Strong Dependence of Point Defect Properties in Metal Halide Perovskites on Description of van der Waals Interaction
Weaker than ionic and covalent bonding, van der Waals (vdW) interactions can have a significant impact on structure and function of molecules and materials, including stabilities of conformers and phases, chemical reaction pathways, electro-optical response, electron-vibrational dynamics, etc. Metal...
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2024
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| _version_ | 1852026003061211137 |
|---|---|
| author | Linjie Deng (13169254) |
| author2 | Jingyi Ran (16438269) Bipeng Wang (7438559) Ariadni Boziki (8554941) Alexandre Tkatchenko (1283865) Jun Jiang (149215) Oleg V. Prezhdo (1235424) |
| author2_role | author author author author author author |
| author_facet | Linjie Deng (13169254) Jingyi Ran (16438269) Bipeng Wang (7438559) Ariadni Boziki (8554941) Alexandre Tkatchenko (1283865) Jun Jiang (149215) Oleg V. Prezhdo (1235424) |
| author_role | author |
| dc.creator.none.fl_str_mv | Linjie Deng (13169254) Jingyi Ran (16438269) Bipeng Wang (7438559) Ariadni Boziki (8554941) Alexandre Tkatchenko (1283865) Jun Jiang (149215) Oleg V. Prezhdo (1235424) |
| dc.date.none.fl_str_mv | 2024-10-11T14:40:15Z |
| dc.identifier.none.fl_str_mv | 10.1021/acs.jpclett.4c02390.s002 |
| dc.relation.none.fl_str_mv | https://figshare.com/articles/dataset/Strong_Dependence_of_Point_Defect_Properties_in_Metal_Halide_Perovskites_on_Description_of_van_der_Waals_Interaction/27212091 |
| dc.rights.none.fl_str_mv | CC BY-NC 4.0 info:eu-repo/semantics/openAccess |
| dc.subject.none.fl_str_mv | Biophysics Biochemistry Medicine Genetics Sociology Infectious Diseases Biological Sciences not elsewhere classified Chemical Sciences not elsewhere classified Physical Sciences not elsewhere classified van der waals midgap state energies metal halide perovskites high defect tolerance common br vacancy chemical reaction pathways excellent optoelectronic properties widely studied cspbbr soft mhp structure local geometric structure point defect properties primarily ionic compounds mhps depend significantly 3 </ sub optical properties widely investigated point defects vibrational coupling total energy strong dependence stemming largely significant impact optical response nl models interstitial defects including stabilities fundamental bandgap covalent bonding although mhps |
| dc.title.none.fl_str_mv | Strong Dependence of Point Defect Properties in Metal Halide Perovskites on Description of van der Waals Interaction |
| dc.type.none.fl_str_mv | Dataset info:eu-repo/semantics/publishedVersion dataset |
| description | Weaker than ionic and covalent bonding, van der Waals (vdW) interactions can have a significant impact on structure and function of molecules and materials, including stabilities of conformers and phases, chemical reaction pathways, electro-optical response, electron-vibrational dynamics, etc. Metal halide perovskites (MHPs) are widely investigated for their excellent optoelectronic properties, stemming largely from high defect tolerance. Although MHPs are primarily ionic compounds, we demonstrate that vdW interactions contribute ∼5% to the total energy, and that static, dynamics, electronic and optical properties of point defects in MHPs depend significantly on the vdW interaction model used. Focusing on widely studied CsPbBr<sub>3</sub> with the common Br vacancy and interstitial defects, we compare the PBE, PBE+D3, PBE+TS, PBE+TS/HI and PBE+MBD-NL models and show that vdW interactions strongly alter the global and local geometric structure, and change the fundamental bandgap, midgap state energies and electron-vibrational coupling. The vdW interaction sensitivity stems from involvement of heavy and highly polarizable chemical elements and the soft MHP structure. |
| eu_rights_str_mv | openAccess |
| id | Manara_575b08483c19fb9979ccf6923dae6f8a |
| identifier_str_mv | 10.1021/acs.jpclett.4c02390.s002 |
| network_acronym_str | Manara |
| network_name_str | ManaraRepo |
| oai_identifier_str | oai:figshare.com:article/27212091 |
| publishDate | 2024 |
| repository.mail.fl_str_mv | |
| repository.name.fl_str_mv | |
| repository_id_str | |
| rights_invalid_str_mv | CC BY-NC 4.0 |
