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Ukuvala ukukhubazeka kusetjenziswe khulu ukwenza ngcono ukusebenza kwamaseli welanga we-lead triiodide perovskite, kodwana umphumela wokukhubazeka okuhlukahlukeneko ekuzinzeni kwesigaba se-α awukacaci; Lapha, sisebenzisa ithiyori yokusebenza kwe-density, sikhomba kokuthoma indlela yokuwohloka kwe-formamidine lead triiodide perovskite ukusuka ku-α-phase ukuya ku-δ-phase begodu sifunda umphumela wokukhubazeka okuhlukahlukeneko esivimbelweni samandla wokutjhuguluka kwesigaba. Imiphumela yokulingisa ibikezela bona iinkhala ze-iodine kungenzeka zibangele ukuwohloka ngombana ziyehlisa khulu isithiyo samandla sokutjhuguluka kwesigaba se-α-δ begodu zinamandla aphasi khulu wokwakheka ebusweni be-perovskite. Ukungeniswa kwesendlalelo esiqinileko se-lead oxalate engancibiliki emanzini ebusweni be-perovskite kuvimbela khulu ukubola kwesigaba se-α, kuvimbela ukufuduka nokuvuvuka kwe-iodine. Phezu kwalokho, iqhinga leli lehlisa khulu ukuhlanganiswa kabutjha okungakhiqizi imisebe begodu likhuphule ukusebenza kuhle kwamaseli welanga ukuya ku-25.39% (okuqinisekiswe ngama-24.92%). Idivayisi engakapakiswa isakwazi ukugcina ukusebenza kwayo kwasekuthomeni okuyi-92% ngemva kokusebenza ngamandla amakhulu ama-awa ama-550 ngaphasi kokukhanya okulinganiselweko kwe-1.5 G yomoya.
Ukusebenza kuhle kokutjhugulula amandla (PCE) wamaseli welanga we-perovskite (ama-PSC) kufikelele irekhodi eliphezulu eliqinisekisiweko lama-26%1. Solo kwango-2015, ama-PSC wesimanjemanje akhetha i-formamidine triiodide perovskite (FAPbI3) njengesendlalelo esidonsa ukukhanya ngebanga lokuzinza kwayo okuhle khulu kokutjhisa kanye ne-bandgap ekhethiweko eduze nomkhawulo we-Shockley-Keisser we-2,3,4. Ngebhadi, amafilimu we-FAPbI3 athatha ukutjhuguluka kwesigaba ukusuka esigabeni esimnyama se-α ukuya esigabeni esiphuzi esingekho-perovskite δ emazingeni womtjhiso wegumbi5,6. Ukukhandela ukwakheka kwesigaba se-delta, kwakhiwe ukwakheka okuhlukahlukeneko kwe-perovskite. Iqhinga elijayelekileko lokunqoba umraro lo kukuhlanganisa i-FAPbI3 nehlanganisela ye-methyl ammonium (MA+), i-cesium (Cs+) kanye ne-bromide (Br-) ions7,8,9. Kodwana, ama-perovskite ahlangeneko ahlushwa yi-bandgap broading kanye nokuhlukaniswa kwesigaba okubangelwa yi-photoinduced, okubeka engozini ukusebenza nokuzinza kokusebenza kwama-PSCs10,11,12.
Iimfundo zamva nje zitjengise bona i-FAPbI3 ye-single crystal ehlanzekileko ngaphandle kokufakwa inokuzinza okuhle khulu ngebanga lobujamo bayo obuhle khulu kanye nokukhubazeka okuphasi13,14. Ngalokho-ke, ukwehlisa ukukhubazeka ngokukhuphula ubukristalu be-FAPbI3 ngobunengi liqhinga eliqakathekileko lokufikelela ama-PSC2,15 asebenzako nazinzileko. Kodwana, ngesikhathi sokusebenza kwe-FAPbI3 PSC, ukuwohloka ukuya esigabeni esingathandekiko se-hexagonal esingasi-perovskite δ kungenzeka16. Ikambiso le ivamise ukuthoma eendaweni eziphezulu kanye nemingcele yeenthoro ezithambekele khulu emanzini, ukutjhisa nokukhanya ngebanga lokuba khona kweendawo ezinengi ezingakalungi17. Ngalokho-ke, ukutjhugululwa kwephasi/kweenhlamvu kuyatlhogeka ukobana kuqiniswe isigaba esimnyama se-FAPbI318. Amaqhinga amanengi wokuphelisa amaphutha, kufaka hlangana ukwethulwa kwama-perovskites aphasi, amamolekhuli we-acid-base Lewis, kanye nama-ammonium halide salts, enze ituthuko ekulu ku-formamidine PSCs19,20,21,22. Bekube nje, pheze zoke iimfundo zitjheje indima yamaphutha ahlukahlukeneko ekunqumeni izakhiwo ze-optoelectronic ezifana nokuhlanganiswa kabutjha kwe-carrier, ubude bokusabalala kanye nesakhiwo sebhendi kumaseli welanga22,23,24. Ukwenza isibonelo, i-density functional theory (DFT) isetjenziselwa ukubikezela amandla wokwakheka kanye namazinga wamandla wokubanjwa kwamaphutha ahlukahlukeneko, okusetjenziswa khulu ukunqophisa umklamo wokungasebenzi20,25,26. Njengoba inani lokukhubazeka lehla, ukuzinza kwedivayisi kuvamise ukuba ngcono. Kodwana, kuma-PSC we-formamidine, iindlela zomthelela wokukhubazeka okuhlukahlukeneko ekuzinzeni kwesigaba kanye nezakhiwo ze-photoelectric kufanele zihluke khulu. Ngokwazi kwethu, ukuzwisisa okusisekelo kokuthi amaphutha abangela njani ukutjhuguluka kwesigaba se-cubic ukuya ku-hexagonal (α-δ) kanye nendima yokungasebenzi kwephasi ekuzinzeni kwesigaba se-α-FAPbI3 perovskite kusazwisiswa kuhle.
