The paper introduces Physics‑Aligned Electronic Ground‑State Models (GSMs) that sit between machine‑learned interatomic potentials and Kohn‑Sham density functional theory in terms of computational cost and accuracy. By aligning GSM learning objectives with KS‑DFT equations and enforcing physical constraints, the authors develop new training techniques—OrthoNormal‑Loss (ON‑Loss), Grassmann Restricted Occupied‑Orbital Training (GROOT), and Residual Optimal‑gauge Conditioning‑aware KS‑Eq. Training (ROCKET)—which dramatically reduce energy and force errors in size‑extrapolation tests from QM9 to QM40. The models also achieve near‑chemical‑accuracy predictions on reactive chemistry benchmarks and demonstrate efficient label‑free self‑consistency fine‑tuning.
whyItMatters":"The work advances the cost‑accuracy frontier for electronic structure predictions, enabling more reliable out‑of‑distribution generalization in drug and material discovery."
By Eike S. Eberhard, Xaver Kainz, Viktor Kotsev, Abdulrahman Aldossary, Stephan G\"unnemann
arXiv:2606. 14498v1 Announce Type: cross Abstract: Predicting the Kohn-Sham Hamiltonian with machine learning can accelerate density functional theory while retaining access to molecular orbitals, energy levels, and electronic-structure observables that energy-only surrogates cannot resolve.
By Yunhong Lou, Xihang Yue, Xinran Wei, Tianqi Deng, Linchao Zhu
The paper presents a neural operator that learns the Kohn–Sham map, directly predicting electron density from the Kohn–Sham potential without orbital diagonalization. Using a domain‑invariant SE(3)‑equivariant Fourier neural operator trained on 8,504 molecules and solids, the model achieves quasi‑linear scaling self‑consistent field (SCF) convergence across diverse systems—including organic molecules, insulators, and metals—while reproducing Kohn–Sham DFT accuracy for densities, spectra, and structural observables. This enables large‑scale simulations, such as magnesium dislocation densities with 82,500 valence electrons, on a single GPU.
By Danish Khan, Maurice D. Hanisch, Nikolai Argatoff, Evan Xie, Sandeep Sharma, Anima Anandkumar
arXiv:2606. 04279v1 Announce Type: new Abstract: Machine-learned (ML) exchange-correlation (XC) functionals aim to replace human-designed density functional approximations by learning directly from reference data, but they still do not consistently outperform traditional $\mathcal{O}(N^4)$-scaling hybrid functionals.
By Eike S. Eberhard, Luca A. Thiede, Abdul Aldossary, Andreas Burger, Nicholas Gao, Vignesh Bhethanabotla, Al\'an Aspuru-Guzik, Stephan G\"unnemann
arXiv:2605.24073v2 Announce Type: replace-cross
Abstract: Machine learning interatomic potentials (MLIPs) require generating computationally expensive, large-scale training datasets to accurately sim...
By Ihor Neporozhnii, Sjoerd Hoogland, Oleksandr Voznyy
The paper introduces OrbFlow, an SE(3)-equivariant generative model that predicts Gaussian-type orbital coefficients for electron density using flow matching. By training with a two-phase trajectory curriculum, OrbFlow improves accuracy on QM9 and MD benchmarks, reducing density errors significantly compared to previous models. The predicted densities also accelerate self-consistent field procedures, cutting iterations by up to 68% and accurately reproducing dipole and quadrupole moments without additional SCF calculations.
By Chenxing Liang, Chengdong Wang, Yuchao Lin, Xiaofeng Qian, Shuiwang Ji
arXiv:2606. 19152v1 Announce Type: cross Abstract: Identifying the lowest-energy surface-adsorbate configuration is critical for modeling heterogeneous catalysis, yet exhaustive exploration with ab initio calculations is computationally prohibitive.
By Zongmin Zhang, Yuyang Lou, Bowen Zhang, Junwu Chen, Ryo Kuroki, Xuan Vu Nguyen, Edvin Fako, Lixue Cheng, Philippe Schwaller
Identifying the lowest-energy surface-adsorbate configuration is critical for modeling heterogeneous catalysis, yet exhaustive exploration with ab initio calculations is computationally prohibitive. Machine-learning force fields (MLFFs) accelerate structural relaxation but leave the search over the vast configurational space a major bottleneck, and open-loop large language model (LLM) agents lack a physics-grounded feedback mechanism to correct erroneous initial guesses.
arXiv:2601.00581v3 Announce Type: replace-cross
Abstract: We introduce AceFF, a pre-trained machine learning interatomic potential (MLIP) optimized for small molecule drug discovery. While MLIPs have...
By Stephen E. Farr, Stefan Doerr, Antonio Mirarchi, Alireza Moradzadeh, Francesc Sabanes Zariquiey, Saee Paliwal, Gianni De Fabritiis
arXiv:2610.19946v1 Announce Type: new
Abstract: Energy-based models can represent distributions over discrete structures such as molecular graphs, but an energy that is accurate at equilibrium need n...
By Amartya Banerjee, Xingyu Xu, Caroline Moosm\"uller, Harlin Lee
Automated materials discovery requires evaluating large pools of candidate configurations, with density functional theory (DFT) as a major throughput bottleneck. Pretrained machine-learned interatomic...
arXiv:2606. 24990v1 Announce Type: new Abstract: Reinforcement Learning (RL) has become a powerful paradigm for de novo molecular design, enabling Chemical Language Models (CLMs) to navigate and explore the chemical space while optimizing specific desired properties.
By Borja Medina, Jon Paul Janet