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Gukoresha ingirabuzimafatizo mu gupima ubusembwa byakoreshejwe cyane mu kunoza imikorere y’uturemangingo tw’izuba twa triiodide perovskite, ariko ingaruka z’ubusembwa butandukanye ku guhagarara kw’uturemangingo tw’izuba ntizisobanutse neza; Aha, dukoresheje inyigisho y’imikorere y’ubucucike, tugaragaza bwa mbere inzira yo kwangirika kwa formamidine lead triiodide perovskite kuva kuri α-phase kugera kuri δ-phase no kwiga ingaruka z’ubusembwa butandukanye ku nzitizi y’impinduka z’uturemangingo. Ibisubizo bya simulation bigaragaza ko icyuho cya iyode gishobora gutera kwangirika kuko bigabanya cyane imbogamizi y’ingufu ku mpinduka z’uturemangingo tw’izuba kandi bifite ingufu nke cyane ku buso bwa perovskite. Kwinjizwa k’urwego rwinshi rwa oxalate y’amazi idashobora gushonga ku buso bwa perovskite bibuza cyane kwangirika kw’uturemangingo tw’izuba, bikabuza kwimuka no guhinduka kwa iyode. Byongeye kandi, iyi ngamba igabanya cyane gusubiranamo kw’uturemangingo tw’izuba kandi yongera ubushobozi bw’uturemangingo tw’izuba kugeza kuri 25.39% (byemewe na 24.92%). Igikoresho gipakuruwe gishobora gukomeza gukora neza ku kigero cya 92% nyuma yo gukora ku ngufu ntarengwa mu gihe cy'amasaha 550 hakoreshejwe imirasire y'umwuka ya 1.5 G.
Ubushobozi bwo guhindura ingufu (PCE) bw'uturemangingo tw'izuba twa perovskite (PSCs) bwageze ku rwego rwo hejuru rwa 26% 1. Kuva mu 2015, PSCs zigezweho zakunze formamidine triiodide perovskite (FAPbI3) nk'urwego rufata urumuri bitewe n'ubushyuhe bwayo bwiza kandi icyuho cyayo kiri hafi y'umupaka wa Shockley-Keisser wa 2,3,4. Ikibabaje ni uko filime za FAPbI3 zikoresha thermodynamically zinyura mu mpinduka kuva ku gice cy'umukara cya α zijya ku gice cy'umuhondo kitari perovskite δ ku bushyuhe bw'icyumba5,6. Kugira ngo hirindwe iremwa rya delta phase, hakozwe imiterere itandukanye ikomeye ya perovskite. Ingamba zikunze gukoreshwa mu gukemura iki kibazo ni ukuvanga FAPbI3 n'uruvange rwa methyl ammonium (MA+), cesium (Cs+) na bromide (Br-) ions7,8,9. Ariko, perovskites zo mu bwoko bwa hybrid zihura n’ikibazo cyo kwaguka kw’icyuho no gutandukana kw’ibyiciro bikomoka ku isanzure, ibyo bikaba byangiza imikorere n’imikorere ya PSCs10,11,12 zikomokaho.
Ubushakashatsi buherutse bwerekanye ko FAPbI3 y’ikirahure kimwe gusa kidafite doping ifite umutekano mwiza bitewe n’ubuziranenge bwayo bwiza n’ubusembwa buke13,14. Kubwibyo, kugabanya ubusembwa binyuze mu kongera ubuziranenge bwa FAPbI3 ni ingamba yingenzi yo kugera kuri PSC2,15 nziza kandi ihamye. Ariko, mu gihe cyo gukora kwa FAPbI3 PSC, kwangirika ku gice cy’umuhondo cya hexagonal kidakenewe cya perovskite δ gishobora kubaho16. Ubusanzwe iyi gahunda itangirira ku buso n’imbibi z’ibinyampeke bishobora kwibasirwa cyane n’amazi, ubushyuhe n’urumuri bitewe n’ahantu henshi habi17. Kubwibyo, guhindagurika kw’ubuso/ubuso bw’ibinyampeke ni ngombwa kugira ngo FAPbI318 ikomeze guhagarara neza. Ingamba nyinshi zo guhindagurika kw’ubusembwa, harimo no gushyiramo perovskites zo mu rugero rwo hasi, aside-base Lewis molecules, n’imyunyungugu ya ammonium halide, byateye imbere cyane muri formamidine PSC19,20,21,22. Kugeza ubu, hafi ya ubushakashatsi bwose bwibanze ku ruhare rw'inenge zitandukanye mu kugena imiterere ya optoelectronic nko gusubiramo kwa carrier, uburebure bwo gukwirakwira no gushyiraho umugozi mu turemangingo tw'izuba22,23,24. Urugero, inyigisho y'imikorere y'ubucucike (DFT) ikoreshwa mu guhanura ingufu zo gushinga no gufata urwego rw'ingufu z'inenge zitandukanye, ikoreshwa cyane mu kuyobora imiterere y'ingufu 20,25,26. Uko umubare w'inenge ugabanuka, ubusanzwe impagarara y'igikoresho iratera imbere. Ariko, muri formamidine PSCs, uburyo impagarara zitandukanye ziterwa n'inenge ku miterere y'impagarara n'iy'amashanyarazi y'ifoto zigomba kuba zitandukanye rwose. Uko tubizi neza, gusobanukirwa kw'ibanze uburyo impagarara zitera ihinduka ry'impinduka ya cubic kugera kuri hexagonal (α-δ) kandi uruhare rw'impagarara yo hejuru ku miterere ya phase ya α-FAPbI3 perovskite ntirurasobanuka neza.
