. The demonstrated framework of combining MOBO with HITL feedback can be adapted to a wide range of multi-objective experimental problems that have interconnected inputs and high experimental failure rates to generate usable results for machine learning models.

cs.ET↗

arXiv2025

Virtual Laboratories: Domain-agnostic workflows for research

Many scientific disciplines have traditionally advanced by iterating over hypotheses using labor-intensive trial-and-error, which is a slow and expensive process. Recent advances in computing, digitalization, and machine learning have introduced tools that promise to make scientific research faster by assisting in this iterative process. However, these advances are scattered across disciplines and only loosely connected, with specific computational methods being primarily developed for narrow domain-specific applications. Virtual Laboratories are being proposed as a unified formulation to help researchers navigate this increasingly digital landscape using common AI technologies. While conceptually promising, VLs are not yet widely adopted in practice, and concrete implementations remain limited.This paper explains how the Virtual Laboratory concept can be implemented in practice by introducing the modular software library VAILabs, designed to support scientific discovery. VAILabs provides a flexible workbench and toolbox for a broad range of scientific domains. We outline the design principles and demonstrate a proof-of-concept by mapping three concrete research tasks from differing fields as virtual laboratory workflows.

cs.OH↗

arXiv2024

Learning Relevant Contextual Variables Within Bayesian Optimization

Contextual Bayesian Optimization (CBO) efficiently optimizes black-box functions with respect to design variables, while simultaneously integrating contextual information regarding the environment, such as experimental conditions. However, the relevance of contextual variables is not necessarily known beforehand. Moreover, contextual variables can sometimes be optimized themselves at an additional cost, a setting overlooked by current CBO algorithms. Cost-sensitive CBO would simply include optimizable contextual variables as part of the design variables based on their cost. Instead, we adaptively select a subset of contextual variables to include in the optimization, based on the trade-off between their relevance and the additional cost incurred by optimizing them compared to leaving them to be determined by the environment. We learn the relevance of contextual variables by sensitivity analysis of the posterior surrogate model while minimizing the cost of optimization by leveraging recent developments on early stopping for BO. We empirically evaluate our proposed Sensitivity-Analysis-Driven Contextual BO (SADCBO) method against alternatives on both synthetic and real-world experiments, together with extensive ablation studies, and demonstrate a consistent improvement across examples.

cs.LG↗

arXiv2023

Using Scalable Computer Vision to Automate High-throughput Semiconductor Characterization

High-throughput materials synthesis methods have risen in popularity due to their potential to accelerate the design and discovery of novel functional materials, such as solution-processed semiconductors. After synthesis, key material properties must be measured and characterized to validate discovery and provide feedback to optimization cycles. However, with the boom in development of high-throughput synthesis tools that champion production rates up to $10^4$ samples per hour with flexible form factors, most sample characterization methods are either slow (conventional rates of $10^1$ samples per hour, approximately 1000x slower) or rigid (e.g., designed for standard-size microplates), resulting in a bottleneck that impedes the materials-design process. To overcome this challenge, we propose a set of automated material property characterization (autocharacterization) tools that leverage the adaptive, parallelizable, and scalable nature of computer vision to accelerate the throughput of characterization by 85x compared to the non-automated workflow. We demonstrate a generalizable composition mapping tool for high-throughput synthesized binary material systems as well as two scalable autocharacterization algorithms that (1) autonomously compute the band gap of 200 unique compositions in 6 minutes and (2) autonomously compute the degree of degradation in 200 unique compositions in 20 minutes, generating ultra-high compositional resolution trends of band gap and stability. We demonstrate that the developed band gap and degradation detection autocharacterization methods achieve 98.5% accuracy and 96.9% accuracy, respectively, on the FA$_{1-x}$MA$_{x}$PbI$_3$, $0\leq x \leq 1$ perovskite semiconductor system.

eess.IV↗

arXiv2021

Predicting antimicrobial activity of conjugated oligoelectrolyte molecules via machine learning

