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I-Defect passivation isetyenziswa kakhulu ukuphucula ukusebenza kweeseli zelanga ze-lead triiodide perovskite, kodwa isiphumo seziphene ezahlukeneyo kuzinzo lwe-α-phase asikacaci; Apha, sisebenzisa ithiyori yokusebenza koxinano, sichonga okokuqala indlela yokubola kwe-formamimidine lead triiodide perovskite ukusuka kwi-α-phase ukuya kwi-δ-phase kwaye sifunde isiphumo seziphene ezahlukeneyo kwi-phase transition energy barrier. Iziphumo zokulinganisa ziqikelela ukuba izithuba ze-iodine zinokubangela ukubola kuba zinciphisa kakhulu umqobo wamandla kwi-α-δ phase transition kwaye zinamandla okwakheka aphantsi kumphezulu we-perovskite. Ukungeniswa komaleko oxineneyo we-lead oxalate enganyibilikiyo emanzini kumphezulu we-perovskite kuthintela kakhulu ukubola kwe-α-phase, kuthintela ukufuduka kunye nokuguquguquka kwe-iodine. Ukongeza, le ndlela inciphisa kakhulu i-interfacial nonradiative recombination kwaye yonyusa ukusebenza kakuhle kweeseli zelanga ukuya kwi-25.39% (iqinisekisiwe yi-24.92%). Isixhobo esingafakwanga sixhobo sisenokugcina ukusebenza kwaso kokuqala kwe-92% emva kokusebenza ngamandla aphezulu kangangeeyure ezingama-550 phantsi kovavanyo lomoya oluyi-1.5 G.
Ukusebenza kakuhle kokuguqulwa kwamandla (PCE) kweeseli zelanga ze-perovskite (ii-PSC) kufikelele kwirekhodi ephezulu eqinisekisiweyo ye-26% 1. Ukusukela ngo-2015, ii-PSC zanamhlanje zikhethe i-formamimidine triiodide perovskite (FAPbI3) njengomaleko ofunxa ukukhanya ngenxa yokuzinza kwayo okuhle kobushushu kunye ne-bandgap ekhethekileyo ekufutshane nomda weShockley-Keisser we-2,3,4. Ngelishwa, iifilimu ze-FAPbI3 thermodynamically zidlula kutshintsho lwesigaba ukusuka kwisigaba se-α esimnyama ukuya kwisigaba se-δ esityheli esingeyiyo i-perovskite kubushushu begumbi5,6. Ukuthintela ukwakheka kwesigaba se-delta, kuye kwaphuhliswa iindlela ezahlukeneyo ze-perovskite ezintsonkothileyo. Icebo eliqhelekileyo lokoyisa le ngxaki kukuxuba i-FAPbI3 kunye nomxube we-methyl ammonium (MA+), i-cesium (Cs+) kunye ne-bromide (Br-) ions7,8,9. Nangona kunjalo, ii-perovskites ezixutyiweyo zinengxaki yokwandiswa kwe-bandgap kunye nokwahlukana kwesigaba esibangelwa yi-photoinduced, nto leyo ebeka emngciphekweni ukusebenza kunye nokuzinza kokusebenza kwe-PSCs10,11,12 ephumayo.
Izifundo zakutshanje zibonise ukuba i-FAPbI3 yekristale ecocekileyo engenalo naluphi na uhlobo lwe-doping inozinzo oluhle kakhulu ngenxa ye-crystallinity yayo egqwesileyo kunye neziphene eziphantsi13,14. Ke ngoko, ukunciphisa iziphene ngokwandisa i-crystallinity ye-bulk FAPbI3 licebo elibalulekileyo lokufezekisa ii-PSC2,15 ezisebenzayo nezizinzileyo. Nangona kunjalo, ngexesha lokusebenza kwe-FAPbI3 PSC, ukonakala ukuya kwisigaba se-δ esityheli esingena-perovskite esingafunekiyo sisenokwenzeka16. Le nkqubo idla ngokuqala kwiindawo eziphezulu kunye nemida yeenkozo ezichaphazeleka lula ngamanzi, ubushushu kunye nokukhanya ngenxa yokubakho kweendawo ezininzi ezineziphene17. Ke ngoko, ukudlula komphezulu/kweenkozo kuyimfuneko ukuzinzisa isigaba esimnyama se-FAPbI318. Iindlela ezininzi zokudlula kweziphene, kubandakanya ukungeniswa kwee-perovskites eziphantsi, iimolekyuli ze-asidi-base Lewis, kunye neetyuwa ze-ammonium halide, zenze inkqubela phambili enkulu kwi-formamimidine PSCs19,20,21,22. Ukuza kuthi ga ngoku, phantse zonke izifundo zigxile kwindima yeziphene ezahlukeneyo ekumiseleni iipropati ze-optoelectronic ezifana nokuhlanganiswa kwe-carrier, ubude bokusasazwa kunye nesakhiwo sebhendi kwiiseli zelanga22,23,24. Umzekelo, ithiyori yokusebenza koxinano (DFT) isetyenziselwa ukuqikelela ngokwethiyori amandla okwakheka kunye namanqanaba amandla okubamba iziphene ezahlukeneyo, esetyenziswa kakhulu ukukhokela uyilo lwe-passivation olusebenzayo20,25,26. Njengoko inani leziphene lincipha, uzinzo lwesixhobo luhlala luphucuka. Nangona kunjalo, kwi-formamimidine PSCs, iindlela zempembelelo yeziphene ezahlukeneyo kuzinzo lwesigaba kunye neepropati ze-photoelectric kufuneka zahluke ngokupheleleyo. Ngokolwazi lwethu, ukuqonda okusisiseko kwendlela iziphene ezibangela ngayo utshintsho lwesigaba se-cubic ukuya kwi-hexagonal (α-δ) kunye nendima ye-passivation yomphezulu kuzinzo lwesigaba se-α-FAPbI3 perovskite ayikaqondwa kakuhle.