Aha, turagaragaza inzira yo kwangirika kwa FAPbI3 perovskite kuva kuri α-phase y'umukara kugera kuri δ-phase y'umuhondo ndetse n'ingaruka z'ubusembwa butandukanye ku nzitizi y'ingufu zo guhindura α-to-δ-phase binyuze muri DFT. I vacances za I, ziboneka byoroshye mu gihe cyo gukora filime no gukora igikoresho, bivugwa ko zishobora gutangiza ihinduka rya α-δ phase. Kubwibyo, twashyizeho urwego rw'amazi rudashonga kandi rudahindagurika mu mikorere rwa α-δ oxalate (PbC2O4) hejuru ya FAPbI3 binyuze mu buryo bwo gukora. Ubuso bwa αxalate ya Lead (LOS) bubuza ikorwa rya I vacances kandi bukarinda kwimuka kwa iyoni za I iyo ziterwa n'ubushyuhe, urumuri, n'amashanyarazi. LOS ivamo igabanya cyane isubiranamo ry'urusobe rw'imirasire hagati y'urusobe rw'imirasire kandi ikongera ubushobozi bwa FAPbI3 PSC kugeza kuri 25.39% (byemewe kuri 24.92%). Igikoresho cya LOS cyari gipakuruwe cyagumanye 92% by'ubushobozi bwacyo bwa mbere nyuma yo gukora ku ngufu ntarengwa (MPP) mu gihe cy'amasaha arenga 550 ku gipimo cy'umwuka (AM) cya 1.5 G cy'imirasire.
Twabanje gukora imibare ya ab initio kugira ngo tubone inzira yo gusenyuka kwa perovskite ya FAPbI3 ijya mu mpinduka kuva kuri phase ya α kugera kuri phase ya δ. Binyuze mu nzira irambuye yo guhindura phase, byagaragaye ko impinduka kuva kuri octahedron yo gusangira impuzandengo eshatu [PbI6] muri cubic α-phase ya FAPbI3 kugera kuri octahedron yo gusangira impande imwe [PbI6] muri hexagonal δ-phase ya FAPbI3 igerwaho. Bica 9. Pb-I ikora umugozi mu ntambwe ya mbere (Int-1), kandi inzitizi yayo y'ingufu igera kuri 0.62 eV/cell, nk'uko bigaragara ku Ishusho ya 1a. Iyo octahedron yimuwe mu cyerekezo cya [0\(\bar{1}\)1], umuyoboro mugufi wa hexagonal waguka kuva kuri 1×1 kugera kuri 1×3, 1×4 hanyuma amaherezo ukinjira muri phase ya δ. Igipimo cy’icyerekezo cy’inzira yose ni (011)α//(001)δ + [100]α//[100]δ. Dukurikije igishushanyo mbonera cy’ikwirakwizwa ry’ingufu, bigaragara ko nyuma y’ishyirwa mu byiciro rya δ phase ya FAPbI3 mu byiciro bikurikira, imbogamizi y’ingufu iba iri hasi ugereranyije n’ihinduka ry’icyiciro cya α, bivuze ko ihinduka ry’icyiciro rizihuta. Birumvikana ko intambwe ya mbere yo kugenzura ihinduka ry’icyiciro ari ingenzi niba dushaka gukumira iyangirika rya α-phase.
Uburyo bwo guhindura icyiciro uhereye ibumoso ujya iburyo – icyiciro cya FAPbI3 cy'umukara (icyiciro cya α), ihuriro rya mbere rya Pb-I (Int-1) hamwe n'irindi ihuriro rya Pb-I (Int-2, Int -3 na Int -4) n'itsinda ry'umuhondo rya FAPbI3 (icyiciro cya delta). b Inzitizi z'ingufu ku ihinduka rya α kugeza kuri δ rya FAPbI3 rishingiye ku busembwa butandukanye bw'ingingo. Umurongo w'utudomo ugaragaza ihuriro ry'ingufu rya kristu nziza (0.62 eV). c Ingufu zo gukora ubusembwa bw'ingingo z'ibanze ku buso bwa perovskite y'amasasu. Umurongo wa abscissa ni ihuriro ry'ingufu z'ihinduka rya α-δ, naho umurongo wa ordinate ni imbaraga zo gukora ubusembwa. Ibice bifite ibara ry'umukara, umuhondo n'icyatsi ni ubwoko bwa I (ubuso bwa EB-hejuru), ubwoko bwa II (ubuso bwa FE) n'ubwoko bwa III (ubuso bwa EB-hejuru), uko bikurikirana. d Ingufu zo gukora ubusembwa VI na LOS bya FAPbI3 mu buyobozi. e I nzitizi ku kwimuka kwa iyoni mu kugenzura na LOS ya FAPbI3. f – Ishusho y’ishusho y’ukwimuka kwa iyoni za I (uduce tw’icunga) na gLOS FAPbI3 (ikijuju, icyuma cy’ubutare; violet (icunga), iyoni (iyoni igendanwa)) mu kugenzura gf (ibumoso: ishusho yo hejuru; iburyo: igice cy’umukara); karuboni; ubururu bwerurutse – azote; umutuku – ogisijeni; umutuku werurutse – hidrojeni). Amakuru y’isoko atangwa mu buryo bwa dosiye z’amakuru y’isoko.
Hanyuma twize ku buryo bwimbitse ingaruka z'ubusembwa butandukanye bw'ingingo (harimo PbFA, IFA, PbI, na IPb antisite occupation; atome za Pbi na II interstitial; na VI, VFA, na VPb vacancies), bifatwa nk'ibintu by'ingenzi, bitera kwangirika k'urwego rwa atome n'ingufu bigaragara ku Ishusho ya 1b n'Imbonerahamwe y'Inyongera ya 1. Igishimishije ni uko ubusembwa bwose bugabanya ubusembwa bw'ingufu z'impinduka y'igice cya α-δ (Ishusho ya 1b). Twizera ko ubusembwa bufite ingufu nke zo mu miterere n'ubusembwa bw'impinduka y'igice cya α-δ bufatwa nk'ubugira ingaruka ku busugire bw'igice. Nkuko byatangajwe mbere, ubuso bukungahaye kuri lisansi muri rusange bufatwa nk'ingirakamaro kuri formamidine PSC27. Kubwibyo, twibanda ku buso bwa PbI2 (100) buri mu bihe by'ubusembwa. Ingufu zo mu miterere y'ubusembwa bw'ingingo z'imbere zigaragara ku Ishusho ya 1c n'Imbonerahamwe y'Inyongera ya 1. Hashingiwe ku busembwa bw'ingufu (EB) n'ingufu zo mu miterere y'igice (FE), ubu busembwa bushyirwa mu moko atatu. Ubwoko bwa I (FE iri hasi ya EB): Nubwo IPb, VFA na VPb bigabanya cyane imbogamizi z'ingufu mu mpinduka z'ibyiciro, bifite ingufu nyinshi zo gukora. Kubwibyo, twizera ko ubwo bwoko bw'inenge bufite ingaruka nke ku mpinduka z'ibyiciro kuko zidakunze kubaho. Ubwoko bwa II (EB iri hejuru): Bitewe n'ingufu z'impinduka z'ibyiciro bya α-δ zazamutse, inenge zo kurwanya ahantu PbI, IFA na PbFA ntizangiza imiterere y'ibyiciro bya perovskite ya α-FAPbI3. Ubwoko bwa III (FE iri hasi ya EB): Inenge za VI, II na Pbi zifite ingufu nke zo gukora zishobora gutera kwangirika kw'ibyiciro by'umukara. Cyane cyane bitewe na FE iri hasi ya EB na EB VI, twizera ko ingamba nziza ari ukugabanya imyanya ya I.
