Understanding solid nitrogen through molecular dynamics simulations with a machine-learning potential

IF 3.7 2区 物理与天体物理 Q1 Physics and Astronomy Physical Review B Pub Date : 2024-11-05 DOI:10.1103/physrevb.110.184107
Marcin Kirsz, Ciprian G. Pruteanu, Peter I. C. Cooke, Graeme J. Ackland
{"title":"Understanding solid nitrogen through molecular dynamics simulations with a machine-learning potential","authors":"Marcin Kirsz, Ciprian G. Pruteanu, Peter I. C. Cooke, Graeme J. Ackland","doi":"10.1103/physrevb.110.184107","DOIUrl":null,"url":null,"abstract":"We construct a fast, transferable, general purpose, machine-learning interatomic potential suitable for large-scale simulations of <mjx-container ctxtmenu_counter=\"60\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-structure=\"(2 0 1)\"><mjx-msub data-semantic-children=\"0,1\" data-semantic- data-semantic-owns=\"0 1\" data-semantic-role=\"latinletter\" data-semantic-speech=\"normal upper N 2\" data-semantic-type=\"subscript\"><mjx-mi data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"2\" data-semantic-role=\"latinletter\" data-semantic-type=\"identifier\"><mjx-c>N</mjx-c></mjx-mi><mjx-script style=\"vertical-align: -0.15em;\"><mjx-mn data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"2\" data-semantic-role=\"integer\" data-semantic-type=\"number\" size=\"s\"><mjx-c>2</mjx-c></mjx-mn></mjx-script></mjx-msub></mjx-math></mjx-container>. The potential is trained only on high quality quantum chemical molecule-molecule interactions; no condensed phase information is used. Although there are no explicit or implicit many-molecule interaction terms, the potential reproduces the experimental phase diagram including the melt curve and the molecular solid phases of nitrogen up to <mjx-container ctxtmenu_counter=\"61\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-structure=\"(4 0 3 2)\"><mjx-mrow data-semantic-annotation=\"clearspeak:unit\" data-semantic-children=\"0,2\" data-semantic-content=\"3\" data-semantic- data-semantic-owns=\"0 3 2\" data-semantic-role=\"implicit\" data-semantic-speech=\"10 upper G upper P a\" data-semantic-type=\"infixop\"><mjx-mn data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"4\" data-semantic-role=\"integer\" data-semantic-type=\"number\"><mjx-c noic=\"true\" style=\"padding-top: 0.642em;\">1</mjx-c><mjx-c style=\"padding-top: 0.642em;\">0</mjx-c></mjx-mn><mjx-mspace data-semantic- data-semantic-operator=\"infixop,⁢\" data-semantic-parent=\"4\" data-semantic-role=\"space\" data-semantic-type=\"operator\" style=\"width: 0.4em;\"></mjx-mspace><mjx-mi data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"4\" data-semantic-role=\"unknown\" data-semantic-type=\"identifier\" space=\"2\"><mjx-c noic=\"true\" style=\"padding-top: 0.669em;\">G</mjx-c><mjx-c noic=\"true\" style=\"padding-top: 0.669em;\">P</mjx-c><mjx-c style=\"padding-top: 0.669em;\">a</mjx-c></mjx-mi></mjx-mrow></mjx-math></mjx-container>. This demonstrates that many-molecule interactions are unnecessary to explain the condensed phases of <mjx-container ctxtmenu_counter=\"62\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-structure=\"(2 0 1)\"><mjx-msub data-semantic-children=\"0,1\" data-semantic- data-semantic-owns=\"0 1\" data-semantic-role=\"latinletter\" data-semantic-speech=\"normal upper N 2\" data-semantic-type=\"subscript\"><mjx-mi data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"2\" data-semantic-role=\"latinletter\" data-semantic-type=\"identifier\"><mjx-c>N</mjx-c></mjx-mi><mjx-script style=\"vertical-align: -0.15em;\"><mjx-mn