Apha, sityhila indlela yokuwohloka kwe-FAPbI3 perovskite ukusuka kwi-α-phase emnyama ukuya kwi-δ-phase etyheli kunye nempembelelo yeziphene ezahlukeneyo kumqobo wamandla wotshintsho lwe-α-to-δ-phase nge-DFT. Izithuba ze-I, eziveliswa lula ngexesha lokwenziwa kwefilimu kunye nokusebenza kwesixhobo, kuqikelelwa ukuba zinokuqalisa utshintsho lwesigaba se-α-δ. Ke ngoko, sazisa umaleko oxineneyo we-lead oxalate (PbC2O4) onganyibilikiyo emanzini kwaye ozinzileyo ngokweekhemikhali phezu kwe-FAPbI3 ngokusebenzisa i-in situ reaction. Umphezulu we-lead oxalate (LOS) uthintela ukwakheka kwezithuba ze-I kwaye uthintela ukufuduka kwee-ion ze-I xa zivuselelwa bubushushu, ukukhanya, kunye namasimi ombane. I-LOS ephumayo inciphisa kakhulu i-interfacial nonradiative recombination kwaye iphucula ukusebenza kakuhle kwe-FAPbI3 PSC ukuya kwi-25.39% (iqinisekiswe kwi-24.92%). Isixhobo se-LOS esingafakwanga sigcine i-92% yokusebenza kwaso kokuqala emva kokusebenza kwindawo yamandla ephezulu (MPP) kangangeeyure ezingaphezu kwama-550 kwi-simulated air mass (AM) ye-1.5 G yemitha.
Siqale senza izibalo ze-ab initio ukuze sifumane indlela yokubola kwe-FAPbI3 perovskite ukuya ekutshintsheni ukusuka kwisigaba se-α ukuya kwisigaba se-δ. Ngenkqubo yokuguqula isigaba eneenkcukacha, kufunyaniswe ukuba utshintsho oluvela kwi-octahedron yekona enemilinganiselo emithathu [PbI6] kwisigaba se-cubic α se-FAPbI3 ukuya kwi-octahedron yecala elinye [PbI6] kwisigaba se-δ secala elineemilo ezi-hexagonal se-FAPbI3 luyafezekiswa. luphula u-9. I-Pb-I yenza ikhonkco kwinyathelo lokuqala (Int-1), kwaye umqobo wayo wamandla ufikelela kwi-0.62 eV/iseli, njengoko kubonisiwe kuMfanekiso 1a. Xa i-octahedron itshintshelwa kwicala le-[0\(\bar{1}\)1], ikhonkco elifutshane elineemilo ezi-hexagonal landa ukusuka kwi-1×1 ukuya kwi-1×3, 1×4 kwaye ekugqibeleni lingena kwisigaba se-δ. Umlinganiselo wolwalathiso lwendlela yonke yi (011)α//(001)δ + [100]α//[100]δ. Ukusuka kumzobo wokusasazwa kwamandla, kunokufunyaniswa ukuba emva kwe-nucleation yesigaba se-δ se-FAPbI3 kumanqanaba alandelayo, umqobo wamandla uphantsi kunowotshintsho lwesigaba se-α, oko kuthetha ukuba utshintsho lwesigaba luya kukhawuleziswa. Ngokucacileyo, inyathelo lokuqala lokulawula utshintsho lwesigaba lubalulekile ukuba sifuna ukuthintela ukuwohloka kwesigaba se-α.
Inkqubo yokuguqulwa kweSigaba ukusuka ekhohlo ukuya ekunene – isigaba esimnyama se-FAPbI3 (isigaba se-α), ukuqhekeka kwebhondi yokuqala ye-Pb-I (Int-1) kunye nokuqhekeka kwebhondi ye-Pb-I (Int-2, Int -3 kunye ne-Int -4) kunye nesigaba esityheli se-FAPbI3 (isigaba se-delta). b Izithintelo zamandla kwinguqu yesigaba se-α ukuya kwi-δ ye-FAPbI3 ngokusekelwe kwiimpazamo ezahlukeneyo zangaphakathi. Umgca onamachaphaza ubonisa umqobo wamandla wekristale efanelekileyo (0.62 eV). c Amandla okwenziwa kweziphene zamanqaku aphambili kumphezulu we-lead perovskite. I-abscissa axis ngumqobo wamandla wenguqu yesigaba se-α-δ, kwaye i-ordinate axis ngamandla okwenziwa kweziphene. Iindawo ezifakwe umbala ongwevu, otyheli kunye noluhlaza ziintlobo I (i-EB ephantsi-phezulu ye-FE), uhlobo II (i-FE ephezulu) kunye nohlobo III (i-EB ephantsi-phantsi ye-FE), ngokwahlukeneyo. d Amandla okwenziwa kweziphene VI kunye ne-LOS ye-FAPbI3 kulawulo. Umqobo we-e I ekufudukeni kwee-ion kulawulo kunye ne-LOS ye-FAPbI3. f – ukubonakaliswa kwesicwangciso sokufuduka kwee-ion ze-I (ii-orenji ze-spheres) kunye ne-gLOS FAPbI3 (grey, lead; violet (orenji), i-ayodini (i-mobile iodine)) kulawulo lwe-gf (ekhohlo: umbono ophezulu; ekunene: icandelo elinqamlezileyo, mdaka); ikhabhoni; luhlaza okwesibhakabhaka olukhanyayo – i-nitrogen; bomvu – ioksijini; pinki olukhanyayo – i-hydrogen). Idatha yomthombo ibonelelwa ngohlobo lweefayile zedatha yomthombo.
