Yɛda mo ase sɛ moakɔ Nature.com. Browser no nkyerɛase a wode redi dwuma no wɔ CSS mmoa kakraa bi. Sɛ wopɛ sɛ wunya nea eye sen biara a, yɛhyɛ nyansa sɛ fa wo browser no foforo di dwuma (anaasɛ dum compatibility mode wɔ Internet Explorer mu). Saa bere yi de, sɛnea ɛbɛyɛ a yɛbɛhwɛ ma wɔakɔ so aboa no, yɛrekyerɛ sait no a yɛmfa styling anaa JavaScript nka ho.
Wɔde sintɔ pasivation adi dwuma kɛse de ama lead triiodide perovskite owia nkwammoaa no adwumayɛ atu mpɔn, nanso nkɛntɛnso ahorow a sintɔ ahorow nya wɔ α-phase stability so no da so ara yɛ nea wontumi nhu; Ɛha yi, yɛde density functional theory di dwuma no, yehu nea edi kan a formamidine lead triiodide perovskite no sɛe kwan fi α-fase so kɔ δ-fase so na yesua nkɛntɛnso a sintɔ ahorow nya wɔ phase nsakrae ahoɔden akwanside no so. Simulation aba no kyerɛ sɛ iodine vacancies na ɛda adi kɛse sɛ ɛde ɔsɛeɛ bɛba ɛfiri sɛ ɛbrɛ ahoɔden akwansideɛ a ɛwɔ α-δ phase nsakraeɛ no ase kɛseɛ na ɛwɔ formation ahoɔden a ɛba fam koraa wɔ perovskite ani. Kɔbere oxalate a nsu ntumi nkɔ mu a ɛyɛ den a wɔde ba perovskite no ani no siw α-fase no a ɛporɔw no ano kɛse, na esiw iodine a ɛkɔ baabi foforo na ɛyɛ hyew no ano. Bio nso, saa kwan yi brɛ interfacial nonradiative recombination ase kɛseɛ na ɛma owia nkwammoaa a ɛyɛ adwuma yie kɔ soro kɔduru 25.39% (wɔagye atom sɛ ɛyɛ 24.92%). Afiri a wɔankyekyere no da so ara tumi kura ne mfitiase 92% adwumayɛ mu bere a ayɛ adwuma wɔ ahoɔden a ɛsen biara mu nnɔnhwerew 550 wɔ mframa a ɛyɛ den a wɔayɛ no sɛ 1.5 G ase akyi.
Tumi a wɔdannan no yie (PCE) a ɛwɔ perovskite owia nkwammoaa (PSCs) mu no adu nea wɔagye atom sɛ ɛyɛ 26%1. Efi afe 2015 no, nnɛyi PSC ahorow no apɛ formamidine triiodide perovskite (FAPbI3) sɛ hann-absorbing layer esiane sɛ ɛyɛ hyew yiye a ɛyɛ den ne bandgap a wɔpɛ a ɛbɛn Shockley-Keisser anohyeto a ɛyɛ 2,3,4 nti. Awerɛhosɛm ne sɛ, FAPbI3 sini ahorow thermodynamically fa phase nsakrae fi tuntum α fase kɔ kɔkɔɔ a ɛnyɛ perovskite δ fase wɔ dan mu hyew5,6. Nea ɛbɛyɛ na wɔasiw delta fã no ano no, wɔayɛ perovskite ahorow a ɛyɛ den. Ɔkwan a wɔtaa fa so di ɔhaw yi so ne sɛ wɔde FAPbI3 fra methyl ammonium (MA+), cesium (Cs+) ne bromide (Br-) ions a wɔaka abom7,8,9. Nanso, hybrid perovskites hu amane wɔ bandgap broadening ne photoinduced phase separation, a ɛma PSCs a efi mu ba no adwumayɛ ne adwumayɛ mu pintinn yɛ basaa10,11,12.
