First-principles Investigation of Optoelectronic Structure and Thermodynamic Properties of Ruddlesden-Popper halide perovskites for optoelectronic applications

First-principles Investigation of Optoelectronic Structure and Thermodynamic Properties of Ruddlesden-Popper halide perovskites for optoelectronic applications | 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 Research Article First-principles Investigation of Optoelectronic Structure and Thermodynamic Properties of Ruddlesden-Popper halide perovskites for optoelectronic applications Izaz Ul Haq, A. Abdelkader, Yahia A. H. Obaidat, Refka Ghodhbani, and 2 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-4658606/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 21 Aug, 2024 Read the published version in Journal of Inorganic and Organometallic Polymers and Materials → Version 1 posted 10 You are reading this latest preprint version Abstract The structure optimization, nuclear magnetic resonance (NMR) shielding, optoelectronic and thermodynamic properties of 2D layered Ruddlesden-Popper Cs 2 CdX 4 (X = Cl, Br, I) are computed using first-principles simulations. The crystal structure is composed of 2D [CdX 4 ] n 2n− plane constructed by CdX 6 octahedral vertices and inorganic spacer cation (Cs + ) separates the octahedral layers. At the VB edge, X-p and Cd-p orbitals are strongly hybridized, which play a key role in the optoelectronic applications of these compounds owing to the excitation of their valence electrons to the conduction band (CB) with minimum photon’s energy. The pseudo-direct and tunable band gaps of the understudy 2D layered RP-HPs are well-suited for optoelectronic applications. The numerical values of Debye temperature illustrates that each compound excites with different Debye frequency, corresponds to the unit cell size and phonon’s wavelength. The specific heat capacity curves are consistent with equipartition theorem of classical mechanics and obey the Dulong-Petit law at high temperature. The positive entropy change (ΔS) spirits negative change in Gibb’s free energy (ΔG), confirming the stability of these materials. The isotropic chemical shift depends on Cd and halides coordinates therefore, Cd-δ iso is decreases and X-δ iso increases with the halide increments. The Cs-p, Cd-d, and X-s orbital play a key role in NMR shielding owing to their existence in lower valence band (VB). First principles calculation Ruddlesden-Popper phase Optoelectronics Specific heat capacity Thermal entropy Debye Model NMR shielding Full Text Additional Declarations No competing interests reported. Cite Share Download PDF Status: Published Journal Publication published 21 Aug, 2024 Read the published version in Journal of Inorganic and Organometallic Polymers and Materials → Version 1 posted Editorial decision: Revision requested 25 Jul, 2024 Reviews received at journal 11 Jul, 2024 Reviews received at journal 09 Jul, 2024 Reviewers agreed at journal 01 Jul, 2024 Reviewers agreed at journal 01 Jul, 2024 Reviewers agreed at journal 01 Jul, 2024 Reviewers invited by journal 01 Jul, 2024 Editor assigned by journal 01 Jul, 2024 Submission checks completed at journal 01 Jul, 2024 First submitted to journal 29 Jun, 2024 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. 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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-4658606","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":325872176,"identity":"c13a90bf-cc02-424a-beee-75af77d758ae","order_by":0,"name":"Izaz Ul Haq","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAuklEQVRIiWNgGAWjYBACNigtByIOPCBFizFYSwIptiU2gEiitPDxH378madiW/r8sMMPgbbYyek2EHTYMQNjnjO3czfeTjMAakk2NjtASAtjg0EybxtQy+wEkJYDidsIamFm/3AYqCXdcHb6ByK1sPEYNgO1JMhL5xBrCw9PMeOcM7cNN0jnFBxIMCDCL/L9xzd/eFNxW15+dvrmDx8q7OQIaoEDA7BKA2KVg61rIEX1KBgFo2AUjCgAAKdFQvIF0sFpAAAAAElFTkSuQmCC","orcid":"","institution":"University of Malakand","correspondingAuthor":true,"prefix":"","firstName":"Izaz","middleName":"Ul","lastName":"Haq","suffix":""},{"id":325872177,"identity":"4d8fada0-3c23-4a54-a748-f9c4fa04afd5","order_by":1,"name":"A. 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Haj Ismail","email":"","orcid":"","institution":"Ajman University","correspondingAuthor":false,"prefix":"","firstName":"A.","middleName":"Haj","lastName":"Ismail","suffix":""},{"id":325872181,"identity":"b0d37a0f-a620-49ba-8d09-2029a25ff4a4","order_by":5,"name":"Imad Khan","email":"","orcid":"","institution":"University of Malakand","correspondingAuthor":false,"prefix":"","firstName":"Imad","middleName":"","lastName":"Khan","suffix":""}],"badges":[],"createdAt":"2024-06-29 09:26:44","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-4658606/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-4658606/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1007/s10904-024-03338-3","type":"published","date":"2024-08-21T15:57:24+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":63300167,"identity":"1005bd2a-ab12-4bb8-81a0-3e194542fd0a","added_by":"auto","created_at":"2024-08-26 16:12:09","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":2867826,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-4658606/v1_covered_39e92b1b-76a2-4d0d-95e9-19e147ec67aa.pdf"}],"financialInterests":"No competing interests reported.","formattedTitle":"First-principles Investigation of Optoelectronic Structure and Thermodynamic Properties of Ruddlesden-Popper halide perovskites for optoelectronic