| spelling | Strong Dependence of Point Defect Properties in Metal Halide Perovskites on Description of van der Waals InteractionLinjie Deng (13169254)Jingyi Ran (16438269)Bipeng Wang (7438559)Ariadni Boziki (8554941)Alexandre Tkatchenko (1283865)Jun Jiang (149215)Oleg V. Prezhdo (1235424)BiophysicsBiochemistryMedicineGeneticsSociologyInfectious DiseasesBiological Sciences not elsewhere classifiedChemical Sciences not elsewhere classifiedPhysical Sciences not elsewhere classifiedvan der waalsmidgap state energiesmetal halide perovskiteshigh defect tolerancecommon br vacancychemical reaction pathwaysexcellent optoelectronic propertieswidely studied cspbbrsoft mhp structurelocal geometric structurepoint defect propertiesprimarily ionic compoundsmhps depend significantly3 </ suboptical propertieswidely investigatedpoint defectsvibrational couplingtotal energystrong dependencestemming largelysignificant impactoptical responsenl modelsinterstitial defectsincluding stabilitiesfundamental bandgapcovalent bondingalthough mhpsWeaker than ionic and covalent bonding, van der Waals (vdW) interactions can have a significant impact on structure and function of molecules and materials, including stabilities of conformers and phases, chemical reaction pathways, electro-optical response, electron-vibrational dynamics, etc. Metal halide perovskites (MHPs) are widely investigated for their excellent optoelectronic properties, stemming largely from high defect tolerance. Although MHPs are primarily ionic compounds, we demonstrate that vdW interactions contribute ∼5% to the total energy, and that static, dynamics, electronic and optical properties of point defects in MHPs depend significantly on the vdW interaction model used. Focusing on widely studied CsPbBr<sub>3</sub> with the common Br vacancy and interstitial defects, we compare the PBE, PBE+D3, PBE+TS, PBE+TS/HI and PBE+MBD-NL models and show that vdW interactions strongly alter the global and local geometric structure, and change the fundamental bandgap, midgap state energies and electron-vibrational coupling. The vdW interaction sensitivity stems from involvement of heavy and highly polarizable chemical elements and the soft MHP structure.2024-10-11T14:40:15ZDatasetinfo:eu-repo/semantics/publishedVersiondataset10.1021/acs.jpclett.4c02390.s002https://figshare.com/articles/dataset/Strong_Dependence_of_Point_Defect_Properties_in_Metal_Halide_Perovskites_on_Description_of_van_der_Waals_Interaction/27212091CC BY-NC 4.0info:eu-repo/semantics/openAccessoai:figshare.com:article/272120912024-10-11T14:40:15Z |
| spellingShingle | Strong Dependence of Point Defect Properties in Metal Halide Perovskites on Description of van der Waals Interaction Linjie Deng (13169254) Biophysics Biochemistry Medicine Genetics Sociology Infectious Diseases Biological Sciences not elsewhere classified Chemical Sciences not elsewhere classified Physical Sciences not elsewhere classified van der waals midgap state energies metal halide perovskites high defect tolerance common br vacancy chemical reaction pathways excellent optoelectronic properties widely studied cspbbr soft mhp structure local geometric structure point defect properties primarily ionic compounds mhps depend significantly 3 </ sub optical properties widely investigated point defects vibrational coupling total energy strong dependence stemming largely significant impact optical response nl models interstitial defects including stabilities fundamental bandgap covalent bonding although mhps |
| status_str | publishedVersion |
| title | Strong Dependence of Point Defect Properties in Metal Halide Perovskites on Description of van der Waals Interaction |
| title_full | Strong Dependence of Point Defect Properties in Metal Halide Perovskites on Description of van der Waals Interaction |
| title_fullStr | Strong Dependence of Point Defect Properties in Metal Halide Perovskites on Description of van der Waals Interaction |
| title_full_unstemmed | Strong Dependence of Point Defect Properties in Metal Halide Perovskites on Description of van der Waals Interaction |
| title_short | Strong Dependence of Point Defect Properties in Metal Halide Perovskites on Description of van der Waals Interaction |
| title_sort | Strong Dependence of Point Defect Properties in Metal Halide Perovskites on Description of van der Waals Interaction |
| topic | Biophysics Biochemistry Medicine Genetics Sociology Infectious Diseases Biological Sciences not elsewhere classified Chemical Sciences not elsewhere classified Physical Sciences not elsewhere classified van der waals midgap state energies metal halide perovskites high defect tolerance common br vacancy chemical reaction pathways excellent optoelectronic properties widely studied cspbbr soft mhp structure local geometric structure point defect properties primarily ionic compounds mhps depend significantly 3 </ sub optical properties widely investigated point defects vibrational coupling total energy strong dependence stemming largely significant impact optical response nl models interstitial defects including stabilities fundamental bandgap covalent bonding although mhps |