Lapha, siveza indlela yokuwohloka kwe-FAPbI3 perovskite ukusuka ku-α-phase emnyama ukuya ku-δ-phase ephuzi kanye nomthelela wokukhubazeka okuhlukahlukeneko esivimbelweni samandla sokutjhuguluka kwe-α-kuya-δ-phase nge-DFT. Izikhala ze-I, ezikhiqizwa lula ngesikhathi sokwenza ifilimu nokusebenza kwedivayisi, kuqagelwa bona zizokuthoma ukutjhuguluka kwesigaba se-α-δ. Ngalokho-ke, sethule isendlalelo esiqinileko se-lead oxalate (PbC2O4) esingancibiliki emanzini nesizinzileko ngamakhemikhali phezu kwe-FAPbI3 ngokusebenzisa ukusabela kwe-in situ. I-lead oxalate surface (LOS) ivimbela ukwakheka kwe-I vacancies begodu ivimbela ukufuduka kwe-I ions lokha nayikhuthazwa mtjhiso, ukukhanya, kanye namasimu kagesi. I-LOS ephumelako yehlisa khulu ukuhlanganiswa kabutjha okungasikho kwemisebe begodu yenza ngcono ukusebenza kuhle kwe-FAPbI3 PSC ukuya ku-25.39% (okuqinisekiswe ku-24.92%). Idivayisi ye-LOS engakapakiswa igcine i-92% yokusebenza kwayo kwasekuthomeni ngemva kokusebenza endaweni yamandla aphezulu (i-MPP) ama-awa angaphezu kwama-550 ngobukhulu bomoya (AM) obuyi-1.5 G yemisebe.
Sithome ngokwenza ukubala kwe-ab initio ukuthola indlela yokubola ye-FAPbI3 perovskite ukutjhuguluka ukusuka esigabeni se-α ukuya esigabeni se-δ. Ngendlela yokutjhugulula isigaba eneenkcukacha, kutholakala bona ukutjhuguluka ukusuka ku-octahedron ye-3-dimensional corner-sharing [PbI6] ku-cubic α-phase ye-FAPbI3 ukuya ku-one-dimensional edge-sharing [PbI6] octahedron ku-hexagonal δ-phase ye-FAPbI3 kuyafezwa. ukuphuka 9. I-Pb-I yakha isibopho esigabeni sokuthoma (i-Int-1), begodu isithiyo sayo samandla sifinyelela ku-0.62 eV/iseli, njengombana kutjengiswe kuMfanekiso 1a. Lokha i-octahedron nayitjhugululwa ngendlela [0\(\bar{1}\)1], iketango elifitjhani le-hexagonal liyakhula ukusuka ku-1×1 ukuya ku-1×3, 1×4 begodu ekugcineni lingena esigabeni se-δ. Izinga lokutjhuguluka kwendlela yoke ngu-(011)α//(001)δ + [100]α//[100]δ. Ukusuka emdwebeni wokusabalalisa amandla, kungatholakala bona ngemva kokubunjwa kwesigaba se-δ se-FAPbI3 emazingeni alandelako, isithiyo samandla siphasi kunaleso sesigaba se-α sokutjhuguluka, okutjho bona ukutjhuguluka kwesigaba kuzokurhaba. Ngokusobala, igadango lokuthoma lokulawula ukutjhuguluka kwesigaba liqakathekile nangabe sifuna ukugandelela ukuwohloka kwesigaba se-α.
ikambiso yokutjhuguluka kwesigaba ukusuka kwesokunxele ukuya kwesokudla – isigaba esimnyama se-FAPbI3 (isigaba se-α), ukuhlukaniswa kokuthoma kwe-Pb-I (Int-1) kanye nokuhlukaniswa kwebhondi ye-Pb-I (Int-2, Int -3 kanye ne-Int -4) kanye nesigaba esiphuzi se-FAPbI3 (isigaba se-delta). b Iinqabo zamandla ekutjhugulukeni kwesigaba se-α ukuya ku-δ se-FAPbI3 ngokuya ngeemraro ezihlukahlukeneko zangaphakathi. Umugqa onamachashazi utjengisa isithiyo samandla sekristalu efaneleko (0.62 eV). c Amandla wokwakheka kwamaphutha wephuzu lokuthoma ebusweni be-perovskite ye-lead. I-abscissa axis yi-energy barrier yokutjhuguluka kwesigaba se-α-δ, begodu i-ordinate axis yi-energy yokwakheka kwesiphambeko. Iingcenye ezifakwe umthunzi ompunga, ophuzi noluhlaza mhlobo I (i-EB ephasi-i-FE ephezulu), ihlobo II (i-FE ephezulu) kanye nehlobo III (i-EB ephasi-i-FE ephasi), ngokulandelana. d Amandla wokwakheka kwamaphutha VI kanye ne-LOS ye-FAPbI3 ekulawuleni. e I isithiyo sokufuduka kwe-ion ekulawuleni kanye ne-LOS ye-FAPbI3. f – ukujanyelwa kwehlelo lokufuduka kwama-ayoni we-I (ama-orange spheres) kanye ne-gLOS FAPbI3 (grey, lead; violet (orange), iodine (mobile iodine)) kulawulo lwe-gf (kwesokunxele: ukubuka phezulu; kwesokudla: isigaba esiphambanweni, ensundu); ikhabhoni; oluhlaza okwesibhakabhaka – inayitrojini; obomvu – i-oksijini; pinki ekhanyako – i-hydrogen). Idatha yomthombo inikelwa ngendlela yamafayela wedatha yomthombo.
