The Inference Report

We describe a neural network architecture and training procedure designed to model electronic ground and excited states of arbitrary molecular systems. By indirectly learning a latent, implicit basis representation of the electronic-state Hamiltonian, the model offers a unified treatment of multiple electronic states, conical intersections, and non-adiabatic couplings. The formalism can be further extended to learn consistent latent representations of additional operators such as transition dipole moments, for example. To demonstrate the general capabilities of our architecture, we train and evaluate networks on two realistic photochemical systems, thymine and azobenzene. The resulting models accurately reproduce energies and oscillator strengths for the ground- and low-lying excited states relevant to the photochemistry of these systems. We highlight the performance of the trained networks by studying critical molecular geometries, including conical intersections and excited state minima. By construction, the proposed framework also recovers the emergence of Berry phase accumulation around conical intersections. By pairing key mathematical structure from quantum chemistry with the representation learning power of transformers, the presented architecture offers a qualitatively new path toward fast and accurate ground- and excited-state simulations.

Electrolyte additive discovery remains challenging because experimentally validated molecules are sparse, whereas accessible chemical spaces are vast and largely unlabeled. This challenge is amplified in lithium-ion batteries, where additive performance arises from coupled interfacial reactions rather than a single molecular property. Here, we develop a prototype-guided molecular intelligence, ProtoMI, a literature-driven framework that learns transferable structural priors from reported electrolyte additives and uses them to prioritize candidates in unlabeled chemical space. For boron-containing additives, ProtoMI combines 126 literature-reported molecules with 179,977 unlabeled candidates. Graph contrastive learning identifies seven chemically interpretable prototypes from the reported additives, and prototype guided semi-supervised contrastive learning adapts these prototypes to the candidate space under source-target distribution mismatch. In retrospective temporal validation, ProtoMI achieves enrichment factors of 9.2-45.6 while screening less than 2% of the candidate space. A subsequent translation step identifies four commercially accessible candidates. One representative candidate, 4,4,5,5-Tetramethyl-2-[10-(1naphthyl)anthracen-9-yl]-1,3,2-dioxaborolane (TNDB), improves high-temperature LiFePO4||graphite cycling at 55 °C by 34.93% relative to the baseline electrolyte. An arsenal of characterizations and operando optical fiber Fourier transform infrared spectroscopy suggest that TNDB forms B-containing, F/P/O-modified inorganic interphases, suppresses solvent decomposition and reduces Fe deposition on graphite. This case study shows how sparse literature knowledge can guide experimentally efficient molecular discovery in data-scarce battery-additive spaces.

Polymeric materials are central to modern technologies, with applications ranging from energy to health and transportation. Although AI has made significant advances in materials discovery, the hierarchical structure of polymers across multiple length scales makes them inherently difficult to represent in a unified and physically meaningful way. Here we introduce HiPoly, a polymer-native AI framework that processes complete polymer descriptions through a three-level hierarchical graph architecture built on the G2RINS representation. HiPoly encodes stochastic inter-monomer connectivity, composition, and molecular weight directly within its architecture, using physically motivated design principles that mirror the multi-scale nature of polymeric systems. The framework establishes an end-to-end AI-driven workflow from experimental formulation data to property prediction, generative molecular design, and physics-based validation through molecular simulations, all unified by a single polymer representation. We demonstrate state-of-the-art prediction accuracy for thermophysical properties of multi-component polymer systems, with ablation studies confirming that each hierarchical design choice contributes independently to model performance. As an example, the generative design pathway is applied here to the discovery of sustainable alternatives to persistent fluorinated polymers, where it is possible to identify and independently validate PFAS-free candidates with target surface-energy properties. This work demonstrates how polymer-native AI can accelerate discovery by linking representation, prediction, and design across complex polymer chemistries.