Kugira ngo tugabanye VI, twakoze urwego rw'ubucucike bwa PbC2O4 kugira ngo twongere ubuso bwa FAPbI3. Ugereranije n'uduce tw'umunyu wa halide nka phenylethylammonium iodide (PEAI) na n-octylammonium iodide (OAI), PbC2O4, idafite iyoni za halogen zigenda, irahamye mu buryo bwa shimi, ntishongera mu mazi, kandi irafungwa byoroshye iyo itangiye gukangurwa. Ituza neza ubushuhe bwo hejuru n'amashanyarazi ya perovskite. Ubushuhe bwa PbC2O4 mu mazi ni 0.00065 g/L gusa, ari na yo iri hasi kurusha iya PbSO428. Ikirenzeho, urwego rw'ubucucike kandi rungana rwa LOS rushobora gutegurwa buhoro buhoro kuri filimi za perovskite hakoreshejwe uburyo bwo gukora ibintu (reba hepfo). Twakoze simulation za DFT z'ubucucike hagati ya FAPbI3 na PbC2O4 nk'uko bigaragara ku Ishusho y'Inyongera ya 1. Imbonerahamwe y'Inyongera ya 2 igaragaza ingufu zo gukora inenge nyuma yo guterwa LOS. Twasanze LOS idakomeza gusa ingufu zo gukora za VI defects kuri 0.69–1.53 eV (Ishusho ya 1d), ahubwo yongera ingufu zo gukora za I ku buso bwo kwimuka no gusohoka (Ishusho ya 1e). Mu cyiciro cya mbere, I ions zimuka ku buso bwa perovskite, zigasiga VI ions mu mwanya wa lattice hamwe n'ingufu ziva kuri 0.61 eV. Nyuma yo kwinjiza LOS, bitewe n'ingaruka zo kubangamira steric, ingufu zo gukora zimuka za I ions ziyongera kugera kuri 1.28 eV. Mu gihe cyo kwimuka kwa I ions ziva ku buso bwa perovskite, ingufu ziva kuri VOC nazo ziba ziri hejuru kurusha mu rugero rwo kugenzura (Ishusho ya 1e). Imbonerahamwe z'imbonerahamwe z'inzira zo kwimuka kwa I ions mu kugenzura na LOS FAPbI3 zigaragazwa ku Ishusho ya 1 f na g, uko bikurikirana. Ibisubizo bya simulation bigaragaza ko LOS ishobora kubuza iremwa rya VI defects no guhinduka kwa I, bityo ikabuza nucleation y'impinduka ya α kuri δ phase.
Uburyo aside oxalic na perovskite ya FAPbI3 byageragejwe. Nyuma yo kuvanga ibisubizo bya aside oxalic na FAPbI3, habayeho ingano nini y'umweru, nk'uko bigaragara ku Ishusho y'Inyongera ya 2. Ifu yabonetse nk'ibikoresho bya PbC2O4 byuzuye hakoreshejwe X-ray diffraction (XRD) (Ishusho y'Inyongera ya 3) na Fourier transform infrared spectroscopy (FTIR) (Ishusho y'Inyongera ya 4). Twasanze aside oxalic ishongera cyane muri isopropyl alcohol (IPA) ku bushyuhe bw'icyumba hamwe n'umushongi wa 18 mg / mL, nk'uko bigaragara ku Ishusho y'Inyongera ya 5. Ibi bituma gutunganya nyuma byoroha kuko IPA, nk'ikintu gisanzwe gikoreshwa mu gufunga, idatuma urwego rwa perovskite rwangirika nyuma y'igihe gito29. Kubwibyo, mu kwinjiza agace ka perovskite mu gisubizo cya aside oxalic cyangwa mu gusiga agace ka aside oxalic kuri perovskite, PbC2O4 yoroheje kandi ikomeye ishobora kuboneka vuba ku buso bwa agace ka perovskite hakurikijwe ikigereranyo gikurikira cy’imiti: H2C2O4 + FAPbI3 = PbC2O4 + FAI + HI. FAI ishobora gushonga muri IPA bityo igakurwaho mu gihe cyo guteka. Ubunini bwa LOS bushobora kugenzurwa hakoreshejwe igihe cyo gukora n’uburyo bubanziriza.