Nnansa yi nhwehwɛmu ada no adi sɛ ahwehwɛ biako a ɛho tew FAPbI3 a enni doping biara wɔ ahoɔden a ɛkyɛn so esiane ne crystallinity a eye kyɛn so ne sintɔ ahorow a ɛba fam nti13,14. Enti, sintɔ ahorow a wɔbɛtew so denam FAPbI3 a ɛdɔɔso no ahwehwɛ a wɔbɛma akɔ soro so no yɛ ɔkwan a ɛho hia a wɔfa so nya PSC ahorow a ɛyɛ adwuma yiye na ɛyɛ den2,15. Nanso, bere a FAPbI3 PSC no reyɛ adwuma no, ɔsɛe a ɛkɔ hexagonal hexagonal non-perovskite δ phase a wɔmpɛ no mu no da so ara betumi aba16. Adeyɛ no taa fi ase wɔ mmeae a ɛwɔ soro ne aburow ahye a ɛyɛ mmerɛw sɛ nsu, ɔhyew ne hann bɛba esiane mmeae pii a asɛe nti17. Enti, ɛho hia sɛ wɔyɛ surface/grain passivation na ama FAPbI318 no fã tuntum no agyina. Defect passivation akwan pii, a nea ɛka ho ne perovskites a ɛba fam, acid-base Lewis molecules, ne ammonium halide nkyene a wɔde aba no anya nkɔso kɛse wɔ formamidine PSCs mu19,20,21,22. Ɛde besi nnɛ no, ɛkame ayɛ sɛ nhwehwɛmu nyinaa atwe adwene asi dwuma a sintɔ ahorow di wɔ optoelectronic su te sɛ carrier recombination, diffusion tenten ne band structure wɔ owia nkwammoaa mu a wɔkyerɛ mu22,23,24. Sɛ nhwɛsoɔ no, wɔde density functional theory (DFT) di dwuma de kyerɛ sɛnea formation ahoɔden ne trapping ahoɔden dodoɔ a ɛwɔ sintɔ ahodoɔ mu, a wɔde di dwuma kɛseɛ de kyerɛ practical passivation design20,25,26. Bere a sintɔ dodow so tew no, mpɛn pii no, sɛnea afiri no gyina pintinn no tu mpɔn. Nanso, wɔ formamidine PSCs mu no, ɛsɛ sɛ akwan horow a sintɔ ahorow nya wɔ phase stability ne photoelectric su so no yɛ soronko koraa. Sɛnea yenim no, ntease titiriw a ɛfa sɛnea sintɔ ahorow ma cubic to hexagonal (α-δ) phase nsakrae ne dwuma a surface passivation di wɔ α-FAPbI3 perovskite phase stability so no da so ara nte ase yiye.
Ɛha yi, yɛda ɔkwan a FAPbI3 perovskite sɛe fi tuntum α-fase kɔ kɔkɔɔ δ-fase ne nkɛntɛnso a sintɔ ahorow nya wɔ ahoɔden akwanside a α-kɔ-δ-fase nsakrae denam DFT so adi. Wɔahyɛ nkɔm sɛ I vacancies, a ɛnyɛ den sɛ wobenya bere a wɔreyɛ sini ne mfiri reyɛ adwuma no, na ɛda adi kɛse sɛ ebefi α-δ phase nsakrae no ase. Enti, yɛde kɔbere oxalate (PbC2O4) a ɛyɛ den a nsu ntumi nkɔ mu na nnuru ntumi nkɔ mu bae wɔ FAPbI3 atifi denam in situ adeyɛ so. Lead oxalate surface (LOS) siw I mmeae a ɛda hɔ kwa no kwan na esiw I ions a ɛkɔ baabi foforo ano bere a ɔhyew, hann, ne anyinam ahoɔden kanyan no no. LOS a efi mu ba no brɛ interfacial nonradiative recombination ase kɛse na ɛma FAPbI3 PSC adwumayɛ tu mpɔn kodu 25.39% (wɔagye atom sɛ ɛyɛ 24.92%). LOS afiri a wɔankyekyere no kuraa ne mfitiaseɛ adwumayɛ mu 92% wɔ berɛ a ɛyɛɛ adwuma wɔ tumi a ɛkyɛn soɔ (MPP) bɛboro nnɔnhwereɛ 550 wɔ mframa dodoɔ a wɔayɛ no sɛdeɛ ɛteɛ (AM) a ɛyɛ 1.5 G mframa akyi.
