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Ukungasebenzi kahle kwe-defect passivation kuye kwasetshenziswa kabanzi ukuthuthukisa ukusebenza kwamaseli elanga e-lead triiodide perovskite, kodwa umphumela wamaphutha ahlukahlukene ekuzinzeni kwe-α-phase awucaci; Lapha, sisebenzisa ithiyori yokusebenza kobuningi, sithola okokuqala indlela yokuwohloka kwe-formamimidine lead triiodide perovskite kusuka ku-α-phase kuya ku-δ-phase futhi sifunde umphumela wamaphutha ahlukahlukene ku-phase transition energy barrier. Imiphumela yokulingisa ibikezela ukuthi izikhala ze-iodine cishe zingabangela ukuwohloka ngoba zehlisa kakhulu isithiyo samandla sokuguqulwa kwesigaba se-α-δ futhi zinamandla okwakheka aphansi kakhulu ebusweni be-perovskite. Ukwethulwa kwengqimba ebanzi ye-lead oxalate enganyibiliki emanzini ebusweni be-perovskite kuvimbela kakhulu ukuwohloka kwesigaba se-α, kuvimbele ukufuduka kanye nokuguquguquka kwe-iodine. Ngaphezu kwalokho, leli cebo linciphisa kakhulu ukuhlanganiswa kwe-interfacial nonradiative futhi landisa ukusebenza kahle kwamaseli elanga ku-25.39% (kuqinisekiswe ngo-24.92%). Idivayisi engapakishiwe isengagcina ukusebenza kwayo kwasekuqaleni okungu-92% ngemuva kokusebenza ngamandla aphezulu amahora angu-550 ngaphansi kokukhanya komoya okungu-1.5 G okulingisiwe.
Ukusebenza kahle kokuguqulwa kwamandla (i-PCE) kwamaseli elanga e-perovskite (ama-PSC) kufinyelele irekhodi eliphakeme eliqinisekisiwe elingu-26%1. Kusukela ngo-2015, ama-PSC anamuhla akhethe i-formamidinine triiodide perovskite (FAPbI3) njengesendlalelo esimunca ukukhanya ngenxa yokuqina kwayo okuhle kokushisa kanye ne-bandgap ekhethwayo eduze komkhawulo we-Shockley-Keisser ongu-2,3,4. Ngeshwa, amafilimu e-FAPbI3 adlula ngokushintsha kwesigaba kusuka esigabeni se-α esimnyama kuya esigabeni se-δ esiphuzi esingeyona i-perovskite ekushiseni kwegumbi5,6. Ukuvimbela ukwakheka kwesigaba se-delta, kuye kwasungulwa ukwakheka okuhlukahlukene okuyinkimbinkimbi kwe-perovskite. Isu elivame kakhulu lokunqoba le nkinga ukuxuba i-FAPbI3 nenhlanganisela ye-methyl ammonium (MA+), i-cesium (Cs+) kanye ne-bromide (Br-) ions7,8,9. Kodwa-ke, ama-perovskite axubile ahlushwa ukwanda kwe-bandgap kanye nokuhlukaniswa kwesigaba esibangelwa yi-photoinduced, okuphazamisa ukusebenza kanye nokuzinza kokusebenza kwama-PSC10,11,12 aphumayo.
Izifundo zamuva nje zibonise ukuthi i-FAPbI3 emsulwa emsulwa ngaphandle kokusebenzisa i-doping inokuqina okuhle kakhulu ngenxa yobukristalu bayo obuhle kakhulu kanye namaphutha aphansi13,14. Ngakho-ke, ukunciphisa amaphutha ngokwandisa ubukristalu be-FAPbI3 eningi kuyisu elibalulekile lokufeza ama-PSC2,15 asebenzayo futhi azinzile. Kodwa-ke, ngesikhathi sokusebenza kwe-FAPbI3 PSC, ukuwohloka kwesigaba se-δ esiphuzi esingenanxantathu esingafuneki kusengaqhubeka nokwenzeka16. Inqubo ivame ukuqala ezindaweni kanye nemingcele yokusanhlamvu esengozini enkulu yamanzi, ukushisa nokukhanya ngenxa yokuba khona kwezindawo eziningi ezinephutha17. Ngakho-ke, ukuphambuka kobuso/kokusanhlamvu kuyadingeka ukuze kuzinziswe isigaba esimnyama se-FAPbI318. Amasu amaningi okuphambuka kwamaphutha, okuhlanganisa nokwethulwa kwama-perovskites aphansi, ama-molecule e-Lewis ane-acid-base, kanye nosawoti we-ammonium halide, enze intuthuko enkulu kuma-PSC e-formamimidine19,20,21,22. Kuze kube manje, cishe zonke izifundo zigxile endimeni yamaphutha ahlukahlukene ekunqumeni izakhiwo ze-optoelectronic ezifana nokuhlanganiswa kwe-carrier, ubude bokusabalalisa kanye nesakhiwo sebhendi kumaseli elanga22,23,24. Isibonelo, i-density functional theory (DFT) isetshenziselwa ukubikezela ngokomqondo amandla okwakheka kanye namazinga wamandla okubamba amaphutha ahlukahlukene, okusetshenziswa kabanzi ukuqondisa ukwakheka kwe-passivation okusebenzayo20,25,26. Njengoba inani lamaphutha lehla, ukuzinza kwedivayisi kuvame ukuthuthuka. Kodwa-ke, kuma-PSC e-formamimidine, izindlela zethonya lamaphutha ahlukahlukene ekuzinzeni kwesigaba kanye nezakhiwo ze-photoelectric kufanele zihluke ngokuphelele. Ngokwazi kwethu okuhle, ukuqonda okuyisisekelo kokuthi amaphutha abangela kanjani ukuguquka kwesigaba se-cubic kuya ku-hexagonal (α-δ) kanye nendima ye-passivation ebusweni ekuzinzeni kwesigaba se-α-FAPbI3 perovskite kusaqondwa kahle.