Amashusho ya mikoroskopi ya elegitoroniki yo gupima (SEM) y’ubugenzuzi na firime za LOS perovskite agaragara ku Ishusho ya 2a, b. Ibisubizo bigaragaza ko imiterere y’ubuso bwa perovskite ibitswe neza, kandi umubare munini w’uduce duto dushyirwa ku buso bw’ingano, byagombye kuba bigaragaza urwego rwa PbC2O4 rukozwe n’uburyo bwo gukora ibintu muri situ. Filimi ya LOS perovskite ifite ubuso bworoshye gato (Ishusho y’inyongera ya 6) n’inguni nini y’amazi ugereranije na firime yo kugenzura (Ishusho y’inyongera ya 7). Mikoroskopi ya elegitoroniki yo gupima ifite ubushobozi bwo hejuru (HR-TEM) yakoreshejwe mu gutandukanya urwego rw’ubuso bw’umusaruro. Ugereranije na firime yo kugenzura (Ishusho ya 2c), urwego ruto kandi rurerure rufite ubugari bwa nm 10 rugaragara neza hejuru ya LOS perovskite (Ishusho ya 2d). Hakoreshejwe mikorosikopi ya elegitoroniki yo gupima ikirere cy’umwijima (HAADF-STEM) ifite angle yo hejuru kugira ngo harebwe aho PbC2O4 na FAPbI3 ihurira, kuba hari uturere twa kristu twa FAPbI3 n’uturere tudafite ishusho ya PbC2O4 bishobora kugaragara neza (Ishusho y’inyongera ya 8). Imiterere y’ubuso bwa perovskite nyuma yo kuvurwa na aside oxalic yagaragajwe n’ibipimo bya X-ray photoelectron spectroscopy (XPS), nk’uko bigaragara ku Mashusho ya 2e–g. Mu Ishusho ya 2e, uburebure bwa C 1s buri hafi 284.8 eV na 288.5 eV ni bimwe mu bimenyetso byihariye bya CC na FA, uko bikurikirana. Ugereranyije n’uburyo bwo kugenzura, imiterere ya LOS yagaragaje uburebure bw’inyongera kuri 289.2 eV, iterwa na C2O42-. Umwimerere wa O 1s wa LOS perovskite ugaragaza imisozi itatu itandukanye ya O 1s mu buryo bwa shimi kuri 531.7 eV, 532.5 eV, na 533.4 eV, bihuye na COO yavuyemo protonated, C=O ya atome za oxalate 30 na O z’igice cya OH (Ishusho ya 2e). )). Ku cyitegererezo cyo kugenzura, hagaragaye umusozi muto wa O 1s gusa, ushobora guterwa na ogisijeni ikoreshwa mu gupima ku buso. Imiterere y’urusobe rw’igenzura rwa Pb 4f7/2 na Pb 4f5/2 iherereye kuri 138.4 eV na 143.3 eV, uko bikurikirana. Twabonye ko LOS perovskite igaragaza impinduka y’umubare wa Pb wa 0.15 eV ugana ku ngufu nyinshi zo gufatanya, bigaragaza imikoranire ikomeye hagati ya atome za C2O42- na Pb (Ishusho ya 2g).
a Amashusho ya SEM y'igenzura na b filime za LOS perovskite, icyerekezo cyo hejuru. c Mikroskopi ya elegitoroniki yohereza amashanyarazi ifite ubushobozi bwo hejuru (HR-TEM) y'igenzura na d filime za LOS perovskite. XPS ifite ubushobozi bwo hejuru ya e C 1s, f O 1s na g Pb 4f perovskite filime. Amakuru y'inkomoko atangwa mu buryo bwa dosiye y'amakuru y'inkomoko.
Dukurikije ibyavuye mu bushakashatsi bwa DFT, byavuzwe ko inenge za VI n’impinduka za I bitera ihinduka ry’icyiciro kuva kuri α kugera kuri δ. Raporo zabanje zagaragaje ko I2 irekurwa vuba cyane kuva kuri firime za perovskite zishingiye kuri PC mu gihe cyo kwibiza mu kirere nyuma yo gushyira firime ku mucyo n’ubushyuhe 31,32,33. Kugira ngo twemeze ingaruka nziza za oxalate y’icyiciro cya α cya perovskite, twinjije firime za control na LOS perovskite mu macupa y’ikirahure abonerana arimo toluene, hanyuma tuyashyiramo urumuri rw’izuba 1 mu gihe cy’amasaha 24. Twapimye uburyo bwo kwinjiza imirasire ya ultraviolet n’urumuri rugaragara (UV-Vis). ) toluene, nk’uko bigaragara ku Ishusho ya 3a. Ugereranije n’icyitegererezo cyo kwinjiza, imbaraga nke cyane zo kwinjiza imirasire ya I2 zagaragaye mu gihe cya LOS-perovskite, bigaragaza ko LOS nto ishobora kubuza I2 kurekurwa muri firime ya perovskite mu gihe cyo kwibiza mu kirere. Amafoto ya firime za control za kera na LOS perovskite agaragara mu mashusho ya 3b na c. Perovskite ya LOS iracyari umukara, mu gihe igice kinini cy’igenzura cyahindutse umuhondo. Imiterere y’urumuri rwa UV igaragara muri firime yinjijwe igaragara ku ishusho ya 3b, c. Twabonye ko uburyo bwo kwinjiza urumuri bujyanye na α muri firime y’igenzura bwagabanutse cyane. Ibipimo bya X-ray byakozwe kugira ngo hamenyekane imiterere ya kristu. Nyuma y’amasaha 24 y’urumuri, firime y’igenzura yagaragaje ikimenyetso gikomeye cy’umuhondo wa δ (11.8°), mu gihe firime ya LOS perovskite ikomeje kuba umukara mwiza (Ishusho ya 3d).
Imiterere y’urumuri rwa toluene igaragara mu buryo bwa UV aho firime igenzura n’ifirime ya LOS byinjijwe munsi y’izuba rimwe mu gihe cy’amasaha 24. Ishusho yerekana agacupa aho buri firime yinjijwe mu gipimo kingana cya toluene. b Imiterere y’urumuri rwa UV-Vis igenzura n’ifirime ya LOS mbere na nyuma y’amasaha 24 yo kwinjizwa munsi y’izuba rimwe. Ishusho igaragaza ifoto ya firime igerageza. d Imiterere ya diffraction ya X-ray y’igenzura n’ifirime za LOS mbere na nyuma y’amasaha 24 yo kwinjizwa. Amashusho ya SEM ya firime igenzura e na firime f LOS nyuma y’amasaha 24 yo kwinjizwa. Amakuru y’inkomoko atangwa mu buryo bwa dosiye y’amakuru y’inkomoko.
