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difεkt pasivεshכn dεn bin yuz am plεnti fכ impruv di pεrformεns fכ lid triiodide pεrכvskεyt solar sεl dεm, bכt di ifekt we difrεn difεkt dεm gεt pan α-fεz stεbiliti stil nכ klia; Hia, yuz density fכnshכnal tiori, wi aydentify fכ di fכs tεm di dεgradashכn path fכ fכmamidin lid triiodide pεrכvskayt frכm α-fεz to δ-fεz εn stכdi di ifekt fכ difrεn difεkt dεm pan di fεz transishכn εnεji barεri. Simulεshכn risכlt prεdikt se ayodin vakεns dεm kin mכst lεk fכ mek dεgradashכn biכs dεn sכmtεm lכs di enεji barεri fכ di α-δ fεz transishכn εn gεt di lכs fכmeshכn enεji na di pεrovskite sεf. di introdכkshכn fכ wan dense layεr fכ wata-insכlubul lid oksalat pan di pεrכvskayt sεf de sכmtεm inhεbit di dεkכmpozishכn fכ di α-fεz, we de prεvεnt di maygrεshכn εn volatilayzεshכn fכ ayodin. apat frכm dat, dis stratεji de ridyus intafεshal nכnraydyutiv rεkombinεshכn bכku bכku wan εn i de inkrεs di solar sεl efyushכn to 25.39% (sεtifiket 24.92%). Di divays we nɔ pak kin stil mentɛn in ɔrijinal 92% efyushɔn afta i dɔn ɔpreshɔn pan maksimal pawa fɔ 550 awa ɔnda simul 1.5 G ay mas iradyeshɔn.
Di pawa kɔnvɔshɔn efyushɔn (PCE) fɔ perovskite solar sɛl (PSC) dɔn rich wan sɛtifiket rɛkɛd ay we na 26%1. Sins 2015, di mכdan PSC dεn dכn prεfεr fכmamidin triiodide pεrכvskayt (FAPbI3) as layt-absכb layεr biכs fכ in εksεlεnt tεmral stεbiliti εn prεfrεns bכndgap we de nia di Shockley-Keisser limit we na 2,3,4. כnכfכs, FAPbI3 film dεm tεmכdaynamikli de כnda wan fεz transishכn frכm wan blak α fεz to wan yכlכ nכn-pεrovskayt δ fεz na rum tεmprachכ5,6. fכ mek di dεlta fεz nכ fכm, dεn dכn divεlכp difrεn kכmpleks pεrכvskit kכmכshכn dεm. di mכst kכmכn stratεji fכ כvakom dis prכblεm na fכ miks FAPbI3 wit wan kכmbaynshכn fכ mεtil amoniכm (MA+), sεsium (Cs+) εn bromid (Br-) ayכn7,8,9. כltu, haybrid pεrכvskayt dεm de sכfa frכm bandgap bכdinin εn fכtoindyus fεz separeshכn, we kכmprכmis di pεrformεns εn opεreshכnal stεbiliti fכ di rizultant PSC dεm10,11,12.
stכdi dεm we dεn jכs du dεn sho se pure single crystal FAPbI3 we nכ gεt εni doping gεt εksεlεnt stεbiliti biכs fכ in εksεlεnt kristכliniti εn lכw difεkt dεm13,14. fכ dat, fכ ridyus difεkt bay we yu inkrεs di kristכliniti fכ bכlk FAPbI3 na imכtant stratεji fכ achy efyushכn εn stebul PSC dεm2,15. כltu, di tεm we di FAPbI3 PSC de כpεrayshכn, dεgradashכn to di כndasaybul yכlכ hεksagכnal nכn-pεrovskayt δ fεz kin stil apin16. di prכsεs kin bigin na di sכfa dεm εn di gren bכnda dεm we kin mכr sכsεptibl fכ wata, כt εn layt biכs fכ di prεsεns fכ plεnti difεktiv εria dεm17. כl dis mek, sכfayz/grεn pasivεshכn nid fכ stεbyul di blak fεz fכ FAPbI318. bכku difεkt pasivεshכn stratεji dεm, inklud di introdכkshכn כf lכw-dimεnshכnal pεrכvskayt, asid-bεys Lεys mכlikul dεm, εn amoniכm halid sכlt dεm, dεn mek big prכgrεs insay fכmamidin PSC dεm19,20,21,22. te naw, kכlכsכl כl di stכdi dεn dכn fכkus pan di rol we difrεn difεkt dεm de ple fכ ditarmin optoεlektrכnik prכpati dεm lεk kכria rεkombinεshכn, difyushכn lεngth εn bכnd strכkchכ insay solar sεl dεm22,23,24. fכ egzampl, dεn de yuz dεnsiti fכnshכnal tiori (DFT) fכ tiori prεdikt di fכmeshכn εnεji dεm εn trap εnεji lεvεl dεm fכ difrεn dεfεkt dεm, we dεn de yuz plεnti fכ gayd prεktikal pasivεshכn disayn20,25,26. As di nɔmba fɔ di tin dɛn we nɔ fayn de go dɔŋ, di tin we di divays kin tinap tranga wan kin bɛtɛ. כltu, insay fכmamidin PSC dεm, di mεkanism dεm fכ di inflכεns fכ difrεn difεkt dεm pan fεz stεbiliti εn fכtoεlektrik prכpati dεm fכ bi komplit difrεnt. Fכ di bεst we wi no, di fכndamεntכl כndastandin כf aw dεfεkt dεm de indyuz di kubik to hεksagכnal (α-δ) fεz transishכn εn di rol we sכfayz pasivεshכn de ple pan di fεz stεbiliti fכ α-FAPbI3 pεrכvskayt stil nכ כndastand am fayn.