Lapha, sembula indlela yokuwohloka kwe-FAPbI3 perovskite kusuka ku-α-phase emnyama kuya ku-δ-phase ephuzi kanye nomthelela weziphambeko ezahlukahlukene kusithiyo samandla sokushintsha kwe-α-to-δ-phase nge-DFT. Izikhala ze-I, ezikhiqizwa kalula ngesikhathi sokwenziwa kwefilimu nokusebenza kwedivayisi, kubikezelwa ukuthi zizoqala ushintsho lwesigaba se-α-δ. Ngakho-ke, sethule ungqimba oluqinile lwe-lead oxalate (PbC2O4) olungancibiliki emanzini futhi oluzinzile ngamakhemikhali phezu kwe-FAPbI3 ngokusebenzisa ukusabela kwe-in situ. I-lead oxalate surface (LOS) ivimbela ukwakheka kwezikhala ze-I futhi ivimbele ukufuduka kwama-ion e-I lapho ivuselelwa ukushisa, ukukhanya, kanye nezinkundla zikagesi. I-LOS ephumelayo inciphisa kakhulu i-interfacial nonradiative recombination futhi ithuthukisa ukusebenza kahle kwe-FAPbI3 PSC ku-25.39% (okuqinisekiswe ku-24.92%). Idivayisi ye-LOS engapakishwanga igcine u-92% wokusebenza kwayo kwasekuqaleni ngemuva kokusebenza endaweni yamandla ephezulu (i-MPP) amahora angaphezu kwangu-550 ngesisindo somoya esilingisiwe (i-AM) esingu-1.5 G semisebe.
Okokuqala senze izibalo ze-ab initio ukuthola indlela yokubola kwe-perovskite ye-FAPbI3 ukuya ekuguqukeni kusuka esigabeni se-α ukuya esigabeni se-δ. Ngenqubo yokuguqulwa kwesigaba eningiliziwe, kutholakale ukuthi ukuguqulwa kusuka ku-octahedron yokwabelana ngamakhona amathathu [PbI6] esigabeni se-cubic α se-FAPbI3 kuya ku-octahedron yokwabelana ngamaphethelo eyodwa [PbI6] esigabeni se-hexagonal δ se-FAPbI3 kufezwa. kuphula u-9. I-Pb-I yakha isibopho esinyathelweni sokuqala (Int-1), futhi isithiyo sayo samandla sifinyelela ku-0.62 eV/iseli, njengoba kuboniswe kuMfanekiso 1a. Lapho i-octahedron ishintshwa ohlangothini lwe-[0\(\bar{1}\)1], uchungechunge olufushane lwe-hexagonal luyanda kusuka ku-1×1 kuya ku-1×3, 1×4 futhi ekugcineni lungena esigabeni se-δ. Isilinganiso sokuqondiswa kwendlela yonke siyi-(011)α//(001)δ + [100]α//[100]δ. Kusukela kumdwebo wokusabalalisa amandla, kungatholakala ukuthi ngemva kokwakheka kwesigaba se-δ se-FAPbI3 ezigabeni ezilandelayo, isithiyo samandla siphansi kunesoshintsho lwesigaba se-α, okusho ukuthi ushintsho lwesigaba luzosheshiswa. Ngokusobala, isinyathelo sokuqala sokulawula ushintsho lwesigaba sibalulekile uma sifuna ukucindezela ukuwohloka kwesigaba se-α.
Inqubo yokuguqulwa kwesigaba kusukela kwesobunxele kuya kwesokudla – isigaba esimnyama se-FAPbI3 (isigaba se-α), ukuhlukana kwesibopho sokuqala se-Pb-I (Int-1) kanye nokuhlukana kwesibopho se-Pb-I okuqhubekayo (Int-2, Int -3 kanye ne-Int -4) kanye nesigaba esiphuzi se-FAPbI3 (isigaba se-delta). b Izithiyo zamandla ekuguqukeni kwesigaba se-α kuya ku-δ se-FAPbI3 ngokusekelwe ezicini ezahlukahlukene zamaphuzu angaphakathi. Umugqa onamachashazi ukhombisa isithiyo samandla sekristalu elifanele (0.62 eV). c Amandla okwakheka kwezici eziyinhloko zamaphuzu ebusweni be-lead perovskite. I-abscissa axis iyisithiyo samandla sokuguquka kwesigaba se-α-δ, kanti i-axis eqondisiwe ingamandla okwakheka kwezici. Izingxenye ezifakwe umbala ompunga, ophuzi noluhlaza ziyi-type I (low EB-high FE), uhlobo II (high FE) kanye nohlobo III (low EB-low FE), ngokulandelana. d Amandla okwakheka kwezici VI kanye ne-LOS ye-FAPbI3 ekulawuleni. Isithiyo se-e I sokufuduka kwama-ion ekulawuleni kanye ne-LOS ye-FAPbI3. f – ukumelwa kwesithombe sokufuduka kwama-ion e-I (izimbulunga eziwolintshi) kanye ne-gLOS FAPbI3 (grey, lead; violet (orenji), i-iodine (i-iodine yeselula)) ekulawuleni kwe-gf (kwesobunxele: umbono ophezulu; kwesokudla: isigaba esiphambeneyo, onsundu); ikhabhoni; okuluhlaza okwesibhakabhaka okukhanyayo – i-nitrogen; obomvu – i-oxygen; okupinki okukhanyayo – i-hydrogen). Idatha yomthombo inikezwa ngesimo samafayela edatha yomthombo.
Sabe sesifunda ngokuhlelekile ithonya lamaphutha ahlukahlukene angaphakathi (kufaka phakathi i-PbFA, i-IFA, i-PbI, kanye ne-IPb antisite occupies; ama-athomu angaphakathi e-Pbi kanye ne-Ii; kanye nezikhala ze-VI, i-VFA, kanye ne-VPb), ezibhekwa njengezici ezibalulekile. ezibangela ukuwohloka kwesigaba se-athomu kanye nezinga lamandla ziboniswe ku-Figure 1b kanye ne-Supplementary Table 1. Ngokuthakazelisayo, akuwona wonke amaphutha anciphisa isithiyo samandla soguquko lwesigaba se-α-δ (Figure 1b). Sikholelwa ukuthi amaphutha anamandla okwakheka aphansi kanye nezithiyo zamandla okuguquka kwesigaba se-α-δ eziphansi abhekwa njengalimaza ukuzinza kwesigaba. Njengoba kubikiwe ngaphambilini, izindawo ezicebile nge-lead ngokuvamile zibhekwa njengezisebenza kahle ku-formamimidine PSC27. Ngakho-ke, sigxila ebusweni obuqediwe be-PbI2 (100) ngaphansi kwezimo ezicebile nge-lead. Amandla okwakheka kwamaphutha amaphutha angaphakathi angaphakathi aboniswe ku-Figure 1c kanye ne-Supplementary Table 1. Ngokusekelwe kusithiyo samandla (EB) kanye namandla okwakheka kwe-phase transition (FE), la maphutha ahlukaniswa ngezinhlobo ezintathu. Uhlobo I (i-FE ephansi ye-EB-high): Nakuba i-IPb, i-VFA kanye ne-VPb kunciphisa kakhulu isithiyo samandla ekushintsheni kwesigaba, zinamandla aphezulu okwakheka. Ngakho-ke, sikholelwa ukuthi lezi zinhlobo zamaphutha zinomthelela olinganiselwe ekushintsheni kwesigaba njengoba zingakhiwanga kakhulu. Uhlobo II (i-EB ephezulu): Ngenxa yesithiyo samandla sokuguqulwa kwesigaba se-α-δ esithuthukisiwe, amaphutha okulwa nesayithi i-PbI, i-IFA kanye ne-PbFA awawonakalisi ukuzinza kwesigaba se-α-FAPbI3 perovskite. Uhlobo III (i-FE ephansi ye-EB-low): amaphutha e-VI, II kanye ne-Pbi anamandla okwakheka aphansi kakhulu angabangela ukuwohloka kwesigaba esimnyama. Ikakhulukazi uma sibheka i-FE ephansi kakhulu kanye ne-EB VI, sikholelwa ukuthi isu elisebenza kahle kakhulu ukunciphisa izikhala ze-I.