Emva koko sifunde ngokucwangcisiweyo impembelelo yeziphene ezahlukeneyo ze-intrinsic point (kubandakanya i-PbFA, i-IFA, i-PbI, kunye ne-IPb antisite occupancy; ii-atoms ze-Pbi kunye ne-Ii interstitial; kunye ne-VI, i-VFA, kunye ne-VPb vacancies), ezithathwa njengezinto eziphambili. ezibangela ukuwohloka kwesigaba se-atomic kunye ne-energy level ziboniswe kuMfanekiso 1b kunye neTheyibhile eyoNgezelelweyo 1. Okunomdla kukuba, ayizizo zonke iziphene ezinciphisa umqobo wamandla wotshintsho lwesigaba se-α-δ (Umfanekiso 1b). Sikholelwa ukuba iziphene ezine-low formation energy kunye ne-α-δ phase transition energy barriers eziphantsi zithathwa njengezinobungozi kuzinzo lwesigaba. Njengoko bekuxeliwe ngaphambili, iindawo ezityebileyo nge-lead ngokubanzi zithathwa njengezisebenzayo kwi-formamimidine PSC27. Ke ngoko, sigxila kumphezulu we-PbI2-terminated (100) phantsi kweemeko ezityebileyo nge-lead. Amandla okwakheka kweziphene ze-intrinsic point defects yomphezulu aboniswe kuMfanekiso 1c kunye neTheyibhile eyoNgezelelweyo 1. Ngokusekelwe kumqobo wamandla (EB) kunye namandla okwakhiwa kwesigaba soguquko (FE), ezi ziphene zahlulwe zibe ziintlobo ezintathu. Uhlobo I (i-EF ephantsi-ephezulu ye-EB): Nangona i-IPb, i-VFA kunye ne-VPb zinciphisa kakhulu umqobo wamandla kwinguqu yesigaba, zinamandla aphezulu okwakheka. Ke ngoko, sikholelwa ukuba olu hlobo lweziphene lunempembelelo encinci kwiinguqu zesigaba kuba azifane zenziwe. Uhlobo II (i-EB ephezulu): Ngenxa yomqobo wamandla okuguquka kwesigaba se-α-δ ophuculweyo, iziphene ze-anti-site PbI, IFA kunye ne-PbFA aziwonakalisi uzinzo lwesigaba se-α-FAPbI3 perovskite. Uhlobo III (i-EF ephantsi-ephantsi ye-EB): iziphene ze-VI, Ii kunye ne-Pbi ezinamandla okwakheka aphantsi zinokubangela ukuwohloka kwesigaba esimnyama. Ingakumbi xa sijonga i-FE ephantsi kunye ne-EB VI, sikholelwa ukuba icebo elisebenzayo kukunciphisa izithuba ze-I.
Ukuze sinciphise i-VI, senze umaleko oxineneyo we-PbC2O4 ukuphucula umphezulu we-FAPbI3. Xa kuthelekiswa nee-organic halide salt passivators ezifana ne-phenylethylammonium iodide (PEAI) kunye ne-n-octylammonium iodide (OAI), i-PbC2O4, engenazo ii-halogen ions ezihambayo, izinzile ngokweekhemikhali, ayinyibiliki emanzini, kwaye ivalwa lula xa ivuselelwa. Ukuzinziswa kakuhle komswakama womphezulu kunye nombane we-perovskite. Ukunyibilika kwe-PbC2O4 emanzini yi-0.00065 g/L kuphela, ephantsi nakweye-PbSO428. Okubaluleke ngakumbi, iileya ezixineneyo nezifanayo ze-LOS zinokulungiswa kancinci kwiifilimu ze-perovskite kusetyenziswa ii-in situ reactions (jonga ngezantsi). Senze ii-DFT simulations zokudibanisa phakathi kwe-FAPbI3 kunye ne-PbC2O4 njengoko kubonisiwe kwi-Supplementary Figure 1. Itheyibhile eyongezelelweyo 2 ibonisa amandla okwakheka kwesiphene emva kokufakwa kwe-LOS. Sifumanise ukuba i-LOS ayinyusi nje kuphela amandla okwenziwa kweempazamo ze-VI nge-0.69–1.53 eV (Umfanekiso 1d), kodwa ikwanyusa amandla okusebenza e-I kumphezulu wokufuduka kunye nomphezulu wokuphuma (Umfanekiso 1e). Kwinqanaba lokuqala, ii-ion ze-I ziyafuduka kumphezulu we-perovskite, zishiya ii-ion ze-VI kwindawo ye-lattice ene-energy barrier ye-0.61 eV. Emva kokungeniswa kwe-LOS, ngenxa yesiphumo sothintelo lwe-steric, amandla okusebenza okufuduka kwee-ion ze-I ayanda ukuya kwi-. 1.28 eV. Ngexesha lokufuduka kwee-ion ze-I zishiya umphezulu we-perovskite, i-energy barrier kwi-VOC nayo iphezulu kunakwisampuli yokulawula (Umfanekiso 1e). Iidayagram ze-schematic zeendlela zokufuduka kwee-ion ze-I kulawulo kunye ne-LOS FAPbI3 ziboniswe kuMfanekiso 1 f kunye no-g, ngokulandelelana. Iziphumo zokulinganisa zibonisa ukuba i-LOS inokuthintela ukwakheka kweempazamo ze-VI kunye nokuguquguquka kwe-I, ngaloo ndlela ithintela i-nucleation yotshintsho lwesigaba se-α ukuya kwi-δ.
Isiphumo phakathi kwe-oxalic acid kunye ne-FAPbI3 perovskite sivavanyiwe. Emva kokuxuba izisombululo ze-oxalic acid kunye ne-FAPbI3, kwavela inani elikhulu le-white precipitate, njengoko kubonisiwe kuMfanekiso oNgezelelweyo 2. Imveliso yomgubo ichongiwe njengezinto ezicocekileyo ze-PbC2O4 kusetyenziswa i-X-ray diffraction (XRD) (Umfanekiso oNgezelelweyo 3) kunye ne-Fourier transform infrared spectroscopy (FTIR) (Umfanekiso oNgezelelweyo 4). Sifumanise ukuba i-oxalic acid inyibilika kakhulu kwi-isopropyl alcohol (IPA) kubushushu begumbi kunye nokunyibilika okumalunga ne-18 mg/mL, njengoko kubonisiwe kuMfanekiso oNgezelelweyo 5. Oku kwenza ukucutshungulwa okulandelayo kube lula kuba i-IPA, njengesinyibilikisi esiqhelekileyo se-passivation, ayonakalisi umaleko we-perovskite ngaphaya kwexesha elifutshane29. Ngoko ke, ngokuntywilisela ifilimu ye-perovskite kwisisombululo se-oxalic acid okanye ngokuyisonga nge-spin-coating isisombululo se-oxalic acid kwi-perovskite, i-PbC2O4 encinci nexineneyo ingafumaneka ngokukhawuleza kumphezulu wefilimu ye-perovskite ngokwe-equation yekhemikhali elandelayo: H2C2O4 + FAPbI3 = PbC2O4 + FAI + HI. I-FAI inokunyibilikiswa kwi-IPA kwaye ngaloo ndlela isuswe ngexesha lokupheka. Ubukhulu be-LOS bunokulawulwa lixesha lokuphendula kunye noxinzelelo lwangaphambi kwexesha.