New antibiotics are needed to battle growing antibiotic resistance, but the development process from hit, to lead, and ultimately to a useful drug, takes decades. Although progress in molecular property prediction using machine-learning methods has opened up new pathways for aiding the antibiotics development process, many existing solutions rely on large datasets and finding structural similarities to existing antibiotics. Challenges remain in modelling of unconventional antibiotics classes that are drawing increasing research attention. In response, we developed an antimicrobial activity prediction model for conjugated oligoelectrolyte molecules, a new class of antibiotics that lacks extensive prior structure-activity relationship studies. Our approach enables us to predict minimum inhibitory concentration for E. coli K12, with 21 molecular descriptors selected by recursive elimination from a set of 5,305 descriptors. This predictive model achieves an R2 of 0.65 with no prior knowledge of the underlying mechanism. We find the molecular representation optimum for the domain is the key to good predictions of antimicrobial activity. In the case of conjugated oligoelectrolytes, a representation reflecting the 3-dimensional shape of the molecules is most critical. Although it is demonstrated with a specific example of conjugated oligoelectrolytes, our proposed approach for creating the predictive model can be readily adapted to other novel antibiotic candidate domains.

physics.app-ph↗

arXiv2021

Opportunities for Machine Learning to Accelerate Halide Perovskite Commercialization and Scale-Up

While halide perovskites attract significant academic attention, examples of at-scale industrial production are still sparse. In this perspective, we review practical challenges hindering the commercialization of halide perovskites, and discuss how machine-learning (ML) tools could help: (1) active-learning algorithms that blend institutional knowledge and human expertise could help stabilize and rapidly update baseline manufacturing processes; (2) ML-powered metrology, including computer imaging, could help narrow the performance gap between large- and small-area devices; and (3) inference methods could help accelerate root-cause analysis by reconciling multiple data streams and simulations, focusing research effort on areas with highest probability for improvement. We conclude that to satisfy many of these challenges, incremental -- not radical -- adaptations of existing ML and statistical methods are needed. We identify resources to help develop in-house data-science talent, and propose how industry-academic partnerships could help adapt "ready-now" ML tools to specific industry needs, further improve process control by revealing underlying mechanisms, and develop "gamechanger" discovery-oriented algorithms to better navigate vast materials combination spaces and the literature.

cond-mat.mtrl-sci↗

arXiv2021

Discovering Equations that Govern Experimental Materials Stability under Environmental Stress using Scientific Machine Learning

While machine learning (ML) in experimental research has demonstrated impressive predictive capabilities, inductive reasoning and knowledge extraction remain elusive tasks, in part because of the difficulty extracting fungible knowledge representations from experimental data. In this manuscript, we use ML to infer the underlying dynamical differential equation (DE) from experimental data of degrading organic-inorganic methylammonium lead iodide (MAPI) perovskite thin films under environmental stressors (elevated temperature, humidity, and light). We apply a sparse regression algorithm that automatically identifies the differential equation describing the dynamics from time-series data. We find that the underlying DE governing MAPI degradation across a broad temperature range of 35 to 85°C is described minimally with three terms (specifically, a second-order polynomial), and not a simple single-order reaction (i.e. 0th, 1st, or 2nd-order reaction). We demonstrate how computer-derived results can aid the researcher to develop profound mechanistic insights. This DE corresponds to the Verhulst logistic function, which describes reaction kinetics analogous in functional form to autocatalytic or self-propagating reactions, suggesting future strategies to suppress MAPI degradation. We examine the robustness of our conclusions to experimental luck-of-the-draw variance and Gaussian noise using a combination of experiment and simulation, and describe the experimental limits within which this methodology can be applied. Our study demonstrates the application of scientific ML in experimental chemical and materials systems, highlighting the promise and challenges associated with ML-aided scientific discovery.

cond-mat.mtrl-sci↗

arXiv2021

Benchmarking the Performance of Bayesian Optimization across Multiple Experimental Materials Science Domains

In the field of machine learning (ML) for materials optimization, active learning algorithms, such as Bayesian Optimization (BO), have been leveraged for guiding autonomous and high-throughput experimentation systems. However, very few studies have evaluated the efficiency of BO as a general optimization algorithm across a broad range of experimental materials science domains. In this work, we evaluate the performance of BO algorithms with a collection of surrogate model and acquisition function pairs across five diverse experimental materials systems, namely carbon nanotube polymer blends, silver nanoparticles, lead-halide perovskites, as well as additively manufactured polymer structures and shapes. By defining acceleration and enhancement metrics for general materials optimization objectives, we find that for surrogate model selection, Gaussian Process (GP) with anisotropic kernels (automatic relevance detection, ARD) and Random Forests (RF) have comparable performance and both outperform the commonly used GP without ARD. We discuss the implicit distributional assumptions of RF and GP, and the benefits of using GP with anisotropic kernels in detail. We provide practical insights for experimentalists on surrogate model selection of BO during materials optimization campaigns.

cond-mat.mtrl-sci↗