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Kucitsa emaphutsa kusetjentiswe kakhulu kwenta ncono kusebenta kwemangcamuzane elanga e-lead triiodide perovskite, kepha umphumela wemaphutsa lehlukahlukene ekusimameni kwe-α-phase solo awucaci; Lapha, sisebentisa density theory lokusebenta, sikhomba kwekucala indlela yekubola kwe-formamidine lead triiodide perovskite kusuka ku-α-sigaba kuya ku-δ-sigaba bese sifundza umphumela wetici letehlukahlukene esivimbelweni semandla ekugucuka kwesigaba. Imiphumela yekulingisa ibiketela kutsi tikhala te iodine tingabangela kakhulu kubola ngoba tehlisa kakhulu sivimbelo semandla sekugucuka kwesigaba se α-δ futsi tinemandla laphansi ekwakheka endzaweni ye perovskite. Kwetfulwa kwelucwencwe lolucinile lwe lead oxalate lengancibiliki emantini etulu kwe perovskite kuvimbela kakhulu kubola kwe α-phase, kuvikela kuhamba kanye nekugucuka kwe iodine. Ngetulu kwaloko, lelisu linciphisa kakhulu kuhlanganiswa kabusha kwe-interfacial nonradiative futsi likhulisa kusebenta kahle kwemaseli elanga kuya ku-25.39% (kucinisekisiwe 24.92%). Ledivaysi lengakapakishwa isakhona kugcina kusebenta kwayo kwekucala lokungu 92% ngemuva kwekusebenta ngemandla lamakhulu emahora langu 550 ngaphansi kwekulingisa kwemoya we 1.5 G.
Kusebenta kahle kwekugucula emandla (i-PCE) kwemaseli elanga e-perovskite (ema-PSC) sekufinyelele esigabeni lesiphakeme lesicinisekisiwe se-26%1. Kusukela nga 2015, ema PSC esimanje akhetsa i-formamidine triiodide perovskite (FAPbI3) njengelucwencwe lolutsatsa kukhanya ngenca yekusimama kwayo lokuhle kakhulu kwekushisa kanye nekukhetsa ibhande lesedvute nemkhawulo we Shockley-Keisser we 2,3,4. Ngelishwa, emafilimu e-FAPbI3 ngendlela yekushisa ahamba ngesigaba sekushintja kusuka esigabeni se-α lesimnyama kuya esigabeni se-δ lesimtfubi lesingasiyo i-perovskite ngesikhatsi sekushisa kweligumbi5,6. Kuvikela kwakheka kwesigaba se delta, kwakhiwa kwetintfo letehlukene letiyinkimbinkimbi te perovskite. Lisu lelivame kakhulu lekuncoba lenkinga kuhlanganisa iFAPbI3 ngenhlanganisela ye-methyl ammonium (MA+), i-cesium (Cs+) kanye ne-bromide (Br-) ions7,8,9. Kepha, ema perovskites lahlanganisiwe ahlushwa bandgap kwandziswa kanye nekuhlukaniswa kwesigaba photoinduced, lokucedza kusebenta kanye nekusimama kwekusebenta kwe PSCs10,11,12 lephumelako.
Tifundvo takamuva tikhombise kutsi i-FAPbI3 lehlantekile ye-crystal yinye ngaphandle kwe-doping inekusimama lokuhle kakhulu ngenca ye-crystallinity yayo lenhle kakhulu kanye netici letiphansi13,14. Ngako-ke, kunciphisa emaphutsa ngekukhulisa i-crystallinity ye-FAPbI3 lenkhulu lisu lelibalulekile lekufeza PSCs2,15 lesebenta kahle nalezinzile. Kepha, ngesikhatsi sekusebenta kwe-FAPbI3 PSC, kwehliswa kwesigaba se-hexagonal lesingatsandzeki lesingasiyo i-perovskite δ kungenteka16. Lenchubo ivame kucala etindzaweni letingetulu kanye nemincele yetinhlavu letsatseka kalula emanti, kushisa kanye nekukhanya ngenca yekubakhona kwetindzawo letiningi letinesici17. Ngakoke, kukhishwa kwemhlabatsi/kwetinhlavu kuyadzingeka kwentela kusimamisa sigaba lesimnyama se FAPbI318. Emasu lamanyenti ekucedza sici, kufaka ekhatsi kwetfulwa kwema-perovskites laphansi, emamolekhyuli e-Lewis lane-esidi, kanye netinsawoti te-ammonium halide, kwente inchubekelembili lenkhulu kuma-PSCs e-formamidine19,20,21,22. Kuze kube ngumanje, cishe tonkhe tifundvo tigcile endzimeni yetici letehlukahlukene ekuncumeni timphahla te-optoelectronic letifana nekuhlanganiswa kabusha kwetitfwali, budze bekusakateka kanye nesakhiwo sebhande kumaseli elanga22,23,24. Sibonelo, ithiyori lesebentako ye-density (DFT) isetjentiselwa kucagela ngekwetifundvo emandla ekwakheka kanye nekubamba emazinga emandla etici letehlukahlukene, letisetjentiswa kakhulu kucondzisa umklamo we-passivation losebentako20,25,26. Njengobe linani letici lincipha, kusimamisa ledivayisi kuvame kuba ncono. Kepha, ku formamidine PSCs, tindlela tekutsintsa kwetici letehlukahlukene ekusimameni kwesigaba kanye netimphahla te-photoelectric kufanele tihluke ngalokuphelele. Ngekwati kwetfu, kuvisisa lokusisekelo kwekutsi tici tikhutsata njani kugucuka kwesigaba se-cubic kuya ku-hexagonal (α-δ) kanye nendzima ye-passivation yemhlabatsi ekusimameni kwesigaba se-α-FAPbI3 perovskite solo akukacondzakali kahle.
