Synthesis of Paracrystalline Diamond

Synthesis of Paracrystalline Diamond | 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 Physical Sciences - Article Synthesis of Paracrystalline Diamond Howard Sheng, Hu Tang, Xiaohong Yuan, Yong Cheng, Hongzhan Fei, and 7 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-438542/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 24 Nov, 2021 Read the published version in Nature → Version 1 posted You are reading this latest preprint version Abstract Solids in nature can be generally classified into crystalline and non-crystalline states, depending on whether long-range lattice periodicity is present in the material. The differentiation of the two states, however, could face fundamental challenges if the degree of long-range order in crystals is significantly reduced. Here we report a unique paracrystalline state of diamond that is distinct from either crystalline or amorphous diamond. The paracrystalline diamond reported in this work, consisting of sub-nanometer-sized paracrystals that possess a well-defined crystalline medium-range order up to a few atomic shells, was synthesized in high-pressure high-temperature conditions (e.g., 30 GPa, 1600 K) employing fcc-C60 as a precursor. The structural characteristics of paracrystalline diamond was identified through a combination of X-ray diffraction, high-resolution transmission microscopy, and advanced molecular dynamics simulation. The formation of paracrystalline diamond is a result of densely distributed nucleation sites developed in compressed C60 as well as pronounced second-nearest-neighbor short-range order in amorphous diamond due to strong sp3 bonding. The discovery of paracrystalline diamond adds a new diamond form to the enriched carbon family, which exhibits distinguishing physical properties and can be furthered exploited to develop new materials. Furthermore, this work reveals the missing link in the length-scale between amorphous and crystalline states across the structural landscape, which has profound implications for recognizing complex structures arising from amorphous materials. Computational Physics Hard Condensed-matter Physics Soft Condensed-matter Physics paracrystalline diamond amorphous materials solids Figures Figure 1 Figure 2 Figure 3 Figure 4 Full Text Due to technical limitations, full-text HTML conversion of this manuscript could not be completed. However, the manuscript can be downloaded and accessed as a PDF. Additional Declarations There is NO Competing Interest. Supplementary Files SI202104019.docx Supplementary Note ExtendedDataFigures202104019.docx Extended Data Figures 1-13 GrowingMROwithannealingtimeat1600K30GPa.mp4 Supplementary Video Cite Share Download PDF Status: Published Journal Publication published 24 Nov, 2021 Read the published version in Nature → Version 1 posted 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. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. 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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-438542","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Physical Sciences - Article","associatedPublications":[],"authors":[{"id":25437487,"identity":"342e2a9c-abbe-4b08-b722-89c989372a62","order_by":0,"name":"Howard 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University","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Mingsheng","middleName":"","lastName":"Wang","suffix":""},{"id":25437497,"identity":"624ac3bb-7029-4bc8-9485-f4e244a48f16","order_by":10,"name":"Tomoo Katsura","email":"","orcid":"","institution":"University of Bayreuth","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Tomoo","middleName":"","lastName":"Katsura","suffix":""},{"id":25437498,"identity":"21555e4b-44b6-456d-85d6-59ffd731bce0","order_by":11,"name":"Huiyang Gou","email":"","orcid":"","institution":"Center for High Pressure Science and Technology Advanced Research","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Huiyang","middleName":"","lastName":"Gou","suffix":""}],"badges":[],"createdAt":"2021-04-19 00:35:41","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-438542/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-438542/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1038/s41586-021-04122-w","type":"published","date":"2021-11-24T05:00:00+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":8931596,"identity":"c239cea4-c4ca-4c31-9d6f-af33b3ad700a","added_by":"auto","created_at":"2021-05-07 19:19:42","extension":"jpg","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":72096,"visible":true,"origin":"","legend":"Synthesizing fully sp3-bonded carbon samples at 30 GPa and 1200–1600 K for 10 min. a, XRD patterns indicate direct synthesis of disordered carbon from C60 under 30 GPa. With increasing temperature, the first main diffraction peak shifts from 2.89 to 2.95 Å-1, suggesting an increased density at higher temperatures. Inset: a typic optical photograph of the transparent bulk sample (~1 mm in diameter) obtained at 30 GPa and 1600 K. b, XRD pattern of the C60 precursor (Fm\"3\" ̅m). Inset: Corresponding HRTEM image and selected area electron diffraction (SAED) pattern. c, Visible Raman (Wavelength of 532 nm) spectra of samples recovered from different temperatures. The samples annealed