Yɛdii kan yɛɛ ab initio akontabuo de hwehwɛɛ FAPbI3 perovskite no porɔwee kwan a ɛkɔ nsakraeɛ firi α fa mu kɔ δ fa mu. Ɛnam fase nsakraeɛ nhyehyɛeɛ a ɛkɔ akyiri so no, wɔhunu sɛ nsakraeɛ a ɛfiri afã mmiɛnsa a ɛkyɛ ntwea so [PbI6] octahedron a ɛwɔ cubic α-fase a ɛwɔ FAPbI3 mu kɔ ɔfa baako a ɛkyɛ ano [PbI6] octahedron a ɛwɔ hexagonal δ-fase a ɛwɔ FAPbI3 mu no yɛ nea ɛba. breaking 9. Pb-I yɛ nkitahodi wɔ anammɔn a edi kan no mu (Int-1), na n’ahoɔden akwanside no du 0.62 eV/cell, sɛnea wɔakyerɛ wɔ Mfonini 1a mu no. Sɛ wɔdannan octahedron no kɔ [0\(\bar{1}\)1] kwan so a, nkɔnsɔnkɔnsɔn tiawa a ɛwɔ ahinanan no trɛw fi 1×1 kosi 1×3, 1×4 na awiei koraa no ɛhyɛn δ fa no mu. Ɔkwan no nyinaa kwankyerɛ nsusuwii ne (011)α//(001)δ + [100]α//[100]δ. Efi ahoɔden kyekyɛ mfonini no mu no, yebetumi ahu sɛ bere a wɔayɛ FAPbI3 δ fa no nucleation akyi wɔ akwan a edidi so yi mu no, ahoɔden akwanside no sua sen α fase nsakrae no, a ɛkyerɛ sɛ fase nsakrae no bɛyɛ ntɛmntɛm. Ɛda adi pefee sɛ, anammɔn a edi kan a yɛde bedi phase nsakrae no so no ho hia kɛse sɛ yɛpɛ sɛ yesiw α-phase degradation ano a.
a Phase nsakraeɛ kwan a ɛfiri benkum kɔ nifa – tuntum FAPbI3 phase (α-phase), Pb-I bond cleavage a ɛdi kan (Int-1) ne Pb-I bond cleavage foforɔ (Int-2, Int -3 ne Int -4) ne yellow phase FAPbI3 (delta phase). b Ahoɔden akwansideɛ a ɛmma α kɔ δ fase nsakraeɛ a ɛwɔ FAPbI3 mu a egyina intrinsic point sintɔ ahodoɔ so. Ntrɛwmu a ɛyɛ nsensanee no kyerɛ ahoɔden akwanside a ɛwɔ ahwehwɛ a eye (0.62 eV) mu. c Ahoɔden a ɛma ɛyɛ mfitiaseɛ nsɛntitiriw sintɔ wɔ kɔbere perovskite ani. Abscissa axis no yɛ ahoɔden akwansideɛ a ɛwɔ α-δ phase nsakraeɛ no mu, na ordinate axis no yɛ ahoɔden a ɛma sintɔ hyehyɛ. Afã horow a wɔde grey, yellow ne green ayɛ no sunsuma ne type I (low EB-high FE), type II (high FE) ne type III (low EB-low FE), sɛnea ɛte biara. d Ahoɔden a ɛma wɔhyehyɛ sintɔ VI ne LOS a ɛwɔ FAPbI3 mu wɔ control no mu. e I akwanside a ɛmma ion tu kɔ baabi foforo wɔ FAPbI3 sohwɛ ne LOS mu. f – I ions (orange spheres) ne gLOS FAPbI3 (akuturuku, kɔbere; violet (orange), iodine (mobile iodine)) a ɛkɔ baabi foforo wɔ gf control no mu (benkum: atifi hwɛ; nifa: cross section, brown); carbon a ɛyɛ hyew; bruu a ɛyɛ hann – nitrogen; kɔkɔɔ – oxygen; pink a ɛyɛ hann – hydrogen). Wɔde Source data ma wɔ source data fael ahorow mu.