Lapha, siveta indlela yekubola kwe-FAPbI3 perovskite kusuka ku-α-sigaba lesimnyama kuya ku-δ-sigaba lesimtfubi kanye nemtselela wemaphutsa lehlukahlukene esivimbelweni semandla se-α-kuya-δ-sigaba sekugucuka nge-DFT. I tikhala, letikhicitwa kalula ngesikhatsi sekwakha ifilimu kanye nekusebenta kwetintfo tekusebenta, kubiketelwa kutsi kungenteka kakhulu kutsi ticale kugucuka kwesigaba se-α-δ. Ngako-ke, setfula lucwencwe lolucinile lolungancibiliki emantini futsi lolucinile ngemakhemikhali lwe-lead oxalate (PbC2O4) ngetulu kwe-FAPbI3 ngekuphendvula kwe-in situ. Lead oxalate surface (LOS) ivimbela kwakheka kwetikhala te I futsi ivimbela kuhamba kwe I ions uma ikhutsatwa kushisa, kukhanya, kanye nemasimu agezi. I-LOS lephumelako inciphisa kakhulu kuhlanganiswa kabusha lokungekho emisebeni ye-interfacial futsi yenta ncono kusebenta kahle kwe-FAPbI3 PSC ku-25.39% (kucinisekisiwe ku-24.92%). Ledivayisi ye-LOS lengakapakishwa igcine 92% wekusebenta kwayo kwekucala ngemuva kwekusebenta endzaweni lephakeme yemandla (MPP) emahora langetulu kwa-550 ngesikhatsi semoya lolingisiwe (AM) we-1.5 G wemisebe.
Sicale senta tibalo te-ab initio kutfola indlela yekubola kwe-FAPbI3 perovskite kuya ekugucukeni kusuka esigabeni se-α kuya esigabeni se-δ. Ngenchubo yekugucula sigaba lesinemininingwane, kutfolakala kutsi kugucuka kusuka ku-octahedron lenetigaba letintsatfu tekwabelana ekhoneni [PbI6] ku-cubic α-sigaba se-FAPbI3 kuya ku-octahedron lenetigaba letintsatfu [PbI6] ku-hexagonal δ-sigaba se-FAPbI3. kwephuka 9. I-Pb-I yakha sibopho esinyatselweni sekucala (Int-1), futsi sivimbo sayo semandla sifinyelela ku-0.62 eV/cell, njengoba kukhonjisiwe kuMfanekiso 1a. Uma i-octahedron ishintjwa ngendlela [0\(\bar{1}\)1], le-chain lemfisha le-hexagonal iyakhula kusuka ku-1×1 kuya ku-1×3, 1×4 bese ekugcineni ingena esigabeni se-δ. Silinganiso sekucondziswa kwayo yonkhe indlela ngu (011) α / / (001) δ + [100] α / / [100] δ. Kusukela emdvwebeni wekusabalalisa emandla, kungatfolakala kutsi ngemuva kwe-nucleation yesigaba se-δ se-FAPbI3 kuletigaba letilandzelako, sivimbelo semandla siphansi kunaleso sekugucuka kwesigaba se-α, lokusho kutsi kugucuka kwesigaba kutawusheshiswa. Kuyacaca kutsi sinyatselo sekucala sekulawula kugucuka kwesigaba sibaluleke kakhulu nangabe sifuna kucindzetela kwehla kwesigaba se-α.
a Inchubo yekugucula Sigaba kusuka ngasencele kuya ngasekudla – sigaba se-FAPbI3 lesimnyama (α-sigaba), kuhlukaniswa kwekucala kwesibopho se-Pb-I (Int-1) kanye nekuhlukaniswa kwesibopho se-Pb-I lokunye (Int-2, Int -3 kanye ne-Int -4) kanye nesigaba lesimtfubi se-FAPbI3 (sigaba se-delta). b Tihibe temandla ku α kuya ku δ sigaba sekugucuka kwe FAPbI3 lokusekelwe ekukhubatekeni lokuhlukahlukene kwemaphuzu langaphakathi. Umugca lonemachashazi ukhombisa sivimbelo semandla se-crystal lefanele (0.62 eV). c Amandla ekwakheka kwemaphuzu layinhloko emaphuzu ebusweni perovskite umholi. I-abscissa axis ngumkhawulo wemandla we-α-δ sigaba sekugucuka, bese i-ordinate axis ngumfutfo wekwakheka kwesici. Letincenye letinemtfunti lompunga, lomtfubi kanye naloluhlata luhlobo I (EB-low-high FE), luhlobo II (FE lephakeme) kanye neluhlobo III (EB-low-low FE), ngekulandzelana. d Amandla ekwakheka kwetici VI kanye LOS of FAPbI3 ekulawuleni. e I sivimbelo sekufuduka kwe-ion ekulawuleni kanye ne-LOS ye-FAPbI3. f – kumelelwa kweluhlelo lwekufuduka kwema-ions e-I (tinhlavu letiwolintshi) kanye ne-gLOS FAPbI3 (lempunga, umthofu; violet (wolintshi), iodine (iodine lehambako)) ekulawuleni kwe-gf (ngasencele: kubuka ngetulu; ngasekudla: sigaba lesiphambukile, lesinsundvu); ikhabhoni; luhlata sasibhakabhaka lolukhanyako – initrogen; lobovu – umoya-mpilo; pinki lokhanyako – i-hydrogen). Idatha umtfombo iniketwa ngendlela amafayela idatha umtfombo.
Sibe sesifundza ngendlela lehlelekile umtselela wekukhubateka kwemaphuzu lehlukahlukene langekhatsi (kufaka ekhatsi kuhlala kwe-PbFA, IFA, PbI, kanye ne-IPb antisite; ema-athomu e-Pbi kanye ne-Ii lasemkhatsini; kanye netikhala te-VI, VFA, kanye ne-VPb), letitsatfwa njengetintfo letibalulekile. letibangela kwehla kwesigaba se-athomu kanye nemandla tikhonjiswe kuMfanekiso 1b kanye neLithebula Lelengetiwe 1. Kuyajabulisa kutsi akusito tonkhe tici letinciphisa umkhawulo wemandla wekushintja kwesigaba se-α-δ (Umfanekiso 1b). Sikholelwa kutsi tici letinemandla laphansi ekwakheka kanye netihibe temandla ekugucuka kwesigaba se-α-δ letiphansi titsatfwa njengaletilimatako ekusimameni kwesigaba. Njengobe kubikwe ngaphambilini, tindzawo leticebile ngekuhola tivame kutsatfwa njengaletisebenta kahle ku-formamidine PSC27. Ngako-ke, sigcila ebusweni be-PbI2-lephelile (100) ngaphansi kwetimo leticebile tekuhola. Amandla ekwakheka kwesici setici temaphuzu langekhatsi langetulu akhonjisiwe kuMfanekiso 1c kanye neLithebula Lelengetiwe 1. Kususelwa esivimbelweni semandla (EB) kanye nemandla ekwakheka kwekugucuka kwesigaba (FE), letici tihlukaniswe ngetinhlobo letintsatfu. Luhlobo I (low EB-high FE): Noma IPb, VFA kanye ne VPb kunciphisa kakhulu sivimbelo semandla kuya ekugucukeni kwesigaba, banemandla laphakeme ekwakheka. Ngako-ke, sikholwa kutsi letinhlobo tetici tinemtselela lomncane ekugucukeni kwesigaba njengoba tingakavami kwakheka. Luhlobo II (EB lephakeme): Ngenca yesivimbelo semandla ekugucuka kwesigaba se-α-δ lephucukile, emaphutsa e-anti-site PbI, IFA kanye ne-PbFA akulimati kusimamisa kwesigaba se-α-FAPbI3 perovskite. Luhlobo III (EB-low FE): VI, Ii kanye ne Pbi emaphutsa lanemandla laphansi ekwakheka kungabangela kwehla kwesigaba lesimnyama. Ikakhulukati uma kuniketwa i-FE ne-EB VI lephansi kakhulu, sikholwa kutsi lisu leliphumelelako kakhulu kunciphisa tikhala te-I.
