arXiv subjects

Ole Schütt

Publications and source records attributed to Ole Schütt.

7 recordsLinked to original sources

arXiv2026

CP2K: An electronic structure and molecular dynamics software package - Dynamics, Transport, and Spectroscopic Response

One of the distinguishing aspects of CP2K is its seamless integration of diverse structural and transition-state optimization techniques with advanced sampling approaches including Monte Carlo, molecular dynamics, and metadynamics, enabling the efficient exploration of complex potential- and free-energy landscapes, including rare events. These capabilities are combined with a broad hierarchy of energy and force evaluation methods, ranging from classical and machine-learned interaction potentials and mixed quantum-classical multiscale and semiempirical schemes, to highly accurate quantum-mechanical electronic-structure approaches. At the heart of the latter lies the Gaussian and plane-wave framework, along with its augmented all-electron generalization, which have been described in detail in our previous code review [T. D. Kühne et al., J. Chem. Phys. 152, 194103 (2020)]. Building on this foundation, the present work revisits the methods within CP2K that turn electronic structure into dynamics, transport, and spectroscopic response. Particular emphasis is placed on the coupling between static response calculations and nuclear motion: spectra may be evaluated at optimized structures, averaged over thermally sampled configurations, obtained from time-correlation functions along ab-initio or path integral molecular trajectories, or followed in real time together with electronic and nuclear dynamics. The same modular structure also enables equilibrium and biased transport simulations, from Kubo-type linear response to open-boundary approaches under external potentials, highlighting CP2K's unique capability to unify quantum chemistry with quantum and statistical mechanics within a versatile, holistic simulation environment.

physics.chem-ph↗

arXiv2025

The CP2K Program Package Made Simple

CP2K is a versatile open-source software package for simulations across a wide range of atomistic systems, from isolated molecules in the gas phase to low-dimensional functional materials and interfaces, as well as highly symmetric crystalline solids, disordered amorphous glasses, and weakly interacting soft-matter systems in the liquid state and in solution. This review highlights CP2K's capabilities for computing both static and dynamical properties using quantum-mechanical and classical simulation methods. In contrast to the accompanying theory and code paper [J. Chem. Phys. 152, 194103 (2020)], the focus here is on the practical usage and applications of CP2K, with underlying theoretical concepts introduced only as needed.

physics.comp-ph↗

arXiv2022

Roadmap on Electronic Structure Codes in the Exascale Era

Electronic structure calculations have been instrumental in providing many important insights into a range of physical and chemical properties of various molecular and solid-state systems. Their importance to various fields, including materials science, chemical sciences, computational chemistry and device physics, is underscored by the large fraction of available public supercomputing resources devoted to these calculations. As we enter the exascale era, exciting new opportunities to increase simulation numbers, sizes, and accuracies present themselves. In order to realize these promises, the community of electronic structure software developers will however first have to tackle a number of challenges pertaining to the efficient use of new architectures that will rely heavily on massive parallelism and hardware accelerators. This roadmap provides a broad overview of the state-of-the-art in electronic structure calculations and of the various new directions being pursued by the community. It covers 14 electronic structure codes, presenting their current status, their development priorities over the next five years, and their plans towards tackling the challenges and leveraging the opportunities presented by the advent of exascale computing.

cond-mat.mtrl-sci↗

arXiv2022

Towards Electronic Structure-Based Ab-Initio Molecular Dynamics Simulations with Hundreds of Millions of Atoms

We push the boundaries of electronic structure-based \textit{ab-initio} molecular dynamics (AIMD) beyond 100 million atoms. This scale is otherwise barely reachable with classical force-field methods or novel neural network and machine learning potentials. We achieve this breakthrough by combining innovations in linear-scaling AIMD, efficient and approximate sparse linear algebra, low and mixed-precision floating-point computation on GPUs, and a compensation scheme for the errors introduced by numerical approximations. The core of our work is the non-orthogonalized local submatrix method (NOLSM), which scales very favorably to massively parallel computing systems and translates large sparse matrix operations into highly parallel, dense matrix operations that are ideally suited to hardware accelerators. We demonstrate that the NOLSM method, which is at the center point of each AIMD step, is able to achieve a sustained performance of 324 PFLOP/s in mixed FP16/FP32 precision corresponding to an efficiency of 67.7% when running on 1536 NVIDIA A100 GPUs.

physics.comp-ph↗

arXiv2020

AiiDAlab -- an ecosystem for developing, executing, and sharing scientific workflows

Cloud platforms allow users to execute tasks directly from their web browser and are a key enabling technology not only for commerce but also for computational science. Research software is often developed by scientists with limited experience in (and time for) user interface design, which can make research software difficult to install and use for novices. When combined with the increasing complexity of scientific workflows (involving many steps and software packages), setting up a computational research environment becomes a major entry barrier. AiiDAlab is a web platform that enables computational scientists to package scientific workflows and computational environments and share them with their collaborators and peers. By leveraging the AiiDA workflow manager and its plugin ecosystem, developers get access to a growing range of simulation codes through a python API, coupled with automatic provenance tracking of simulations for full reproducibility. Computational workflows can be bundled together with user-friendly graphical interfaces and made available through the AiiDAlab app store. Being fully compatible with open-science principles, AiiDAlab provides a complete infrastructure for automated workflows and provenance tracking, where incorporating new capabilities becomes intuitive, requiring only Python knowledge.

cond-mat.mtrl-sci↗

arXiv2020

Materials Cloud, a platform for open computational science

Materials Cloud is a platform designed to enable open and seamless sharing of resources for computational science, driven by applications in materials modelling. It hosts 1) archival and dissemination services for raw and curated data, together with their provenance graph, 2) modelling services and virtual machines, 3) tools for data analytics, and pre-/post-processing, and 4) educational materials. Data is citable and archived persistently, providing a comprehensive embodiment of the FAIR principles that extends to computational workflows. Materials Cloud leverages the AiiDA framework to record the provenance of entire simulation pipelines (calculations performed, codes used, data generated) in the form of graphs that allow to retrace and reproduce any computed result. When an AiiDA database is shared on Materials Cloud, peers can browse the interconnected record of simulations, download individual files or the full database, and start their research from the results of the original authors. The infrastructure is agnostic to the specific simulation codes used and can support diverse applications in computational science that transcend its initial materials domain.

cond-mat.mtrl-sci↗

arXiv2020

CP2K: An Electronic Structure and Molecular Dynamics Software Package -- Quickstep: Efficient and Accurate Electronic Structure Calculations

CP2K is an open source electronic structure and molecular dynamics software package to perform atomistic simulations of solid-state, liquid, molecular and biological systems. It is especially aimed at massively-parallel and linear-scaling electronic structure methods and state-of-the-art ab-initio molecular dynamics simulations. Excellent performance for electronic structure calculations is achieved using novel algorithms implemented for modern high-performance computing systems. This review revisits the main capabilities of CP2k to perform efficient and accurate electronic structure simulations. The emphasis is put on density functional theory and multiple post-Hartree-Fock methods using the Gaussian and plane wave approach and its augmented all-electron extension.

physics.chem-ph↗