Bese sifunda ngokuhlelekileko umthelela wokukhubazeka okuhlukahlukeneko (okufaka hlangana i-PbFA, i-IFA, i-PbI, kanye ne-IPb antisite occupancy; i-Pbi ne-Ii ama-athomu we-interstitial; kanye ne-VI, VFA, ne-VPb vacancies), okuthathwa njengezinto eziqakathekileko. ezibangela ukuwohloka kwesigaba sezinga le-athomu nelamandla zitjengiswe kuMfanekiso 1b kanye neThebuli yokuNgezelelako 1. Ngokuthakazelisako, akusibo boke ubujamo obunciphisa isithiyo samandla sokutjhuguluka kwesigaba se-α-δ (Umfanekiso 1b). Sikholelwa bona ukukhubazeka okunamandla aphasi wokwakheka kanye nemikhawulo yamandla wokutjhuguluka kwesigaba se-α-δ aphasi kuthathwa njengokulimaza ukuzinza kwesigaba. Njengombana kubikwe ngaphambilini, iindawo ezine-lead zithathwa njengezisebenza kuhle ku-formamidine PSC27. Ngalokho-ke, sidzimelele ebusweni obuphelileko be-PbI2 (100) ngaphasi kweemeko ezine-lead. Amandla wokwakheka kwephutha lephutha langaphakathi lendawo atjengiswe kuMfanekiso 1c kanye neThebuli lokuNgezelelako 1. Ngokuya ngesivimbelo samandla (EB) kanye namandla wokwakheka kokutjhuguluka kwesigaba (FE), amaphutha la ahlukaniswe ngemihlobo emithathu. Umhlobo I (i-EB ephasi-i-FE ephezulu): Nanyana i-IPb, i-VFA ne-VPb yehlisa khulu isithiyo samandla ekutjhugulukeni kwesigaba, inamandla aphezulu wokwakheka. Ngalokho-ke, sikholelwa bona imihlobo le yokukhubazeka inomthelela omncani ekutjhugulukeni kwesigaba ngombana ayikavami ukwakheka. Umhlobo we-II (i-EB ephezulu): Ngebanga lokuthuthuka kwesithiyo samandla wokutjhuguluka kwesigaba se-α-δ, ukukhubazeka kwe-anti-site PbI, IFA kanye ne-PbFA akulimazi ukuzinza kwesigaba se-α-FAPbI3 perovskite. Umhlobo we-III (i-EB ephasi-i-FE ephasi): VI, Ii kanye ne-Pbi ukukhubazeka okunamandla aphasi wokubunjwa kungabangela ukuwohloka kwesigaba esimnyama. Khulukhulu nakuqalwa i-FE ephasi khulu ne-EB VI, sikholelwa bona isu elisebenzako khulu kukwehlisa iinkhala ze-I.
Ukwehlisa i-VI, sakha isendlalelo esiqinileko se-PbC2O4 ukwenza ngcono ubuso be-FAPbI3. Nayiqathaniswa nama-organic halide salt passivators afana ne-phenylethylammonium iodide (PEAI) kanye ne-n-octylammonium iodide (OAI), i-PbC2O4, enganawo ama-halogen ions ahambako, izinzile ngokwekhemikhali, ayincibiliki emanzini, begodu iyacinywa lula lokha nayivuselelwako. Ukuzinza okuhle komswakama wangaphezulu kanye nensimu kagesi ye-perovskite. Ukuncibilika kwe-PbC2O4 emanzini kungu-0.00065 g/L kwaphela, okuphasi khulu kune-PbSO428. Okuqakatheke khulu, amalayini aminyeneko nafanako we-LOS angalungiswa ngokuthambileko kumafilimu we-perovskite kusetjenziswa ukusabela kwe-in situ (qala ngenzasi). Senze ukulingiswa kwe-DFT kokuhlangana hlangana kwe-FAPbI3 ne-PbC2O4 njengombana kutjengiswe kuMfanekiso wokuNgezelelako 1. Ithebula lokuNgezelelako 2 liveza amandla wokwakheka kwesiphambeko ngemva kokujovwa kwe-LOS. Sithole bona i-LOS ayikhuphuli kwaphela amandla wokwakheka kwe-VI nge-0.69–1.53 eV (Umfanekiso 1d), kodwana ikhuphula namandla wokusebenza we-I endaweni yokufuduka nendawo yokuphuma (Umfanekiso 1e). Esigabeni sokuthoma, ama-ayoni we-I atjhinga ebusweni be-perovskite, atjhiya ama-ayoni we-VI asesikhundleni se-lattice esinesithiyo samandla esingu-0.61 eV. Ngemva kokungeniswa kwe-LOS, ngonobangela womphumela wokuvimbela kwe-steric, amandla wokusebenza wokufuduka kwama-ayoni we-I akhuphuka abe. 1.28 eV. Ngesikhathi sokufuduka kwama-ayoni we-I atjhiya ubuso be-perovskite, isithiyo samandla ku-VOC naso siphezulu kunasesampula yokulawula (Umfanekiso 1e). Imifanekiso yeendlela zokufuduka kwe-I ion ekulawuleni kanye ne-LOS FAPbI3 itjengiswe kuMfanekiso 1 f no-g, ngokulandelana. Imiphumela yokulingisa itjengisa bona i-LOS ingavimbela ukwakheka kwamaphutha we-VI nokuvuvuka kwe-I, ngaleyo ndlela ivimbele ukutjhuguluka kwesigaba se-α ukuya ku-δ.
Ukusabela hlangana kwe-oxalic acid ne-FAPbI3 perovskite kwahlolwa. Ngemva kokuhlanganisa iinsombululo ze-oxalic acid ne-FAPbI3, kwakhiwa inani elikhulu le-white precipitate, njengombana kutjengiswe ku-Supplementary Figure 2. Umkhiqizo we-powder wabonwa njenge-PbC2O4 ehlanzekileko kusetjenziswa i-X-ray diffraction (XRD) (I-Supplementary Figure 3) kanye ne-Fourier transform infrared spectroscopy (FT) (Supplementary Figure 4). Sithole bona i-oxalic acid incibilika khulu ku-isopropyl alcohol (IPA) emazingeni womtjhiso wegumbi ngokuncibilika okulinganiselwa ku-18 mg/mL, njengombana kutjengiswe ku-Supplementary Figure 5. Lokhu kwenza bona ukusebenza okulandelako kube lula ngombana i-IPA, njenge-passivation solvent ejayelekileko, ayilimazi isendlalelo se-perovskite ngemva kwesikhathi esifitjhani. Ngalokho-ke, ngokucwilisa ifilimu ye-perovskite ngaphakathi kwesisombululo se-oxalic acid nofana ngokutjhugulula isisombululo se-oxalic acid phezu kwe-perovskite, i-PbC2O4 encani neminyeneko ingatholwa msinyana ebusweni befilimu ye-perovskite ngokuya nge-equation yamakhemikhali elandelako: H2C2O4 + FAPI3 = PbI3 + FAIO I-FAI ingancibilika ku-IPA begodu isuswe ngesikhathi sokupheka. Ubukhulu be-LOS bungalawulwa sikhathi sokuphendula kanye nokugxila kwe-precursor.