Kunciphisa VI, satfutfukisa ungqimba eminyene PbC2O4 kwenta ncono ebusweni FAPbI3. Nawucatsanisa netintfo letiphilako letifaka luswayi lwe halide letifana ne phenylethylammonium iodide (PEAI) kanye ne n-octylammonium iodide (OAI), iPbC2O4, lete ema halogen ions lahambako, icinile ngemakhemikhali, ayincibiliki emantini, futsi iyacinywa kalula uma ivuselela. Kusimama lokuhle umswakama ebusweni kanye ensimini kagesi perovskite. Kuncibilika kwe PbC2O4 emantini ngu 0.00065 g/L kuphela, lokuphansi kakhulu kunaleyo ye PbSO428. Lokubaluleke kakhulu, tincenye letiminyene naletifanako te LOS tingalungiswa kancane kumafilimu e perovskite kusetjentiswa kuphendvula kwe in situ (buka ngephansi). Senta kulingisa kwe-DFT kwekubopha kwe-interfacial emkhatsini we-FAPbI3 ne-PbC2O4 njengobe kukhonjisiwe kuMfanekiso Longetiwe 1. Lithebula Lelengetiwe 2 letfula emandla ekwakheka kwesici ngemuva kwekujovwa kwe-LOS. Sitfole kutsi i-LOS ayikhulisi kuphela emandla ekwakheka kwetici te-VI nga-0.69–1.53 eV (Umfanekiso 1d), kepha iphindze ikhulise emandla ekusebenta e-I endzaweni yekufuduka kanye nendzawo yekuphuma (Umfanekiso 1e). Esigabeni sekucala, ema-ion e-I afuduka eceleni kwemhlabatsi we-perovskite, ashiya ema-ion e-VI esimeni se-lattice ngesivimbelo semandla se-0.61 eV. Ngemuva kwekwetfulwa kwe-LOS, ngenca yemphumela wekuvimbela kwe-steric, emandla ekusebenta ekufudukeni kwe-I ions ayakhula kuya ku. 1.28 eV. Ngesikhatsi sekufuduka kwe I ions leshiya ebusweni be perovskite, sivimbo semandla ku VOC siphindze sibe ngetulu kunalesisampula yekulawula (Fig. 1e). Imidvwebo ye-Schematic yetindlela tekufuduka te-I ion ekulawuleni kanye ne-LOS FAPbI3 ikhonjiswe kuMfanekiso 1 f na g, ngekulandzelana. Imiphumela yekulingisa ikhombisa kutsi i-LOS ingavimbela kwakheka kwetici te-VI kanye nekugucuka kwe-I, ngaleyo ndlela kuvimbele i-nucleation ye-α kuya ku-δ sigaba sekugucuka.
Kuphendvula emkhatsini we-oxalic esidi kanye ne-FAPbI3 perovskite kwahlolwa. Ngemuva kwekuhlanganisa tisombululo te-oxalic acid kanye ne-FAPbI3, kwakhiwa linani lelikhulu le-precipitate lemhlophe, njengoba kukhonjisiwe kuMfanekiso Longetiwe 2. Umkhicito wemphuphu wakhonjwa njengentfo lehlantekile ye-PbC2O4 kusetjentiswa i-X-ray diffraction (XRD) (Umfanekiso Longetiwe 3) kanye ne-Fourier Umfanekiso Longetiwe). Sitfole kutsi i-oxalic acid incibilika kakhulu ku-isopropyl alcohol (IPA) ngesikhatsi sekushisa ekamelweni ngekuncibilika lokucishe kube ngu-18 mg/mL, njengobe kukhonjisiwe ku-Supplementary Umfanekiso 5. Ngakoke, ngekucwilisa lefilimu ye perovskite esixazululweni se oxalic esidi noma ngekujika-kugcoka lesisombululo se oxalic esidi kule perovskite, iPbC2O4 lencane naleminyene ingatfolakala ngekushesha etulu kwefilimu ye perovskite ngekuya kwesilinganiso sekhemikhali lesilandzelako: H2C2O4 + PAPbI +3. I-FAI ingancibilikiswa ku-IPA ngaleyondlela isuswe ngesikhatsi sekupheka. Kugcizelela kwe LOS kungalawulwa sikhatsi sekuphendvula kanye nekuhlushwa kwe precursor.