at 1200 K and 1400 K have similar Raman features with the DLC films having a high sp3 fraction27, suggesting a trace amount of sp2 carbon remaining in these samples. d, EELS spectra of samples recovered from different temperatures and cubic diamond crystal. The features at 285 and 292 eV are due to transitions of 1s electron to π* and σ*, corresponding to sp2 and sp3 bonding, respectively. The 1400 K sample has a residual 5.2% of sp2 bonding, analyzed from the ratio of π* and σ* features using single-crystal graphite for calibration28.","description":"","filename":"1.jpg","url":"https://assets-eu.researchsquare.com/files/rs-438542/v1/bdc748468e92ea33a2f03395.jpg"},{"id":8931865,"identity":"1f1b9cc3-6ee2-4505-84cf-9198da47aad9","added_by":"auto","created_at":"2021-05-07 19:22:43","extension":"jpg","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":123709,"visible":true,"origin":"","legend":"TEM characterization of samples recovered from 30 GPa and 1200-1600 K. a-b, c-d, and e-f, Typical HRTEM images of samples and the corresponding inverse FFT images, respectively. Insets: FFT patterns corresponding to the white boxes (7.0 × 7.0 nm2) in (a), (c), and (e), respectively. The cyan and red circles in (d and f) indicate crystal-like MRO clusters. Note that the circles only serve as a guide for the eye. MRO clusters are discernable in (f), where the lattice fringes marked by the cyan and red solid lines match CD- and HD-like (111) and (100) crystal planes, respectively. g-h, FFT patterns, corresponding to the red and cyan boxes (2.0 × 2.0 nm2) in (f), respectively. The brighter spots on the diffuse halos indicated by the colored arrows confirm the existence of CD and HD-like MRO clusters illustrated in (f). ","description":"","filename":"2.jpg","url":"https://assets-eu.researchsquare.com/files/rs-438542/v1/a4d199c6285d07c692bb26e3.jpg"},{"id":8931296,"identity":"204bd67c-6fdd-45ea-9ef2-51989d56acc3","added_by":"auto","created_at":"2021-05-07 19:16:43","extension":"jpg","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":113365,"visible":true,"origin":"","legend":"Identification of p-D. a, Simulated structure factor S(Q) of a-D and p-D (f = 70%). b, Top: Experimental S(Q) of the recovered samples. Bottom: Simulated S(Q) of p-D with 50% paracrystals in comparison to the experimental data. c, Intensity ratio of the first peak (~2.9 Å-1) to the second peak (~5.4 Å-1) as a function of volume percentage of paracrystals. d, Structural model of p-D with 70% paracrystals from MD simulation. Colors represent different types of atomic packing. Based on CNA analysis, the turquoise, gold, and red atoms represent CD-, HD-like, and disordered atomic packing within two atomic shells, respectively. The typical size and atomic arrangement of the paracrystals are illustrated in the circles on the left. e, Simulated HRTEM image from the paracrystalline model presented in (d). The cyan and yellow circles indicate CD and HD-like clusters, respectively, in agreement with the experimental HRTEM image shown in Fig. 2f.","description":"","filename":"3.jpg","url":"https://assets-eu.researchsquare.com/files/rs-438542/v1/e9aabba3e52db65f0c07e06a.jpg"},{"id":8931597,"identity":"f9be5272-e5e1-4f8a-aac2-704abcd82019","added_by":"auto","created_at":"2021-05-07 19:19:43","extension":"jpg","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":166741,"visible":true,"origin":"","legend":"Distinguishing p-D from a-D. a, Atomic structure of p-D vs. a-D, visualized based on their respective degree of MRO represented by the CNA index and orientational order parameter . For a-D, the images present monotonous colors (red and blue), indicating the absence of crystal-like MRO clusters. In contrast, high-fraction MRO CD and HD-like clusters populate and become the main feature in p-D. b, The radial distribution function (top) and orientational correlation function (bottom) of p-D and a-D, respectively.","description":"","filename":"4.jpg","url":"https://assets-eu.researchsquare.com/files/rs-438542/v1/c2e0fdb7673022e0b5924320.jpg"},{"id":15886802,"identity":"b13114e7-e385-4830-9bb8-a937c7681a40","added_by":"auto","created_at":"2021-11-25 08:07:21","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":1540236,"visible":true,"origin":"","legend":"","description":"","filename":"Paracrystallinediamond20210419.pdf","url":"https://assets-eu.researchsquare.com/files/rs-438542/v1_covered.pdf"},{"id":13629361,"identity":"c90afe77-a1be-4d90-9502-8ea7a2b21f04","added_by":"auto","created_at":"2021-09-17 08:05:49","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":1535142,"visible":true,"origin":"","legend":"","description":"","filename":"Paracrystallinediamond20210419.pdf","url":"https://assets-eu.researchsquare.com/files/rs-438542/v1_covered.pdf"},{"id":8932196,"identity":"e122dd7f-adc2-40ce-8038-71dc09f5447b","added_by":"auto","created_at":"2021-05-07 19:25:49","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":1329263,"visible":true,"origin":"","legend":"","description":"","filename":"Paracrystallinediamond20210419.pdf","url":"https://assets-eu.researchsquare.com/files/rs-438542/v1_stamped.pdf"},{"id":8931599,"identity":"c785165f-47bd-4971-9b17-a470e7874193","added_by":"auto","created_at":"2021-05-07 