data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"normal\" data-semantic- data-semantic-parent=\"2\" data-semantic-role=\"integer\" data-semantic-type=\"number\" size=\"s\"><mjx-c>2</mjx-c></mjx-mn></mjx-script></mjx-msub></mjx-math></mjx-container>. With increased pressure, transitions are observed from cubic <mjx-container ctxtmenu_counter=\"63\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-children=\"1\" data-semantic-content=\"0,2\" data-semantic- data-semantic-owns=\"0 1 2\" data-semantic-role=\"leftright\" data-semantic-speech=\"left parenthesis alpha right parenthesis\" data-semantic-structure=\"(3 0 1 2)\" data-semantic-type=\"fenced\"><mjx-mo data-semantic- data-semantic-operator=\"fenced\" data-semantic-parent=\"3\" data-semantic-role=\"open\" data-semantic-type=\"fence\" style=\"vertical-align: -0.02em;\"><mjx-c>(</mjx-c></mjx-mo><mjx-mi data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"italic\" data-semantic- data-semantic-parent=\"3\" data-semantic-role=\"greekletter\" data-semantic-type=\"identifier\"><mjx-c>𝛼</mjx-c></mjx-mi><mjx-mo data-semantic- data-semantic-operator=\"fenced\" data-semantic-parent=\"3\" data-semantic-role=\"close\" data-semantic-type=\"fence\" style=\"vertical-align: -0.02em;\"><mjx-c>)</mjx-c></mjx-mo></mjx-math></mjx-container>, which optimizes quadrupole-quadrupole interactions, through tetragonal <mjx-container ctxtmenu_counter=\"64\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-children=\"1\" data-semantic-content=\"0,2\" data-semantic- data-semantic-owns=\"0 1 2\" data-semantic-role=\"leftright\" data-semantic-speech=\"left parenthesis gamma right parenthesis\" data-semantic-structure=\"(3 0 1 2)\" data-semantic-type=\"fenced\"><mjx-mo data-semantic- data-semantic-operator=\"fenced\" data-semantic-parent=\"3\" data-semantic-role=\"open\" data-semantic-type=\"fence\" style=\"vertical-align: -0.02em;\"><mjx-c>(</mjx-c></mjx-mo><mjx-mi data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"italic\" data-semantic- data-semantic-parent=\"3\" data-semantic-role=\"greekletter\" data-semantic-type=\"identifier\"><mjx-c>𝛾</mjx-c></mjx-mi><mjx-mo data-semantic- data-semantic-operator=\"fenced\" data-semantic-parent=\"3\" data-semantic-role=\"close\" data-semantic-type=\"fence\" style=\"vertical-align: -0.02em;\"><mjx-c>)</mjx-c></mjx-mo></mjx-math></mjx-container>, which allows more efficient packing, to monoclinic <mjx-container ctxtmenu_counter=\"65\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-children=\"1\" data-semantic-content=\"0,2\" data-semantic- data-semantic-owns=\"0 1 2\" data-semantic-role=\"leftright\" data-semantic-speech=\"left parenthesis lamda right parenthesis\" data-semantic-structure=\"(3 0 1 2)\" data-semantic-type=\"fenced\"><mjx-mo data-semantic- data-semantic-operator=\"fenced\" data-semantic-parent=\"3\" data-semantic-role=\"open\" data-semantic-type=\"fence\" style=\"vertical-align: -0.02em;\"><mjx-c>(</mjx-c></mjx-mo><mjx-mi data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"italic\" data-semantic- data-semantic-parent=\"3\" data-semantic-role=\"greekletter\" data-semantic-type=\"identifier\"><mjx-c>𝜆</mjx-c></mjx-mi><mjx-mo data-semantic- data-semantic-operator=\"fenced\" data-semantic-parent=\"3\" data-semantic-role=\"close\" data-semantic-type=\"fence\" style=\"vertical-align: -0.02em;\"><mjx-c>)</mjx-c></mjx-mo></mjx-math></mjx-container>, which packs still more efficiently. On heating, we obtain the hcp three-dimensional (3D) rotor phase <mjx-container ctxtmenu_counter=\"66\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-children=\"1\" data-semantic-content=\"0,2\" data-semantic- data-semantic-owns=\"0 1 2\" data-semantic-role=\"leftright\" data-semantic-speech=\"left parenthesis beta