Ukuze sinciphise i-VI, sakhe ungqimba oluqinile lwe-PbC2O4 ukuze sithuthukise ubuso be-FAPbI3. Uma kuqhathaniswa nama-passivator kasawoti we-halide we-organic njenge-phenylethylammonium iodide (PEAI) kanye ne-n-octylammonium iodide (OAI), i-PbC2O4, engenawo ama-halogen ion ahambayo, izinzile ngamakhemikhali, ayincibiliki emanzini, futhi ivalwa kalula uma ishukunyiswa. Ukuzinza okuhle komswakama womphezulu kanye nensimu kagesi ye-perovskite. Ukuncibilika kwe-PbC2O4 emanzini kungu-0.00065 g/L kuphela, okuphansi ngisho nangokwe-PbSO428. Okubaluleke kakhulu, izendlalelo eziqinile nezifanayo ze-LOS zingalungiswa kalula kumafilimu e-perovskite kusetshenziswa ukusabela kwe-in situ (bheka ngezansi). Senze ukulingisa kwe-DFT kokubopha okuphakathi kwe-FAPbI3 kanye ne-PbC2O4 njengoba kuboniswe ku-Supplementary Figure 1. Ithebula Elingeziwe 2 liveza amandla okwakheka kwesici ngemva kokujova kwe-LOS. Sithole ukuthi i-LOS ayikhulisi nje kuphela amandla okwakheka kwamaphutha e-VI ngo-0.69–1.53 eV (Isithombe 1d), kodwa futhi ikhulisa amandla okusebenza e-I endaweni yokufuduka kanye nendawo yokuphuma (Isithombe 1e). Esigabeni sokuqala, ama-ion e-I ayafuduka eduze kwendawo ye-perovskite, eshiya ama-ion e-VI endaweni ye-lattice enesithiyo samandla esingu-0.61 eV. Ngemva kokwethulwa kwe-LOS, ngenxa yomphumela wokuvimbela okuqinile, amandla okusebenza okufuduka kwama-ion e-I ayanda abe ngu-1.28 eV. Ngesikhathi sokufuduka kwama-ion e-I eshiya indawo ye-perovskite, isithiyo samandla ku-VOC siphakeme kakhulu kunasesibonelweni sokulawula (Isithombe 1e). Imidwebo ye-schematic yezindlela zokufuduka kwama-ion e-I ekulawuleni kanye ne-LOS FAPbI3 iboniswe ku-Isithombe 1 f kanye no-g, ngokulandelana. Imiphumela yokulingisa ikhombisa ukuthi i-LOS ingavimbela ukwakheka kwamaphutha e-VI kanye nokuguquguquka kwe-I, ngaleyo ndlela ivimbele i-nucleation yokuguquka kwesigaba se-α kuya ku-δ.
Ukusabela phakathi kwe-oxalic acid kanye ne-FAPbI3 perovskite kwahlolwa. Ngemva kokuxuba izixazululo ze-oxalic acid kanye ne-FAPbI3, kwakheka inani elikhulu le-white precipitate, njengoba kuboniswe ku-Supplementary Figure 2. Umkhiqizo wempuphu wahlonzwa njengento emsulwa ye-PbC2O4 kusetshenziswa i-X-ray diffraction (XRD) (Supplementary Figure 3) kanye ne-Fourier transform infrared spectroscopy (FTIR) (Supplementary Figure 4). Sithole ukuthi i-oxalic acid incibilika kakhulu ku-isopropyl alcohol (IPA) ekushiseni kwegumbi okunokuncibilika okungaba ngu-18 mg/mL, njengoba kuboniswe ku-Supplementary Figure 5. Lokhu kwenza ukucubungula okulandelayo kube lula njengoba i-IPA, njenge-passivation solvent evamile, ingalimazi ungqimba lwe-perovskite ngaphezu kwesikhathi esifushane. Ngakho-ke, ngokucwilisa ifilimu ye-perovskite esixazululweni se-oxalic acid noma ngokumboza isisombululo se-oxalic acid ku-perovskite, i-PbC2O4 encane futhi ebanzi ingatholakala ngokushesha ebusweni befilimu ye-perovskite ngokwesilinganiso samakhemikhali esilandelayo: i-H2C2O4 + FAPbI3 = PbC2O4 + FAI +HI. I-FAI ingancibilikiswa ku-IPA ngaleyo ndlela isuswe ngesikhathi sokupheka. Ubukhulu be-LOS bungalawulwa isikhathi sokuphendula kanye nokuhlushwa kwangaphambili.
