arXiv subjects

Megan Stanley

Publications and source records attributed to Megan Stanley.

5 recordsLinked to original sources

arXiv2025

Accurate and scalable exchange-correlation with deep learning

Density Functional Theory (DFT) underpins much of modern computational chemistry and materials science. Yet, the reliability of DFT-derived predictions of experimentally measurable properties remains fundamentally limited by the need to approximate the unknown exchange-correlation (XC) functional. The traditional paradigm for improving accuracy has relied on increasingly elaborate hand-crafted functional forms. This approach has led to a longstanding trade-off between computational efficiency and accuracy, which remains insufficient for reliable predictive modelling of laboratory experiments. Here we introduce Skala, a deep learning-based XC functional that surpasses state-of-the-art hybrid functionals in accuracy across the main-group chemistry benchmark set GMTKN55 with an error of 2.8 kcal/mol, while retaining the lower computational cost characteristic of semi-local DFT. This demonstrated departure from the historical trade-off between accuracy and efficiency is enabled by learning non-local representations of electronic structure directly from data, bypassing the need for increasingly costly hand-engineered features. Leveraging an unprecedented volume of high-accuracy reference data from wavefunction-based methods, we establish that modern deep learning enables systematically improvable neural exchange-correlation models as training datasets expand, positioning first-principles simulations to become progressively more predictive.

physics.chem-ph↗

arXiv2024

A Foundation Model for the Earth System

Reliable forecasts of the Earth system are crucial for human progress and safety from natural disasters. Artificial intelligence offers substantial potential to improve prediction accuracy and computational efficiency in this field, however this remains underexplored in many domains. Here we introduce Aurora, a large-scale foundation model for the Earth system trained on over a million hours of diverse data. Aurora outperforms operational forecasts for air quality, ocean waves, tropical cyclone tracks, and high-resolution weather forecasting at orders of magnitude smaller computational expense than dedicated existing systems. With the ability to fine-tune Aurora to diverse application domains at only modest computational cost, Aurora represents significant progress in making actionable Earth system predictions accessible to anyone.

physics.ao-ph↗

arXiv2023

Re-evaluating Retrosynthesis Algorithms with Syntheseus

Automated Synthesis Planning has recently re-emerged as a research area at the intersection of chemistry and machine learning. Despite the appearance of steady progress, we argue that imperfect benchmarks and inconsistent comparisons mask systematic shortcomings of existing techniques, and unnecessarily hamper progress. To remedy this, we present a synthesis planning library with an extensive benchmarking framework, called syntheseus, which promotes best practice by default, enabling consistent meaningful evaluation of single-step models and multi-step planning algorithms. We demonstrate the capabilities of syntheseus by re-evaluating several previous retrosynthesis algorithms, and find that the ranking of state-of-the-art models changes in controlled evaluation experiments. We end with guidance for future works in this area, and call the community to engage in the discussion on how to improve benchmarks for synthesis planning.

cs.LG↗

arXiv2021

Shapley explainability on the data manifold

Explainability in AI is crucial for model development, compliance with regulation, and providing operational nuance to predictions. The Shapley framework for explainability attributes a model's predictions to its input features in a mathematically principled and model-agnostic way. However, general implementations of Shapley explainability make an untenable assumption: that the model's features are uncorrelated. In this work, we demonstrate unambiguous drawbacks of this assumption and develop two solutions to Shapley explainability that respect the data manifold. One solution, based on generative modelling, provides flexible access to data imputations; the other directly learns the Shapley value-function, providing performance and stability at the cost of flexibility. While "off-manifold" Shapley values can (i) give rise to incorrect explanations, (ii) hide implicit model dependence on sensitive attributes, and (iii) lead to unintelligible explanations in higher-dimensional data, on-manifold explainability overcomes these problems.

cs.LG↗

arXiv2014

Frequency stabilization of the zero-phonon line of a quantum dot via phonon-assisted active feedback

We report on the feedback stabilization of the zero-phonon emission frequency of a single InAs quantum dot. The spectral separation of the phonon-assisted component of the resonance fluorescence provides a probe of the detuning between the zero-phonon transition and the resonant driving laser. Using this probe in combination with active feedback, we stabilize the zero-phonon transition frequency against environmental fluctuations. This protocol reduces the zero-phonon fluorescence intensity noise by a factor of 22 by correcting for environmental noise with a bandwidth of 191 Hz, limited by the experimental collection efficiency. The associated sub-Hz fluctuations in the zero-phonon central frequency are reduced by a factor of 7. This technique provides a means of stabilizing the quantum dot emission frequency without requiring access to the zero-phonon emission.

cond-mat.mes-hall↗