Hia, wi rivεl di dεgradashכn path fכ FAPbI3 perovskite frכm blak α-fεz to yכlכ δ-fεz εn di inflכεns fכ difrεn difεkt dεm pan di enεji barεri fכ α-to-δ-fεz transishכn via DFT. I vakɛns, we izi fɔ jenarayz di tɛm we dɛn de mek fim ɛn divays ɔpreshɔn, dɛn prɛdikt se dɛn go mɔs initiate di α-δ faz transishɔn. So, wi introdכks wan wata-insכlubul εn kεmikכl stebul dεns layεr כf lid כksalet (PbC2O4) pan tap כf FAPbI3 tru wan in situ riakshכn. Lid oxalate surface (LOS) de inhibit di fכmeshכn fכ I vakεnsi dεm εn de mek di I ayכn dεm nכ de muv we di hεt, layt, εn ilektrikal fil dεm de stimul am. di rizultant LOS sכmtεm ridyus intafεshal nכnraydyutiv rεkombinεshכn εn impruv FAPbI3 PSC efyushכn to 25.39% (sεtifiket to 24.92%). Di LOS divays we nɔ pak bin kip 92% pan in ɔrijinal efyushɔn afta i dɔn wok na di maksimal pawa pɔynt (MPP) fɔ pas 550 awa pan wan simul ɛya mas (AM) we na 1.5 G redyushɔn.
Wi fכs pεrform ab initio kכlkyulεshכn fכ fכnd di dεkכmpכzishכn pat fכ di FAPbI3 pεrovskite fכ transishכn frכm di α fεz to di δ fεz. tru wan ditayl fεz transfכmeshכn prכsεs, dεn fכnshכn se di transfכmeshכn frכm wan tri-dimεnshכnal kכna-shεrin [PbI6] כktahεdrכn insay di kubik α-fεz fכ FAPbI3 to wan-dimεnshכnal edj-shεrin [PbI6] כktahεdrכn insay di hεksagכnal δ-fεz fכ FAPbI3 de achy. brek 9. Pb-I de fכm wan bכnd insay di fכs step (Int-1), εn in enεji barεri de rich 0.62 eV/sεl, lεk aw dεn sho na fכg 1a. We di ɔktahedrɔn shift na di [0\(\bar{1}\)1] dairekshɔn, di heksagɔnal shɔt chen de ɛkspɛn frɔm 1×1 to 1×3, 1×4 ɛn dɔn i de go insay di δ faz. Di oriɛnteshɔn rεshɔn fɔ di ɔl pat na (011)α//(001)δ + [100]α//[100]δ. frכm di enεji distribushכn dayagram, dεn kin fכnshכn se afta di nyukliashכn fכ di δ fεz fכ FAPbI3 insay di fכlכw stej dεm, di enεji barεri de lכs pas di wan fכ di α fεz transishכn, we min se di fεz transishכn go aksεlεrat. i klia se di fכs step fכ kכntrכl di fεz transishכn na krichכ if wi want fכ sכpres α-fεz dεgradashכn.
a Faz transfכmeshכn prכsεs frכm lεft to rayt – blak FAPbI3 fεz (α-faz), fכs Pb-I bכnd klivεj (Int-1) εn fכda Pb-I bכnd klivεj (Int-2, Int -3 εn Int -4) εn yכlכ fεz FAPbI3 (delta fεz). b Enεji barεri dεm to di α to δ fεz transishכn fכ FAPbI3 bays pan difrεn intrinsik pכynt dεfεkt dεm. Di dot layn sho di enaji barɛri fɔ wan ideal kristal (0.62 eV). c Enerji fכ fכmeshכn fכ praymar pכynt dεfεkt dεm na di sεf fכ lid pεrכvskayt. di abscissa aks na di enaji barεri fכ di α-δ fεz transishכn, εn di כrdinayt aks na di enεji fכ difεkt fכmeshכn. Di pat dɛn we dɛn shed wit grey, yɔlɔ ɛn grɛn na tayp I (lɔ EB-ay FE), tayp II (ay FE) ɛn tayp III (lɔ EB-lɔ FE), rispɛktvɔli. d Enerji fכ fכmeshכn fכ difεkt VI εn LOS fכ FAPbI3 na di kכntrכl. e I barεri fכ ayכn maygrεshכn in kכntrכl εn LOS fכ FAPbI3. f – skematik ripreshɔn fɔ di maykreshɔn fɔ I ayɔn dɛn (ɔrɛnj sfɛra) ɛn gLOS FAPbI3 (grey, lid; vayɛl (ɔrɛnj), ayodin (mobayl ayodin)) na di gf kɔntrol (lɛft: tɔp we yu si; rayt: krɔs sɛkshɔn, brawn); kabɔn; layt blu – naytrɔjen; rɛd – ɔksijɛn; layt pink – haydrojɛn). Sɔs data de gi insay di fɔm fɔ sɔs data fayl dɛn.
We den sistamatli stכdi di inflכεns כf difrεn intrinsik pכynt dεfεkt dεm (inklud PbFA, IFA, PbI, εn IPb antisayt כkupεshכn; Pbi εn Ii intastitial atכm dεm; εn VI, VFA, εn VPb vakεns dεm), we dεn kכnsidr fכ bi ki fכktכr. we de mek atכmik εn enεji lεvεl fεz dεgradashכn dεn sho am na fכg 1b εn Supplementary Table 1. i intrestin fכ no se nכto כl difεkt dεm de ridyus di enεji barεri fכ di α-δ fεz transishכn (Figure 1b). Wi biliv se difεkt dεm we gεt כl tu lכw fכmeshכn εnεji εn lכw α-δ fεz transishכn εnεji barεri dεm dεn kin kכnsidr dεm as dεtrimental to fεz stεbiliti. as dεn bin ripot bifo, lid-rich sεf dεm dεn jεnarali kכnsidrεm as ifektiv fכ fכmamidin PSC27. כl dis mek wi de fכkus pan di PbI2-tεrminεt (100) sεf כnda lid-rich kכndishכn dεm. Di difεkt fכmeshכn εnεji fכ di sכfayz intrinsik pכynt difεkt dεm dεn sho am na Fig 1c εn Supplementary Table 1. Bays pan di enεji barεri (EB) εn fεz transishכn fכmeshכn εnεji (FE), dεn kכl dεn difεkt ya insay tri tכyp. Tayp I (lɔ EB-hay FE): pan ɔl we IPb, VFA ɛn VPb rili ridyus di ɛnaji barɛri fɔ faz transishɔn, dɛn gɛt ay fɔmɛshɔn ɛnaji. So, wi biliv se dɛn kayn difrɛns ya gɛt smɔl impak pan di faz transishɔn bikɔs dɛn nɔ kin fɔm. Tayp II (high EB): biכs fכ di improv α-δ fεz transishכn εnεji barεri, di anti-sayt dεfεkt PbI, IFA εn PbFA nכ de damej di fεz stεbiliti fכ α-FAPbI3 pεrכvskayt. Tayp III (lɔ EB-lɔ FE): VI, Ii ɛn Pbi difrɛns wit rili lɔw fɔmɛshɔn ɛnaji kin mek blak faz dɛgradɛshɔn. Ɛspɛshali we wi gi di FE ɛn EB VI we smɔl pas ɔl, wi biliv se di strateji we go wok pas ɔl na fɔ ridyus I vakɛns.