Imifanekiso ye-scanning electron microscopy (SEM) yokulawula kunye neefilimu ze-LOS perovskite iboniswe kwiMifanekiso 2a,b. Iziphumo zibonisa ukuba imo yomphezulu we-perovskite igcinwe kakuhle, kwaye inani elikhulu lamasuntswana amancinci abekwe kumphezulu weenkozo, ekufuneka amele umaleko we-PbC2O4 owenziwe yi-in-situ reaction. Ifilimu ye-LOS perovskite inomphezulu othambileyo kancinci (Umfanekiso oNcedisayo 6) kunye ne-engile enkulu yokunxibelelana namanzi xa ithelekiswa nefilimu yokulawula (Umfanekiso oNcedisayo 7). I-high-resolution transmission transmission electron microscopy (HR-TEM) yasetyenziswa ukwahlula umaleko womphezulu wemveliso. Xa kuthelekiswa nefilimu yokulawula (Umfanekiso 2c), umaleko obhityileyo ofanayo noxineneyo onobukhulu obumalunga ne-10 nm ubonakala ngokucacileyo phezu kwe-LOS perovskite (Umfanekiso 2d). Ukusebenzisa i-high-angle annular dark-field scanning electron microscopy (HAADF-STEM) ukuhlola ujongano phakathi kwe-PbC2O4 kunye ne-FAPbI3, ubukho beendawo zekristale ze-FAPbI3 kunye neendawo ezingabonakaliyo ze-PbC2O4 zinokubonwa ngokucacileyo (Umfanekiso ongezelelweyo 8). Ukwakheka komphezulu we-perovskite emva konyango lwe-oxalic acid kwabonakaliswa yimilinganiselo ye-X-ray photoelectron spectroscopy (XPS), njengoko kubonisiwe kwiMifanekiso 2e–g. KwiMifanekiso 2e, iincopho ze-C1s ezijikeleze i-284.8 eV kunye ne-288.5 eV zezempawu ezithile ze-CC kunye ne-FA, ngokwahlukeneyo. Xa kuthelekiswa ne-control membrane, i-LOS membrane ibonise incopho eyongezelelweyo kwi-289.2 eV, ebangelwa yi-C2O42-. I-O 1s spectrum ye-LOS perovskite ibonisa iincopho ezintathu ze-O 1s ezahlukileyo ngokweekhemikhali kwi-531.7 eV, 532.5 eV, kunye ne-533.4 eV, ezihambelana ne-COO e-deprotonated, i-C=O yamaqela e-oxalate angapheliyo angama-30 kunye nee-athomu ze-O ze-OH component (Umzobo 2e). )). Kwisampulu yokulawula, kuphela incopho encinci ye-O 1s ebonwe, enokuthi ibangelwe yi-oxygen chemisorbed kumphezulu. Iimpawu ze-control membrane ze-Pb 4f7/2 kunye ne-Pb 4f5/2 zifumaneka kwi-138.4 eV kunye ne-143.3 eV, ngokulandelelana. Siqaphele ukuba i-LOS perovskite ibonisa utshintsho lwencopho ye-Pb malunga ne-0.15 eV ukuya kumandla aphezulu okubopha, okubonisa ukusebenzisana okunamandla phakathi kwee-athomu ze-C2O42- kunye ne-Pb (Umzobo 2g).
imifanekiso ye-SEM yolawulo kunye neefilimu ze-b ze-LOS perovskite, umbono ophezulu. c I-high-resolution cross-sectional transmission electron microscopy (HR-TEM) yolawulo kunye neefilimu ze-d ze-LOS perovskite. I-XPS ephezulu ye-e C 1s, f O 1s kunye neefilimu ze-g Pb 4f perovskite. Idatha yomthombo inikezelwa ngohlobo lweefayile zedatha yomthombo.
Ngokweziphumo ze-DFT, kuqikelelwa ngokwethiyori ukuba iimpazamo ze-VI kunye nokufuduka kwe-I kubangela ngokulula utshintsho lwesigaba ukusuka kwi-α ukuya kwi-δ. Iingxelo zangaphambili zibonise ukuba i-I2 ikhutshwa ngokukhawuleza kwiifilimu ze-perovskite ezisekwe kwi-PC ngexesha lokuntywiliselwa nge-photo emva kokubeka iifilimu kuxinzelelo lokukhanya nobushushu31,32,33. Ukuqinisekisa isiphumo sokuzinza kwe-oxalate ye-lead kwisigaba se-α se-perovskite, sintywilisele iifilimu ze-control kunye ne-LOS perovskite kwiibhotile zeglasi ezicacileyo ezine-toluene, ngokulandelanayo, saza sazikhanyisa nge-1 sunlight kangangeeyure ezingama-24. Silinganise ukufunxwa kwe-ultraviolet kunye nokukhanya okubonakalayo (UV-Vis). ) isisombululo se-toluene, njengoko kubonisiwe kuMfanekiso 3a. Xa kuthelekiswa nesampulu yokulawula, amandla okufunxwa kwe-I2 aphantsi kakhulu abonwe kwimeko ye-LOS-perovskite, okubonisa ukuba i-compact LOS inokuthintela ukukhululwa kwe-I2 kwifilimu ye-perovskite ngexesha lokuntywiliselwa kokukhanya. Iifoto zeefilimu ze-control ezindala kunye ne-LOS perovskite ziboniswe kwi-insets zeMifanekiso 3b kunye no-c. I-LOS perovskite isemnyama, ngelixa uninzi lwefilimu yokulawula lujike lwaba tyheli. I-UV–visible absorption spectra yefilimu entywilisiweyo iboniswe kwiMifanekiso 3b, c. Siqaphele ukuba ukufunxwa okuhambelana ne-α kwifilimu yokulawula kuncitshisiwe ngokucacileyo. Ukulinganiswa kwe-X-ray kwenziwe ukuze kubhalwe ukuguquka kwesakhiwo sekristale. Emva kweeyure ezingama-24 zokukhanya, i-control perovskite ibonise isignali ye-δ-phase etyheli enamandla (11.8°), ngelixa i-LOS perovskite isagcina isigaba esimnyama esihle (Umfanekiso 3d).
