English (United Kingdom)

https://curated-unify.zendy.io/wp-json/zendy-region/v1/featured_content/oa?rat=en

https://curated-unify.zendy.io/wp-json/zendy-region/v1/highlighted_journal/

Global: Zendy Tools annual

Presents the keyphrase highlighting as premium feature

Keyphrase Highlighting

Presents the summarisation as premium feature

Summarisation

Insights

Presents the pdf analysis as premium feature

PDF Analysis

Presents the zaia usage as premium feature

ZAIA

Global: Zendy Tools monthly

Global: Zendy Plus monthly

Presents the access of premium content as premium feature

Premium Content

Global: Zendy Plus annual

Global: Zendy Free Plan

Path integral molecular dynamics simulations, combined with an ab initioevaluation of interactions using electronic structure theory, incorporate thequantum mechanical nature of both the electrons and nuclei, which are essentialto accurately describe systems containing light nuclei. However, path integralsimulations have traditionally required a computational cost around two ordersof magnitude greater than treating the nuclei classically, making themprohibitively costly for most applications. Here we show that the cost of pathintegral simulations can be dramatically reduced by extending our ring polymercontraction approach to ab initio molecular dynamics simulations. By usingdensity functional tight binding as a reference system, we show that our abinitio ring polymer contraction (AI-RPC) scheme gives rapid and systematicconvergence to the full path integral density functional theory result. Wedemonstrate the efficiency of this approach in ab initio simulations of liquidwater and the reactive protonated and deprotonated water dimer systems. We findthat the vast majority of the nuclear quantum effects are accurately capturedusing contraction to just the ring polymer centroid, which requires the samenumber of density functional theory calculations as a classical simulation.Combined with a multiple time step scheme using the same reference system,which allows the time step to be increased, our implementation is as fast as atypical classical ab initio molecular dynamics simulation and 35$\times$ fasterthan a full path integral calculation, while still exactly including thequantum sampling of nuclei. This development thus offers a route to routinelyinclude nuclear quantum effects in ab initio molecular dynamics simulations atnegligible computational cost.

Ab initio molecular dynamics with nuclear quantum effects at classical cost: ring polymer contraction for density functional theory