Fכ ridyus VI, wi divεlכp wan dense layεr fכ PbC2O4 fכ impruv di sכfayz fכ FAPbI3. we yu kכmpεr wit כrganik halid sכlt pasivεtכ dεm lεk fεnylεtilammonium ayodayd (PEAI) εn n-oktilammonium ayodayd (OAI), PbC2O4, we nכ gεt nכ mobayl halojen ayכn, na kεmikכl stebul, i nכ de sכlv insay wata, εn i izi fכ dεaktiv we dεn stimul am. Gud stebilizayshɔn fɔ sɔfayz mɔstɔ ɛn ilɛktrik fil fɔ perovskite. di sכlubiliti fכ PbC2O4 insay wata na כnli 0.00065 g/L, we ivin lכw pas di wan fכ PbSO428. mכr imכtant, dεn εn yunifכm layεr dεm fכ LOS kin sכftli pripia pan pεrovskite film dεm we de yuz in situ riakshכn (luk dכn). We pεrform DFT simulεshכn כf di intafεshal bכnding bitwin FAPbI3 εn PbC2O4 lεk aw dεn sho na Supplementary Figure 1. Supplementary Table 2 prεzεnt di dεfεkt fכmeshכn εnεji afta LOS injεkshכn. Wi fכnd se LOS nכto כnli inkrεs di fכmeshכn εnεji fכ VI difεkt dεm bay 0.69–1.53 eV (Figure 1d), bכt i de inkrεs di aktibכshכn enεji fכ I na di maygrεshכn sεf εn εkzit sεf (Figure 1e). insay di fכs stej, I ayכn dεm de muv along di pεrכvskayt sεf, we de lεf VI ayכn dεm na lat posishכn wit enεji barεri we na 0.61 eV. afta di introdכkshכn fכ LOS, biכs fכ di ifekt fכ stεrik hindrεns, di aktibכshכn εnεji fכ di maygrεshכn fכ I ayכn dεm de inkrεs to. 1.28 eV. durin di maygrεshכn fכ I ayכn dεm we de kכmכt na di pεrכvskayt sεf, di enεji barεri na di VOC de hכy bak pas di kכntrol sεmpl (Fig. 1e). Skematik dayagram dεm fכ I ayכn maygrεshכn path dεm in kכntrכl εn LOS FAPbI3 dεn sho na Fig 1 f εn g, rispεktivli. di simulεshכn risכlt sho se LOS kin inhεbit di fכmeshכn fכ VI difεkt dεm εn di volatilayzεshכn fכ I, we de mek i nכ de mek di nyuklieshכn fכ di α to δ fεz transishכn.
Di riakshכn bitwin oksalik asid εn FAPbI3 pεrכvskayt bin tεst. Afta we dɛn miks di sɔlvushɔn dɛn fɔ ɔksalik asid ɛn FAPbI3, dɛn fɔm bɔku bɔku wayt prɛsipitayt, lɛk aw dɛn sho na Supplementary Figure 2. Dɛn bin no di pauda prodakt as pure PbC2O4 matirial we dɛn yuz X-ray diffraction (XRD) (Supplementary Figure 3) ɛn Fourier transfɔm infrared spɛktroskɔpi (FTIR) (Supplementary Figure 4). Wi fכnd se oksalik asid de hεli sכlubul insay isopropyl alkol (IPA) na rum tεmprachכ wit sכlubiliti we na aprכksimatli 18 mg/mL, lεk aw dεn sho na Supplementary Figure 5. Dis de mek sכbsεkshכn prכsεsin izi biכs IPA, as kכmכn pasivεshכn sכlvεnt, nכ de damej di pεrכvskayt layεr pas sכt tεm29. So, bay we yu put di perovskite film insay oksalik asid sכlushכn כ spin-kכt di oksalik asid sכlushכn pan di pεrכvskayt, dεn kin gεt tin εn dense PbC2O4 kwik kwik wan pan di sεf fכ di pεrכvskayt film akɔdin to di kεmikכl ikwyushכn we de kam biεn: H2C2O4 + FAPbI3 = PbC2O4 + FAI +HI. FAI kin sɔlv insay IPA ɛn so dɛn kin pul am we dɛn de kuk. di tiknes fכ LOS kin kכntrol bay riakshכn tεm εn prεkursכr kכnsantreshכn.