Izithombe ze-scanning electron microscopy (SEM) zokulawula kanye namafilimu e-LOS perovskite ziboniswe kuZithombe 2a,b. Imiphumela ikhombisa ukuthi isimo sendawo ye-perovskite sigcinwe kahle, futhi inani elikhulu lezinhlayiya ezincane libekwe phezu kobuso bezinhlamvu, okufanele limele ungqimba lwe-PbC2O4 olwakhiwe ukusabela kwe-in-situ. Ifilimu ye-LOS perovskite inobuso obushelela kancane (Isithombe Esingeziwe 6) kanye ne-engeli enkulu yokuxhumana kwamanzi uma kuqhathaniswa nefilimu yokulawula (Isithombe Esingeziwe 7). I-high-resolution transmission transmission electron microscopy (HR-TEM) yasetshenziswa ukuhlukanisa ungqimba lobuso bomkhiqizo. Uma kuqhathaniswa nefilimu yokulawula (Isithombe 2c), ungqimba oluncane olufanayo noluqinile olunobukhulu obungaba ngu-10 nm lubonakala kahle phezu kwe-LOS perovskite (Isithombe 2d). Ukusebenzisa i-high-angle annular dark-field scanning electron microscopy (HAADF-STEM) ukuhlola ukuxhumana phakathi kwe-PbC2O4 ne-FAPbI3, ukuba khona kwezindawo ezikristalu ze-FAPbI3 kanye nezindawo ezi-amorphous ze-PbC2O4 kungabonakala ngokucacile (Isithombe Esingeziwe 8). Ukwakheka kobuso be-perovskite ngemuva kokwelashwa kwe-oxalic acid kwabonakala ngezilinganiso ze-X-ray photoelectron spectroscopy (XPS), njengoba kuboniswe kuZithombe 2e–g. KuZithombe 2e, iziqongo ze-C1s ezizungeze i-284.8 eV kanye ne-288.5 eV zingezezimpawu ezithile ze-CC kanye ne-FA, ngokulandelana. Uma kuqhathaniswa ne-membrane yokulawula, i-membrane ye-LOS ibonise iqongo elengeziwe ku-289.2 eV, elibangelwa yi-C2O42-. I-spectrum ye-O1s ye-LOS perovskite ibonisa iziqongo ezintathu ze-O1s ezihlukile ngamakhemikhali ku-531.7 eV, 532.5 eV, kanye ne-533.4 eV, ezihambisana ne-COO ekhishwe iprotoni, i-C=O yama-athomu e-oxalate angaphelele angu-30 kanye ne-O engxenye ye-OH (Isithombe 2e). )). Kwisampula yokulawula, kwabonwa isiqongo esincane se-O1s kuphela, esingabangelwa yi-oxygen chemisorbed ebusweni. Izici ze-membrane yokulawula ye-Pb 4f7/2 kanye ne-Pb 4f5/2 zitholakala ku-138.4 eV kanye ne-143.3 eV, ngokulandelana. Sibonile ukuthi i-LOS perovskite ibonisa ukushintsha kwesiqongo se-Pb esingaba ngu-0.15 eV siye emandleni aphezulu okubopha, okubonisa ukusebenzisana okunamandla phakathi kwama-athomu e-C2O42- kanye ne-Pb (Isithombe 2g).
Izithombe ze-SEM zokulawula kanye namafilimu e-b e-LOS perovskite, umbono ophezulu. c I-high-resolution cross-sectional transmission electron microscopy (HR-TEM) yokulawula kanye namafilimu e-d e-LOS perovskite. I-XPS ephezulu ye-e C1s, fO1s kanye namafilimu e-g Pb 4f perovskite. Idatha yomthombo inikezwa ngesimo samafayela edatha yomthombo.
Ngokusho kwemiphumela ye-DFT, kubikezelwa ngokwethiyori ukuthi amaphutha e-VI kanye nokufuduka kwe-I kubangela kalula ukuguquka kwesigaba kusuka ku-α kuya ku-δ. Imibiko yangaphambilini ikhombisile ukuthi i-I2 ikhishwa ngokushesha kumafilimu e-perovskite asekelwe ku-PC ngesikhathi sokucwiliswa nge-photo ngemva kokuveza amafilimu ekukhanyeni nasekucindezelweni kokushisa31,32,33. Ukuqinisekisa umphumela wokuzinza we-lead oxalate esigabeni se-α se-perovskite, sicwilise amafilimu e-control kanye ne-LOS perovskite emabhodleleni engilazi acacile aqukethe i-toluene, ngokulandelana, bese siwakhanyisa ngokukhanya kwelanga oku-1 amahora angama-24. Silinganise ukumuncwa kwesisombululo se-toluene se-ultraviolet kanye nokukhanya okubonakalayo (UV-Vis). ), njengoba kuboniswe kuMfanekiso 3a. Uma kuqhathaniswa nesampula yokulawula, kwabonakala ukuqina okuphansi kakhulu kokumuncwa kwe-I2 endabeni ye-LOS-perovskite, okubonisa ukuthi i-compact LOS ingavimbela ukukhishwa kwe-I2 kufilimu ye-perovskite ngesikhathi sokucwiliswa kokukhanya. Izithombe zamafilimu e-control aged kanye ne-LOS perovskite ziboniswa kuzithombe 3b kanye no-c. I-LOS perovskite isemnyama, kuyilapho iningi lefilimu yokulawula seliphenduke eliphuzi. Ama-spectra okumunca abonakalayo e-UV efilimu ecwilisiwe aboniswe ku-Figs. 3b, c. Sibone ukuthi ukumunca okuhambisana ne-α efilimini yokulawula kunciphile ngokusobala. Ukulinganiswa kwe-X-ray kwenziwa ukuze kubhalwe ukuvela kwesakhiwo sekristalu. Ngemva kwamahora angu-24 okukhanya, i-control perovskite ibonise isignali eqinile ye-δ-phase ephuzi (11.8°), kuyilapho i-LOS perovskite isalokhu igcina isigaba esihle esimnyama (Isithombe 3d).
Ama-spectra okumunca abonakalayo e-UV ezixazululo ze-toluene lapho ifilimu yokulawula kanye nefilimu ye-LOS kwacwiliswa ngaphansi kwelanga eli-1 amahora angama-24. I-insert ibonisa ibhodlela lapho ifilimu ngayinye yacwiliswa khona kumthamo olinganayo we-toluene. b Ama-spectra okumunca e-UV-Vis efilimu yokulawula kanye nefilimu ye-c LOS ngaphambi nangemva kwamahora angama-24 okucwiliswa ngaphansi kwelanga eli-1. I-insert ibonisa isithombe sefilimu yokuhlola. d Amaphethini okusabalalisa e-X-ray okulawula kanye namafilimu e-LOS ngaphambi nangemva kwamahora angama-24 okucwiliswa. Izithombe ze-SEM zefilimu yokulawula e kanye nefilimu f LOS ngemva kwamahora angama-24 okucwiliswa. Idatha yomthombo inikezwa ngesimo samafayela edatha yomthombo.