Afei yɛyɛɛ nhyehyɛe suaa nkɛntɛnso a intrinsic point defects ahorow (a PbFA, IFA, PbI, ne IPb antisite occupancy; Pbi ne Ii interstitial atoms; ne VI, VFA, ne VPb vacancies) nya nkɛntɛnso ho ade, a wobu no sɛ ɛyɛ nneɛma atitiriw. a ɛde atom ne ahoɔden level phase degradation ba no wɔakyerɛ wɔ Mfonini 1b ne Supplementary Table 1. Nea ɛyɛ anigye no, ɛnyɛ sintɔ nyinaa na ɛtew ahoɔden akwanside a ɛwɔ α-δ phase nsakrae no so (Mfonini 1b). Yɛgye di sɛ wɔbu sintɔ a ɛwɔ ahoɔden a ɛba fam wɔ formation ahoɔden ne α-δ phase transition ahoɔden akwansideɛ a ɛba fam nyinaa sɛ ɛsɛe phase stability. Sɛnea yɛadi kan abɔ amanneɛ no, wɔtaa bu mmeae a kɔbere pii wom sɛ etu mpɔn ma formamidine PSC27. Enti, yɛde yɛn adwene si PbI2-awie (100) soro wɔ tebea horow a kɔbere pii wom mu. Wɔakyerɛ ahoɔden a ɛma mfomsoɔ ba wɔ soro intrinsic point defects mu wɔ Mfonini 1c ne Supplementary Table 1. Wɔgyina ahoɔden akwansideɛ (EB) ne phase transition formation energy (FE) so, wɔkyekyɛ saa sintɔ yi mu ahodoɔ mmiɛnsa. Type I (low EB-high FE): Ɛwom sɛ IPb, VFA ne VPb tew ahoɔden akwanside a ɛmma phase nsakrae ano no ase kɛse de, nanso wɔwɔ ahoɔden a ɛkorɔn a ɛma wɔhyehyɛ. Enti, yegye di sɛ saa sintɔ ahorow yi nni nkɛntɛnso kakraa bi wɔ phase transitions so efisɛ wɔntaa nhyehyɛ. Type II (EB a ɛkorɔn): Esiane α-δ phase transition energy barrier a wɔatu mpɔn nti, anti-site sintɔ PbI, IFA ne PbFA nsɛe α-FAPbI3 perovskite phase stability. Type III (low EB-low FE): VI, Ii ne Pbi sintɔ a ɛwɔ formation ahoɔden a ɛba fam koraa no betumi ama black phase degradation aba. Titiriw sɛ yɛhwɛ FE ne EB VI a ɛba fam koraa a, yegye di sɛ ɔkwan a etu mpɔn sen biara ne sɛ yɛbɛtew I adwuma a ɛda hɔ no so.
Sɛnea ɛbɛyɛ a yɛbɛtew VI so no, yɛyɛɛ PbC2O4 a ɛyɛ den a ɛbɛma FAPbI3 no ani atu mpɔn. Sɛ wɔde toto organic halide nkyene pasivators te sɛ phenylethylammonium iodide (PEAI) ne n-octylammonium iodide (OAI) ho a, PbC2O4 a enni halogen ions a ɛkɔ baabiara no yɛ nea nnuru a ɛyɛ den, entumi nwura nsu mu, na ɛnyɛ den sɛ ɛbɛma ayɛ adwuma bere a wɔkanyan no. Pa stabilization a ɛwɔ soro nsuo ne anyinam ahoɔden field a perovskite. PbC2O4 a ɛtumi nwura nsuo mu no yɛ 0.00065 g/L pɛ, a ɛba fam mpo sene PbSO428 deɛ. Nea ɛho hia kɛse no, wobetumi asiesie LOS a ɛyɛ den na ɛyɛ pɛ wɔ perovskite sini ahorow so denam in situ reactions so (hwɛ ase hɔ). Yɛyɛɛ DFT simulations a ɛfa interfacial bonding a ɛda FAPbI3 ne PbC2O4 ntam sɛnea wɔakyerɛ wɔ Supplementary Figure 1. Supplementary Table 2 