Skanin εlektrכn maykroskכpi (SEM) imej dεm fכ kכntrol εn LOS pεrכvskayt film dεm dεn sho na Fig 2a,b. di risalts sho se di perovskite surface mכfכlכji de prεsiv fayn fayn wan, εn big nכmba fכ fayn patikyula dεm de dכn dכn pan di gren sεf, we fכ riprizent wan PbC2O4 layεr we di in-situ riakshכn fכm. Di LOS perovskite film gɛt smɔl smol sɔfays (Supplementary Figure 6) ɛn big wata kɔntakt angle we yu kɔmpia am wit di kɔntrol film (Supplementary Figure 7). Dɛn yuz ay-rɛzolushɔn transvas transmishɔn ilɛktron maykroskɔpi (HR-TEM) fɔ difrɛns di sɔfayz layt fɔ di prɔdak. we yu kכmpεr wit di kכntrol film (Fig. 2c), wan yunifכm εn dense tin layεr wit tik we bכt 10 nm de klia wan pan tap di LOS pεrovskite (Fig. 2d). yuz ay-angle anulכr dak-fild skan εlektrכn maykroskכpi (HAADF-STEM) fכ egzamin di intafεys bitwin PbC2O4 εn FAPbI3, di prεsεns fכ kristalin rijyכn dεm fכ FAPbI3 εn amorphous rijyכn dεm fכ PbC2O4 kin klia wan (Supplementary Figure 8). Di surface kompozishun fכ di perovskite afta oxalic acid tritmεnt bin kכntribyut bay X-ray fכtoεlektrכn spεktroskopi (XPS) mεzjכmεnt, lεk aw dεn sho na Fig 2e–g. insay Fig 2e, di C 1s pik dεm arawnd 284.8 eV εn 288.5 eV de pan di spεsifi k CC εn FA signal dεm, rispεktivli. we yu kכmpεr wit di kכntrol mεmbran, di LOS mεmbran sho wan adishכnal pik na 289.2 eV, we dεn atribyut to C2O42-. Di O 1s spεktrum fכ LOS perovskite de sho tri kεmikכl difrεnt O 1s pik dεm na 531.7 eV, 532.5 eV, εn 533.4 eV, we kכrεspכnd to diprotonated COO, C=O fכ intakt oksalayt grup 30 εn O atכm dεm fכ di OH kכmכpכnt (Fig. 2e ). )). Fכ di kכntrol sεmpl, na כnli sכm O 1s pik dεn bin obsεv, we kin atribyut to כksijεn kεmisכrb pan di sכfa. di kכntrol mεmbran kכntribyushכn dεm fכ Pb 4f7/2 εn Pb 4f5/2 de na 138.4 eV εn 143.3 eV, rispεktivli. Wi obsכv se di LOS perovskite de sho shift pan di Pb pik we de bכt 0.15 eV tכwεd hכy binding enεji, we sho se strכng intarakshכn bitwin di C2O42- εn Pb atכm dεm (Fig. 2g).
a SEM imej dɛn fɔ kɔntrol ɛn b LOS perovskite film dɛn, ɔp viu. c Ha-rεsכlushכn kכros-sekshכnal transmishכn εlektrכn maykroskכpi (HR-TEM) כf kכntrכl εn d LOS pεrכvskayt film dεm. High-rezolushɔn XPS fɔ e C 1s, f O 1s ɛn g Pb 4f perovskite film dɛn. Sɔs data de gi insay di fɔm fɔ sɔs data fayl dɛn.
Akɔdin to di DFT rizɔlt, dɛn tiori prɛdikt se VI difrɛns ɛn I maykreshɔn izi fɔ mek di faz transishɔn frɔm α to δ. di ripot dεm we bin de bifo dεn sho se I2 de rilis kwik kwik wan frכm PC-bεys pεrכvskayt film dεm we dεn de fכto-imεshכn afta dεn εkspכz di film dεm to layt εn tεmכl strεs31,32,33. Fכ kכnfכm di stεbyulεshכn ifekt we lid oksalayt gεt pan di α-fεz fכ pεrכvskεyt, wi imers di kכntrכl εn LOS pεrכvskεyt film dεm insay transparent glas bכtul dεm we kכntεn toluεn, rispεktivli, εn afta dat wi iradiet dεm wit 1 san layt fכ 24 h. Wi bin mɛzhɔ di absɔpshɔn fɔ ɔltra vayolɛt ɛn visible layt (UV-Vis). ) toluene sכlushכn, lεk aw dεn sho na fכg 3a. Kכmpεr wit di kכntrol sεmpl, dεn obsεv bכku lכw I2 absכpshכn intensiti in di kes fכ LOS-perovskite, we sho se kompakt LOS kin inhεbit di rilis fכ I2 frכm di perovskite film di tεm we layt imεshכn. fכtograf dεm fכ di ol kכntrכl εn LOS pεrכvskit film dεm dεn sho na di insεt dεm na Fig 3b εn c. Di LOS perovskite stil blak, we bɔku pan di kɔntrol fim dɔn tɔn yɔlɔ. Di UV–visible absכpshכn spεktra fכ di imers film dεn sho na Figs. 3b, c. Wi obsכv se di absכpshכn we kכrεspכnd to α insay di kכntrol film bin klia wan dεkrεs. X-ray mεzhɔmεnt dεn bin du fכ dכkument di evolushכn כf di kristכl strכkchכ. Afta 24 awa we di layt de shayn, di kɔntrol perovskite sho wan strɔng yɔlɔ δ-faz signal (11.8°), we di LOS perovskite stil de mentɛn gud blak faz (Figure 3d).
UV-visible absכpshכn spεktra fכ toluene sכlushכn we di kכntrol film εn LOS film bin imersh כnda 1 san layt fכ 24 awa. Di inset sho wan vayl we dɛn bin put ɛni fim insay wan ikwal volyum we gɛt toluɛn. b UV-Vis absכpshכn spεktra fכ kכntrol film εn c LOS film bifo εn afta 24 h fכ imershכn כnda 1 san layt. Di inset sho wan foto fɔ di tɛst fim. d X-ray difrεkshכn patεn dεm fכ kכntrol εn LOS film dεm bifo εn afta 24 h we dεn εkspכz. SEM imej dεm fכ kכntrol film e εn film f LOS afta 24 awa we dεn εkspכz. Sɔs data de gi insay di fɔm fɔ sɔs data fayl dɛn.