Iinthombe ze-elekthronikhi ye-elekthronikhi (SEM) yokulawula kanye namafilimu we-LOS perovskite zitjengiswe emifanekisweni 2a,b. Imiphumela itjengisa bona ubujamo bendawo ye-perovskite bulondolozwe kuhle, begodu inani elikhulu leenhlayiya ezincani zifakwe ebusweni beenthoro, okufanele zijamele isendlalelo se-PbC2O4 esakhiwe ngokusabela kwe-in-situ. Ifilimu ye-LOS perovskite inendawo ebuthakathaka kancani (Isithombe esingezelelweko 6) kanye ne-engeli ekulu yokuthintana namanzi nayiqathaniswa nefilimu yokulawula (Isithombe esingezelelweko 7). I-high-resolution transverse transmission electron microscopy (HR-TEM) yasetjenziselwa ukuhlukanisa isendlalelo sangaphezulu somkhiqizo. Nawuqathanisa nefilimu yokulawula (Umfanekiso 2c), isendlalelo esincani esifanako nesiminyeneko esinobukhulu obungaba yi-10 nm sibonakala kuhle phezu kwe-LOS perovskite (Umfanekiso 2d). Ukusebenzisa i-high-angle annular dark-field scanning electron microscopy (HAADF-STEM) ukuhlola isikhombisi phakathi kwe-PbC2O4 ne-FAPbI3, ubukhona bezindawo ze-crystalline ze-FAPbI3 kanye nezindawo ezingekho emthethweni ze-PbC2O4 kungabonwa ngokucacile (Isithombe esingezelelweko 8). Ukwakheka kwe-perovskite ngemva kokwelatjhwa nge-oxalic acid kwabonakala ngokulinganisa kwe-X-ray photoelectron spectroscopy (XPS), njengombana kutjengisiwe ku-Figure 2e–g. Emfanekisweni 2e, i-C 1s iqophelo elizungeze i-284.8 eV kanye ne-288.5 eV ngeyamatshwayo we-CC ne-FA, ngokulandelana. Nayiqathaniswa ne-membrane yokulawula, i-LOS membrane itjengise i-peak eyengeziweko ku-289.2 eV, ehlobene ne-C2O42-. I-O 1s spectrum ye-LOS perovskite itjengisa amakhemikhali amathathu ahlukileko we-O 1s ku-531.7 eV, 532.5 eV, kanye no-533.4 eV, okuhambelana ne-COO e-deprotonated, C=O yamaqembu we-oxalate 30 kanye nama-O athomu we-OH (Fig. 2). )). Ngesampula yokulawula, kwabonwa isiqongo esincani se-O 1s, okungabangelwa yi-oksijini edonswe ngamakhemikhali ebusweni. Iimfanelo ze-membrane yokulawula ye-Pb 4f7/2 ne-Pb 4f5/2 zitholakala ku-138.4 eV kanye ne-143.3 eV, ngokulandelana. Sitjheje bona i-LOS perovskite itjengisa ukutjhuguluka kwe-Pb peak engaba ngu-0.15 eV ukuya emandleni aphezulu wokubopha, okutjengisa ukusebenzisana okunamandla hlangana nama-athomu we-C2O42- ne-Pb (Isithombe 2g).
a Iinthombe ze-SEM zokulawula kanye b namafilimu we-LOS perovskite, umbono ophezulu. c I-high-resolution cross-sectional transmission electron microscopy (HR-TEM) yokulawula kanye d namafilimu we-LOS perovskite. I-XPS ephezulu ye-e C 1s, f O 1s kanye ne-g Pb 4f amafilimu we-perovskite. Idatha yomthombo inikelwa ngendlela yamafayela wedatha yomthombo.
Ngokuya ngemiphumela ye-DFT, kwabikezelwa bona ukukhubazeka kwe-VI nokufuduka kwe-I kubangela lula ukutjhuguluka kwesigaba ukusuka ku-α ukuya ku-δ. Imibiko edlulileko itjengise bona i-I2 ikhutjhwa msinyana emafilimini we-perovskite asekelwe ku-PC ngesikhathi sokucwiliswa ngemva kokuveza amafilimu ekukhanyeni nokugandeleleka kokutjhisa31,32,33. Ukuqinisekisa umphumela wokuzinzisa we-lead oxalate ku-α-phase ye-perovskite, sacwilisa amafilimu wokulawula ne-LOS perovskite emabhodleleni weklasi akhanyako ane-toluene, ngokulandelana, bese siwakhanyisa ngokukhanya kwelanga oku-1 ama-awa ama-24. Silinganise ukumunywa kwe-ultraviolet nokukhanya okubonakalako (UV-Vis). ) isisombululo se-toluene, njengombana kutjengiswe kuMfanekiso 3a. Nawuqathaniswa nesampula yokulawula, ukumuncwa kwe-I2 okuphasi khulu kwabonwa endabeni ye-LOS-perovskite, okutjengisa bona i-LOS encani ingavimbela ukukhutjhwa kwe-I2 kusuka kufilimu ye-perovskite ngesikhathi sokucwilisa ukukhanya. Iinthombe zamafilimu we-old control kanye ne-LOS perovskite zitjengiswe ngaphakathi kwemifanekiso 3b no-c. I-LOS perovskite isemnyama, kuthi inengi lefilimu yokulawula sele iphenduke ibe mthubi. I-UV-ebonakalako yokumuncwa kwefilimu ecwilisiweko itjengiswe kuma-Figs. 3b, c. Sitjheje bona ukumuncwa okuhambisana ne-α kufilimu yokulawula kwehle khulu. Iinlinganiso ze-X-ray zenziwa ukutlola ukutjhuguluka kwesakhiwo sekristalu. Ngemva kwama-awa ama-24 wokukhanyisa, i-perovskite yokulawula itjengise isignali eqinileko ye-δ-phase ephuzi (11.8°), ngesikhathi i-LOS perovskite isagcina isigaba esihle esimnyama (Umfanekiso 3d).
I-UV-visible absorption spectra ye-toluene solutions lapho ifilimu yokulawula nefilimu ye-LOS ifakwe ngaphasi kokukhanya kwelanga oku-1 ama-awa ama-24. I-inset itjengisa isitja lapho ifilimu ngayinye gade icwiliswe ngaphakathi kwevolumu elinganako ye-toluene. b I-UV-Vis yokumuncwa kwefilimu yokulawula kanye ne-c yefilimu ye-LOS ngaphambi nangemva kwama-awa ama-24 wokucwiliswa ngaphasi kokukhanya kwelanga oku-1. I-inset itjengisa isithombe sefilimu yokuhlolwa. d Amaphetheni wokuphambuka kwe-X-ray wokulawula namafilimu we-LOS ngaphambi nangemva kwama-awa ama-24 wokuvezwa. Iinthombe ze-SEM zefilimu yokulawula e nefilimu f LOS ngemva kwama-awa ama-24 wokuvezwa. Idatha yomthombo inikelwa ngendlela yamafayela wedatha yomthombo.