right parenthesis\" data-semantic-structure=\"(3 0 1 2)\" data-semantic-type=\"fenced\"><mjx-mo data-semantic- data-semantic-operator=\"fenced\" data-semantic-parent=\"3\" data-semantic-role=\"open\" data-semantic-type=\"fence\" style=\"vertical-align: -0.02em;\"><mjx-c>(</mjx-c></mjx-mo><mjx-mi data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"italic\" data-semantic- data-semantic-parent=\"3\" data-semantic-role=\"greekletter\" data-semantic-type=\"identifier\"><mjx-c>𝛽</mjx-c></mjx-mi><mjx-mo data-semantic- data-semantic-operator=\"fenced\" data-semantic-parent=\"3\" data-semantic-role=\"close\" data-semantic-type=\"fence\" style=\"vertical-align: -0.02em;\"><mjx-c>)</mjx-c></mjx-mo></mjx-math></mjx-container> and, at pressure, the cubic <mjx-container ctxtmenu_counter=\"67\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-structure=\"0\"><mjx-mi data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"italic\" data-semantic- data-semantic-role=\"greekletter\" data-semantic-speech=\"delta\" data-semantic-type=\"identifier\"><mjx-c>𝛿</mjx-c></mjx-mi></mjx-math></mjx-container> phase which contains both 3D and 2D rotors, tetragonal <mjx-container ctxtmenu_counter=\"68\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-structure=\"(2 0 1)\"><mjx-msup data-semantic-children=\"0,1\" data-semantic- data-semantic-owns=\"0 1\" data-semantic-role=\"greekletter\" data-semantic-speech=\"delta Superscript asterisk\" data-semantic-type=\"superscript\"><mjx-mi data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"italic\" data-semantic- data-semantic-parent=\"2\" data-semantic-role=\"greekletter\" data-semantic-type=\"identifier\"><mjx-c>𝛿</mjx-c></mjx-mi><mjx-script style=\"vertical-align: 0.363em;\"><mjx-mo data-semantic- data-semantic-parent=\"2\" data-semantic-role=\"multiplication\" data-semantic-type=\"operator\" size=\"s\"><mjx-c>*</mjx-c></mjx-mo></mjx-script></mjx-msup></mjx-math></mjx-container> phase with 2D rotors, and the rhombohedral <mjx-container ctxtmenu_counter=\"69\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-structure=\"0\"><mjx-mi data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"italic\" data-semantic- data-semantic-role=\"greekletter\" data-semantic-speech=\"epsilon\" data-semantic-type=\"identifier\"><mjx-c>𝜀</mjx-c></mjx-mi></mjx-math></mjx-container>. Molecular dynamics demonstrates where these phases are indeed rotors, rather than frustrated order. The model supports the metastability of the complex <mjx-container ctxtmenu_counter=\"70\" ctxtmenu_oldtabindex=\"1\" jax=\"CHTML\" overflow=\"linebreak\" role=\"tree\" sre-explorer- style=\"font-size: 100.7%;\" tabindex=\"0\"><mjx-math data-semantic-structure=\"0\"><mjx-mi data-semantic-annotation=\"clearspeak:simple\" data-semantic-font=\"italic\" data-semantic- data-semantic-role=\"greekletter\" data-semantic-speech=\"iota\" data-semantic-type=\"identifier\"><mjx-c>𝜄</mjx-c></mjx-mi></mjx-math></mjx-container> phase, but not the reported existence of the wide range of bond lengths. The thermodynamic transitions involve both shifts of molecular centers and rotations of molecules: the onset of rotation is rapid, whereas motion of molecular centers is inhibited and we suggest that this is the cause of the experimentally observed sluggishness of transitions. Routine density functional theory calculations give a similar picture to the potential.","PeriodicalId":20082,"journal":{"name":"Physical Review B","volume":"44 1","pages":""},"PeriodicalIF":3.7000,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Physical Review B","FirstCategoryId":"101","ListUrlMain":"https://doi.org/10.1103/physrevb.110.184107","RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"Physics and Astronomy","Score":null,"Total":0}