Wi bin du skan εlektrכn maykroskכpi (SEM) mεjכmεnt fכ obsכv di maykrostrכkchכral chenj dεm na di pεrכvskayt film afta 24 awa iluminεshכn, lεk aw dεn sho na Fig 3e,f. In di kontrכl film, big gren dεm bin dεstroy εn tכn to sכm nidul, we kכrεspכnd to di mכfכlכji fכ di δ-fεz prodak FAPbI3 (Fig. 3e). Fכ LOS film dεm, di perovskite gren dεm de stil de insay gud kכndishכn (Figure 3f). di risal dεm kכnfכm se di lכs fכ I de sכmtεm indyuz di transishכn frכm di blak fεz to di yכlכ fεz, we PbC2O4 de stεbyul di blak fεz, we de prεvεnt di lכs fכ I. Bikɔs di vakεns dεnsiti na di sεf de bכku hכy pas di gren bכlk,34 dis fεz de mכr lεk fכ apin na di sεf fכ di gren. wan tεm we i de rilis ayodin εn fכm VI. as dεn prεdikt bay DFT, LOS kin inhεbit di fכmeshכn fכ VI dεfεkt dεm εn prεvεnt di maygrεshכn fכ I ayכn dεm to di pεrovskite sεf.
Apat frɔm dat, dɛn bin stɔdi di ifɛkt we di PbC2O4 layt gɛt pan di mɔstɔ rɛsistɛns fɔ di perovskite film dɛn na atmosfɛrik ɛya (rɛlativ humiditi 30-60%). As yu si na Supplementary Figure 9, di LOS perovskite bin stil blak afta 12 dez, we di kontrכl film bin tכn yכlכ. insay XRD mεjכmεnt, di kכntrol film sho wan strכng pik na 11.8° we kכrεspכnd to di δ fεz fכ FAPbI3, we di LOS pεrovskite de rεtεn di blak α fεz fayn fayn wan (Supplementary Figure 10).
Stedi-stet fotoluminesεns (PL) εn tεm-rεsolv fכtoluminesεns (TRPL) bin yuz fכ stכdi di pasivεshכn ifekt כf lid כksalet pan di pεrכvskεyt sεf. In Fig. Figure 4a sho se di LOS film dɔn inkrisayz PL intensiti. Insay di PL map imej, di intensiti fɔ di LOS film ova di ɔl eria we na 10 × 10 μm2 ay pas di wan fɔ di kɔntrol film (Supplementary Figure 11), we sho se PbC2O4 yunifom pasiv di perovskite film. di kεriכn layf tεm dεn de ditarεmin bay we dεn aprכksimat di TRPL dεkayshכn wit wan singl εkspכnεshכnal fכnshכn (Fig. 4b). di kכria layf tεm fכ di LOS film na 5.2 μs, we bכku lכng pas di kכntrol film wit kכriכ layf tεm we na 0.9 μs, we sho se di rεdכks sכfayz nכnraydiεtiv rεkombinεshכn.
Stedi-stet PL ɛn b-spɛktra fɔ tɛmporari PL fɔ perovskite film dɛn pan glas sabstret dɛn. c SP kεrv כf di divays (FTO/TiO2/SnO2/perovskite/spiro-OMeTAD/Au). d EQE spɛktrum ɛn Jsc EQE spɛktrum intagret frɔm di mɔs efishɔnal divays. d Dipεndεns כf layt intensiti כf wan pεrכvskayt divays pan di Voc dayagram. f Tipik MKRC analisis we yuz wan ITO/PEDOT:PSS/perovskite/PCBM/Au klin ol divays. VTFL na di maksimal trap filin vɔlɔt. Frɔm dɛn data ya wi kɔl di trap density (Nt). Sɔs data de gi insay di fɔm fɔ sɔs data fayl dɛn.
Fכ stכdi di ifekt we di lid oksalayt layt gεt pan di divays pεrformεns, dεn yuz wan tradishכnal FTO/TiO2/SnO2/perovskite/spiro-OMeTAD/Au kכntakt strכkchכ. Wi de yuz formamidine chloride (FACl) as aditiv to di perovskite precursor insted of methylamine hydrochloride (MACl) fɔ ajɔst bɛtɛ divays pefɔmɛns, bikɔs FACl kin gi bɛtɛ kristal kwaliti ɛn avɔyd di band gap fɔ FAPbI335 (luk Supplementary Figures 1 ɛn 2 fɔ ditayli kɔmpiashɔn). ). 12-14). IPA bin pik as di antisolvent bikɔs i de gi bɛtɛ kristal kwaliti ɛn prɛferɛd ɔryenteshɔn insay perovskite film dɛn kɔmpia to diethyl ether (DE) ɔ klorobenzene (CB)36 (Supplementary Figures 15 ɛn 16). Di tiknes fɔ PbC2O4 bin tek tɛm ɔptimayz fɔ wɛl balans difɛkt pasivɛshɔn ɛn chaj transpɔt bay we dɛn adjɔst di ɔksalik asid kɔnsɛntreshɔn (Supplementary Figure 17). Krɔs-sekshɔnal SEM imej dɛn fɔ di ɔptimayz kɔntrol ɛn LOS divays dɛn sho na Supplementary Figure 18. Tipik kɔrɛnt dɛnsiti (CD) kɔv fɔ kɔntrol ɛn LOS divays dɛn sho na Fig 4c, ɛn di paramita dɛn we dɛn pul kɔmɔt na di Supplementary Table 3. Maksimal pawa kɔnvɔshɔn efyushɔn (PCE) kɔntrol sɛl dɛn 23.43% (22.94%), Jsc 25.75 mA cm-2 (25.74 mA cm-2), Voc 1.16 V (1.16 V) ɛn rivays (fɔwad) skan. Di fil faktɔ (FF) na 78.40% (76.69%). Maksimal PCE LOS PSC na 25.39% (24.79%), Jsc na 25.77 mA cm-2, Voc na 1.18 V, FF na 83.50% (81.52%) frɔm rivas (fɔwad Skan to). Di LOS divays ajɔst wan sɛtifiket fotovoltayk pefɔmɛns we na 24.92% insay wan trɔst tɔd-pati fotovoltayk laboratori (Saplimɛnt Fig 19). Di eksternal kwantum efyushɔn (EQE) gi wan intagreted Jsc we na 24.90 mA cm-2 (kɔntrol) ɛn 25.18 mA cm-2 (LOS PSC), rispɛktvɔli, we bin de insay gud agrimɛnt wit di Jsc we dɛn mɛzhɔ insay di standad AM 1.5 G spɛktrum (Fig. .4d). ) . Di statystik distribyushɔn fɔ di PCE dɛn we dɛn mɛzhɔ fɔ kɔntrol ɛn LOS PSC dɛn de sho na Suplimɛnt Fig 20.