Senze izilinganiso ze-scanning electron microscopy (SEM) ukuze sibone izinguquko zesakhiwo sefilimu ye-perovskite ngemva kwamahora angu-24 okukhanya, njengoba kuboniswe kuZithombe 3e,f. Efilimini yokulawula, izinhlamvu ezinkulu zabhujiswa futhi zaguqulwa zaba izinaliti ezincane, ezihambisana nokwakheka komkhiqizo we-δ-phase FAPbI3 (Isithombe 3e). Kumafilimu e-LOS, izinhlamvu ze-perovskite zihlala zisesimweni esihle (Isithombe 3f). Imiphumela iqinisekisile ukuthi ukulahlekelwa yi-I kubangela kakhulu ukuguquka kusuka esigabeni esimnyama kuya esigabeni esiphuzi, kuyilapho i-PbC2O4 izinzisa isigaba esimnyama, ivimbela ukulahleka kwe-I. Njengoba ubuningi besikhala ebusweni buphakeme kakhulu kunobuningi bezinhlamvu,34 lesi sigaba kungenzeka kakhulu ukuthi senzeke ebusweni bezinhlamvu. 34 sikhipha i-iodine ngasikhathi sinye futhi sakhe i-VI. Njengoba kubikezelwe yi-DFT, i-LOS ingavimbela ukwakheka kwamaphutha e-VI futhi ivimbele ukufuduka kwama-ion e-I ebusweni be-perovskite.
Ngaphezu kwalokho, kufundwe umphumela wesendlalelo se-PbC2O4 ekumelaneni nomswakama kwamafilimu e-perovskite emoyeni womoya (umswakama ohlobene 30-60%). Njengoba kuboniswe ku-Supplementary Figure 9, i-LOS perovskite yayisemnyama ngemva kwezinsuku ezingu-12, kuyilapho ifilimu yokulawula iphenduke iphuzi. Ezilinganisweni ze-XRD, ifilimu yokulawula ikhombisa ukuphakama okunamandla ku-11.8° okuhambisana nesigaba se-δ se-FAPbI3, kuyilapho i-LOS perovskite igcina kahle isigaba se-α esimnyama (Isithombe Esingeziwe 10).
I-Steady-state photoluminescence (PL) kanye ne-time-resolved photoluminescence (TRPL) kusetshenziswe ukutadisha umphumela we-passivation we-lead oxalate ebusweni be-perovskite. Ku-Fig. Isibalo 4a sibonisa ukuthi ifilimu ye-LOS ikhuphule amandla e-PL. Esithombeni sokumapha se-PL, amandla efilimu ye-LOS kuyo yonke indawo engu-10 × 10 μm2 aphezulu kunalawo efilimu yokulawula (Isibalo Esingeziwe 11), okubonisa ukuthi i-PbC2O4 i-passivate efanayo yefilimu ye-perovskite. Isikhathi sokuphila sokuthwala sinqunywa ngokulinganisa ukubola kwe-TRPL ngomsebenzi owodwa we-exponential (Isibalo 4b). Isikhathi sokuphila sokuthwala sefilimu ye-LOS singama-5.2 μs, okude kakhulu kunefilimu yokulawula enesikhathi sokuphila sokuthwala esingama-0.9 μs, okubonisa ukuncipha kokuhlanganiswa kwe-surface nonradiative.
I-PL ezinzile kanye ne-b-spectra ye-PL yesikhashana yamafilimu e-perovskite kuma-substrate engilazi. c Ijika le-SP ledivayisi (i-FTO/TiO2/SnO2/perovskite/spiro-OMeTAD/Au). d I-spectrum ye-EQE kanye ne-spectrum ye-Jsc EQE ehlanganiswe kusuka kudivayisi esebenza kahle kakhulu. d Ukuxhomekeka kokukhanya okukhulu kwedivayisi ye-perovskite ku-Voc diagram. f Ukuhlaziywa okuvamile kwe-MKRC kusetshenziswa idivayisi ye-ITO/PEDOT:PSS/perovskite/PCBM/Au ehlanzekile. I-VTFL yi-voltage ephezulu yokugcwalisa i-trap. Kusukela kule datha sibale ubuningi be-trap (Nt). Idatha yomthombo inikezwa ngesimo samafayela edatha yomthombo.
Ukuze kufundwe umphumela wesendlalelo se-lead oxalate ekusebenzeni kwedivayisi, kusetshenziswe isakhiwo sokuxhumana sendabuko se-FTO/TiO2/SnO2/perovskite/spiro-OMeTAD/Au. Sisebenzisa i-formamidine chloride (FACl) njengesithasiselo ku-precursor ye-perovskite esikhundleni se-methylamine hydrochloride (MACl) ukuze sifinyelele ukusebenza okungcono kwedivayisi, njengoba i-FACl inganikeza ikhwalithi engcono yekristalu futhi igweme igebe lebhendi le-FAPbI335 (bheka Izibalo Ezingeziwe 1 no-2 ukuze uthole ukuqhathanisa okuningiliziwe). ). 12-14). I-IPA ikhethwe njenge-antisolvent ngoba inikeza ikhwalithi engcono yekristalu kanye nokuqondiswa okuthandwayo kumafilimu e-perovskite uma kuqhathaniswa ne-diethyl ether (DE) noma i-chlorobenzene (CB)36 (Izibalo Ezingeziwe 15 no-16). Ubukhulu be-PbC2O4 bulungiselelwe ngokucophelela ukuze kulinganiswe kahle ukudlula kwesici kanye nokuthuthwa kweshaja ngokulungisa ukuhlushwa kwe-oxalic acid (Isithombe Esingeziwe 17). Izithombe ze-SEM ezinqamulayo zamadivayisi okulawula alungiselelwe kanye ne-LOS ziboniswe ku-Supplementary Figure 18. Ama-current density ajwayelekile (CD) ama-control kanye namadivayisi e-LOS aboniswe ku-Figure 4c, kanti amapharamitha akhishwe anikezwe ku-Supplementary Table 3. Amaseli okulawula okuguqulwa kwamandla aphezulu (PCE) angu-23.43% (22.94%), Jsc 25.75 mA cm-2 (25.74 mA cm-2), Voc 1.16 V (1.16 V) kanye ne-reverse (forward) scan. I-fill factor (FF) ingu-78.40% (76.69%). I-PCE LOS PSC ephezulu ingu-25.39% (24.79%), Jsc ingu-25.77 mA cm-2, Voc ingu-1.18 V, FF ingu-83.50% (81.52%) kusukela emuva (forward Scan kuya). Idivayisi ye-LOS ithole ukusebenza kwe-photovoltaic okuqinisekisiwe okungu-24.92% elabhorethri ye-photovoltaic yomuntu wesithathu ethembekile (Isithombe Esingeziwe 19). Ukusebenza kahle kwe-quantum yangaphandle (i-EQE) kunikeze i-Jsc ehlanganisiwe engu-24.90 mA cm-2 (ukulawula) kanye no-25.18 mA cm-2 (i-LOS PSC), ngokulandelana, okwakuvumelana kahle ne-Jsc elinganiswe ku-standard AM 1.5 G spectrum (Isithombe .4d). ). Ukusatshalaliswa kwezibalo kwama-PCE alinganisiwe okulawula kanye nama-LOS PSC kuboniswe ku-Supplementary Figure 20.