引用次数: 0

Abstract

We construct a fast, transferable, general purpose, machine-learning interatomic potential suitable for large-scale simulations of N2. The potential is trained only on high quality quantum chemical molecule-molecule interactions; no condensed phase information is used. Although there are no explicit or implicit many-molecule interaction terms, the potential reproduces the experimental phase diagram including the melt curve and the molecular solid phases of nitrogen up to 10GPa. This demonstrates that many-molecule interactions are unnecessary to explain the condensed phases of N2. With increased pressure, transitions are observed from cubic (𝛼), which optimizes quadrupole-quadrupole interactions, through tetragonal (𝛾), which allows more efficient packing, to monoclinic (𝜆), which packs still more efficiently. On heating, we obtain the hcp three-dimensional (3D) rotor phase (𝛽) and, at pressure, the cubic 𝛿 phase which contains both 3D and 2D rotors, tetragonal 𝛿* phase with 2D rotors, and the rhombohedral 𝜀. Molecular dynamics demonstrates where these phases are indeed rotors, rather than frustrated order. The model supports the metastability of the complex 𝜄 phase, but not the reported existence of the wide range of bond lengths. The thermodynamic transitions involve both shifts of molecular centers and rotations of molecules: the onset of rotation is rapid, whereas motion of molecular centers is inhibited and we suggest that this is the cause of the experimentally observed sluggishness of transitions. Routine density functional theory calculations give a similar picture to the potential.
查看原文
分享 分享
微信好友 朋友圈 QQ好友 复制链接
本刊更多论文
通过具有机器学习潜力的分子动力学模拟了解固态氮
我们构建了一种适合大规模模拟 N2 的快速、可转移、通用的机器学习原子间势。该势垒仅根据高质量的量子化学分子-分子相互作用进行训练;未使用凝聚相信息。虽然没有显式或隐式多分子相互作用项,但该势能重现了实验相图,包括熔融曲线和高达 10GPa 的氮分子固相。这表明多分子相互作用在解释 N2 凝聚相时是不必要的。随着压力的增加,可以观察到从立方体(𝛼)到四方体(𝛾)的转变,立方体能优化四极-四极相互作用,四方体能更有效地堆积,而单斜体(𝜆)则能更有效地堆积。加热时,我们得到了 hcp 三维转子相(绊脚石),在压力作用下,得到了同时包含三维和二维转子的立方体𝛿 相、包含二维转子的四方体𝛿* 相以及斜方体𝜀 相。分子动力学证明了这些相确实是转子,而不是受挫阶。该模型支持复杂的𝜄相的可转移性,但不支持报告中存在的宽键长范围。热力学转变涉及分子中心的移动和分子的旋转:旋转的开始是快速的,而分子中心的运动则受到抑制,我们认为这是实验观察到的转变迟缓的原因。常规密度泛函理论计算也给出了与电位类似的结果。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 去求助
来源期刊
Physical Review B
Physical Review B 物理-物理:凝聚态物理
CiteScore
6.70
自引率
32.40%
发文量
0
审稿时长
3.0 months
期刊介绍: Physical Review B (PRB) is the world’s largest dedicated physics journal, publishing approximately 100 new, high-quality papers each week. The most highly cited journal in condensed matter physics, PRB provides outstanding depth and breadth of coverage, combined with unrivaled context and background for ongoing research by scientists worldwide. PRB covers the full range of condensed matter, materials physics, and related subfields, including: -Structure and phase transitions -Ferroelectrics and multiferroics -Disordered systems and alloys -Magnetism -Superconductivity -Electronic structure, photonics, and metamaterials -Semiconductors and mesoscopic systems -Surfaces, nanoscience, and two-dimensional materials -Topological states of matter
期刊最新文献
Interconnected skyrmions in a nanowire structure: Micromagnetic simulations Spin-deformation coupling in two-dimensional polar materials Superconductivity and strain-enhanced phase stability of Janus tungsten chalcogenide hydride monolayers Two-dimensional higher-order topological metals Absorption of electromagnetic waves in a screened two-dimensional electron system
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
已复制链接
已复制链接
快去分享给好友吧!
我知道了
×
扫码分享
扫码分享
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1