Twakoze ibipimo bya scanning electron microscopy (SEM) kugira ngo turebe impinduka mu miterere ya firime ya perovskite nyuma y'amasaha 24 y'urumuri, nk'uko bigaragara ku Mashusho ya 3e, f. Muri firime yo kugenzura, ibinyampeke binini byarangiritse bihinduka urushinge ruto, bihuye n'imiterere y'umusaruro wa δ-phase FAPbI3 (Ishusho ya 3e). Kuri firime za LOS, ibinyampeke bya perovskite biguma mu mimerere myiza (Ishusho ya 3f). Ibisubizo byemeje ko kubura kwa I bitera cyane ihinduka kuva ku cyiciro cy'umukara kugera ku gice cy'umuhondo, mu gihe PbC2O4 ikomeza igice cy'umukara, ikarinda kubura kwa I. Kubera ko ubucucike bw'imyanda ku buso buri hejuru cyane ugereranyije n'ingano,34 iki cyiciro gishobora kubaho ku buso bw'ibinyampeke icyarimwe, kikarekura iyode igakora VI. Nk'uko byahanuwe na DFT, LOS ishobora kubuza ikorwa ry'ibinyampeke bya VI no gukumira kwimuka kwa iyoni za I ku buso bwa perovskite.
Byongeye kandi, hakozwe ubushakashatsi ku ngaruka z'urwego rwa PbC2O4 ku bushyuhe bwa filimi za perovskite mu kirere (ubushyuhe bungana na 30-60%). Nk'uko bigaragara ku Ishusho y'Inyongera ya 9, perovskite ya LOS yari ikiri umukara nyuma y'iminsi 12, mu gihe filimi y'igenzura yahindutse umuhondo. Mu bipimo bya XRD, filimi y'igenzura igaragaza uburebure bukomeye kuri 11.8° bujyanye n'igice cya δ cya FAPbI3, mu gihe perovskite ya LOS igumana ikiraro cya α cy'umukara (Ishusho y'Inyongera ya 10).
Ishusho y'urumuri rwa steady-state (PL) na photoluminescence ya TRPL (TRPL) byakoreshejwe mu kwiga ingaruka zo kudakora neza kwa oxalate y'icuma ku buso bwa perovskite. Ku ishusho ya 4a, filime ya LOS yongereye imbaraga za PL. Mu ishusho ya PL, imbaraga za filime ya LOS ku buso bwose bwa 10 × 10 μm2 ziruta iz'ishusho y'igenzura (Ishusho y'inyongera ya 11), bigaragaza ko PbC2O4 igabanya imbaraga za filime ya perovskite. Igihe cyo gutwara kigenwa no kwegereza kubora kwa TRPL hakoreshejwe imikorere imwe y'igaragaza (Ishusho ya 4b). Igihe cyo gutwara cya filime ya LOS ni 5.2 μs, kikaba kirekire cyane kurusha filime y'igenzura ifite igihe cyo gutwara cya 0.9 μs, bigaragaza ko kugabanuka k'ubuso butari imirasire.
PL ihoraho na b-spectra bya PL y'igihe gito ya filime za perovskite ku bidukikije by'ikirahure. c Umurongo wa SP w'igikoresho (FTO/TiO2/SnO2/perovskite/spiro-OMeTAD/Au). d EQE spectrum na Jsc EQE spectrum bihujwe n'igikoresho gikora neza cyane. d Gushingira ku bushyuhe bw'urumuri rw'igikoresho cya perovskite ku gishushanyo cya Voc. f Isesengura risanzwe rya MKRC rikoresheje igikoresho cya ITO/PEDOT:PSS/perovskite/PCBM/Au gisukuye. VTFL ni voltage ntarengwa yo kuzuza trap. Duhereye kuri aya makuru twabaze ubucucike bw'umutego (Nt). Amakuru y'isoko atangwa mu buryo bwa dosiye z'amakuru y'isoko.
Kugira ngo twige ingaruka z'urwego rwa oxalate y'icyitegererezo ku mikorere y'igikoresho, hakoreshejwe imiterere gakondo ya FTO/TiO2/SnO2/perovskite/spiro-OMeTAD/Au. Dukoresha formamidine chloride (FACl) nk'inyongera ku gice cya mbere cya perovskite aho gukoresha methylamine hydrochloride (MACl) kugira ngo tugere ku mikorere myiza y'igikoresho, kubera ko FACl ishobora gutanga kristalo nziza no kwirinda icyuho cya FAPbI335 (reba Ishusho y'inyongera ya 1 na 2 kugira ngo tugereranye neza). ). 12-14). IPA yatoranyijwe nk'umuti urwanya solvent kuko itanga kristalo nziza kandi ikunda kwerekezwa muri filimi za perovskite ugereranije na diethyl ether (DE) cyangwa chlorobenzene (CB)36 (Ishusho y'inyongera ya 15 na 16). Ubunini bwa PbC2O4 bwatunganyijwe neza kugira ngo buringanize neza uburyo ikibazo kigenda gihinduka no gutwara charge binyuze mu guhindura ingano ya aside oxalic (Ishusho y'inyongera ya 17). Amashusho ya SEM y’ibikoresho byabugenewe byo kugenzura neza n’ibikoresho bya LOS agaragara ku Ishusho y’inyongera ya 18. Imirongo isanzwe y’ubucucike bw’amashanyarazi (CD) ku bikoresho byo kugenzura na LOS igaragara ku Ishusho ya 4c, kandi ibipimo byakuwemo bigaragazwa mu Imbonerahamwe y’inyongera ya 3. Ubushobozi ntarengwa bwo guhindura imbaraga (PCE) ni 23.43% (22.94%), Jsc 25.75 mA cm-2 (25.74 mA cm-2), Voc 1.16 V (1.16 V) na scan reverse (imbere). Factor yo kuzuza (FF) ni 78.40% (76.69%). PCE LOS PSC ntarengwa ni 25.39% (24.79%), Jsc ni 25.77 mA cm-2, Voc ni 1.18 V, FF ni 83.50% (81.52%) uhereye inyuma (imbere Scan kugeza). Igikoresho cya LOS cyabonye imikorere yemewe ya 24.92% muri laboratwari yizewe ya fotovoltaic y’uruhande rwa gatatu (Ishusho y’inyongera ya 19). Ubuhanga bwa quantum bwo hanze (EQE) bwatanze Jsc ihuriweho ya 24.90 mA cm-2 (igenzura) na 25.18 mA cm-2 (LOS PSC), uko bikurikirana, byari bihuye neza na Jsc yapimwe muri AM 1.5 G spectrum isanzwe (Ishusho ya .4d). ). Ikwirakwizwa ry’imibare rya PCE zapimwe zo kugenzura na LOS PSCs rigaragazwa mu Ishusho y’inyongera ya 20.