Njengoba kuboniswe kuMfanekiso 4e, ubudlelwano phakathi kwe-Voc kanye nokukhanya kwabalwa ukuze kufundwe umphumela we-PbC2O4 ekuhlanganisweni kabusha kwendawo okusizwa yi-trap. Ukuthambeka komugqa ofakiwe wedivayisi ye-LOS kungu-1.16 kBT/sq, okuphansi kunomthambeka womugqa ofakiwe wedivayisi yokulawula (1.31 kBT/sq), okuqinisekisa ukuthi i-LOS iyasiza ekuvimbeleni ukuthambeka kabusha kwendawo ngama-decoys. Sisebenzisa ubuchwepheshe bokukhawulela ukushaja kwesikhala (SCLC) ukuze silinganise ngobuningi ubukhulu besici sefilimu ye-perovskite ngokulinganisa isici se-IV esimnyama sedivayisi yembobo (ITO/PEDOT:PSS/perovskite/spiro-OMeTAD/Au) njengoba kuboniswe kumfanekiso. 4f Bonisa. Ubuningi be-trap bubalwa ngefomula ethi Nt = 2ε0εVTFL/eL2, lapho i-ε iyi-dielectric constant ehlobene yefilimu ye-perovskite, i-ε0 iyi-dielectric constant ye-vacuum, i-VTFL iyi-voltage ekhawulelayo yokugcwalisa i-trap, i-e iyi-charge, i-L iyi-thickness yefilimu ye-perovskite (650 nm). Ubuningi be-defect yedivayisi ye-VOC bubalwa bungu-1.450 × 1015 cm–3, okungaphansi kobuningi be-defect yedivayisi yokulawula, obungu-1.795 × 1015 cm–3.
Idivayisi engapakishwanga ihlolwe endaweni yamandla ephezulu (i-MPP) ngaphansi kokukhanya kwelanga okugcwele ngaphansi kwe-nitrogen ukuhlola ukuzinza kwayo kokusebenza kwesikhathi eside (Isithombe 5a). Ngemva kwamahora angu-550, idivayisi ye-LOS yaqhubeka nokusebenza kahle kwayo okuphezulu okungu-92%, kuyilapho ukusebenza kwedivayisi yokulawula kwehle kwaya ku-60% kokusebenza kwayo kwasekuqaleni. Ukusatshalaliswa kwezinto kudivayisi endala kwalinganiswa nge-time-of-flight secondary ion mass spectrometry (ToF-SIMS) (Isithombe 5b, c). Ukuqongelela okukhulu kwe-iodine kungabonakala endaweni yokulawula ephezulu yegolide. Izimo zokuvikelwa kwegesi engasebenzi azibandakanyi izinto ezonakalisa imvelo njengomswakama nomoya-mpilo, okuphakamisa ukuthi izindlela zangaphakathi (okungukuthi, ukufuduka kwama-ion) yizo ezibangela lokho. Ngokusho kwemiphumela ye-ToF-SIMS, ama-I- kanye nama-AuI2-ion atholakale ku-electrode ye-Au, okubonisa ukusabalala kwe-I kusuka ku-perovskite kuya ku-Au. Ukuqina kwesignali kwama-I- kanye nama-AuI2-ion kudivayisi yokulawula kuphakeme cishe ngokuphindwe kayishumi kunokwesampula ye-VOC. Imibiko yangaphambilini ikhombisile ukuthi ukugeleza kwama-ion kungaholela ekunciphiseni okusheshayo kokuhamba kwemigodi ye-spiro-OMeTAD kanye nokugqwala kwamakhemikhali kwengqimba ephezulu ye-electrode, ngaleyo ndlela kubohloza ukuxhumana kwe-interfacial kudivayisi37,38. I-Au electrode yasuswa futhi ungqimba lwe-spiro-OMeTAD lwahlanzwa kusuka ku-substrate ngesisombululo se-chlorobenzene. Sabe sesichaza ifilimu sisebenzisa i-grazing incidence X-ray diffraction (GIXRD) (Isithombe 5d). Imiphumela ikhombisa ukuthi ifilimu yokulawula ine-diffraction peak ecacile ku-11.8°, kuyilapho kungekho-diffraction peak entsha evelayo kusampula ye-LOS. Imiphumela ikhombisa ukuthi ukulahlekelwa okukhulu kwama-I ama-ion kufilimu yokulawula kuholela ekwakhiweni kwesigaba se-δ, kuyilapho kufilimu ye-LOS le nqubo ivinjelwe ngokusobala.
Amahora angu-575 okulandelela okuqhubekayo kwe-MPP kwedivayisi engavaliwe emoyeni we-nitrogen kanye nokukhanya kwelanga oku-1 ngaphandle kwesihlungi se-UV. Ukusatshalaliswa kwe-ToF-SIMS kwama-b I- kanye nama-c AuI2-ions kudivayisi yokulawula ye-LOS MPP kanye nedivayisi yokuguga. Imibala ephuzi, eluhlaza okotshani kanye ne-orenji ihambelana ne-Au, i-Spiro-OMeTAD kanye ne-perovskite. d I-GIXRD yefilimu ye-perovskite ngemuva kokuhlolwa kwe-MPP. Idatha yomthombo inikezwa ngesimo samafayela edatha yomthombo.