Iispectra zokufunxa ezibonakalayo ze-UV zezisombululo ze-toluene apho ifilimu yokulawula kunye nefilimu ye-LOS zantywiliselwa phantsi kwelanga eli-1 iiyure ezingama-24. I-inset ibonisa ibhotile apho ifilimu nganye yantywiliselwa khona kumthamo olinganayo we-toluene. b Iispectra zokufunxa ze-UV-Vis zefilimu yokulawula kunye nefilimu ye-c LOS ngaphambi nasemva kweeyure ezingama-24 zokuntywiliselwa phantsi kwelanga eli-1. I-inset ibonisa ifoto yefilimu yovavanyo. d Iipateni ze-diffraction ze-X-ray zolawulo kunye neefilimu ze-LOS ngaphambi nasemva kweeyure ezingama-24 zokutywiliselwa. Imifanekiso ye-SEM yefilimu yokulawula e kunye nefilimu f LOS emva kweeyure ezingama-24 zokutywiliselwa. Idatha yomthombo ibonelelwa ngohlobo lweefayile zedatha yomthombo.
Senze ukulinganisa i-scanning electron microscopy (SEM) ukujonga utshintsho lwesakhiwo sefilimu ye-perovskite emva kweeyure ezingama-24 zokukhanya, njengoko kubonisiwe kwiMifanekiso 3e,f. Kwifilimu yokulawula, iinkozo ezinkulu zatshatyalaliswa zaza zaguqulwa zaba ziinaliti ezincinci, ezihambelana nokwakheka kwemveliso ye-δ-phase FAPbI3 (Umzobo 3e). Kwiifilimu ze-LOS, iinkozo ze-perovskite zihlala zikwimeko entle (Umfanekiso 3f). Iziphumo ziqinisekisile ukuba ukulahleka kwe-I kubangela kakhulu utshintsho ukusuka kwisigaba esimnyama ukuya kwisigaba esityheli, ngelixa i-PbC2O4 izinzisa isigaba esimnyama, ithintela ukulahleka kwe-I. Ekubeni uxinano lwesithuba kumphezulu luphezulu kakhulu kunobuninzi bengqolowa,34 esi sigaba sinokwenzeka ngakumbi kumphezulu wengqolowa. ngaxeshanye sikhupha i-iodine kwaye senze i-VI. Njengoko kuxelwe kwangaphambili yi-DFT, i-LOS inokuthintela ukwakheka kweziphene ze-VI kwaye ithintele ukufuduka kwee-ion ze-I kumphezulu we-perovskite.
Ukongeza, isiphumo somaleko we-PbC2O4 ekuchaseni ukufuma kweefilimu ze-perovskite emoyeni womoya (ukufuma okulinganiselweyo yi-30-60%) kufundwe. Njengoko kubonisiwe kuMfanekiso oNcedisayo 9, i-LOS perovskite yayisemnyama emva kweentsuku ezili-12, ngelixa ifilimu yokulawula yajika yaba tyheli. Kwimilinganiselo ye-XRD, ifilimu yokulawula ibonisa incopho enamandla kwi-11.8° ehambelana nesigaba se-δ se-FAPbI3, ngelixa i-LOS perovskite igcina kakuhle isigaba se-α esimnyama (Umfanekiso oNcedisayo 10).
I-photoluminescence ye-Steady-state (PL) kunye ne-photoluminescence esonjululwe ngexesha (TRPL) zisetyenzisiwe ukufunda isiphumo sokudlula kwe-oxalate ye-lead kumphezulu we-perovskite. KuMfanekiso 4a ubonisa ukuba ifilimu ye-LOS inyuse i-PL intensity. Kumfanekiso we-PL mapping, intensity yefilimu ye-LOS kuyo yonke indawo ye-10 × 10 μm2 iphezulu kuneyo yefilimu yokulawula (Umfanekiso ongezelelweyo 11), obonisa ukuba i-PbC2O4 iyadlula ngokufanayo ifilimu ye-perovskite. Ubomi bomthwali bumiselwa ngokuqikelela ukubola kwe-TRPL ngomsebenzi omnye we-exponential (Umfanekiso 4b). Ubomi bomthwali wefilimu ye-LOS yi-5.2 μs, ende kakhulu kunefilimu yokulawula enempilo yomthwali ye-0.9 μs, ebonisa ukuncipha kokuphinda kuhlangane komphezulu ongeyiyo imitha.
I-PL ezinzileyo kunye ne-b-spectra ye-PL yexeshana yeefilimu ze-perovskite kwi-substrates zeglasi. c I-SP curve yesixhobo (FTO/TiO2/SnO2/perovskite/spiro-OMeTAD/Au). d I-spectrum ye-EQE kunye ne-Jsc EQE spectrum ezidityaniswe kwisixhobo esisebenza kakuhle. d Ukuxhomekeka kokukhanya okukhulu kwesixhobo se-perovskite kwi-Voc diagram. f Uhlalutyo oluqhelekileyo lwe-MKRC kusetyenziswa isixhobo se-ITO/PEDOT:PSS/perovskite/PCBM/Au esicocekileyo. I-VTFL yeyona voltage iphezulu yokuzalisa i-trap. Kule datha sibalele uxinano lwe-trap (Nt). Idatha yemvelaphi ibonelelwa ngendlela yeefayile zedatha yemvelaphi.
