Related papers: Second-order self-consistent field algorithms: fro…
According to the modern paradigms of software engineering, standard tasks are best accomplished by reusable open source libraries. We describe OpenOrbitalOptimizer: a reusable open source C++ library for the iterative solution of coupled…
The convergence of self-consistent field equations in mean-field nuclear-electronic orbital methods strongly depends on the choice of initial guesses for quantum nuclei. Although several such guesses have been proposed in the literature, a…
This paper proposes a homogeneous second-order descent framework (HSODF) for nonconvex and convex optimization based on the generalized homogeneous model (GHM). In comparison to the Newton steps, the GHM can be solved by extremal symmetric…
We present high-probability (and expectation) complexity bounds for two versions of stochastic adaptive regularization methods with cubics (SARC), also known as regularized Newton methods. The first algorithm aims to find first-order…
The self-consistent procedure in electronic structure calculations is revisited using a highly efficient and robust algorithm for solving the non-linear eigenvector problem i.e. H({{\psi}}){\psi} = E{\psi}. This new scheme is derived from a…
This work is on constrained large-scale non-convex optimization where the constraint set implies a manifold structure. Solving such problems is important in a multitude of fundamental machine learning tasks. Recent advances on Riemannian…
Second-order methods are of great importance for composite convex optimization problems due to their local super-linear convergence rates (under appropriate assumptions). However, the presence of even a simple nonsmooth function in the…
In this work we investigate methods to improve the efficiency and scalability of quantum algorithms for quantum chemistry applications. We propose a transformation of the electronic structure Hamiltonian in the second quantization framework…
We extend our recently developed semiclassical strong-field Herman-Kluk propagator (SFHK) method to calculate high-order harmonic generation (HHG) for atoms in intense lasers. We show that our method, based on a combination of the…
In this paper, through a very intuitive vanilla proximal method perspective, we derive accelerated high-order optimization algorithms for minimizing a convex function that has H\"{o}lder continuous derivatives. In this general convex…
A new scheme to study the properties of finite nuclei is proposed based on the Dirac-Brueckner-Hartree-Fock (DBHF) approach starting from a bare nucleon-nucleon interaction. The relativistic structure of the nucleon self-energies in nuclear…
We propose a novel general algorithm LHAC that efficiently uses second-order information to train a class of large-scale l1-regularized problems. Our method executes cheap iterations while achieving fast local convergence rate by exploiting…
The theory of spectral filtering is a remarkable tool to understand the statistical properties of learning with kernels. For least squares, it allows to derive various regularization schemes that yield faster convergence rates of the excess…
Self-consistent field theory (SCFT) has proven to be a powerful tool for modeling equilibrium microstructures of soft materials, particularly for multiblock polymers. A very successful approach to numerically solving the SCFT set of…
Doping compounds can be considered a perturbation to the nuclear charges in a molecular Hamiltonian. Expansions of this perturbation in a Taylor series, i.e. quantum alchemy, has been used in literature to assess millions of derivative…
This paper provides a theoretical and numerical comparison of classical first-order splitting methods for solving smooth convex optimization problems and cocoercive equations. From a theoretical point of view, we compare convergence rates…
We develop a new method for equality constrained optimization problems based on a sequential cubic programming framework. Each iteration utilizes a step decomposition based on the Jacobian of the constraints into a normal and a tangential…
The self-consistent field (SCF) iteration, combined with its variants, is one of the most widely used algorithms in quantum chemistry. We propose a procedure to adapt the SCF iteration for the p-Laplacian eigenproblem, which is an important…
Minimizing loss functions is central to machine-learning training. Although first-order methods dominate practical applications, higher-order techniques such as Newton's method can deliver greater accuracy and faster convergence, yet are…
In this paper, we study Newton-conjugate gradient (Newton-CG) methods for minimizing a nonconvex function $f$ whose Hessian is $(H_f,\nu)$-H\"older continuous with modulus $H_f>0$ and exponent $\nu\in(0,1]$. Recently proposed Newton-CG…