As yu si na Fig 4e, di rilayshכn bitwin Voc εn layt intensiti bin kכl fכ stכdi di ifekt we PbC2O4 gεt pan trap-asist surface rεkombinεshכn. Di slɔp fɔ di fit layn fɔ di LOS divays na 1.16 kBT/sq, we smɔl pas di slɔp fɔ di fit layn fɔ di kɔntrol divays (1.31 kBT/sq), we kɔnfyus se LOS yusful fɔ inhibit sɔfayz rikombineshɔn bay dɛkɔy. Wi de yuz spɛs chaj kɔrɛnt limitin (SCLC) teknɔlɔji fɔ kwantiti fɔ mɛzhɔ di difrɛns dɛnsiti fɔ wan perovskite film bay we wi de mɛzhɔ di dak IV karakta fɔ wan ol divays (ITO/PEDOT:PSS/perovskite/spiro-OMeTAD/Au) lɛk aw dɛn sho na di figa. 4f Sho. Di trap density na di fɔmula Nt = 2ε0εVTFL/eL2, usay ε na di rilitiv dayelɛktrik kɔnstant fɔ di perovskite film, ε0 na di dayelɛktrik kɔnstant fɔ vaykum, VTFL na di limitin vɔlɔt fɔ ful di trap, e na di chaj, L na di tiknes fɔ di perovskite film (650 nm). di difεkt dεnsiti fכ di VOC divays dεn kכl am fכ bi 1.450 × 1015 cm–3, we lכw pas di difεkt dεnsiti fכ di kכntrol divays, we na 1.795 × 1015 cm–3.
Di divays we nɔ pak bin tɛst na di maksimal pawa pɔynt (MPP) ɔnda ful de layt ɔnda naytrɔjen fɔ ɛgzamin in lɔng tɛm pefɔmɛns stebiliti (Figure 5a). Afta 550 awa, di LOS divays stil bin de mentɛn 92% pan in maksimal efyushɔn, we di kɔntrol divays in pefɔmɛns bin dɔn drɔp to 60% pan in ɔrijinal pefɔmɛns. Di distribushɔn fɔ di ɛlimɛnt dɛn na di ol divays bin mɛzhɔ bay tɛm-ɔf-flay sɛkɔndari ayɔn mas spɛktrometri (ToF-SIMS) (Fig. 5b, c). yu kin si big akumuleshכn fכ ayodin na di כp gold kכntrכl εria. Di kondishɔn dɛm fɔ inɛt gas protɛkshɔn nɔ de inklud tin dɛm we de pwɛl di envayrɔmɛnt lɛk mɔstɔ ɛn ɔksijɛn, we de sho se intanɛnt mɛkanism dɛm (dat na, ayɔn maykreshɔn) na dɛn de ripɔtabl. Akɔdin to ToF-SIMS rizɔlt, dɛn bin detekt I- ɛn AuI2- ayɔn dɛn na di Au ilɛktrɔd, we sho di difyushɔn fɔ I frɔm di perovskite insay Au. di signal intensiti fכ I- εn AuI2- ayכn dεm na di kכntrol divays na aprכksimatli 10 tεm hכy pas di wan fכ di VOC sεmpl. di ripot dεm we dεn bin dכn du bifo dis tεm dεn sho se ayכn pεrmieshכn kin mek di ol kכnduktiviti fכ spiro-OMeTAD dכn kwik kwik wan εn kεmikכl kכrכshכn fכ di tכp εlektrod layεr, we de mek di intafεshal kכntakt na di divays de dכn37,38. Di Au ilɛktrɔd bin kɔmɔt ɛn di spiro-OMeTAD layt bin klin frɔm di sabstret wit wan klorobenzin sɔlvushɔn. We den karaktaiz di film yuz grazing insidɛns X-ray difrakshɔn (GIXRD) (Figure 5d). di risalts sho se di kontrכl film gεt klia difrεkshכn pik na 11.8°, we nכ nyu difrεkshכn pik de apia na di LOS sεmpl. di risalts sho se big lכs dεm fכ I ayכn dεm na di kכntrol film de lid to di jεnereshכn fכ di δ fεz, we insay di LOS film dis prכsεs de inhεbit klia wan.
575 awa kɔntinyu MPP trak fɔ wan divays we nɔ sial na naytrɔjen atmosfɛs ɛn 1 san layt we nɔ gɛt UV filta. ToF-SIMS distribyushɔn fɔ b I- ɛn c AuI2- ayɔn dɛn na di LOS MPP kɔntrol divays ɛn ol divays. Di shed dɛm fɔ yɔlɔ, grɛn ɛn ɔrɛnj kɔrɛspɔnd to Au, Spiro-OMeTAD ɛn perovskite. d GIXRD di perovskite film afta MPP test. Sɔs data de gi insay di fɔm fɔ sɔs data fayl dɛn.
Tεmprachכ-dipεndεnt kכnduktiviti bin mεzj fכ kכnfכm se PbC2O4 kin inhεbit ayכn maygrεshכn (Supplementary Figure 21). Di aktibyushɔn ɛnaji (Ea) fɔ ayɔn maykreshɔn de ditarmin bay we dɛn mɛzhɔ di chenj in kɔnduktiviti (σ) na di FAPbI3 film na difrɛn tɛmpracha (T) ɛn yuz di Nernst-Einstein rileshɔn: σT = σ0exp(−Ea/kBT), usay σ0 na kɔnstant, kB na di Boltzmann kɔnstant. Wi gɛt di valyu fɔ Ea frɔm di slɔp fɔ ln(σT) versus 1/T, we na 0.283 eV fɔ di kɔntrol ɛn 0.419 eV fɔ di LOS divays.