Ukuze kufundwe impembelelo yomaleko we-lead oxalate ekusebenzeni kwesixhobo, kusetyenziswe isakhiwo soqhagamshelwano se-FTO/TiO2/SnO2/perovskite/spiro-OMeTAD/Au sendabuko. Sisebenzisa i-formamidine chloride (FACl) njengesithako kwi-perovskite precursor endaweni ye-methylamine hydrochloride (MACl) ukuze sifezekise ukusebenza ngcono kwesixhobo, kuba i-FACl inokubonelela ngomgangatho ongcono wekristale kwaye iphephe umsantsa webhendi ye-FAPbI335 (jonga iMifanekiso eyoNgezelelweyo 1 kunye no-2 ukuze uthelekise iinkcukacha). ). 12-14). I-IPA ikhethwe njenge-antisolvent kuba ibonelela ngomgangatho ongcono wekristale kunye nolwalathiso olukhethwayo kwiifilimu ze-perovskite xa kuthelekiswa ne-diethyl ether (DE) okanye i-chlorobenzene (CB)36 (IMifanekiso eyoNgezelelweyo 15 kunye no-16). Ubukhulu be-PbC2O4 bulungiselelwe ngononophelo ukulinganisela kakuhle i-defect passivation kunye nokuthuthwa kwetshaja ngokulungelelanisa uxinaniso lwe-oxalic acid (Umfanekiso oyoNgezelelweyo 17). Imifanekiso ye-SEM enqamlezileyo yezixhobo zolawulo olulungisiweyo kunye ne-LOS iboniswe kwi-Supplementary Figure 18. Ii-currents eziqhelekileyo ze-current density (CD) zezixhobo zolawulo kunye ne-LOS ziboniswe kwi-Figure 4c, kwaye iiparameters ezikhutshiweyo zinikwe kwi-Supplementary Table 3. Iiseli zolawulo lwe-Maximum power conversion efficiency (PCE) 23.43% (22.94%), Jsc 25.75 mA cm-2 (25.74 mA cm-2), Voc 1.16 V (1.16 V) kunye ne-reverse (forward) scan. I-fill factor (FF) yi-78.40% (76.69%). I-PCE LOS PSC ephezulu yi-25.39% (24.79%), Jsc yi-25.77 mA cm-2, Voc yi-1.18 V, FF yi-83.50% (81.52%) ukusuka ngasemva (forward Scan ukuya). Isixhobo se-LOS sifumene ukusebenza kwe-photovoltaic okuqinisekisiweyo kwe-24.92% kwilebhu ye-photovoltaic yomntu wesithathu ethembekileyo (Umfanekiso oNcedisayo 19). Ukusebenza kwe-quantum yangaphandle (i-EQE) kunike i-Jsc edibeneyo ye-24.90 mA cm-2 (ulawulo) kunye ne-25.18 mA cm-2 (i-LOS PSC), ngokwahlukeneyo, eyayivumelana kakuhle ne-Jsc elinganiswe kwi-standard AM 1.5 G spectrum (Umzobo .4d). ). Ukusasazwa kwezibalo ze-PCE ezilinganisiweyo zolawulo kunye ne-LOS PSCs kuboniswe kwi-Supplementary Figure 20.
Njengoko kubonisiwe kuMfanekiso 4e, ubudlelwane phakathi kweVoc kunye nokukhanya kwabalwa ukuze kufundwe isiphumo sePbC2O4 kwi-trap-assisted surface recombination. I-slope yomgca ofakelweyo wesixhobo se-LOS yi-1.16 kBT/sq, engaphantsi kwe-slope yomgca ofakelweyo wesixhobo solawulo (1.31 kBT/sq), eqinisekisa ukuba i-LOS iluncedo ekuthinteleni i-surface recombination ngama-decoys. Sisebenzisa itekhnoloji ye-space charge current limiting (SCLC) ukulinganisa ngobuninzi i-defect density yefilimu ye-perovskite ngokulinganisa uphawu lwe-dark IV lwesixhobo se-hole (ITO/PEDOT:PSS/perovskite/spiro-OMeTAD/Au) njengoko kubonisiwe kumfanekiso. 4f Bonisa. Uxinano lwetraphu lubalwa ngefomula ethi Nt = 2ε0εVTFL/eL2, apho i-ε yi-dielectric constant ehambelanayo yefilimu ye-perovskite, i-ε0 yi-dielectric constant ye-vacuum, i-VTFL yi-voltage enomda wokugcwalisa i-trap, i-e yitshaja, i-L yi-thickness yefilimu ye-perovskite (650 nm). Uxinano lwe-defect yesixhobo se-VOC lubalwa ukuba yi-1.450 × 1015 cm–3, engaphantsi kunoxinano lwe-defect yesixhobo solawulo, oluyi-1.795 × 1015 cm–3.
Isixhobo esingafakwanga sivavanyiwe kwindawo yamandla ephezulu (MPP) phantsi kokukhanya kwelanga phantsi kwe-nitrogen ukuze kuhlolwe uzinzo lwaso lokusebenza ixesha elide (Umfanekiso 5a). Emva kweeyure ezingama-550, isixhobo se-LOS sisagcine i-92% yokusebenza kwaso okuphezulu, ngelixa ukusebenza kwesixhobo solawulo kwehle ukuya kwi-60% yokusebenza kwaso kokuqala. Ukusasazwa kwezinto kwisixhobo esidala kulinganiswe nge-time-of-flight secondary ion mass spectrometry (ToF-SIMS) (Umfanekiso 5b, c). Ukuqokelelwa okukhulu kwe-iodine kunokubonwa kwindawo ephezulu yolawulo lwegolide. Iimeko zokhuseleko lwegesi olungasebenziyo azibandakanyi izinto ezonakalisa okusingqongileyo ezifana nokufuma kunye neoksijini, nto leyo ebonisa ukuba iindlela zangaphakathi (oko kukuthi, ukufuduka kwe-ion) zinoxanduva. Ngokweziphumo ze-ToF-SIMS, ii-I- kunye ne-AuI2-ions zifunyenwe kwi-Au electrode, nto leyo ebonisa ukusasazeka kwe-I ukusuka kwi-perovskite ukuya kwi-Au. Ubunzulu besignali ye-I- kunye ne-AuI2-ions kwisixhobo solawulo buphezulu ngokuphindwe kalishumi kunobo besampulu ye-VOC. Iingxelo zangaphambili zibonise ukuba ukugqobhoza kwee-ion kunokukhokelela ekunciphiseni ngokukhawuleza kokuqhuba kwemingxuma ye-spiro-OMeTAD kunye nokubola kweekhemikhali kwileya ephezulu ye-electrode, ngaloo ndlela kubonakalise unxibelelwano oluphakathi kwisixhobo37,38. I-Au electrode isusiwe kwaye ileya ye-spiro-OMeTAD icocwe kwi-substrate ngesisombululo se-chlorobenzene. Emva koko sachaza ifilimu sisebenzisa i-grazing incidence X-ray diffraction (GIXRD) (Umfanekiso 5d). Iziphumo zibonisa ukuba ifilimu yokulawula inencopho yokugqabhuka ecacileyo kwi-11.8°, ngelixa kungekho ncopho intsha yokugqabhuka ebonakala kwisampulu ye-LOS. Iziphumo zibonisa ukuba ilahleko enkulu yee-ion ze-I kwifilimu yokulawula ikhokelela ekuvelisweni kwesigaba se-δ, ngelixa kwifilimu ye-LOS le nkqubo ithintelwe ngokucacileyo.