Senze iinlinganiso ze-elekthronikhi ye-elekthronikhi (i-SEM) ukuqala amatjhuguluko we-microstructural yefilimu ye-perovskite ngemva kwama-awa ama-24 wokukhanyisa, njengombana kutjengisiwe emifanekisweni 3e,f. Efilimini yokulawula, iinhlamvu ezinkulu zabhujiswa begodu zatjhugululwa zaba ziinaliti ezincani, ebezihambelana nendlela umkhiqizo we-δ-phase FAPbI3 (Umfanekiso 3e). Emafilimini we-LOS, iinhlamvu ze-perovskite zihlala zisebujameni obuhle (Umfanekiso 3f). Imiphumela iqinisekise bona ukulahlekelwa kwe-I kubangela khulu ukutjhuguluka ukusuka esigabeni esimnyama ukuya esigabeni esiphuzi, lokha i-PbC2O4 iqinisa isigaba esimnyama, ivimbele ukulahlekelwa kwe-I. Njengombana ukuminyana kwesikhala ebusweni kuphezulu khulu kunasesigabeni seenthoro,34 isigaba lesi kungenzeka bona senzeke ebusweni beenthoro. ngesikhathi sinye ukukhupha i-iodine nokwakha i-VI. Njengombana kubikezelwe yi-DFT, i-LOS ingavimbela ukwakheka kwamaphutha we-VI begodu ivimbele ukufuduka kwama-ayoni we-I ukuya ebusweni be-perovskite.
Ukungezelela, umphumela wesendlalelo se-PbC2O4 ekujamelaneni nomswakama wamafilimu we-perovskite emoyeni womkhathi (umswakama ohlobene 30-60%) wafundwa. Njengombana kutjengisiwe emfanekisweni wokungezelela 9, i-LOS perovskite beyisesemnyama ngemva kwamalanga ali-12, ngesikhathi ifilimu yokulawula itjhuguluka ibe mthubi. Ekulinganisweni kwe-XRD, ifilimu yokulawula itjengisa isiqongo esinamandla ku-11.8° ehambelana nesigaba se-δ se-FAPbI3, lokha i-LOS perovskite igcina isigaba esimnyama se-α kuhle (Isithombe esingezelelweko 10).
I-Steady-state photoluminescence (PL) kanye ne-time-resolved photoluminescence (TRPL) kwasetjenziselwa ukufunda umphumela wokungasebenzi kwe-lead oxalate ebusweni be-perovskite. Ku-Fig. Umfanekiso 4a utjengisa bona ifilimu ye-LOS ikhuphule amandla we-PL. Emfanekisweni we-PL, ukuqina kwefilimu ye-LOS phezu kwendawo yoke ye-10 × 10 μm2 kuphezulu kunaleyo yefilimu yokulawula (Isithombe esingezelelweko 11), okutjengisa bona i-PbC2O4 yenza ifilimu ye-perovskite ibe yinto efanako. Isikhathi sokuphila komthwali sinqunywa ngokulinganisa ukubola kwe-TRPL ngomsebenzi owodwa we-exponential (Umfanekiso 4b). Isikhathi sokuphila sefilimu ye-LOS siyi-5.2 μs, okude khulu kunefilimu yokulawula enesikhathi sokuphila sesithwali esiyi-0.9 μs, okutjengisa ukwehlisa ukuhlanganiswa kabutjha okungasikho kwemisebe.
I-PL engaguqukiko kanye ne-b-spectra ye-PL yesikhatjhana yamafilimu we-perovskite phezu kweengilazi. c Ijika le-SP ledivayisi (FTO/TiO2/SnO2/perovskite/spiro-OMeTAD/Au). d I-EQE spectrum kanye ne-Jsc EQE spectrum ehlanganiswe ukusuka kudivayisi esebenza kuhle khulu. d Ukuthembela kokukhanya okukhulu kwedivayisi ye-perovskite emfanekisweni we-Voc. f Ukuhlaziywa kwe-MKRC okujayelekileko kusetjenziswa isisetjenziswa sokuhlanza umgodi we-ITO/PEDOT:PSS/perovskite/PCBM/Au. I-VTFL yivoltheji ephezulu yokugcwalisa umgibe. Ukusuka kiledatha sibale ukuminyana kwesithiyo (Nt). Idatha yomthombo inikelwa ngendlela yamafayela wedatha yomthombo.
Ukufunda umphumela we-lead oxalate layer ekusebenzeni kwedivayisi, kwasetjenziswa isakhiwo sokuthintana se-FTO/TiO2/SnO2/perovskite/spiro-OMeTAD/Au. Sisebenzisa i-formamidine chloride (FACl) njengesengezo ku-perovskite precursor esikhundleni se-methylamine hydrochloride (MACl) ukufezekisa ukusebenza kuhle kwedivayisi, ngombana i-FACl inganikela ngekhwalithi engcono ye-crystal begodu ibalekele isikhala se-band se-FAPbI335 (qala imifanekiso yokungezelela 1 no-2 ukumadanisa okunabileko). ). 12-14). I-IPA yakhethwa njenge-antisolvent ngombana inikela ngekhwalithi engcono yamakristalu begodu ikhetha ukuqondiswa kumafilimu we-perovskite nayiqathaniswa ne-diethyl ether (DE) nofana i-chlorobenzene (CB)36 (Iinthombe ezingezelelweko 15 no-16). Ukuqina kwe-PbC2O4 kwalungiswa ngokutjheja ukulinganisa kuhle ukungasebenzi nokuthuthwa kwe-charge ngokulungisa ukugxila kwe-oxalic acid (Isithombe esingezelelweko 17). Iinthombe ze-SEM eziphambukileko zedivayisi yokulawula ne-LOS zitjengiswe ku-Supplementary Figure 18. Amagoba we-current density (CD) ajwayelekileko wamadivayisi wokulawula ne-LOS atjengiswa ku-Supplementary Table 3. Ukusebenza kuhle okukhulu kokuguqulwa kwamandla (PCE) amaseli (34%, 24%, 34%, J.C.). 25.75 mA cm-2 (25.74 mA cm-2), i-Voc 1.16 V (1.16 V) kanye ne-reverse (forward) scan. I-fill factor (FF) ngu-78.40% (76.69%). I-PCE ephezulu ye-LOS PSC yi-25.39% (24.79%), i-Jsc yi-25.77 mA cm-2, i-Voc yi-1.18 V, i-FF yi-83.50% (81.52%) ukusuka emuva (kuya phambili Skena ukuya). Idivayisi ye-LOS ifinyelele ukusebenza okuqinisekisiweko kwe-photovoltaic kwama-24.92% elabhorethri ye-photovoltaic ethembekileko (Isithombe esingezelelweko 19). I-external quantum efficiency (EQE) yanikela i-Jsc ehlangeneko ye-24.90 mA cm-2 (ukulawula) kanye ne-25.18 mA cm-2 (LOS PSC), ngokulandelana, ebeyivumelana kuhle ne-Jsc elinganiswe ku-AM 1.5 G spectrum (Umfanekiso .4d). ) . Ukusabalala kwezibalo zama-PCE alinganisiweko wokulawula kanye nama-LOS PSC kutjengiswe kuMfanekiso wokuNgezelela 20.