Nkuko bigaragara ku Ishusho ya 4e, isano iri hagati ya Voc n'ubukana bw'urumuri yapimwe kugira ngo yige ingaruka za PbC2O4 ku gusubiranamo kw'ubuso bufashijwe na trap. Uburebure bw'umurongo ushyizwemo ku gikoresho cya LOS ni 1.16 kBT/sq, buri munsi y'uburebure bw'umurongo ushyizwemo ku gikoresho cyo kugenzura (1.31 kBT/sq), byemeza ko LOS ifite akamaro mu gukumira gusubiranamo kw'ubuso hakoreshejwe decoys. Dukoresha ikoranabuhanga rigabanya amashanyarazi y'umwanya (SCLC) kugira ngo dupime ubucucike bw'inenge bwa filimi ya perovskite dupima imiterere yijimye ya IV y'igikoresho cy'umwobo (ITO/PEDOT:PSS/perovskite/spiro-OMeTAD/Au) nk'uko bigaragara ku ishusho. 4f Erekana. Ubucucike bw'umutego bubarwa hakoreshejwe formula Nt = 2ε0εVTFL/eL2, aho ε ari constant dielectric ya filime ya perovskite, ε0 ni constant dielectric ya vacuum, VTFL ni voltage igabanya yo kuzuza umutego, e ni charge, L ni ubunini bwa filime ya perovskite (650 nm). Ubucucike bw'inenge bw'igikoresho cya VOC bubarwa kuri 1.450 × 1015 cm–3, buri munsi y'ubucucike bw'inenge bw'igikoresho cyo kugenzura, ari cyo 1.795 × 1015 cm–3.
Igikoresho cyari gipakuruwe cyageragejwe ku ngufu ntarengwa (MPP) munsi y'izuba ryinshi munsi ya azote kugira ngo harebwe uburyo gihagaze neza mu gihe kirekire (Ishusho ya 5a). Nyuma y'amasaha 550, igikoresho cya LOS cyakomeje kugumana 92% by'ubushobozi bwacyo ntarengwa, mu gihe imikorere y'igikoresho cyo kugenzura yari yagabanutse ikagera kuri 60% by'imikorere yacyo ya mbere. Ikwirakwizwa ry'ibintu mu gikoresho gishaje ryapimwe hakoreshejwe igihe cyo kuguruka kwa secondary ion mass spectrometry (ToF-SIMS) (Ishusho ya 5b, c). Ingano nini ya ayode igaragara mu gace ko hejuru ka zahabu. Imiterere yo kurinda imyuka idafite ingufu ntikuraho ibintu byangiza ibidukikije nk'ubushuhe na ogisijeni, bigaragaza ko uburyo bw'imbere (ni ukuvuga kwimuka kwa ayoni) ari byo bitera. Dukurikije ibyavuye muri ToF-SIMS, iyoni za I- na AuI2 zabonetse muri electrode ya Au, bigaragaza ko I iva muri perovskite ijya muri Au. Ubukana bw'ikimenyetso cya iyoni za I- na AuI2 mu gikoresho cyo kugenzura buri hejuru y'inshuro 10 ugereranyije n'icyitegererezo cya VOC. Raporo zabanjirije iyi zagaragaje ko kwinjira kwa iyoni bishobora gutuma spiro-OMeTAD igenda igabanuka vuba mu buryo bwo gutwara imyobo ndetse no kwangirika kw'icyiciro cyo hejuru cya electrode, bityo bikangiza uburyo bwo guhuza igikoresho mu gikoresho37,38. Electrode ya Au yakuweho maze urwego rwa spiro-OMeTAD rusukurwa muri substrate hakoreshejwe umuti wa chlorobenzene. Hanyuma twashyize filime ku murongo w'imashini ya X-ray diffraction (GIXRD) (Ishusho ya 5d). Ibisubizo bigaragaza ko filime igenzura ifite uburebure bugaragara bwa diffraction kuri 11.8°, mu gihe nta uburebure bushya bwa diffraction bugaragara mu gipimo cya LOS. Ibisubizo bigaragaza ko igihombo kinini cya iyoni za I muri filime igenzura gituma habaho δ phase, mu gihe muri filime ya LOS iyi nzira igaragara ko ihagaritswe.
Amasaha 575 yo gukurikirana MPP igikoresho kidafunze mu kirere cya azote n'izuba rimwe ridafite akayunguruzo ka UV. Ikwirakwizwa rya ToF-SIMS rya b I- na c AuI2- ions mu gikoresho cyo kugenzura LOS MPP n'igikoresho gishaje. Amabara y'umuhondo, icyatsi n'umuhondo ahuye na Au, Spiro-OMeTAD na perovskite. d GIXRD ya firime ya perovskite nyuma yo gupimwa na MPP. Amakuru y'isoko atangwa mu buryo bwa dosiye z'amakuru y'isoko.
Uburyo bwo gutwara amashanyarazi bushingiye ku bushyuhe bwapimwe kugira ngo hemezwe ko PbC2O4 ishobora kubuza uburyo iyoni yimuka (Ishusho y'inyongera ya 21). Ingufu zo gukora (Ea) z'uburyo iyoni yimuka zigenwa no gupima impinduka mu buryo bwo gutwara amashanyarazi (σ) bwa filime ya FAPbI3 ku bushyuhe butandukanye (T) no gukoresha isano ya Nernst-Einstein: σT = σ0exp(−Ea/kBT), aho σ0 ari ikintu gihoraho, kB ni ikintu gihoraho cya Boltzmann. Tubona agaciro ka Ea uhereye ku ruhande rwa ln(σT) ugereranyije na 1/T, ari byo 0.283 eV yo kugenzura na 0.419 eV yo gukoresha igikoresho cya LOS.