Iiyure ezingama-575 zokulandelela okuqhubekayo kwe-MPP kwesixhobo esingavalwanga kwindawo ene-nitrogen kunye nokukhanya kwelanga oku-1 ngaphandle kwesihluzi se-UV. Ukusasazwa kwe-ToF-SIMS kwee-b I- kunye ne-c AuI2- ions kwisixhobo sokulawula se-LOS MPP kunye nesixhobo sokuguga. Imibala etyheli, eluhlaza kunye ne-orenji ihambelana ne-Au, Spiro-OMeTAD kunye ne-perovskite. d GIXRD yefilimu ye-perovskite emva kovavanyo lwe-MPP. Idatha yomthombo inikezelwa ngendlela yeefayile zedatha yomthombo.
Ulawulo oluxhomekeke kubushushu lulinganiswe ukuqinisekisa ukuba i-PbC2O4 inokuthintela ukufuduka kwee-ion (Umfanekiso Ongezelelweyo 21). Amandla okusebenza (i-Ea) okufuduka kwee-ion amiselwa ngokulinganisa utshintsho kwi-conductivity (σ) yefilimu ye-FAPbI3 kumaqondo obushushu ahlukeneyo (T) kunye nokusebenzisa ulwalamano lwe-Nernst-Einstein: σT = σ0exp(−Ea/kBT), apho i-σ0 iyi-constant, i-kB yi-constant ye-Boltzmann. Sifumana ixabiso le-Ea kwi-slope ye-ln(σT) ngokuchasene ne-1/T, eyi-0.283 eV yolawulo kunye ne-0.419 eV yesixhobo se-LOS.
Ngamafutshane, sinikezela ngesakhelo sethiyori sokuchonga indlela yokuwohloka kwe-FAPbI3 perovskite kunye nempembelelo yeziphene ezahlukeneyo kumqobo wamandla wotshintsho lwesigaba se-α-δ. Phakathi kwezi ziphene, iziphene ze-VI ziqikelelwa ngokwethiyori ukuba zingabangela ngokulula utshintsho lwesigaba ukusuka kwi-α ukuya kwi-δ. Umaleko oxineneyo we-PbC2O4 onganyibilikiyo emanzini nozinzileyo ngokweekhemikhali ungeniswa ukuzinzisa isigaba se-α se-FAPbI3 ngokuthintela ukwakheka kwezithuba ze-I kunye nokufuduka kwee-ion ze-I. Esi sicwangciso sinciphisa kakhulu ukuhlanganiswa kwe-interfacial non-radiative, sonyusa ukusebenza kakuhle kweeseli zelanga ukuya kwi-25.39%, kwaye siphucula uzinzo lokusebenza. Iziphumo zethu zibonelela ngesikhokelo sokufezekisa ii-PSC ze-formamidine ezisebenzayo nezizinzileyo ngokuthintela utshintsho lwesigaba se-α olubangelwa ziziphene ukuya kwi-δ.
I-Titanium(IV) isopropoxide (TTIP, 99.999%) ithengwe kwiSigma-Aldrich. I-Hydrochloric acid (HCl, 35.0–37.0%) kunye ne-ethanol (anhydrous) zithengwe kwiGuangzhou Chemical Industry. I-SnO2 (15 wt% tin(IV) oxide colloidal dispersion) ithengwe kwiAlfa Aesar. I-Lead(II) iodide (PbI2, 99.99%) ithengwe kwiTCI Shanghai (China). I-Formamidine iodide (FAI, ≥99.5%), i-formamimidine chloride (FACl, ≥99.5%), i-methylamine hydrochloride (MACl, ≥99.5%), i-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%), i-4-tert -butylpyridine (tBP, 96%) ithengwe kwiXi'an Polymer Light Technology Company (eTshayina). 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). Ithengwe kwiSigma-Aldrich. I-Oxalic acid (H2C2O4, 99.9%) ithengwe kwiMacklin. Zonke iikhemikhali zisetyenziswe njengoko zifunyenwe ngaphandle kolunye utshintsho.
Ii-substrates ze-ITO okanye ze-FTO (1.5 × 1.5 cm2) zicocwe nge-ultrasonic ngesepha, i-acetone, kunye ne-ethanol imizuzu eli-10, ngokulandelelana, zaze zomiswa phantsi komjelo we-nitrogen. Umaleko oxineneyo we-TiO2 barrier ubekwe kwi-substrate ye-FTO kusetyenziswa isisombululo se-titanium diisopropoxybis (acetylacetonate) kwi-ethanol (1/25, v/v) ebekwe kwi-500 °C imizuzu engama-60. I-SnO2 colloidal dispersion ixutywe ngamanzi anyibilikisiweyo kumlinganiselo we-1:5. Kwi-substrate ecocekileyo ephathwe nge-UV ozone imizuzu engama-20, ifilimu encinci ye-SnO2 nanoparticles ibekwe kwi-4000 rpm imizuzwana engama-30 yaze yatshiswa kwi-150 °C imizuzu engama-30. Kwisisombululo se-perovskite precursor, i-275.2 mg FAI, i-737.6 mg PbI2 kunye ne-FACl (20 mol%) zinyibilikisiwe kwi-DMF/DMSO (15/1) mixed solvent. Umaleko we-perovskite walungiswa ngokufaka isisombululo se-perovskite esingama-40 μL phezu komaleko we-SnO2 ophathwe yi-UV-ozone kwi-5000 rpm emoyeni ongqongileyo imizuzwana engama-25. Imizuzwana emi-5 emva kwexesha lokugqibela, i-50 μL yesisombululo se-MACl IPA (4 mg/mL) yaphoswa ngokukhawuleza kwi-substrate njengesinyibilikisi. Emva koko, iifilimu ezisandula ukulungiswa zafakwa kwi-150°C imizuzu engama-20 zaza emva koko kwi-100°C imizuzu eli-10. Emva kokupholisa ifilimu ye-perovskite kubushushu begumbi, isisombululo se-H2C2O4 (1, 2, 4 mg enyibilikiswe kwi-1 mL IPA) safakwa kwi-4000 rpm imizuzwana engama-30 ukuze kuphumzwe umphezulu we-perovskite. Isisombululo se-spiro-OMeTAD esilungiselelwe ngokuxuba i-72.3 mg ye-spiro-OMeTAD, i-1 ml ye-CB, i-27 µl tBP kunye ne-17.5 µl ye-Li-TFSI (520 mg kwi-1 ml ye-acetonitrile) yafakwa kwifilimu nge-4000 rpm ngaphakathi kwemizuzwana engama-30. Ekugqibeleni, umaleko we-Au onobukhulu obuyi-100 nm wasuswa kwi-vacuum ngesantya se-0.05 nm/s (0~1 nm), 0.1 nm/s (2~15 nm) kunye ne-0.5 nm/s (16~100 nm).