Kuskena ngesibonakhulu se-electron (SEM) titfombe tekulawula kanye nemafilimu e-LOS perovskite akhonjiswe kuTibalo 2a,b. Imiphumela ikhombisa kutsi le perovskite surface morphology igcinwe kahle, futsi linani lelikhulu letinhlayiya letincane tifakwa etulu kwetinhlavu, lokufanele kutsi kumele luhlaka lwe PbC2O4 lolwakhiwa ngukuphendvula kwe in-situ. Lefilimu ye LOS perovskite inendzawo lebushelelezi kancane (Umfanekiso Longetiwe 6) kanye ne engela lenkhulu yekutsintsana nemanti uma kucatsaniswa nefilimu yekulawula (Umfanekiso Longetiwe 7). I-electron microscopy yekudluliswa kwe-electron (HR-TEM) lenesisombululo lesiphakeme yasetjentiswa kwehlukanisa lucwencwe lwemhlabatsi lwalomkhicito. Nawucatsanisa nefilimu yekulawula (Fig. 2c), luhlaka loluncane lolufanako futsi loluminyene lolunebukhulu lobungaba ngu 10 nm lubonakala kahle ngetulu kwe LOS perovskite (Fig. 2d). Kusebentisa sibonakhulu se-electron lesine-angle lesetulu (HAADF-STEM) kuhlola sikhombisi emkhatsini we-PbC2O4 ne-FAPbI3, kuba khona kwetifundza te-crystalline te-FAPbI3 kanye netifundza te-amorphous te-PbC2O4 kungabonakala ngalokucacile (Umfanekiso Longetiwe 8). Kubunjwa kwemhlabatsi we perovskite ngemuva kwekwelashwa kwe oxalic acid kwabonakala ngekukala kwe X-ray photoelectron spectroscopy (XPS), njengoba kukhonjisiwe ku Tibalo 2e–g. KuMfanekiso 2e, ticoco te C 1s letitungelete 284.8 eV kanye na 288.5 eV tingetimphawu letitsite te CC kanye ne FA, ngekulandzelana. Nawucatsanisa nelucwencwe lwekulawula, ulwelwesi lwe-LOS lwakhombisa sicoco lesengetiwe ku-289.2 eV, lesihlobene ne-C2O42-. I-O 1s spectrum ye-LOS perovskite ikhombisa ticoco letintsatfu te-O 1s letihlukile ngemakhemikhali ku-531.7 eV, 532.5 eV, kanye na-533.4 eV, letihambisana ne-COO lekhishiwe, C=O yemacembu e-oxalate langakaphatfwa 30 kanye nema-athomu e-O engcenye ye-OH2e (Fig. ). )). Kulesampula yekulawula, kwabonakala kuphela sicoco lesincane se O 1s, lesingabangelwa yi oxygen chemisorbed etulu. Timphawu telucwencwe lwekulawula lwe Pb 4f7/2 kanye ne Pb 4f5/2 tikhona ku 138.4 eV na 143.3 eV, ngekulandzelana. Sibonile kutsi i-LOS perovskite ikhombisa kushintja kwesicoco se-Pb lesingaba ngu-0.15 eV kuya emandla laphakeme ekubopha, lokukhombisa kusebentisana lokucinile emkhatsini wema-athomu e-C2O42- kanye ne-Pb (Fig. 2g).
a SEM imifanekiso yekulawula kanye b LOS perovskite emafilimu, umbono phezulu. c Sibonakhulu se-elekthronikhi sekudluliswa kwetigaba letiphambukile (HR-TEM) sekulawula kanye d nemafilimu e-LOS perovskite. I-XPS lesetulu ye-e C 1s, f O 1s kanye ne-g Pb 4f emafilimu e-perovskite. Idatha umtfombo iniketwa ngendlela amafayela idatha umtfombo.
Ngekuya kwemiphumela ye-DFT, kubikezelwa ngekwemcondvo kutsi emaphutsa e-VI kanye nekufuduka kwe-I kubangela kalula kugucuka kwesigaba kusuka ku-α kuya ku-δ. Imibiko yangaphambilini ikhombise kutsi i-I2 ikhululwa ngekushesha kusuka kumafilimu e-perovskite lasekelwe ku-PC ngesikhatsi sekucwiliswa ngesithombe ngemuva kwekuveta lamafilimu ekukhanyeni nasekucindzetelekeni lokushisako31,32,33. Kucinisekisa umphumela wekusimamisa we-oxalate leholako ku-α-sigaba se-perovskite, sacwilisa emafilimu ekulawula kanye ne-LOS perovskite emabhodleleni engilazi labonakalako lacuketse i-toluene, ngekulandzelana, bese siyabakhanyisa ngekukhanya kwelanga loku-1 24 h. Silinganise kumuncwa kwe-ultraviolet kanye nekukhanya lokubonakalako (UV-Vis). ) sisombululo se-toluene, njengobe kukhonjisiwe kuMfanekiso 3a. Nawucatsanisa nesampula yekulawula, kucinisa lokuphansi kakhulu kwekutsatsa I2 kwabonwa esimeni se-LOS-perovskite, lokukhombisa kutsi i-LOS lencane ingavimbela kukhishwa kwe-I2 kusuka kufilimu ye-perovskite ngesikhatsi sekucwiliswa lokukhanyako. Titfombe tekulawula lokugugile kanye nemafilimu eLOS perovskite tikhonjiswa kuma insets eTibalo 3b na c. Le LOS perovskite solo imnyama, kantsi liningi lefilimu yekulawula seliphenduke libe mtfubi. Le UV–lebonakalako yekutsatsa spectra yefilimu lecwilisiwe ikhonjiswe ku Figs. 3b, c. Sibonile kutsi kumunwa lokuhambisana ne-α kufilimu yekulawula kwancishiswa ngalokucacile. Tilinganiso te-X-ray tentiwa kute kubhalwe phansi kutigucukela kwemvelo kwesakhiwo se-crystal. Ngemuva kwemahora lamashumi lamabili nakune ekukhanya, le perovskite yekulawula yakhombisa luphawu lolucinile lwe δ-phase loluphuti (11.8°), kantsi le perovskite ye LOS isagcina sigaba lesihle lesimnyama (Umfanekiso 3d).
I-UV-lebonakalako yekutsatsa spectra yetisombululo te toluene lapho khona ifilimu yekulawula kanye nefilimu ye LOS kwacwiliswa ngaphansi kwekukhanya kwelanga lokungu 1 emahora langu 24. Le inset ikhombisa i-vial lapho ifilimu ngayinye yayicwiliswa khona ngevolumu lelinganako ye-toluene. b I-UV-Vis yekutsatsa spectra yefilimu yekulawula kanye nefilimu ye-c LOS ngaphambi nangemuva kwema-24 h ekucwiliswa ngaphansi kwekukhanya kwelanga loku-1. Le inset ikhombisa sitfombe sefilimu yekuhlola. d Emaphethini e-X-ray diffraction ekulawula kanye nemafilimu e-LOS ngaphambi nangemuva kwema-24 h ekuchayeka. SEM imifanekiso yekulawula ifilimu e kanye nefilimu f LOS ngemuva kwemahora langu-24 ekuchayeka. Idatha umtfombo iniketwa ngendlela amafayela idatha umtfombo.
