Density functional theory (DFT) is a fundamental method for simulating quantum chemical properties, but it remains expensive due to the iterative self-consistent field (SCF) process required to solve the Kohn-Sham equations. Recently, deep learning methods are gaining attention as a way to bypass this step by directly predicting the Hamiltonian. However, they rely on deterministic regression and do not consider the highly structured nature of Hamiltonians. In this work, we propose QHFLOW, a high-order equivariant flow matching framework that generates Hamiltonian matrices conditioned on molecular geometry. Flow matching models continuous-time trajectories between simple priors and complex targets, learning the structured distributions over Hamiltonians instead of direct regression. To further incorporate symmetry, we use a neural architecture that predicts SE(3)-equivariant vector fields, improving accuracy and generalization across diverse geometries. To further enhance physical fidelity, we additionally introduce a fine-tuning scheme to align predicted orbital energies with the target. QHFLOW achieves state-of-the-art performance, reducing Hamiltonian error by 73% on MD17 and 53% on QH9 compared to the previous best model. Moreover, we further show that QHFLOW accelerates the DFT process without trading off the solution quality when initializing SCF iterations with the predicted Hamiltonian, significantly reducing the number of iterations and runtime.

Recent works proposed amortizing the cost by learning generalized wave functions across different structures and compounds instead of solving each problem independently.

However, GCNs involve unnecessary nonlinearity and deep architecture. We also verify that molecular GCNs are based on a poor basis function set compared with the standard one used in theoretical calculations or quantum chemical simulations. From these observations, we describe the quantum deep field (QDF), a machine learning (ML) model based on an underlying quantum physics, in particular the density functional theory (DFT).

We introduce fermionic neural Gibbs states (fNGS), a variational framework for modeling finite-temperature properties of strongly interacting fermions. fNGS starts from a reference mean-field thermofield-double state and uses neural-network transformations together with imaginary-time evolution to systematically build strong correlations. Applied to the doped Fermi-Hubbard model, a minimal lattice model capturing essential features of strong electronic correlations, fNGS accurately reproduces thermal energies over a broad range of temperatures, interaction strengths, even at large dopings, for system sizes beyond the reach of exact methods. These results demonstrate a scalable route to studying finite-temperature properties of strongly correlated fermionic systems beyond one dimension with neural-network representations of quantum states.

Spin plays a fundamental role in understanding electronic structure, yet many real-space wavefunction methods fail to adequately consider it. We introduce the Spin-Adapted Antisymmetrization Method (SAAM), a general procedure that enforces exact total spin symmetry for antisymmetric many-electron wavefunctions in real space. In the context of neural network-based quantum Monte Carlo (NNQMC), SAAM leverages the expressiveness of deep neural networks to capture electron correlation while enforcing exact spin adaptation via group representation theory. This framework provides a principled route to embed physical priors into otherwise black-box neural network wavefunctions, yielding a compact representation of correlated system with neural network orbitals. Compared with existing treatments of spin in NNQMC, SAAM is more accurate and efficient, achieving exact spin purity without any additional tunable hyperparameters. To demonstrate its effectiveness, we apply SAAM to study the spin ladder of iron-sulfur clusters, a long-standing challenge for many-body methods due to their dense spectrum of nearly degenerate spin states. Our results reveal accurate resolution of low-lying spin states and spin gaps in [Fe$_2$S$_2$] and [Fe$_4$S$_4$] clusters, offering new insights into their electronic structures. In sum, these findings establish SAAM as a robust, hyperparameter-free standard for spin-adapted NNQMC, particularly for strongly correlated systems.