Ukusebenza kwe-SC kweeseli zelanga ze-perovskite kulinganiswe kusetyenziswa i-Keithley 2400 meter phantsi kokukhanya kwe-solar simulator (SS-X50) kubunzulu bokukhanya obuyi-100 mW/cm2 kwaye kwaqinisekiswa kusetyenziswa iiseli zelanga ze-silicon ezilinganisiweyo. Ngaphandle kokuba kuchazwe ngenye indlela, ii-SP curves zilinganiswe kwibhokisi yeglavu egcwele i-nitrogen kubushushu begumbi (~25°C) kwiindlela zokuskena eziya phambili nezibuyela umva (inyathelo le-voltage 20 mV, ixesha lokulibaziseka yi-10 ms). Imaski yomthunzi isetyenzisiwe ukumisela indawo esebenzayo ye-0.067 cm2 kwi-PSC elinganisiweyo. Ukulinganiswa kwe-EQE kwenziwe emoyeni ojikelezileyo kusetyenziswa inkqubo ye-PVE300-IVT210 (i-Industrial Vision Technology(s) Pte Ltd) kunye nokukhanya oku-monochromatic okugxile kwisixhobo. Ukuze isixhobo sizinze, uvavanyo lweeseli zelanga ezingafakwanga luqhutywe kwibhokisi yeglavu ye-nitrogen kuxinzelelo lwe-100 mW/cm2 ngaphandle kwesihluzi se-UV. I-ToF-SIMS ilinganiswa kusetyenziswa i-PHI nanoTOFII time-of-flight SIMS. Uvavanyo lobunzulu lufunyenwe kusetyenziswa umpu we-Ar ion we-4 kV onendawo ye-400×400 µm.
Ukulinganiswa kwe-X-ray photoelectron spectroscopy (XPS) kwenziwe kwinkqubo yeThermo-VG Scientific (ESCALAB 250) kusetyenziswa i-monochromatized Al Kα (kwimo ye-XPS) kuxinzelelo lwe-5.0 × 10–7 Pa. I-scanning electron microscopy (SEM) yenziwe kwinkqubo ye-JEOL-JSM-6330F. Imo yobuso kunye nobunzima beefilimu ze-perovskite zilinganiswe kusetyenziswa i-atomic force microscopy (AFM) (Bruker Dimension FastScan). I-STEM kunye ne-HAADF-STEM zigcinwe kwi-FEI Titan Themis STEM. I-UV-Vis absorption spectra zilinganiswe kusetyenziswa i-UV-3600Plus (Shimadzu Corporation). I-Space charge limiting current (SCLC) irekhodwe kwi-Keithley 2400 meter. I-Steady-state photoluminescence (PL) kunye ne-time-resolved photoluminescence (TRPL) ye-carrier lifetime decay zilinganiswe kusetyenziswa i-FLS 1000 photoluminescence spectrometer. Imifanekiso yemephu ye-PL ilinganiswe kusetyenziswa inkqubo yeHoriba LabRam Raman i-HR Evolution. I-Fourier transform infrared spectroscopy (FTIR) yenziwe kusetyenziswa inkqubo yeThermo-Fisher Nicolet NXR 9650.
Kulo msebenzi, sisebenzisa indlela yesampulu yendlela ye-SSW ukufunda indlela yenguqu yesigaba ukusuka kwi-α-phase ukuya kwi-δ-phase. Kwindlela ye-SSW, intshukumo yomphezulu wamandla anokubakho imiselwa yindlela ye-random soft mode (i-derivative yesibini), evumela uphando oluneenkcukacha nolujolise kumphezulu wamandla anokubakho. Kulo msebenzi, isampuli yendlela yenziwa kwi-supercell ye-atom engama-72, kwaye ngaphezulu kwe-100 initial/final state (IS/FS) pairs ziqokelelwa kwinqanaba le-DFT. Ngokusekelwe kwiseti yedatha ye-IS/FS pairwise, indlela edibanisa isakhiwo sokuqala kunye nesakhiwo sokugqibela inokugqitywa ngokuhambelana phakathi kwee-athomu, kwaye emva koko intshukumo yeendlela ezimbini kumphezulu weyunithi eguquguqukayo isetyenziselwa ukumisela ngokutyibilikayo indlela yenguquko yesimo. (VK-DESV). Emva kokukhangela imeko yenguquko, indlela enethintelo esezantsi inokugqitywa ngokubeka imiqobo yamandla kwindawo.
Zonke izibalo ze-DFT zenziwe kusetyenziswa i-VASP (uhlobo 5.3.5), apho unxibelelwano lwe-electron-ion lwee-athomu ze-C, N, H, Pb, kunye ne-I zimelwe yi-projected amplified wave (PAW). Umsebenzi wokudibanisa uchazwa yi-generalized gradient approximation kwi-Perdue-Burke-Ernzerhoff parametrization. Umda wamandla wamaza endiza wawumiselwe kwi-400 eV. Igridi ye-k-point yeMonkhorst-Pack inobukhulu be-(2 × 2 × 1). Kuzo zonke izakhiwo, i-lattice kunye neendawo ze-athomu zalungiswa ngokupheleleyo de i-maximum stress component yayingaphantsi kwe-0.1 GPa kwaye i-maximum force component yayingaphantsi kwe-0.02 eV/Å. Kwimodeli yomphezulu, umphezulu we-FAPbI3 uneeleya ezi-4, umaleko osezantsi uneeleya ezizinzileyo ezilinganisa umzimba we-FAPbI3, kwaye iileya ezintathu eziphezulu zinokuhamba ngokukhululekileyo ngexesha lenkqubo yokwenza ngcono. Umaleko we-PbC2O4 ungqindilili obuyi-1 ML kwaye ufumaneka kumphezulu we-I-terminal we-FAPbI3, apho i-Pb ibotshelelwe kwi-1 I kunye ne-4 O.
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