applications","fulltext":[],"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":true,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"journal-of-inorganic-and-organometallic-polymers-and-materials","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"joip","sideBox":"Learn more about [Journal of Inorganic and Organometallic Polymers and Materials](https://www.springer.com/journal/10904)","snPcode":"10904","submissionUrl":"https://submission.nature.com/new-submission/10904/3","title":"Journal of Inorganic and Organometallic Polymers and Materials","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"First principles calculation, Ruddlesden-Popper phase, Optoelectronics, Specific heat capacity, Thermal entropy, Debye Model, NMR shielding","lastPublishedDoi":"10.21203/rs.3.rs-4658606/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-4658606/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eThe structure optimization, nuclear magnetic resonance (NMR) shielding, optoelectronic and thermodynamic properties of 2D layered Ruddlesden-Popper Cs\u003csub\u003e2\u003c/sub\u003eCdX\u003csub\u003e4\u003c/sub\u003e (X = Cl, Br, I) are computed using first-principles simulations. The crystal structure is composed of 2D [CdX\u003csub\u003e4\u003c/sub\u003e]\u003csub\u003en\u003c/sub\u003e\u003csup\u003e2n−\u003c/sup\u003e plane constructed by CdX\u003csub\u003e6\u003c/sub\u003e octahedral vertices and inorganic spacer cation (Cs\u003csup\u003e+\u003c/sup\u003e) separates the octahedral layers. At the VB edge, X-p and Cd-p orbitals are strongly hybridized, which play a key role in the optoelectronic applications of these compounds owing to the excitation of their valence electrons to the conduction band (CB) with minimum photon’s energy. The pseudo-direct and tunable band gaps of the understudy 2D layered RP-HPs are well-suited for optoelectronic applications. The numerical values of Debye temperature illustrates that each compound excites with different Debye frequency, corresponds to the unit cell size and phonon’s wavelength. The specific heat capacity curves are consistent with equipartition theorem of classical mechanics and obey the Dulong-Petit law at high temperature. The positive entropy change (ΔS) spirits negative change in Gibb’s free energy (ΔG), confirming the stability of these materials. The isotropic chemical shift depends on Cd and halides coordinates therefore, Cd-δ\u003csub\u003eiso\u003c/sub\u003e is decreases and X-δ\u003csub\u003eiso\u003c/sub\u003e increases with the halide increments. The Cs-p, Cd-d, and X-s orbital play a key role in NMR shielding owing to their existence in lower valence band (VB).\u003c/p\u003e","manuscriptTitle":"First-principles Investigation of Optoelectronic Structure and Thermodynamic Properties of Ruddlesden-Popper halide perovskites for optoelectronic applications","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2024-07-23 05:04:12","doi":"10.21203/rs.3.rs-4658606/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"decision","content":"Revision requested","date":"2024-07-26T01:28:01+00:00","index":"","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2024-07-11T22:02:25+00:00","index":"hide","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2024-07-09T17:27:01+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"79247954615013293536383685815257310633","date":"2024-07-02T02:27:58+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"7880263386713329638465199302277667878","date":"2024-07-01T17:09:07+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"325738012126106324980952623502578994396","date":"2024-07-01T14:58:14+00:00","index":"hide","fulltext":""},{"type":"reviewersInvited","content":"","date":"2024-07-01T13:33:54+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2024-07-01T07:44:09+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2024-07-01T07:03:56+00:00","index":"","fulltext":""},{"type":"submitted","content":"Journal of Inorganic and Organometallic Polymers and Materials","date":"2024-06-29T09:25:20+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"journal-of-inorganic-and-organometallic-polymers-and-materials","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"joip","sideBox":"Learn more about [Journal of Inorganic and Organometallic Polymers and Materials](https://www.springer.com/journal/10904)","snPcode":"10904","submissionUrl":"https://submission.nature.com/new-submission/10904/3","title":"Journal of Inorganic and Organometallic Polymers and Materials","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"cd085014-ab32-45ab-a83e-74de0ae2663f","owner":[],"postedDate":"July 23rd, 2024","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[],"tags":[],"updatedAt":"2024-08-26T16:01:56+00:00","versionOfRecord":{"articleIdentity":"rs-4658606","link":"https://doi.org/10.1007/s10904-024-03338-3","journal":{"identity":"journal-of-inorganic-and-organometallic-polymers-and-materials","isVorOnly":false,"title":"Journal of Inorganic and Organometallic Polymers and Materials"},"publishedOn":"2024-08-21 15:57:24","publishedOnDateReadable":"August 21st, 2024"},"versionCreatedAt":"2024-07-23 05:04:12","video":"","vorDoi":"10.1007/s10904-024-03338-3","vorDoiUrl":"https://doi.org/10.1007/s10904-024-03338-3","workflowStages":[]},"version":"v1","identity":"rs-4658606","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-4658606","identity":"rs-4658606","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}