Predicting thermal stability during handling and storage is essential for the design of safe and reliable energetic materials. However, experimental measurements vary significantly across laboratories due to differences in protocols and analysis methods, making it difficult to train reliable predictive models. We address this challenge through differential learning. Rather than predicting absolute decomposition temperatures, we instead train message passing neural networks to predict relative differences between pairs of molecules. This approach reduces sensitivity to systematic experimental errors and achieves >85% accuracy in ranking compounds by thermal stability, outperforming conventional regression methods on the same heterogeneous dataset. To understand what drives these predictions, we compare neural network models with interpretable alternatives built from descriptors derived from ab initio calculations and cheminformatics software. This analysis identifies bond dissociation enthalpy as a key determinant of thermal stability rankings, providing further insight into the complex chemistry of thermal decomposition. The differential learning framework generalizes across model architectures, from graph neural networks to classical descriptor-based approaches. Our results demonstrate that learning relative properties rather than absolute values offers a practical solution for modeling noisy experimental data, with direct applications in materials design where thermal stability predictions inform safety protocols.

Kohn--Sham density functional theory (DFT) underpins electronic-structure simulations, but repeated orbital diagonalizations lead to cubic scaling, restricting quantum calculations to modest scales only. Eliminating these auxiliary orbitals while retaining Kohn--Sham accuracy is the central goal of orbital-free DFT, but both analytical and machine-learning methods have so far fallen short. Prior learning approaches either try to learn the variational kinetic-energy functionals, which are ill-conditioned, or directly predict the ground state, which extrapolate poorly to larger systems. Instead, we identify the Kohn--Sham map as the right learning target for orbital-free DFT. It maps a Kohn--Sham potential directly to the corresponding density and noninteracting kinetic energy, quantities otherwise obtained through an orbital diagonalization. Focusing on the density component in this work, a domain-invariant $\mathrm{SE}(3)$-equivariant Fourier neural operator learns to predict it from the potential as input on real-space grids, enabling stable quasi-linear scaling SCFs. Trained jointly on 8,504 molecules and solids, a single model generalizes to out-of-distribution organic molecules, insulators, and metals. For the first time, the same method converges SCFs across these systems without explicitly constructing Kohn--Sham orbitals, while reproducing densities, electronic spectra, and structural observables at Kohn--Sham DFT accuracy. Linear-scaling SCFs additionally allow converging magnesium dislocation densities containing up to 82,500 valence electrons on a single GPU.

Coupled-cluster theory defines the accuracy standard for molecular electronic-structure properties but scales too steeply for routine application, whereas density-functional theory is affordable yet systematically biased. We resolve this trade-off with a single equivariant network, MEHnet-MG, that predicts an effective one-electron Hamiltonian from one inexpensive B3LYP/def2-SVP calculation and derives a broad suite of properties from it (energy, optical gap, dipole, quadrupole, polarizability, Mulliken atomic charges, and Mayer bond orders) at coupled-cluster accuracy across nine main-group elements, including the under-served phosphorus, sulfur, and chlorine chemistries. The model is trained on a new in-house dataset of multi-property labels computed at the CCSD(T) level for all nine elements. On a held-out test set, it reduces the error of every property by a factor of 3.8 to 230 relative to semi-local, hybrid, and double-hybrid DFT (referenced to composite CCSD(T)/cc-pVTZ; Methods), while adding only ~25 ms wall time per molecule, delivering coupled-cluster-quality predictions at the cost of a single DFT calculation. Critically, deriving every property from a predicted Hamiltonian rather than pooling per-atom features builds the correct size-scaling into the model architecture: on pi-conjugated oligothiophenes it matches finite-field CCSD polarizability and the EOM-CCSD optical gap to ~2% at the largest sizes where those references remain affordable (44 and 37 atoms, where a single CCSD field point already costs ~500x the model's entire inference) and extrapolates the corrected trends to 58-atom chains, a regime where pooling-based architectures fail by construction. Accurate extrapolation is therefore set by the model's inductive bias rather than by the training data.