Highly Accurate Many-Body Theory Reaches 2D Materials

Highly Accurate Many-Body Theory Reaches 2D Materials | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Highly Accurate Many-Body Theory Reaches 2D Materials Nicole Spanedda, Anouar Benali, Fernando A. Reboredo, Jaron T. Krogel This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-6473408/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 26 Sep, 2025 Read the published version in Scientific Reports → Version 1 posted 14 You are reading this latest preprint version Abstract Quantum confinement in 2D materials strongly enhances electronic correlation effects. Therefore, predicting the properties of these unique materials, with both a high level of accuracy and computational efficiency, without relying on adjustable parameters or functionals, remains an outstanding theoretical challenge. The majority of theoretical studies are based on the approximations of density functional theory (DFT). The reliability of DFT predictions are heavily dependent on the choice of an approximated exchange-correlation functional. Here, we perform and compare, state-of-the-art sCI and quantum Monte Carlo extrapolated calculations for the quintessential 2D material, graphene. We demonstrate that Self-Healing Diffusion Monte Carlo (SHDMC) obtains a very compact, but high-quality wavefunction for 2D materials that lacks the strong basis set dependence displayed by state of the art quantum chemistry methods. The SHDMC wavefunction is of higher quality compared to that obtained from sCI, in the same orbital basis, while being ~1000 times smaller in terms of determinant count compared to sCI. We also demonstrate that extrapolating SHDMC results to the infinite determinant limit compares extremely well with complete basis set extrapolated sCI. Our work paves the way for future applications of SHDMC to challenging 2D materials. Physical sciences/Physics/Quantum physics Physical sciences/Physics/Condensed matter physics Physical sciences/Physics/Condensed matter physics/Electronic properties and materials Full Text Additional Declarations No competing interests reported. Supplementary Files shdmcsupplementaryinfo.pdf Cite Share Download PDF Status: Published Journal Publication published 26 Sep, 2025 Read the published version in Scientific Reports → Version 1 posted Editorial decision: Revision requested 26 May, 2025 Reviews received at journal 16 May, 2025 Reviews received at journal 16 May, 2025 Reviews received at journal 16 May, 2025 Reviews received at journal 09 May, 2025 Reviewers agreed at journal 07 May, 2025 Reviewers agreed at journal 06 May, 2025 Reviewers agreed at journal 05 May, 2025 Reviewers agreed at journal 05 May, 2025 Reviewers invited by journal 05 May, 2025 Editor assigned by journal 05 May, 2025 Editor invited by journal 05 May, 2025 Submission checks completed at journal 02 May, 2025 First submitted to journal 17 Apr, 2025 You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. 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Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-6473408","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":453471057,"identity":"592999f7-5048-4e5e-99e7-be17a0041f73","order_by":0,"name":"Nicole Spanedda","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA2ElEQVRIiWNgGAWjYNACNmYgwXwASFiQpIUtAUhIkKSFx4A4LfKzm589+FBmLW/Of+bj48odEgzy7j0GeLUY3DlmbjjjXLrhzhm5mw3PnpFgMDxzhoAWiQQzad62w4wbbvBuk2xsA2qZkZaA32Ez0r9J/207bL/h/JlnxGlhuJFjJs3Ydjhxw4EcNrAWeYnkAwT8cqZMsudcevKGG2nGhkAtPAY8h/FrkZ/dvk3iR5m17Ybzhx8+bGyzkZNvb2zA7zD0iOAxwG8HFi0M8gTsGAWjYBSMgpEHAFUXRtZxDhwXAAAAAElFTkSuQmCC","orcid":"","institution":"Oak Ridge National Laboratory","correspondingAuthor":true,"prefix":"","firstName":"Nicole","middleName":"","lastName":"Spanedda","suffix":""},{"id":453471058,"identity":"b7ff7d26-815e-4d22-befe-86aca7dc6a43","order_by":1,"name":"Anouar Benali","email":"","orcid":"","institution":"Argonne National Laboratory","correspondingAuthor":false,"prefix":"","firstName":"Anouar","middleName":"","lastName":"Benali","suffix":""},{"id":453471059,"identity":"2bceb2b5-c2bd-4d77-ba4d-dcd43ec8f449","order_by":2,"name":"Fernando A. 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