Senta tilinganiso te-electron microscopy (SEM) kute sibone tingucuko tesakhiwo lesincane sefilimu ye-perovskite ngemuva kwemahora langu-24 ekukhanya, njengobe kukhonjisiwe kuTibalo 3e,f. Kulelifilimu lekulawula, tinhlavu letinkhulu tabhujiswa futsi tagucuka taba tinyawo letincane, lebetihambisana ne morphology yemkhicito we δ-phase FAPbI3 (Fig. 3e). Kumafilimu eLOS, letinhlavu te perovskite tihlala tisesimeni lesihle (Umfanekiso 3f). Imiphumela yacinisekisa kutsi kulahleka kwe I kakhulu kukhutsata kugucuka kusuka esigabeni lesimnyama kuya esigabeni lesimtfubi, kantsi iPbC2O4 isimamisa sigaba lesimnyama, ivimbela kulahleka kwe I. Njengobe buningi besikhala emhlabatsini buphakeme kakhulu kunasemhlabatsini wetinhlavu,34 lesigaba kungenteka kakhulu kutsi senteke emhlabatsini we. ngaso sonkhe sikhatsi kukhipha iodine bese kwakha VI. Njengobe kubiketelwe yi DFT, i LOS ingavimbela kwakheka kwetici te VI futsi ivikele kuhamba kwe I ions kuya ebusweni be perovskite.
Ngekwengeta, umphumela we PbC2O4 layer ekumelaneni nemswakama wemafilimu e perovskite emoyeni wemkhatsi (umswakama lohlobene 30-60%) wafundvwa. Njengoba kukhonjisiwe ku Umfanekiso Longetiwe 9, i-LOS perovskite beyisolo imnyama ngemuva kwemalanga langu 12, kantsi ifilimu yekulawula yaphenduka ibe mtfubi. Ekulinganiseni kwe XRD, ifilimu yekulawula ikhombisa sicoco lesinemandla ku 11.8° lehambisana nesigaba se δ se FAPbI3, kantsi i-LOS perovskite igcina kahle sigaba se α lesimnyama (Umfanekiso Longetiwe 10).
Kukhanya lokucinile (PL) kanye nekukhanya lokulungiswa sikhatsi (TRPL) kwasetjentiswa kufundza umphumela wekungasebenti kwe-oxalate leholako ebusweni be-perovskite. Ku Fig. Umfanekiso 4a ukhombisa kutsi ifilimu LOS uye wakhulisa PL umfutho. Esitfombeni se-PL mapping, kucina kwefilimu ye-LOS kuyo yonkhe indzawo lengu-10 × 10 μm2 kuphakeme kunaleyo yefilimu yekulawula (Umfanekiso Longetiwe 11), lokukhombisa kutsi i-PbC2O4 i-pasivates ngendlela lefanako lefilimu ye-perovskite. Sikhatsi sekuphila semtfwali sincunywa ngekulinganisa kubola kwe TRPL ngemsebenti munye we exponential (Fig. 4b). Sikhatsi sekuphila semtfwali wefilimu ye-LOS ngu-5.2 μs, lokuyintfo lendze kakhulu kunefilimu yekulawula lenesikhatsi sekuphila semtfwali we-0.9 μs, lokukhombisa kuncishiswa kwekuhlanganiswa kabusha kwemhlabatsi lokungekho emisebeni.
I-PL lecinile kanye ne-b-spectra ye-PL yesikhashana yemafilimu e-perovskite etindzaweni letiphansi tengilazi. c SP ijika ledivayisi (FTO / TiO2 / SnO2 / i-perovskite / i-spiro-OMeTAD / i-Au). d EQE spectrum kanye Jsc EQE spectrum kuhlanganiswe kusuka kudivayisi esebenta kakhulu. d Kuncika ekukhanyeni kwemandla edivayisi ye-perovskite kumdvwebo we-Voc. f Kuhlatiya lokujwayelekile kwe-MKRC kusetjentiswa intfo yekuhlanta imbobo ye-ITO/PEDOT:PSS/perovskite/PCBM/Au. VTFL ngumgibe esiphezulu ukugcwalisa voltage. Kusukela kulemininingwane sabala buningi besicupho (Nt). Idatha umtfombo iniketwa ngendlela amafayela idatha umtfombo.
Kufundza umphumela wesendlalelo se-oxalate leholako ekusebenteni kwedivayisi, kwasetjentiswa sakhiwo sekutsintsana se-FTO / TiO2 / SnO2 / perovskite / spiro-OMeTAD / Au. Sisebentisa i-formamidine chloride (FACl) njengesengeto ku-perovskite precursor esikhundleni se-methylamine hydrochloride (MACl) kute sifinyelele kusebenta lokuncono kwetintfo tekusebenta, njengoba i-FACl inganiketa lizinga lelincono le-crystal futsi igweme igebe lebhande le-FAPbI335 (bona Tibalo Letengetiwe te-detail2i). ). 12-14). IPA yakhetfwa njengentfo lelwa nekuncibilika ngoba iniketa lizinga le crystal lelincono kanye nekukhetsa kucondziswa kumafilimu eperovskite uma kucatsaniswa ne diethyl ether (DE) noma i-chlorobenzene (CB)36 (Tibalo Letengetiwe 15 na 16). Kucina kwe PbC2O4 kwalungiswa kahle kwentela kulinganisa kahle passivation yesici kanye nekutfutsa kwekushaja ngekulungisa i-oxalic acid lokuhlushwa (Umfanekiso Longetiwe 17). Imifanekiso ye-SEM lephambukile yekulawula lelungiselelwe kanye netintfo te-LOS tikhonjiswe ku-Supplementary Umfanekiso 18. Emajika lajwayelekile e-density (CD) ekulawula kanye netintfo te-LOS akhonjisiwe ku-Figure 4c, futsi emapharamitha lakhishiwe aniketwe ku-Thebula Lelengetiwe 3. Kusebenta kahle kwekuguqulwa kwemandla lamakhulu (%2c2%)43. 25.75 mA cm-2 (25.74 mA cm-2), Voc 1.16 V (1.16 V) kanye nekubuyela emuva (phambili) kwekuskena. Sici sekugcwalisa (FF) ngu-78.40% (76.69%). I-PCE LOS PSC lephakeme ngu-25.39% (24.79%), i-Jsc ngu-25.77 mA cm-2, i-Voc ngu-1.18 V, i-FF ngu-83.50% (81.52%) kusuka emuva (Scan phambili kuya). Ledivaysi ye-LOS ifinyelele kusebenta kwe-photovoltaic lokucinisekisiwe kwa-24.92% elabhorethri ye-photovoltaic yebantfu besitsatfu letsembekile (Umfanekiso Longetiwe 19). Kusebenta kahle kwe-quantum yangaphandle (EQE) kwaniketa i-Jsc lehlanganisiwe ye-24.90 mA cm-2 (kulawula) kanye ne-25.18 mA cm-2 (LOS PSC), ngekulandzelana, lebeyivumelana kahle ne-Jsc lelinganiswa ku-AM 1.5 G spectrum lejwayelekile (Fig. .4d). ) . Kusabalaliswa kwetibalo tema-PCE lalinganisiwe ekulawula kanye nema-PSC e-LOS kukhonjisiwe kuMfanekiso Longetiwe 20.