Ukuqhuba kwe-ion okuncike ekushiseni kulinganiswe ukuqinisekisa ukuthi i-PbC2O4 ingavimbela ukufuduka kwe-ion (Isithombe Esingeziwe 21). Amandla okusebenza (i-Ea) okufuduka kwe-ion anqunywa ngokulinganisa ushintsho ekuqhubeni kwe-ion (σ) kwefilimu ye-FAPbI3 emazingeni okushisa ahlukene (T) nokusebenzisa ubudlelwano be-Nernst-Einstein: σT = σ0exp(−Ea/kBT), lapho i-σ0 iyi-constant, i-kB iyi-constant ye-Boltzmann. Sithola inani le-Ea kusuka emthambekeni we-ln(σT) uma kuqhathaniswa ne-1/T, okungu-0.283 eV yokulawula kanye no-0.419 eV wedivayisi ye-LOS.
Ngamafuphi, sinikeza uhlaka lwethiyori lokuhlonza indlela yokuwohloka kwe-FAPbI3 perovskite kanye nomthelela wamaphutha ahlukahlukene kusithiyo samandla soguquko lwesigaba se-α-δ. Phakathi kwala maphutha, amaphutha e-VI abikezelwa ngokwethiyori ukuthi angabangela kalula ushintsho lwesigaba kusuka ku-α kuya ku-δ. Ingqimba eqinile ye-PbC2O4 engancibiliki emanzini futhi eqinile ngamakhemikhali yethulwa ukuze kuzinziswe isigaba se-α se-FAPbI3 ngokuvimbela ukwakheka kwezikhala ze-I kanye nokufuduka kwama-ion e-I. Leli cebo linciphisa kakhulu ukuhlanganiswa kwe-interfacial non-radiative, landisa ukusebenza kahle kwamaseli elanga ku-25.39%, futhi lithuthukisa ukuzinza kokusebenza. Imiphumela yethu inikeza isiqondiso sokufeza ama-PSC e-formamidine asebenzayo futhi azinzile ngokuvimbela ushintsho lwesigaba se-α olubangelwa amaphutha kuya ku-δ.
I-Titanium(IV) isopropoxide (TTIP, 99.999%) ithengwe kwa-Sigma-Aldrich. I-Hydrochloric acid (HCl, 35.0–37.0%) kanye ne-ethanol (anhydrous) ithengwe kwa-Guangzhou Chemical Industry. I-SnO2 (15 wt% tin(IV) oxide colloidal dispersion) ithengwe kwa-Alfa Aesar. I-Lead(II) iodide (PbI2, 99.99%) ithengwe kwa-TCI Shanghai (China). I-Formamidine iodide (FAI, ≥99.5%), i-formamidine chloride (FACl, ≥99.5%), i-methylamine hydrochloride (MACl, ≥99.5%), 2,2′,7,7′-tetrakis-(N , N-di-p) )-methoxyaniline)-9,9′-spirobifluorene (Spiro-OMeTAD, ≥99.5%), i-lithium bis(trifluoromethane)sulfonylimide (Li-TFSI, 99.95%), 4-tert -butylpyridine (tBP, 96%) ithengwe eXi'an Polymer Light Technology Company (eShayina). I-N,N-dimethylformamide (DMF, 99.8%), i-dimethyl sulfoxide (DMSO, 99.9%), i-isopropyl alcohol (IPA, 99.8%), i-chlorobenzene (CB, 99.8%), i-acetonitrile (ACN). Kuthengwe kwa-Sigma-Aldrich. I-Oxalic acid (H2C2O4, 99.9%) ithengwe kwa-Macklin. Wonke amakhemikhali asetshenziswe njengoba etholakele ngaphandle kwezinye izinguquko.
I-substrates ye-ITO noma ye-FTO (1.5 × 1.5 cm2) yahlanzwa nge-ultrasonic ngensipho, i-acetone, kanye ne-ethanol imizuzu eyi-10, ngokulandelana, yabe isomiswa ngaphansi komfula we-nitrogen. Ingqimba yokuvimba ye-TiO2 ebanzi yafakwa ku-substrate ye-FTO kusetshenziswa isixazululo se-titanium diisopropoxybis (acetylacetonate) ku-ethanol (1/25, v/v) efakwe ku-500 °C imizuzu engama-60. Ukusabalala kwe-SnO2 colloidal kwahlanzwa ngamanzi acwengekile ngesilinganiso sevolumu esingu-1:5. Ku-substrate ehlanzekile ephathwe nge-UV ozone imizuzu engama-20, ifilimu elincane lama-nanoparticles e-SnO2 lafakwa ku-4000 rpm imizuzwana engama-30 bese lishiswa ku-150 °C imizuzu engama-30. Kwisisombululo se-perovskite precursor, i-275.2 mg FAI, i-737.6 mg PbI2 kanye ne-FACl (20 mol%) zancibilikiswa ku-DMF/DMSO (15/1) solvent exubile. Isendlalelo se-perovskite salungiswa ngokufaka isixazululo se-perovskite esingu-40 μL ngaphezulu kwesendlalelo se-SnO2 esiphathwe nge-UV-ozone ku-5000 rpm emoyeni ozungezile imizuzwana engu-25. Imizuzwana emi-5 ngemuva kwesikhathi sokugcina, isixazululo se-MACl IPA esingu-50 μL (4 mg/mL) safakwa ngokushesha kwi-substrate njengesiqeda ukuncibilika. Ngemuva kwalokho, amafilimu asanda kulungiswa afakwa ku-150°C imizuzu engama-20 bese kuba ku-100°C imizuzu eyi-10. Ngemva kokupholisa ifilimu ye-perovskite ekushiseni kwegumbi, isixazululo se-H2C2O4 (1, 2, 4 mg esincibilikisiwe ku-1 mL IPA) safakwa ku-4000 rpm imizuzwana engama-30 ukuze kuncishiswe ubuso be-perovskite. Isixazululo se-spiro-OMeTAD esilungiselelwe ngokuxuba i-spiro-OMeTAD engu-72.3 mg, i-1 ml ye-CB, i-27 µl tBP kanye ne-17.5 µl ye-Li-TFSI (520 mg ku-1 ml ye-acetonitrile) safakwa nge-spin-coating efilimini ku-4000 rpm zingakapheli imizuzwana engama-30. Ekugcineni, ungqimba lwe-Au oluyi-100 nm obukhulu lwashiswa ku-vacuum ngesivinini esingu-0.05 nm/s (0~1 nm), 0.1 nm/s (2~15 nm) kanye no-0.5 nm/s (16~100 nm).