19:19:43","extension":"docx","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":21837,"visible":true,"origin":"","legend":"Supplementary Note","description":"","filename":"SI202104019.docx","url":"https://assets-eu.researchsquare.com/files/rs-438542/v1/ca4b6c6de3d005f71e5d0db7.docx"},{"id":8931600,"identity":"1495985d-eb6d-4bb7-bbdd-b36725877aaa","added_by":"auto","created_at":"2021-05-07 19:19:43","extension":"docx","order_by":2,"title":"","display":"","copyAsset":false,"role":"supplement","size":10016409,"visible":true,"origin":"","legend":"Extended Data Figures 1-13","description":"","filename":"ExtendedDataFigures202104019.docx","url":"https://assets-eu.researchsquare.com/files/rs-438542/v1/3d315556d25d3bd1f03be01c.docx"},{"id":8931866,"identity":"3e6da8d4-547b-4b0a-b518-230aaaf0f8f2","added_by":"auto","created_at":"2021-05-07 19:22:43","extension":"mp4","order_by":3,"title":"","display":"","copyAsset":false,"role":"supplement","size":7625145,"visible":true,"origin":"","legend":"Supplementary Video","description":"","filename":"GrowingMROwithannealingtimeat1600K30GPa.mp4","url":"https://assets-eu.researchsquare.com/files/rs-438542/v1/8024d27428df51a60bdc1b32.mp4"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Synthesis of Paracrystalline Diamond","fulltext":[{"header":"Full Text","content":"\u003cp\u003eDue to technical limitations, full-text HTML conversion of this manuscript could not be completed. However, the manuscript can be downloaded and accessed as a PDF.\u003c/p\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":false,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":true,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"nature-portfolio","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"","title":"Nature Portfolio","twitterHandle":"","acdcEnabled":false,"dfaEnabled":false,"editorialSystem":"ejp","reportingPortfolio":"","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"paracrystalline diamond, amorphous materials, solids","lastPublishedDoi":"10.21203/rs.3.rs-438542/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-438542/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"Solids in nature can be generally classified into crystalline and non-crystalline states, depending on whether long-range lattice periodicity is present in the material. The differentiation of the two states, however, could face fundamental challenges if the degree of long-range order in crystals is significantly reduced. Here we report a unique paracrystalline state of diamond that is distinct from either crystalline or amorphous diamond. The paracrystalline diamond reported in this work, consisting of sub-nanometer-sized paracrystals that possess a well-defined crystalline medium-range order up to a few atomic shells, was synthesized in high-pressure high-temperature conditions (e.g., 30 GPa, 1600 K) employing fcc-C60 as a precursor. The structural characteristics of paracrystalline diamond was identified through a combination of X-ray diffraction, high-resolution transmission microscopy, and advanced molecular dynamics simulation. The formation of paracrystalline diamond is a result of densely distributed nucleation sites developed in compressed C60 as well as pronounced second-nearest-neighbor short-range order in amorphous diamond due to strong sp3 bonding. The discovery of paracrystalline diamond adds a new diamond form to the enriched carbon family, which exhibits distinguishing physical properties and can be furthered exploited to develop new materials. Furthermore, this work reveals the missing link in the length-scale between amorphous and crystalline states across the structural landscape, which has profound implications for recognizing complex structures arising from amorphous materials.","manuscriptTitle":"Synthesis of Paracrystalline Diamond","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2021-05-07 19:16:40","doi":"10.21203/rs.3.rs-438542/v1","editorialEvents":[],"status":"published","journal":{"display":false,"email":"[email protected]","identity":"nature","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"nature","sideBox":"Learn more about [Nature](http://www.nature.com/nature/)","snPcode":"","submissionUrl":"","title":"Nature","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"ejp","reportingPortfolio":"Nature","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"8b706918-d341-4e98-a56f-3401fd9de50a","owner":[],"postedDate":"May 7th, 2021","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[{"id":4169779,"name":"Computational Physics"},{"id":4169780,"name":"Hard Condensed-matter Physics"},{"id":4169781,"name":"Soft Condensed-matter Physics"}],"tags":[],"updatedAt":"2021-11-25T08:07:13+00:00","versionOfRecord":{"articleIdentity":"rs-438542","link":"https://doi.org/10.1038/s41586-021-04122-w","journal":{"identity":"nature","isVorOnly":false,"title":"Nature"},"publishedOn":"2021-11-24 05:00:00","publishedOnDateReadable":"November 24th, 2021"},"versionCreatedAt":"2021-05-07 19:16:40","video":"","vorDoi":"10.1038/s41586-021-04122-w","vorDoiUrl":"https://doi.org/10.1038/s41586-021-04122-w","workflowStages":[]},"version":"v1","identity":"rs-438542","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-438542","identity":"rs-438542","version":["v1"]},"buildId":"rHA-KDH7Qsr4HCuvH75dn","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}