Njengoba kukhonjisiwe ku Figure 4e, budlelwane emkhatsini we Voc kanye nemandla ekukhanya kwabalwa kufundza umphumela we PbC2O4 ekuhlanganisweni kabusha kwemhlabatsi lokusitwa ngumgibe. Umthambeka welayini lefakwe yedivayisi ye LOS ngu 1.16 kBT/sq, lokuphansi kunekuthambeka kwelayini lefakwe yedivayisi yekulawula (1.31 kBT/sq), kucinisekisa kutsi iLOS iyasita ekuvimbeleni kuhlanganiswa kabusha kwemhlabatsi nge decoys. Sisebentisa bucwepheshe bekunciphisa umkhawulo wekushaja kwemkhatsi (SCLC) kute silinganise ngesilinganiso bukhulu besici sefilimu ye-perovskite ngekukala sici se-IV lesimnyama setintfo tembobo (ITO / PEDOT: PSS / perovskite / spiro-OMeTAD / Au) njengobe kukhonjisiwe kulomfanekiso. 4f Khombisa. Lokucina kwesicupho kubalwa ngefomula Nt = 2ε0εVTFL/eL2, lapho ε ngumkhawulo we-dielectric lohlobene nefilimu ye-perovskite, ε0 ngumkhawulo we-dielectric we-vacuum, i-VTFL ngumkhawulo we-voltage yekugcwalisa lomgibe, e ngumshalo, L ngumkhawulo we-perovskite ifilimu). Kucina kwesici kwetintfo te VOC kubalwa kutsi kube ngu 1.450 × 1015 cm–3, lokuphansi kunekucina kwesici kwetintfo tekulawula, lokungu 1.795 × 1015 cm–3.
Ledivayisi lengakapakishwa yahlolwa endzaweni lephakeme yemandla (MPP) ngaphansi kwekukhanya kwemini lokugcwele ngaphansi kwe nitrogen kuhlola kusimamisa kwayo kwekusebenta kwesikhatsi lesidze (Umfanekiso 5a). Ngemuva kwemahora langu-550, idivayisi ye-LOS beyisolo igcina 92% wekusebenta kwayo lokukhulu, kantsi kusebenta kwedivayisi yekulawula bekwehle kwaba ngu-60% wekusebenta kwayo kwekucala. Kusabalaliswa kwetintfo kuledivayisi lendzala kwakalwa ngesikhatsi-sekundiza sesibili se-ion mass spectrometry (ToF-SIMS) (Fig. 5b, c). Kugcwala lokukhulu kwe iodine kungabonakala endzaweni lengetulu yekulawula igolide. Timo tekuvikela igesi lengasebenti tikhipha tintfo leticedza imvelo letifana nemswakama kanye ne oxygen, lokukhombisa kutsi tindlela tangekhatsi (lokusho kutsi, kuhamba kwe ion) ngito letinesibopho. Ngekuya kwemiphumela ye ToF-SIMS, I- kanye ne AuI2- ions yatfolakala ku electrode ye Au, lokukhombisa kusakateka kwe I kusuka ku perovskite kuya ku Au. Kucina kwesiginali ye-I- kanye ne-AuI2- ions kuledivayisi yekulawula kucishe kube tikhatsi letingu-10 kunaleyo yesampula ye-VOC. Imibiko yangaphambilini ikhombise kutsi kungena kwe-ion kungaholela ekuncipheni lokusheshako kwekuhamba kwemgodzi we-spiro-OMeTAD kanye nekugcola kwemakhemikhali kwesendlalelo se-electrode lesetulu, ngaleyo ndlela kucedza kuchumana kwe-interfacial kule-device37,38. Le electrode ye Au yasuswa futsi le spiro-OMeTAD yahlantwa kusuka kulendzawo lephansi ngesisombululo se chlorobenzene. Sibe sesichaza lefilimu sisebentisa i-X-ray yetigameko tekudla (GIXRD) (Umfanekiso 5d). Imiphumela ikhombisa kutsi lefilimu yekulawula inesicoco sekuphambuka lesisobala ku 11.8°, kantsi kute sicoco lesisha sekuphambuka lesivela kusampula ye LOS. Imiphumela ikhombisa kutsi kulahlekelwa lokukhulu kwe-I ions kufilimu yekulawula kuholela ekukhiciteni sigaba se-δ, kantsi kufilimu ye-LOS lenchubo ivinjelwe ngalokucacile.
Emahora langu 575 ekulandzelela kwe MPP lokuchubekako kwetintfo letingakavalwa emkhatsini we nitrogen kanye nekukhanya kwelanga lokungu 1 ngaphandle kwesihlungi se UV. ToF-SIMS kusabalalisa b I- kanye c AuI2- ions ku LOS MPP idivayisi yekulawula kanye idivayisi yekuguga. Lemibala lephuti, leluhlata kanye newolintshi ihambisana ne Au, iSpiro-OMeTAD kanye ne perovskite. d GIXRD yefilimu ye-perovskite ngemuva kwekuhlolwa kwe-MPP. Idatha umtfombo iniketwa ngendlela amafayela idatha umtfombo.
Kudvonsa lokuncike ekushiseni kwalinganiswa kucinisekisa kutsi iPbC2O4 ingavimbela kuhamba kwe-ion (Umfanekiso Longetiwe 21). Amandla ekusebenta (Ea) ekufuduka kwe-ion ancunywa ngekukala lushintjo ekudvonseni (σ) kwefilimu ye-FAPbI3 emazingeni ekushisa lehlukene (T) kanye nekusebentisa buhlobo be-Nernst-Einstein: σT = σ0exp(−Ea/kBT), lapho σ0 njalo, kB njalo Bo. Sitfola linani le-Ea kusuka ekuthambekeni kwe-ln (σT) uma kucatsaniswa ne-1/T, lokungu-0.283 eV wekulawula kanye ne-0.419 eV yedivayisi ye-LOS.