Ukusebenza kwe-SC kwamaseli elanga e-perovskite kukalwe kusetshenziswa i-Keithley 2400 meter ngaphansi kokukhanya kwe-solar simulator (SS-X50) ngamandla okukhanya angu-100 mW/cm2 futhi kwaqinisekiswa kusetshenziswa amaseli elanga e-silicon ajwayelekile alinganisiwe. Ngaphandle kokuthi kuchazwe ngenye indlela, ama-SP curve akalwe ebhokisini legilavu ​​​​eligcwele i-nitrogen ekushiseni kwegumbi (~25°C) ngezindlela zokuskena ezihamba phambili nezibuyela emuva (isinyathelo se-voltage 20 mV, isikhathi sokulibaziseka esingu-10 ms). Imaski yesithunzi yasetshenziswa ukunquma indawo ephumelelayo engu-0.067 cm2 ye-PSC elinganisiwe. Ukulinganiswa kwe-EQE kwenziwa emoyeni ozungezile kusetshenziswa uhlelo lwe-PVE300-IVT210 (Industrial Vision Technology(s) Pte Ltd) ngokukhanya oku-monochromatic okugxile kudivayisi. Ukuze idivayisi izinze, ukuhlolwa kwamaseli elanga angafakwanga kwenziwa ebhokisini legilavu ​​​​le-nitrogen ku-100 mW/cm2 ingcindezi ngaphandle kwesihlungi se-UV. I-ToF-SIMS ikalwa kusetshenziswa i-PHI nanoTOFII time-of-flight SIMS. Ukuhlolwa kokujula kutholakale kusetshenziswa isibhamu se-Ar ion esingu-4 kV esinendawo engu-400×400 µm.
Izilinganiso ze-X-ray photoelectron spectroscopy (XPS) zenziwe ohlelweni lwe-Thermo-VG Scientific (ESCALAB 250) kusetshenziswa i-Al Kα e-monochromatized (yemodi ye-XPS) ngokucindezela okungu-5.0 × 10–7 Pa. I-scanning electron microscopy (SEM) yenziwe ohlelweni lwe-JEOL-JSM-6330F. Ukwakheka kobuso kanye nokuqina kwamafilimu e-perovskite kwalinganiswa kusetshenziswa i-atomic force microscopy (AFM) (Bruker Dimension FastScan). I-STEM kanye ne-HAADF-STEM zigcinwe ku-FEI Titan Themis STEM. I-UV-Vis absorption spectra yalinganiswa kusetshenziswa i-UV-3600Plus (Shimadzu Corporation). I-Space charge limiting current (SCLC) yaqoshwa ku-Keithley 2400 meter. I-Steady-state photoluminescence (PL) kanye ne-time-resolved photoluminescence (TRPL) of carrier lifetime decay yalinganiswa kusetshenziswa i-FLS 1000 photoluminescence spectrometer. Izithombe zemephu ye-PL zilinganiswe kusetshenziswa uhlelo lwe-Horiba LabRam Raman i-HR Evolution. I-Fourier transform infrared spectroscopy (FTIR) yenziwe kusetshenziswa uhlelo lwe-Thermo-Fisher Nicolet NXR 9650.
Kulo msebenzi, sisebenzisa indlela yokulinganisa indlela ye-SSW ukutadisha indlela yokuguquka kwesigaba kusuka ku-α-phase kuya ku-δ-phase. Endleleni ye-SSW, ukunyakaza kobuso bamandla angasethwa kunqunywa yisiqondiso semodi ethambile engahleliwe (i-derivative yesibili), evumela ucwaningo oluningiliziwe nolunenhloso lobuso bamandla angasethwa. Kulo msebenzi, ukulinganisa indlela kwenziwa ku-supercell yama-athomu angu-72, futhi kuqoqwa amabhangqa angaphezu kwe-100 okuqala/okugcina (IS/FS) ezingeni le-DFT. Ngokusekelwe kusethi yedatha ye-IS/FS pairwise, indlela exhumanisa isakhiwo sokuqala kanye nesakhiwo sokugcina inganqunywa ngokuhambisana phakathi kwama-athomu, bese kusetshenziswa ukunyakaza okubili eceleni kobuso beyunithi eguquguqukayo ukuze kunqunywe kahle indlela yesimo sokuguquka. (VK-DESV). Ngemva kokusesha isimo sokuguquka, indlela enesithiyo esiphansi kakhulu inganqunywa ngokubeka izithiyo zamandla ezingeni.
Zonke izibalo ze-DFT zenziwe kusetshenziswa i-VASP (inguqulo 5.3.5), lapho ukusebenzisana kwama-electron-ion kwama-athomu e-C, N, H, Pb, kanye ne-I kumelelwa uhlelo lwe-projected amplified wave (PAW). Umsebenzi wokuxhumana kokushintshana uchazwa yi-generalized gradient approximation ku-Perdue-Burke-Ernzerhoff parametrization. Umkhawulo wamandla wamagagasi endiza usethelwe ku-400 eV. Igridi ye-k-point ye-Monkhorst-Pack inosayizi ongu-(2 × 2 × 1). Kuzo zonke izakhiwo, i-lattice kanye nezikhundla ze-athomu zalungiswa ngokugcwele kuze kube yilapho ingxenye yokucindezeleka ephezulu ingaphansi kuka-0.1 GPa kanti ingxenye yamandla ephezulu ingaphansi kuka-0.02 eV/Å. Kumodeli wobuso, ubuso be-FAPbI3 bunezendlalelo ezi-4, ungqimba olungezansi lunama-athomu aqinile alingisa umzimba we-FAPbI3, futhi izendlalelo ezintathu eziphezulu zingahamba ngokukhululeka ngesikhathi senqubo yokwenza ngcono. Isendlalelo se-PbC2O4 sinobukhulu obuyi-1 ML futhi sitholakala ebusweni be-I-terminal ye-FAPbI3, lapho i-Pb iboshwe khona ku-1 I kanye no-4 O.
Ukuze uthole ulwazi olwengeziwe mayelana nomklamo wocwaningo, bheka i-Natural Portfolio Report Abstract ehlobene nalesi sihloko.
Yonke idatha etholwe noma ehlaziywe phakathi nalolu cwaningo ifakiwe esihlokweni esishicilelwe, kanye nolwazi olusekelayo kanye namafayela edatha eluhlaza. Idatha eluhlaza eyethulwe kulolu cwaningo iyatholakala ku-https://doi.org/10.6084/m9.figshare.2410016440. Idatha yomthombo inikezwe kulesi sihloko.
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