Njengombana kutjengiswe kuMfanekiso 4e, ubudlelwano hlangana ne-Voc nokuqina kokukhanya kwabalwa ukufunda umphumela we-PbC2O4 ekuhlanganisweni kabutjha okusizwa mthiyo. Umthambeka welayini efakwe idivayisi ye-LOS ngu-1.16 kBT/sq, okuphasi kunomthambeka welayini efakwe idivayisi yokulawula (1.31 kBT/sq), okuqinisekisa bona i-LOS ilusizo ekuvimbeleni ukuhlanganiswa kabutjha kwephasi ngama-decoy. Sisebenzisa ithekhnoloji ye-space charge current limiting (SCLC) ukulinganisa ubukhulu be-defect yefilimu ye-perovskite ngokulinganisa ubujamo be-IV emnyama ye-hole device (ITO/PEDOT:PSS/perovskite/spiro-OMeTAD/Au) njengombana kutjengisiwe emfanekisweni. 4f Tjengisa. Ukuminyana kwesithiyo kubalwa ngefomula Nt = 2ε0εVTFL/eL2, lapho ε kuyi-dielectric constant yefilimu ye-perovskite, ε0 kuyi-dielectric constant ye-vacuum, i-VTFL yivoltheji ekhawulela ukuzalisa isithiyo, e yi-charge, L yi-thickness yefilimu ye-perovskite (650 nom). Ukuminyana kwesiphambeko sedivayisi ye-VOC kubalwa ku-1.450 × 1015 cm–3, okungaphasi kobukhulu bokuphazamiseka kwedivayisi yokulawula, okungu-1.795 × 1015 cm–3.
Idivayisi engakapakiswa yahlolwa endaweni yamandla aphezulu (i-MPP) ngaphasi kokukhanya kwemini ngaphasi kwe-nitrogen ukuhlola ukuzinza kwayo kwesikhathi eside (Umfanekiso 5a). Ngemva kwama-awa ama-550, idivayisi ye-LOS isalondoloza i-92% yokusebenza kwayo okuphezulu, ngesikhathi ukusebenza kwedivayisi yokulawula yehlele ku-60% yokusebenza kwayo kwasekuthomeni. Ukusabalala kwezinto ezisetjenzisweni endala kwalinganiswa nge-time-of-flight secondary ion mass spectrometry (ToF-SIMS) (Umfanekiso 5b, c). Ukubuthelela okukhulu kwe-iodine kungabonakala endaweni ephezulu yokulawula igolide. Ubujamo bokuvikelwa kwegesi engasebenziko abufaki izinto ezilimaza ibhoduluko ezifana nomswakama ne-oksijini, okusikisela bona iindlela zangaphakathi (okutjho, ukufuduka kwe-ion) zinomthwalo. Ngokuya ngemiphumela ye-ToF-SIMS, i-I- kanye ne-AuI2- ions zatholakala ku-Au electrode, okutjengisa ukusabalala kwe-I ukusuka ku-perovskite ukuya ku-Au. Ukuqina kwesiginali yama-ayoni we-I- kanye ne-AuI2- esisetjenzisweni sokulawula kungaphezu kwezikhathi ezili-10 kunaleyo yesampula ye-VOC. Imibiko edlulileko itjengise bona ukungena kwe-ayoni kungadosela ekwehleni okurhabako kokudlulisa umgodi we-spiro-OMeTAD kanye nokugqwala kwamakhemikhali kwesendlalelo se-electrode ephezulu, ngaleyindlela kuwohloke ukuthintana kwe-interfacial kudivayisi37,38. I-Electrode ye-Au yasuswa begodu isendlalelo se-spiro-OMeTAD sahlanzwa kusuka ku-substrate ngesisombululo se-chlorobenzene. Bese sihlathulula ifilimu sisebenzisa i-X-ray diffraction (GIXRD) (Umfanekiso 5d). Imiphumela itjengisa bona ifilimu yokulawula ine-peak yokuphambuka ebonakalako ku-11.8°, ngesikhathi kungabi ne-peak etja yokuphambuka esampuleni ye-LOS. Imiphumela itjengisa bona ukulahlekelwa okukhulu kwama-ayoni we-I kufilimu yokulawula kurholela ekukhiqizeni isigaba se-δ, kuthi kufilimu ye-LOS ikambiso le ivinjelwe kuhle.
Ama-awa ama-575 wokulandelela i-MPP okuragela phambili kwedivayisi engakavalwa emmoyeni we-nitrogen kanye nokukhanya kwelanga oku-1 ngaphandle kwesihlungi se-UV. Ukusabalalisa kwe-ToF-SIMS kwama-ion we-b I- kanye ne-c AuI2- kudivayisi yokulawula ye-LOS MPP kanye nedivayisi yokuguga. Imithunzi ephuzi, eluhlaza kanye ne-orenji ihambelana ne-Au, i-Spiro-OMeTAD kanye ne-perovskite. d GIXRD yefilimu ye-perovskite ngemva kokuhlolwa kwe-MPP. Idatha yomthombo inikelwa ngendlela yamafayela wedatha yomthombo.
