Related papers: Gradient type optimization methods for electronic …

We focus on a class of non-smooth optimization problems over the Stiefel manifold in the decentralized setting, where a connected network of $n$ agents cooperatively minimize a finite-sum objective function with each component being weakly…

Standard negative log-likelihood (NLL) for Supervised Fine-Tuning (SFT) applies uniform token-level weighting. This rigidity creates a two-fold failure mode: (i) overemphasizing low-probability targets can amplify gradients on noisy…

Existing analyses of optimization in deep learning are either continuous, focusing on (variants of) gradient flow, or discrete, directly treating (variants of) gradient descent. Gradient flow is amenable to theoretical analysis, but is…

We describe an ab initio method for calculating the electronic structure, electronic transport, and forces acting on the atoms, for atomic scale systems connected to semi-infinite electrodes and with an applied voltage bias. Our method is…

Density functional theory (DFT), one of the most widely utilized methods available to computational chemistry, fails to describe systems with statically correlated electrons. To address this shortcoming, in previous work we transformed DFT…

Kohn-Sham density functional theory (DFT) has long struggled with the accurate description of strongly correlated and open shell systems and improvements have been minor even in the newest hybrid functionals. In this Letter we treat the…

Noncollinear (NC) magnetism and spin-orbit coupling (SOC) are indispensable for predictive ab initio materials simulations with pronounced relativistic effects and magnetic frustration, yet they significantly increase the cost of…

Density Functional Theory (DFT) is one of the most used ab initio theoretical frameworks in materials science. It derives the ground state properties of a multi-atomic ensemble directly from the computation of its one-particle density \nr…

For the computational prediction of core electron binding energies in solids, two distinct kinds of modelling strategies have been pursued: the $\Delta$-Self-Consistent-Field method based on density functional theory (DFT), and the GW…

Deep-learning density functional theory (DFT) shows great promise to significantly accelerate material discovery and potentially revolutionize materials research. However, current research in this field primarily relies on data-driven…

We demonstrate in the present study that self-consistent calculations based on the self-energy functional theory (SFT) are possible for the electronic structure of realistic systems in the context of quantum chemistry. We describe the…

In this paper, we address the optimization problem of minimizing $Q(df_x)$ over a Hadamard manifold ${\cal M}$, where $f$ is a convex function on ${\cal M}$, $df_x$ is the differential of $f$ at $x \in {\cal M}$, and $Q$ is a function on…

The NEPv approach has been increasingly used lately for optimization on the Stiefel manifold arising from machine learning. General speaking, the approach first turns the first order optimality condition, also known as the KKT condition,…

We present an embedding scheme for periodic systems that facilitates the treatment of the physically important part (here the unit cell) with advanced electronic-structure methods, that are computationally too expensive for periodic…

Reliable and robust convergence to the electronic ground state within density functional theory (DFT) Kohn-Sham (KS) calculations remains a thorny issue in many systems of interest. In such cases, charge sloshing can delay or completely…

Density-potential functional theory (DPFT) is an alternative formulation of orbital-free density functional theory that may be suitable for modeling the electronic structure of large systems. To date, DPFT has been applied mainly to quantum…

Linear scaling methods for density-functional theory (DFT) simulations are formulated in terms of localised orbitals in real-space, rather than the delocalised eigenstates of conventional approaches. In local-orbital methods, relative to…

This paper focus on the minimization of a possibly nonsmooth objective function over the Stiefel manifold. The existing approaches either lack efficiency or can only tackle prox-friendly objective functions. We propose a constraint…

We present a fully charge self-consistent implementation of dynamical mean field theory (DMFT) combined with density functional theory (DFT) for electronic structure calculations of materials with strong electronic correlations. The…

Electronic structure calculation of atoms and molecules, in the past few decades has largely been dominated by density functional methods. This is primarily due to the fact that this can account for electron correlation effects in a…