in sכmari, wi provayd wan tiori fכm fכ aydentify di dεgradashכn path fכ FAPbI3 perovskite εn di inflכεns fכ difrεn difεkt dεm pan di enεji barεri fכ di α-δ fεz transishכn. pan dεn difεkt dεm ya, dεn tiori prεdikt VI difεkt dεm fכ izi fכ mek fεz transishכn frכm α to δ. wan wata-insכlubul εn kεmikכl stebul dεns layεr fכ PbC2O4 dεn introdכks fכ stεbyul di α-fεz fכ FAPbI3 bay we i de inhεbit di fכmeshכn fכ I vakεns dεm εn di maygrεshכn fכ I ayכn dεm. Dis strateji de ridyus di intafeshal nכn-raydiativ rεkombinεshכn sכmtεm, i de inkrεs di solar sεl efyushכn to 25.39%, εn i de impruv di כpεrayshכn stεbiliti. di rizulεt dεm we wi gεt de gi gayd fכ achy efyushכn εn stebul fכmamidin PSC dεm bay we dεn de inhεbit di dεfεkt-indyus α to δ fεz transishכn.
Titanium(IV) isopropoxide (TTIP, 99.999%) bin bay frɔm Sigma-Aldrich. Dɛn bin bay haydroklɔrik asid (HCl, 35.0–37.0%) ɛn ɛtɛnol (anhaydrous) frɔm Guangzhou Kɛmikɛl Indastri. SnO2 (15 wt% tin(IV) oksayd kolכyd dispershכn) bin bay frכm Alfa Aesar. Lid(II) ayodayd (PbI2, 99.99%) bin bay frɔm TCI Shanghai (Chaina). Fɔmamidin ayodayd (FAI, ≥99.5%), fɔmamidin klorayd (FACl, ≥99.5%), mɛtylamin haydroklɔrayd (MACl, ≥99.5%), 2,2′,7,7′-tɛtrakis-(N, N-di-p) )-mɛtɔksianilin)-9,9′-spirobifluorin (Spiro-OMeTAD, ≥99.5%), lithium bis(trifluoromethane)sulfonylimide (Li-TFSI, 99.95%), 4-tert -butylpyridine (tBP, 96%) bin bay frɔm Xi'an Polima Layt Tɛknɔlɔji Kɔmni (Chaina). N,N-dimethylformamide (DMF, 99.8%), dimetil salfoksayd (DMSO, 99.9%), isopropyl alkol (IPA, 99.8%), klorobenzine (CB, 99.8%), asetonitril (ACN). Dɛn bay am frɔm Sigma-Aldrich. Oksalik asid (H2C2O4, 99.9%) bin bay frɔm Maklin. Dɛn bin yuz ɔl di kemikal dɛn lɛk aw dɛn bin gɛt dɛn ɛn dɛn nɔ bin mek ɛni ɔda chenj.
ITO ɔ FTO sabstret (1.5 × 1.5 cm2) bin ultrasonically klin wit ditajɛn, asɛtɔn, ɛn ɛtɛnol fɔ 10 min, rispɛktvɔli, ɛn afta dat dɛn drɛy ɔnda wan naytrɔjen strim. A dense TiO2 barɛri layt bin deposit pan wan FTO sabstret yuz wan sɔlvushɔn fɔ taytaniɔm diisopropoxybis(acetylacetonate) insay ɛtɛnol (1/25, v/v) we dɛn deposit na 500 °C fɔ 60 min. Di SnO2 kolכyd dispershכn bin diluted wit deionized wata insay wan volyum rεshכn we na 1:5. Na klin sabstret we dɛn trit wit UV ɔzɔn fɔ 20 minit, dɛn bin put wan tin film we gɛt SnO2 nanopartikul dɛn na 4000 rpm fɔ 30 sɛkɔn ɛn afta dat dɛn bin prɛhɛt am na 150 °C fɔ 30 minit. Fכ di perovskite prεkursכr sכlushכn, 275.2 mg FAI, 737.6 mg PbI2 εn FACl (20 mol%) bin sכlv insay DMF/DMSO (15/1) miks sכlvεnt. Di perovskite layt bin pripia bay we dɛn sɛntrifug 40 μL perovskite prɛkursɔ sɔlshɔn pan tap di UV-ɔzɔn-trit SnO2 layt na 5000 rpm insay ambiɛnt ɛya fɔ 25 s. 5 sekכnd afta di las tεm, 50 μL MACl IPA sכlushכn (4 mg/mL) bin dכp kwik kwik wan pan di sabstεrayt as antisכlvεnt. Afta dat, di films we dɛn jɔs pripia bin anɛl na 150°C fɔ 20 min ɛn afta dat na 100°C fɔ 10 min. Afta we dɛn dɔn kol di perovskite film to rum tɛmpracha, H2C2O4 sɔlvushɔn (1, 2, 4 mg we dɛn sɔlv insay 1 mL IPA) bin sɛntrifug na 4000 rpm fɔ 30 s fɔ pasiv di perovskite sɔfays. Wan spiro-OMeTAD solushɔn we dɛn pripia bay we dɛn miks 72.3 mg spiro-OMeTAD, 1 ml CB, 27 μl tBP ɛn 17.5 μl Li-TFSI (520 mg insay 1 ml asɛtonitril) bin spin-kɔt pan di fim pan 4000 rpm insay 30 s. Fɔ dɔn, dɛn bin ɛvapɔret wan 100 nm tik Au layt insay vaykum pan wan rit we na 0.05 nm/s (0~1 nm), 0.1 nm/s (2~15 nm) ɛn 0.5 nm/s (16~100 nm) . ).
