Accelerating Structure-Property Relationship Discovery with Multimodal Machine Learning and Self-Driving Microscopy

TL;DR

This paper introduces an autonomous microscopy framework combined with deep learning to efficiently explore and map nanoscale structure-property relationships in materials, demonstrated on halide perovskite films.

Contribution

It presents a novel integration of self-driving microscopy with dual-novelty deep kernel learning and dual variational autoencoders for adaptive data collection and representation learning.

Findings

Identified distinct hysteresis behaviors linked to nanoscale structural motifs.

Mapped structure-property relationships in halide perovskite films.

Demonstrated efficient exploration of large spectral datasets.

Abstract

Microscopy combined with local spectroscopy is widely used to correlate nanoscale structure with functional properties in materials, but conventional measurements rely heavily on human-selected sampling locations and predefined targets, limiting dataset diversity and the potential for discovery. Here, we present a framework that integrates autonomous microscopy with a dual-novelty deep kernel learning (DN-DKL) for adaptive data acquisition and a dual variational autoencoder (VAE) for representation learning. DN-DKL actively guides the microscopy toward structurally and spectroscopically novel regions, enabling efficient collection of large spectral datasets. Dual-VAE embeds local structure and spectroscopic responses into a shared latent manifold that serves as a structure-property relationship map. We applied this framework for the investigation of halide perovskite films using conductive atomic force microscopy. The results reveal distinct hysteresis behaviors that are linked to specific nanoscale structural motifs, including grain boundary junction points that show hysteresis under different bias conditions and asymmetric grain boundaries that suppress charge transport. This framework establishes a general strategy that leverages the complementary strengths of self-driving microscopy, machine learning, and human expertise to accelerate scientific discovery in functional materials.