Ngalokufishane, siniketa luhlaka lwetifundvo tekukhomba indlela yekuwohloka kwe-FAPbI3 perovskite kanye nemtselela wemaphutsa lehlukahlukene esivimbelweni semandla sekushintja kwesigaba se-α-δ. Emkhatsini waletici, VI tici theoretically kubikezelwa kalula kubangela sigaba kugucuka kusuka α kuya δ. Lucwencwe lolucinile lolungancibiliki emantini futsi lolucinile ngemakhemikhali lwe PbC2O4 lwetfulwa kwentela kusimamisa α-phase ye FAPbI3 ngekuvimbela kwakheka kwetikhala te I kanye nekufuduka kwe I ions. Lelisu linciphisa kakhulu kuhlanganiswa kabusha lokungekho emisebeni ye-interfacial, kukhulisa kusebenta kahle kwemaseli elanga kuya ku-25.39%, futsi kwenta ncono kusimamisa kusebenta. Imiphumela yetfu iniketa sicondziso sekufeza ema-PSC e-formamidine lasebenta kahle nalacinile ngekuvimbela kugucuka kwesigaba se-α kuya ku-δ lesibangelwa sici.
I-Titanium (IV) i-isopropoxide (TTIP, 99.999%) yatsengwa ku-Sigma-Aldrich. I-esidi yemanti (HCl, 35.0–37.0%) kanye ne ethanol (lete emanti) kwatsengwa eMbonini Yemakhemikhali yase Guangzhou. I-SnO2 (15 wt% yetin (IV) yekusakateka kwe-oxide) yatsengwa ku-Alfa Aesar. I-iodide yekuhola (i-PbI2, 99.99%) yatsengwa e-TCI Shanghai (eShayina). I-yodide ye-Formamidine (i-FAI, ≥99.5%), i-formamidine chlorayide (FACl, ≥99.5%), i-methylamine hydrochloride (MACl, ≥99.5%), i- (I-Spiro-OMeTAD, ≥99.5%), i-lithiamu bis (trifluoromethane) sulfonylimide (i-Li-TFSI, 99.95%), i-4-tert -butylpyridine (tBP, 96%) yatsengwa eNkampanini Yebuchwepheshe Bekukhanya Ye-Polymer Ye-Xi'an (eShayina). I-N,N-i-DMF, 99.8%), i-dimethyl sulfoxide (i-DMSO, 99.9%), i-isopropyl tjwala (i-IPA, 99.8%), i-chlorobenzene (CB, 99.8%), i-acetonitrile (i-ACN). Kutsengwe ku Sigma-Aldrich. I-Oxalic esidi (H2C2O4, 99.9%) yatsengwa eMacklin. Onkhe emakhemikhali asetjentiswa njengobe atfoliwe ngaphandle kwekuguculwa lokunye.
ITO noma FTO tintfo letiphansi (1.5 × 1.5 cm2) tahlantwa nge-ultrasonic ngesibulalimagciwane, i-acetone, kanye ne-ethanol imizuzu lelishumi, ngekulandzelana, bese tomiswa ngaphansi kwemfudlana we-nitrogen. Lucwencwe lwesivimbo lwe TiO2 lolucinile lwafakwa endzaweni lephansi ye FTO kusetjentiswa sisombululo se titanium diisopropoxybis (i-acetylacetonate) ku ethanol (1/25, v/v) lefakwe ku 500 °C imizuzu lengu 60. Le SnO2 colloidal kusakateka kwahlanjululwa ngemanti lakhiwe ngesilinganiso sevolumu ye 1:5. Ku substrate lehlantekile lephatfwe nge UV ozone imizuzu lengemashumi lamabili, ifilimu lencane ye SnO2 nanoparticles yafakwa ku 4000 rpm imizuzwane lengemashumi lamatsatfu bese iyashiswa ku 150 °C imizuzu lengemashumi lamatsatfu. Kulesisombululo sekucala se perovskite, 275.2 mg we FAI, 737.6 mg we PbI2 kanye ne FACl (20 mol%) kwancibilikiswa ku DMF/DMSO (15/1) lokuhlanganisiwe. Lelucwencwe lwe perovskite lwalungiswa ngekutsi kuhlanganiswe 40 μL wesisombululo sekucala se perovskite ngetulu kwelucwencwe lwe SnO2 loluphatfwe nge UV-ozone ku 5000 rpm emoyeni lokhonako ema 25 s. 5 imizuzwane ngemuva kwesikhatsi sekugcina, 50 μL we MACl IPA sisombululo (4 mg / mL) washeshe walahlwa phezu substrate njenge antisolvent. Ngemuva kwaloko, lamafilimu lasanda kulungiswa abe annealed ku 150 ° C 20 min bese ku 100 ° C 10 min. Ngemuva kwekupholisa ifilimu ye perovskite kuya ekushiseni kweligumbi, sisombululo se H2C2O4 (1, 2, 4 mg lesincibilikisiwe ku 1 mL IPA) sacinywa ku 4000 rpm emaminithi lamashumi lamatsatfu kwentela kucitsa indzawo ye perovskite. Sisombululo se spiro-OMeTAD lesilungiselelwe ngekuhlanganisa 72.3 mg we spiro-OMeTAD, 1 ml we CB, 27 μl we tBP kanye na 17.5 μl we Li-TFSI (520 mg ku 1 ml we acetonitrile) sagcotjwa ngekujikeleta kulefilimu nga 4000 rpm ngaphakatsi. Ekugcineni, ungqimba lwe-Au lolukhulu lolungu-100 nm lwahhwamuka esikhaleni ngesilinganiso se-0.05 nm / s (0 ~ 1 nm), 0.1 nm / s (2 ~ 15 nm) kanye na-0.5 nm / s (16 ~ 100 nm) . ).