Ukudlulisa okuthembele emazingeni womtjhiso kwalinganiswa ukuqinisekisa bona i-PbC2O4 ingavimbela ukufuduka kwe-ion (Isithombe esingezelelweko 21). Amandla wokusebenza (Ea) wokufuduka kwe-ayoni anqunywa ngokulinganisa ukutjhuguluka kokudlulisa (σ) kwefilimu ye-FAPbI3 emazingeni womtjhiso ahlukileko (T) begodu kusetjenziswa ubuhlobo be-Nernst-Einstein: σT = σ0exp(−Ea/kBT), lapho i-σ0 iyinto engaguqukiko, i-kB iyinto engaguqukiko ye-Boltman. Sithola inani le-Ea ukusuka emthambekeni we-ln(σT) ngokuqathaniswa ne-1/T, okuyi-0.283 eV yokulawula kanye ne-0.419 eV yedivayisi ye-LOS.
Ngokufingqa, sinikela ngohlaka lwethiyori lokukhomba indlela yokuwohloka kwe-FAPbI3 perovskite kanye nomthelela wokukhubazeka okuhlukahlukeneko esivimbelweni samandla sokutjhuguluka kwesigaba se-α-δ. Hlangana namaphutha la, amaphutha we-VI abikezelwa bona abanga lula ukutjhuguluka kwesigaba ukusuka ku-α ukuya ku-δ. Isendlalelo esiqinileko se-PbC2O4 esingancibiliki emanzini nesizinzileko ngamakhemikhali sethulwa ukuqinisa isigaba se-α se-FAPbI3 ngokuvimbela ukwakheka kwezikhala ze-I nokufuduka kwama-ion we-I. Iqhinga leli lehlisa khulu ukuhlanganiswa okungasikho kwemisebe, likhuphula ukusebenza kuhle kwamaseli welanga ukuya ku-25.39%, begodu lenza ngcono ukuzinza kokusebenza. Imiphumela yethu inikela isiqondiso sokufezekisa ama-PSC we-formamidine asebenzako begodu azinzileko ngokuvimbela ukutjhuguluka kwesigaba se-α ukuya ku-δ esibangelwa yi-defect.
I-Titanium(IV) isopropoxide (TTIP, 99.999%) yathengwa ku-Sigma-Aldrich. I-hydrochloric acid (HCl, 35.0–37.0%) kanye ne-ethanol (enganamanzi) kwathengwa e-Guangzhou Chemical Industry. I-SnO2 (15 wt% tin(IV) oxide colloidal dispersion) yathengwa ku-Alfa Aesar. I-Lead(II) iodide (PbI2, 99.99%) yathengwa ku-TCI Shanghai (China). I-formamidine iodide (FAI, ≥99.5%), i-formamidine chloride (FACl, ≥99.5%), i-methylamine hydrochloride (MACl, ≥99.5%), i-2,2′,7,7′-tetrakis-(N , N-di-p) )-methoxyaniline)-9′-spirofluore (Spiro-OMeTAD, ≥99.5%), i-lithium bis(trifluoromethane)sulfonylimide (Li-TFSI, 99.95%), i-4-tert -butylpyridine (tBP, 96%) yathengwa ku-Xi'an Polymer Light Technology Company (China). 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 ku-Sigma-Aldrich. I-oxalic acid (H2C2O4, 99.9%) yathengwa ku-Macklin. Woke amakhemikhali asetjenziswe njengombana atholwe ngaphandle kokutjhugululwa okunye.
I-ITO nofana i-FTO (1.5 × 1.5 cm2) yahlanzwa nge-ultrasonic nge-detergent, i-acetone, kanye ne-ethanol imizuzu eli-10, ngokulandelana, bese yomiswa ngaphasi komfudlana we-nitrogen. Isendlalelo esiqinileko se-TiO2 sifakwe phezu kwe-FTO kusetjenziswa isisombululo se-titanium diisopropoxybis(acetylacetonate) ku-ethanol (1/25, v/v) ebekwe ku-500 °C isikhathi esingaba mizuzu ema-60. Ukuhlakazeka kwe-SnO2 kwe-colloidal kwahlanjululwa ngamanzi ahlanjululwe nge-volume ratio ye-1:5. Ephasini elihlanzekileko eliphathwe nge-ozone ye-UV imizuzu ema-20, ifilimu encani ye-SnO2 nanoparticles yafakwa ku-4000 rpm imizuzwana ema-30 bese yafuthunyelwa ku-150 °C imizuzu ema-30. Ngesixazululo se-perovskite precursor, i-275.2 mg FAI, 737.6 mg PbI2 kanye ne-FACl (20 mol%) zancibilikiswa ku-DMF/DMSO (15/1) isisombululo esihlanganisiweko. Isendlalelo se-perovskite salungiswa ngokutjhugulula i-40 μL yesixazululo se-perovskite phezu kwesendlalelo se-SnO2 esiphathwe nge-UV-ozone nge-5000 rpm emoyeni ozungezileko ama-25 s. 5 imizuzwana ngemva kwesikhathi sokugcina, i-50 μL yesisombululo se-MACl IPA (4 mg/mL) yalahlwa msinyana phezu kwe-substrate njenge-antisolvent. Bese, amafilimu asanda kulungiswa athonywa ku-150°C imizuzu ema-20 bese kuthi ku-100°C imizuzu eli-10. Ngemva kokupholisa ifilimu ye-perovskite ukuya emazingeni womtjhiso wegumbi, isisombululo se-H2C2O4 (1, 2, 4 mg esincibilikiswe ku-1 mL IPA) satjhugululwa nge-4000 rpm ama-30 s ukuqeda ubuso be-perovskite. Isisombululo se-spiro-OMeTAD esilungiselelwe ngokuhlanganisa i-72.3 mg spiro-OMeTAD, 1 ml CB, 27 μl tBP kanye ne-17.5 μl Li-TFSI (520 mg ku-1 ml acetonitrile) safakwa nge-spin-coated phezu kwefilimu nge-4000 rpm ngaphakathi kwe-spin 300. Ekugcineni, isendlalelo se-Au esibukhulu esingu-100 nm sahwamuka ngaphakathi kwe-vacuum ngezinga elingu-0.05 nm/s (0~1 nm), 0.1 nm/s (2~15 nm) kanye no-0.5 nm/s (16~100 nm) . ).