Di SC pefɔmans fɔ di perovskite solar sɛl dɛn bin mɛzhɔ yuz wan Keithley 2400 mita ɔnda solar simulator iluminɛshɔn (SS-X50) pan layt intensiti we na 100 mW/cm2 ɛn dɛn bin verify yuz kalibrayt standad silikon solar sɛl dɛn. If dɛn nɔ tɔk ɔda tin, dɛn bin mɛzhɔ SP kɔv dɛn insay wan naytrɔjen-ful glɔv bɔks na rum tɛmpracha (~25°C) insay fɔdɔm ɛn rivas skan mɔd (vɔlt stɛp 20 mV, dilɛy tɛm 10 ms). Wan shado mask bin yuz fɔ no wan ifektiv eria we na 0.067 cm2 fɔ di PSC we dɛn mɛzhɔ. EQE mεjכmεnt bin kכriכnt insay ambiεnt εya yuz wan PVE300-IVT210 sistεm (Industrial Vision Technology(s) Pte Ltd) wit monokromatik layt we fכkus pan di divays. Fɔ divays stebiliti, dɛn bin du tɛst fɔ nɔ-ɛnkapsul solar sɛl dɛn insay naytrɔjen glɔvbɔks pan 100 mW/cm2 prɛshɔn we nɔ gɛt UV filta. ToF-SIMS na we dɛn de mɛzhɔ yuz PHI nanoTOFII tɛm-ɔf-flay SIMS. Dip profayl bin ɔbtain yuz wan 4 kV Ar ayɔn gɔn wit wan eria we na 400×400 μm.
X-ray fotoelektrɔn spɛktroskɔpi (XPS) mɛzhɔmɛnt dɛn bin du pan wan Thermo-VG Scientific sistem (ESCALAB 250) we yuz monokromatized Al Kα (fɔ XPS mod) pan prɛshɔn we na 5.0 × 10–7 Pa. Dɛn bin du skan ilɛktron maykroskɔpi (SEM) pan wan JEOL-JSM-6330F sistem. Di surface morphology ɛn roughness fɔ di perovskite film dɛn bin mɛzhɔ yuz atɔmik fɔs maykroskɔpi (AFM) (Bruker Dimension FastScan). STEM ɛn HAADF-STEM de na di FEI Titan Themis STEM. UV–Vis absɔpshɔn spɛktra dɛn bin mɛzhɔ yuz wan UV-3600Plus (Shimadzu Kɔpɔreshɔn). Space charge limiting current (SCLC) bin rikodɔ pan wan Keithley 2400 mita. Stedi-stet fotoluminesεns (PL) εn tεm-rεsolv fכtoluminesεns (TRPL) כf kεriכ layftaym dεkay bin mεzj yuz wan FLS 1000 fotoluminesεns spεktrכmita. PL map imej dɛn bin mɛzhɔ yuz wan Horiba LabRam Raman sistɛm HR Ɛvɔlɔshɔn. Fourier transfɔm infrarɛd spɛktroskɔpi (FTIR) bin de yuz wan Thermo-Fisher Nicolet NXR 9650 sistem.
In dis wok, wi yuz di SSW pat sampling mεtכd fכ stכdi di fεz transishכn pat frכm α-faz to δ-faz. Insay di SSW we, di muvmɛnt fɔ di pɔtɛnɛshɛl ɛnaji sɔfays na di dairekshɔn fɔ di random sɔft mɔd (sɛkɔn dɛrivativ), we de alaw fɔ du ditayl ɛn ɔbjɛktiv stɔdi fɔ di pɔtɛnɛshɛl ɛnaji sɔfays. insay dis wok, dεn de du pat sεmpl pan 72-atכm supεrsεl, εn dεn kכlekt mכr dan 100 initial/faynal stet (IS/FS) pe dεm na di DFT lεvεl. Bays pan di IS/FS pairwise data set, di pat we kɔnɛkt di initial strɔkchɔ ɛn di fayn strɔkchɔ kin bi wit di kɔrɛspɔndɛns bitwin atɔm dɛn, ɛn afta dat dɛn kin yuz di tu-we muvmɛnt along di vɛriɔbul yunit sɔfa fɔ smol smol ditarmin di transishɔn stet we. (VK-DESV) we dɛn kɔl. Afta dɛn dɔn fɛn di transishɔn stet, dɛn kin no di rod we gɛt di lɔs barɛri bay we dɛn rank di ɛnaji barɛri dɛn.
Ɔl di DFT kɔlkyulɛshɔn dɛn bin du yuz VASP (vɛshɔn 5.3.5), usay di ilɛktron–ayɔn intarakshɔn dɛn fɔ C, N, H, Pb, ɛn I atɔm dɛn de riprizent bay wan projɛkt amplifyed wɛv (PAW) skim. Di εkshεnj kכrεleshכn fכnshכn dεn dεskrεb am bay di jεnaralisεd grεdiεnt aprכksimεshכn in di Pεrdue-Bכrkε-Ernzεrכf paramεtrayzεshכn. Di enaji limit fɔ plen wev dɛn bin sɛt to 400 eV. Di Monkhorst–Pack k-point grid gɛt sayz we na (2 × 2 × 1). Fɔ ɔl di strɔkchɔ dɛn, lat ɛn atɔmik pozishɔn dɛn bin ful ɔptimayz te di maksimal strɛs kɔmpɔnɛnt bin de dɔŋ 0.1 GPa ɛn di maksimal fɔs kɔmpɔnɛnt bin de dɔŋ 0.02 eV/Å. insay di sכfayz mכdel, di sכfayz fכ FAPbI3 gεt 4 layεr, di bכtכm layεr gεt fiks atכm dεm we de simul di bכdi fכ FAPbI3, εn di tכp tri layεr dεm kin muv fri wan di tεm we di optimayzεshכn prכsεs de. di PbC2O4 layεr na 1 ML tik εn i de na di I-tεrminal sεf fכ FAPbI3, usay Pb de bכnd to 1 I εn 4 O.
Fɔ no mɔ bɔt di we aw dɛn mek di stɔdi, si di Natural Portfolio Report Abstract we gɛt fɔ du wit dis atikul.
Ɔl di data we dɛn gɛt ɔ analayz we dɛn de du dis stɔdi, de insay di atikul we dɛn dɔn pablish, ɛn bak insay di sɔpɔt infɔmeshɔn ɛn raw data fayl dɛn. Di raw data we dɛn prɛzɛnt na dis stɔdi de na https://doi.org/10.6084/m9.figshare.2410016440. Dɛn gi di sɔs data fɔ dis atikul.
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