Kusebenta kwe SC kwemaseli elanga e perovskite kwakalwa ngekusebentisa iKeithley 2400 imitha ngaphansi kwekukhanya kwe simulator yelanga (SS-X50) ngemandla ekukhanya langu 100 mW/cm2 futsi kwacinisekiswa kusetjentiswa emaseli elanga esilicon lajwayelekile lalinganisiwe. Ngaphandle uma kushiwo ngalenye indlela, emagoba e-SP akalinganiswa ebhokisini lemaglavu lagcwele i-nitrogen ngesikhatsi sekushisa ekamelweni (~ 25 ° C) ngetindlela tekuskena phambili nasemuva (sinyatselo se-voltage 20 mV, sikhatsi sekubambelela 10 ms). Imask yesitfunti yasetjentiswa kutfola indzawo lephumelelako ye 0.067 cm2 ye PSC lelinganisiwe. Kukala kwe-EQE kwentiwa emoyeni lokhona kusetjentiswa luhlelo lwe-PVE300-IVT210 (Buchwepheshe Bembono Wetimboni (ema) Pte Ltd) ngekukhanya lokunembala munye lokugcile kuledivayisi. Kute kusimame idivayisi, kuhlolwa kwemangcamuzane elanga langakahlanganiswa kwentiwa ebhokisini lemaglavu e-nitrogen ngekucindzeteleka lokungu-100 mW/cm2 ngaphandle kwesihlungi se-UV. ToF-SIMS kulinganiswa kusetjentiswa PHI nanoTOFII sikhatsi-sekundiza SIMS. Kujula kwephrofayili kwatfolakala kusetjentiswa sibhamu se 4 kV Ar ion lesinendzawo lengu 400×400 μm.
Kukala kwe-X-ray photoelectron spectroscopy (XPS) kwentiwa kuhlelo lwesayensi lwe-Thermo-VG (ESCALAB 250) kusetjentiswa i-Al Kα le-monochromatized (yemodi ye-XPS) ngekucindzeteleka kwe-5.0 × 10–7 Pa. Lendlela yekwakheka kwemhlabatsi kanye nekuba lukhuni kwemafilimu e-perovskite kwakalwa ngekusebentisa sibonakhulu semandla e-athomu (AFM) (Bruker Dimension FastScan). I-STEM kanye ne-HAADF-STEM ibanjelwe e-FEI Titan Themis i-STEM. I-UV-Vis yekutsatsa emabala yakalwa kusetjentiswa i-UV-3600Plus (Inkampani yaShimadzu). Sikhala sekushaja lokunciphisa nyalo (SCLC) kwabhalwa ku Keithley 2400 imitha. Kukhanya lokucinile (PL) kanye nekukhanya lokucatululwe sikhatsi (TRPL) kwekubola kwemphilo yemtfwali kwakalwa ngekusebentisa i-FLS 1000 spectrometer yekukhanya. PL imifanekiso yekubeka emabalave yakalwa ngekusebentisa luhlelo lweHoriba LabRam Raman HR Kugucuka Kwemvelo. I-FTIR yentiwa kusetjentiswa luhlelo lwe-Thermo-Fisher Nicolet NXR 9650.
Kulomsebenti, sisebentisa indlela yekutsatsa sampula yendlela ye-SSW kute sifundze indlela yekushintja kwesigaba kusuka ku-α-sigaba kuya ku-δ-sigaba. Ngendlela ye-SSW, kuhamba kwendzawo lenemandla langaba khona kuncunywa sicondziso sendlela lethambile lengahleliwe (lesuselwa kwesibili), levumela kufundza lokubanti futsi lokunemgomo kwendzawo lenemandla langaba khona. Kulomsebenti, kusampula kwendlela kwentiwa ku-supercell ye-athomu lengu-72, futsi emabhangqa langetulu kwa-100 ekucala/ekugcina (IS/FS) ahlanganiswa ezingeni le-DFT. Kususelwa kusethi yedatha ye-IS/FS pairwise, indlela lehlanganisa sakhiwo sekucala kanye nesakhiwo sekugcina ingancunywa ngekuhambisana emkhatsini wema-athomu, bese kuhamba kwetindlela letimbili eceleni kwemhlabatsi weyunithi legucukako kusetjentiswa kuncuma kahle indlela yesimo sekugucuka. (I-VK-I-DESV). Ngemuva kwekufuna simo sekugucuka, indlela lenesivimbelo lesiphansi kakhulu ingancunywa ngekubeka tihibe temandla.
Tonkhe tibalo te-DFT tentiwa kusetjentiswa i-VASP (inguqulo 5.3.5), lapho khona kusebentisana kwe-electron–ion kwe-C, N, H, Pb, kanye nema-athomu e-I kumelelwa luhlelo lwe-wave lekhulisiwe (PAW) lekhonjisiwe. Umsebenti wekuhambisana wekushintjana uchazwa ngekulinganisa kwe-gradient jikelele ku-parametry ye-Perdue-Burke-Ernzerhoff. Umkhawulo wemandla emagagasi endiza wabekwa ku-400 eV. Igridi ye Monkhorst-Pack k-phuzu inebukhulu be (2 × 2 × 1). Kuto tonkhe takhiwo, lattice kanye netikhundla te-athomu talungiswa ngalokuphelele kwaze kwaba ngulapho incenye lenkhulu yekucindzeteleka ingaphansi kwa 0.1 GPa kantsi incenye lenkhulu yemandla beyingaphansi kwa 0.02 eV/Å. Kumodeli yemhlabatsi, indzawo ye-FAPbI3 inetinhlaka letingu-4, lesendlalelo lesingephansi sine-athomu lecinile lelingisa umtimba we-FAPbI3, futsi letinhlaka letintsatfu letisetulu tingahamba ngekukhululeka ngesikhatsi senkambo yekusebenta kahle. Lelucwencwe lwe PbC2O4 lungu 1 ML ngebukhulu futsi lusendzaweni ye I-terminal ye FAPbI3, lapho khona iPb iboshelwe ku 1 I na 4 O.
Kute utfole lwati lolubanti mayelana nekwakhiwa kwesifundvo, bona Sifinyeto Sembiko Wephothifoliyo Yemvelo lesihambisana nalesihloko.
Yonkhe idatha letfolakele noma lehlaziywe ngesikhatsi salolucwaningo ifakwe kulesihloko lesishicilelwe, kanye naselwatini lolusekelako kanye nemafayela emininingwane leluhlata. Idatha leluhlata levetwe kulolucwaningo iyatfolakala ku https://doi.org/10.6084/m9.figshare.2410016440. Idatha umtfombo iniketwe lesi sihloko.
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