Ukusebenza kwe-SC kwamaseli welanga we-perovskite kwalinganiswa kusetjenziswa i-Keithley 2400 meter ngaphasi kokukhanya kwelanga (SS-X50) ngokukhanya okukhulu kwe-100 mW/cm2 begodu kwaqinisekiswa kusetjenziswa amaseli welanga we-silicon alinganisiweko. Ngaphandle kobana kutjhiwo ngenye indlela, amajika we-SP alinganiswa ebhokisini lamagilavu ​​azele i-nitrogen emazingeni womtjhiso wegumbi (~25°C) ngendlela yokuskena eya phambili neyabuyela emuva (isinyathelo sevoltheji 20 mV, isikhathi sokulibaziseka 10 ms). Imaski yesithunzi yasetjenziselwa ukuthola indawo esebenzako ye-0.067 cm2 ye-PSC elinganisiweko. Iinlinganiso ze-EQE zenziwa emoyeni ozungezeko kusetjenziswa ihlelo le-PVE300-IVT210 (Industrial Vision Technology(s) Pte Ltd) ngokukhanya kwe-monochromatic okudzimelele esisetjenzisweni. Ukuqinisa idivayisi, ukuhlolwa kwamaseli welanga angafakwanga kwenziwa ngaphakathi kwebhokisi lamagilavu ​​we-nitrogen nge-100 mW/cm2 ngaphandle kwe-UV filter. I-ToF-SIMS ilinganiswa kusetjenziswa i-PHI nanoTOFII time-of-flight SIMS. Ukuhlola ukutjhinga kwatholakala kusetjenziswa isibhamu se-4 kV Ar ion esinendawo engu-400×400 μm.
Iinlinganiso ze-X-ray photoelectron spectroscopy (XPS) zenziwa ku-Thermo-VG Scientific system (ESCALAB 250) kusetjenziswa i-monochromatized Al Kα (ye-XPS mode) ngegandeleleko le-5.0 × 10–7 Pa. I-Scanning electron microscopy (SEM) yenziwa ku-JESM-JJ-303 F system. Ubujamo bephasi kanye nobudisi bamafilimu we-perovskite kwalinganiswa kusetjenziswa i-atomic force microscopy (AFM) (Bruker Dimension FastScan). I-STEM ne-HAADF-STEM zibanjwa e-FEI Titan Themis STEM. I-UV-Vis absorption spectra yalinganiswa kusetjenziswa i-UV-3600Plus (Shimadzu Corporation). I-space charge limiting current (SCLC) yarekhodwa ku-Keithley 2400 meter. I-Steady-state photoluminescence (PL) kanye ne-time-resolved photoluminescence (TRPL) yokubola kwesikhathi sokuphila kwethwali kwalinganiswa kusetjenziswa i-FLS 1000 photoluminescence spectrometer. Iinthombe ze-PL zalinganiswa kusetjenziswa i-Horiba LabRam Raman system HR Evolution. I-Fourier transform infrared spectroscopy (FTIR) yenziwa kusetjenziswa i-Thermo-Fisher Nicolet NXR 9650 system.
Kulomsebenzi, sisebenzisa indlela yokuthatha amasampula wendlela ye-SSW ukufunda indlela yokutjhuguluka kwesigaba ukusuka esigabeni se-α ukuya esigabeni se-δ. Ngendlela ye-SSW, ukunyakaza kwendawo yamandla angaba khona kunqunywa yindlela yendlela ethambileko engakahleleki (ukuvela kwesibili), okuvumela isifundo esinabileko nesiqondileko sendawo yamandla angaba khona. Kulomsebenzi, ukusampula kwendlela kwenziwa ku-supercell yama-athomu ama-72, begodu ama-pair we-IS/FS angaphezu kwe-100 abuthelelwa ezingeni le-DFT. Ngokuya ngesethi yedatha ye-IS/FS ngababili, indlela ehlanganisa isakhiwo sokuthoma nesakhiwo sokugcina ingatholwa ngokubhalelana hlangana nama-athomu, bese kuthi ukunyakaza kweendlela ezimbili ebusweni beyunithi eguquguqukako kusetjenziselwe ukunquma ngokutjhelelako indlela yobujamo bokutjhuguluka. (VK-DESV). Ngemva kokufuna ubujamo bokutjhuguluka, indlela enesithiyo esiphasi khulu ingatholwa ngokubeka iinqabo zamandla.
Zoke iimbalo ze-DFT zenziwa kusetjenziswa i-VASP (inguqulo 5.3.5), lapho ukusebenzisana kwe-elekthroni-ion yama-athomu we-C, N, H, Pb, kanye ne-I kujanyelwe yi-projected amplified wave (PAW) scheme. Umsebenzi wokuhlobana wokutjhinisana uchazwa ngokulinganisa kwe-gradient jikelele ku-Perdue-Burke-Ernzerhoff parametrization. Umkhawulo wamandla wamagagasi wendiza wabekwa ku-400 eV. Igridi ye-Monkhorst-Pack k-point inobukhulu obungu-(2 × 2 × 1). Kizo zoke izakhiwo, i-lattice kanye nezikhundla ze-athomu zalungiswa ngokuzeleko bekwaba kulapho ingcenye yokugandeleleka okukhulu ingaphasi kwe-0.1 GPa begodu ingcenye yamandla aphezulu ibe ngaphasi kwe-0.02 eV/Å. Emfanekisweni wangaphezulu, ubuso be-FAPbI3 buneengaba ezi-4, isendlalelo esingezansi sinama-athomu angaguqukiko alingisa umzimba we-FAPbI3, begodu amasendlalelo amathathu angaphezulu angakhamba ngokutjhaphuluka ngesikhathi senqubo yokwenza ngcono. Isendlalelo se-PbC2O4 sibukhulu obuyi-1 ML begodu sitholakala ebusweni be-I-terminal ye-FAPbI3, lapho i-Pb ibotjhelelwe khona ku-1 I no-4 O.
Ukuthola ilwazi elinabileko malungana nomklamo wesifundo, qala i-Abstract yoMbiko wePhothifoliyo yemvelo ehlotjaniswa ne-atikili le.
Yonke idatha etholwe namkha ehlaziywe ngesikhathi sesifundo lesi ifakwe esihlokweni esigadangisiweko, kanye nelwazi elisekelako namafayela wedatha engakalungiswa. Idatha engakalungiswa ethulwe esifundweni lesi iyatholakala ku-https://doi.org/10.6084/m9.figshare.2410016440. Idatha yomthombo inikelwe esihlokweni lesi.
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