Muri make, dutanga uburyo bwo kumenya inzira yo kwangirika kwa perovskite ya FAPbI3 n'ingaruka z'inenge zitandukanye ku nzitizi y'impinduka ya phase ya α-δ. Muri izi nenge, inenge za VI zivugwa ko zishobora gutera impinduka kuva kuri α kugera kuri δ. Hashyizweho urwego rw'ubucucike bunini bwa PbC2O4 budashonga kandi buhamye mu mazi kugira ngo butuze phase ya α ya FAPbI3 binyuze mu kubuza ishyirwaho ry'imyanya ya I n'iyimuka rya iyoni za I. Iyi ngamba igabanya cyane isubiranamo ry'urusobe rw'imirasire hagati y'urusobe, yongera imikorere myiza y'uturemangingo tw'izuba kugeza kuri 25.39%, kandi ikongera ubudahangarwa bw'imikorere. Ibisubizo byacu bitanga ubuyobozi bwo kugera kuri PSC za formamidine zikora neza kandi zihamye binyuze mu kubuza impinduka ya phase ya α iterwa n'inenge kuva kuri δ.
Isopropoxide ya Titanium (IV) (TTIP, 99.999%) yaguzwe muri Sigma-Aldrich. Aside ya Hydrochloric (HCl, 35.0–37.0%) na ethanol (anhydrous) byaguzwe muri Guangzhou Chemical Industry. SnO2 (15 wt% tin (IV) oxide colloidal dispersion) yaguzwe muri Alfa Aesar. Lead (II) iyode (PbI2, 99.99%) yaguzwe muri TCI Shanghai (Ubushinwa). Formamidine iyode (FAI, ≥99.5%), formamidine chloride (FACl, ≥99.5%), methylamine hydrochloride (MACl, ≥99.5%), 2,2′,7,7′-tetrakis-(N , N-di-p) )-methoxyaniline)-9,9′-spirobifluorene (Spiro-OMeTAD, ≥99.5%), lithium bis(trifluoromethane)sulfonylimide (Li-TFSI, 99.95%), 4-tert -butylpyridine (tBP, 96%) yaguzwe muri Xi'an Polymer Light Technology Company (Ubushinwa). N,N-dimethylformamide (DMF, 99.8%), dimethyl sulfoxide (DMSO, 99.9%), isopropyl alcohol (IPA, 99.8%), chlorobenzene (CB, 99.8%), acetonitrile (ACN). Yaguzwe muri Sigma-Aldrich. Aside oxalic (H2C2O4, 99.9%) yaguzwe muri Macklin. Imiti yose yakoreshejwe uko yakiriwe nta zindi mpinduka.
ITO cyangwa FTO substrates (1.5 × 1.5 cm2) byasukuwe hakoreshejwe ikoranabuhanga hifashishijwe isabune, acetone, na ethanol mu gihe cy'iminota 10, hanyuma byumishwa munsi y'umugezi wa azote. Urukuta rw'urutare rwa TiO2 rwashyizwe ku rukuta rwa FTO hakoreshejwe umuti wa titanium diisopropoxybis (acetylacetonate) muri ethanol (1/25, v/v) washyizwe kuri 500 °C mu gihe cy'iminota 60. Ihindagurika rya SnO2 colloidal ryavanzwe n'amazi ya deionized mu gipimo cya 1:5. Ku rukuta rusukuye rwavuwe na ozone ya UV mu gihe cy'iminota 20, agace gato ka SnO2 nanoparticles kashyizwe kuri 4000 rpm mu gihe cy'amasegonda 30 hanyuma gashyuha kuri 150 °C mu gihe cy'iminota 30. Ku muti wa perovskite precursor, 275.2 mg FAI, 737.6 mg PbI2 na FACl (20 mol%) byashongeshejwe muri DMF/DMSO (15/1) solvent ivanze. Urupapuro rwa perovskite rwateguwe hakoreshejwe centrifuge ya 40 μL y'umuti wa perovskite ubanza hejuru y'urupapuro rwa SnO2 rwavuwe na UV-ozone kuri 5000 rpm mu kirere mu gihe cy'amasegonda 25. Amasegonda 5 nyuma y'igihe cya nyuma, 50 μL y'umuti wa MACl IPA (4 mg/mL) yashyizwe ku butaka nk'umuti ugabanya ubushyuhe. Hanyuma, uduce dushya twateguwe twashyizwe ku bushyuhe bwa 150°C mu gihe cy'iminota 20 hanyuma kuri 100°C mu gihe cy'iminota 10. Nyuma yo gukonjesha agapapuro ka perovskite kugeza ku bushyuhe bw'icyumba, umuti wa H2C2O4 (1, 2, 4 mg yashongeshejwe muri 1 mL IPA) washyizwe ku bushyuhe bwa 4000 rpm mu gihe cy'amasegonda 30 kugira ngo ubuso bwa perovskite buhumeke. Umuti wa spiro-OMeTAD wateguwe hifashishijwe kuvanga 72.3 mg ya spiro-OMeTAD, 1 ml ya CB, 27 µl tBP na 17.5 µl ya Li-TFSI (520 mg muri 1 ml ya acetonitrile) washyizwe kuri firime ku muvuduko wa 4000 rpm mu masegonda 30. Amaherezo, urwego rwa Au rufite ubugari bwa 100 nm rwakuwe mu mwuka mu buryo bwa vacuum ku muvuduko wa 0.05 nm/s (0~1 nm), 0.1 nm/s (2~15 nm) na 0.5 nm/s (16~100 nm).
Imikorere ya SC y'uturemangingo tw'izuba twa perovskite yapimwe hakoreshejwe metero 2400 za Keithley munsi y'urumuri rwa simulator y'izuba (SS-X50) ku bushyuhe bwa 100 mW/cm2 kandi byemezwa hakoreshejwe uturemangingo tw'izuba twa silikoni twagenzuwe. Keretse byavuzwe ukundi, imiyoboro ya SP yapimwe mu gasanduku kuzuye uturindantoki ku bushyuhe bw'icyumba (~25°C) mu buryo bwo gupima imbere n'inyuma (intambwe ya voltage 20 mV, igihe cyo gutinda 10 ms). Hakoreshejwe agapfukamunwa k'igicucu kugira ngo hamenyekane ubuso bufatika bwa cm2 0.067 kuri PSC yapimwe. Ibipimo bya EQE byakorewe mu kirere hakoreshejwe sisitemu ya PVE300-IVT210 (Industrial Vision Technology(s) Pte Ltd) hamwe n'urumuri rumwe rwibanze ku gikoresho. Kugira ngo igikoresho gikomere, igeragezwa ry'uturemangingo tw'izuba tutarapfundikirwa ryakorewe mu gasanduku k'uturindantoki ka azote ku gitutu cya 100 mW/cm2 nta kayunguruzo ka UV. ToF-SIMS ipimwa hakoreshejwe PHI nanoTOFII igihe cyo kuguruka SIMS. Ubujyakuzimu bwabonetse hakoreshejwe imbunda ya Arion ya 4 kV ifite ubuso bwa 400×400 µm.
Ibipimo bya X-ray photoelectron spectroscopy (XPS) byakorewe kuri sisitemu ya Thermo-VG Scientific (ESCALAB 250) hakoreshejwe Al Kα ya monochromatized (kuri XPS mode) ku gitutu cya 5.0 × 10–7 Pa. Mikroskopi ya electron scanning (SEM) yakozwe kuri sisitemu ya JEOL-JSM-6330F. Imiterere y'ubuso n'ubukana bwa filimi za perovskite byapimwe hakoreshejwe mikroskopi ya atome force (AFM) (Bruker Dimension FastScan). STEM na HAADF-STEM bikorerwa kuri FEI Titan Themis STEM. Imiterere ya UV-Vis absorption spectra yapimwe hakoreshejwe UV-3600Plus (Shimadzu Corporation). Umuriro ugabanya charge current (SCLC) wafashwe kuri metero 2400 za Keithley. Umuriro uhoraho (PL) na photoluminescence (TRPL) ya carrier lifetime decay byapimwe hakoreshejwe spectrometer ya FLS 1000 photoluminescence. Amashusho ya PL mapping yapimwe hakoreshejwe sisitemu ya Horiba LabRam Raman HR Evolution. Fourier transform infrared spectroscopy (FTIR) yakozwe hakoreshejwe sisitemu ya Thermo-Fisher Nicolet NXR 9650.
Muri uyu murimo, dukoresha uburyo bwo gukusanya inzira ya SSW kugira ngo twige inzira y’impinduka y’icyiciro kuva kuri α-phase kugera kuri δ-phase. Muri ubwo buryo bwa SSW, ingendo y’ubuso bw’ingufu zishobora kugenwa n’icyerekezo cya random soft mode (icyiciro cya kabiri), bituma habaho inyigo irambuye kandi idafite aho ihuriye n’ubuso bw’ingufu zishobora kugenwa. Muri uyu murimo, gukusanya inzira bikorwa kuri supercell ya atome 72, kandi ibice birenga 100 bya mbere/ibya nyuma (IS/FS) bikusanyirizwa ku rwego rwa DFT. Hashingiwe ku makuru ya IS/FS, inzira ihuza imiterere y’ibanze n’imiterere ya nyuma ishobora kugenwa hamwe n’aho atome zihurira, hanyuma inzira ebyiri ku buso bw’impinduka zikoreshwa kugira ngo hamenyekane neza uburyo bw’impinduka. (VK-DESV). Nyuma yo gushakisha imiterere y’impinduka, inzira ifite imbogamizi ntoya ishobora kugenwa hashyirwa ku rutonde inzitizi z’ingufu.
Imibare yose ya DFT yakozwe hakoreshejwe VASP (version 5.3.5), aho imikoranire ya electron-ion ya atome za C, N, H, Pb, na I ihagarariwe na gahunda ya amplified wave (PAW). Imikorere y'ihindagurika ry'impinduka isobanurwa na generalized gradient approximation muri Perdue-Burke-Ernzerhoff parameterization. Ingufu ntarengwa ku miraba y'indege zashyizwe kuri 400 eV. Monkhorst-Pack k-point grid ifite ingano ya (2 × 2 × 1). Ku miterere yose, lattice na atome positions byakozwe neza kugeza igihe igice cy'umuvuduko ntarengwa cyari munsi ya 0.1 GPa naho igice cy'imbaraga ntarengwa cyari munsi ya 0.02 eV/Å. Mu ishusho y'ubuso, ubuso bwa FAPbI3 bufite imiterere 4, urwego rwo hasi rufite atome zidahinduka zigana umubiri wa FAPbI3, kandi imiterere itatu yo hejuru ishobora kugenda neza mu gihe cyo gutunganya neza. Urusobe rwa PbC2O4 rufite ubugari bwa ML 1 kandi ruri ku buso bwa I-terminal bwa FAPbI3, aho Pb ihujwe na 1 I na 4 O.
Kugira ngo umenye byinshi ku bijyanye n'igishushanyo mbonera cy'ubushakashatsi, reba Incamake ya Raporo y'Ubushakashatsi bw'Ibintu Bisanzwe ijyanye n'iyi nkuru.
Amakuru yose yabonetse cyangwa yasesenguwe muri ubu bushakashatsi ari mu nkuru yasohotse, ndetse no mu makuru y’inyongera n’amadosiye y’amakuru fatizo. Amakuru fatizo yagaragajwe muri ubu bushakashatsi araboneka kuri https://doi.org/10.6084/m9.figshare.2410016440. Amakuru y’inkomoko y’iyi nkuru aratangwa.
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