de sintɔ formation ahoɔden wɔ LOS injection akyi. Yehui sɛ ɛnyɛ sɛ LOS ma VI sintɔ ahorow no formation ahoɔden kɔ soro 0.69–1.53 eV nko (Mfonini 1d), na mmom ɛma I activation ahoɔden nso kɔ soro wɔ migration surface ne exit surface (Mfonini 1e). Wɔ ɔfa a edi kan no mu no, I ions tu fa perovskite no ani, na ɛma VI ions kɔ lattice gyinabea a ahoɔden akwanside a ɛyɛ 0.61 eV. LOS a wɔde aba akyi no, esiane steric akwanside nkɛntɛnso nti, ahoɔden a ɛma I ions tu kɔ baabi foforo no kɔ soro kodu. 1.28 eV na ɛwɔ hɔ. Wɔ I ions a ɛfiri perovskite ani no tu no, ahoɔden akwansideɛ a ɛwɔ VOC no mu nso korɔn sene control sample no mu (Mfonini 1e). Schematic diagrams a ɛkyerɛ I ion migration akwan wɔ control ne LOS FAPbI3 mu no wɔakyerɛ wɔ Mfonini 1 f ne g mu, sɛnea ɛte biara. Nea efii simulation no mu bae no kyerɛ sɛ LOS betumi asiw VI sintɔ ahorow a ɛba ne I a ɛyɛ hyew no ano, na ɛnam so asiw α kɔ δ phase nsakrae no nucleation ano.
Wɔsɔɔ sɛnea oxalic acid ne FAPbI3 perovskite yɛ adwuma no hwɛe. Bere a wɔde oxalic acid ne FAPbI3 aduru frafrae akyi no, nsu fitaa pii bae, sɛnea wɔada no adi wɔ Mfonini a Wɔde Ka Ho 2. Wɔde X-ray diffraction (XRD) (Mfonini a Wɔde Ka Ho 3) ne Fourier transform infrared spectroscopy (FTIR) (Mfonini a Wɔde Ka Ho 4) na ɛkyerɛɛ sɛ powder ade no yɛ PbC2O4 ade a ɛho tew. Yehui sɛ oxalic acid yɛ nea ɛtumi nwura isopropyl alcohol (IPA) mu kɛseɛ wɔ dan mu hyeɛ mu a ɛtumi nwura mu bɛyɛ 18 mg/mL, sɛdeɛ wɔakyerɛ wɔ Supplementary Figure 5. Eyi ma dwumadie a ɛdi akyire no yɛ mmerɛ ɛfiri sɛ IPA, sɛ pasivation solvent a wɔtaa yɛ no, nsɛe perovskite layer no nsen berɛ tiawa Enti, ɛdenam perovskite film no a wɔde bɛhyɛ oxalic acid solution mu anaasɛ wɔde spin-coating oxalic acid solution no so wɔ perovskite no so no, wobetumi anya PbC2O4 a ɛyɛ tratraa na ɛyɛ den ntɛmntɛm wɔ perovskite film no ani sɛnea nnuru nsɛso a edidi so yi kyerɛ no: H2C2O4 + FAPbI3 = PbC2O4 + FAI +HI. Wobetumi apete FAI wɔ IPA mu na wɔnam saayɛ so ayi afi hɔ bere a wɔrenoa aduan no. Wobetumi de bere a wɔde yɛ ade ne nea edi kan no dodow adi LOS no mu duru so.
Scanning electron microscopy (SEM) mfonini ahorow a ɛkyerɛ control ne LOS perovskite films no wɔakyerɛ wɔ Mfonini 2a,b mu. Nea ɛfiri mu baeɛ no kyerɛ sɛ wɔakora perovskite ani nsɛsoɔ so yie, na wɔde nneɛma nketenkete dodoɔ bi agu aburow no ani, a ɛsɛ sɛ egyina hɔ ma PbC2O4 a ɛnam in-situ reaction so na ɛbae. LOS perovskite film no wɔ soro a ɛyɛ torotoro kakra (Supplementary Figure 6) ne nsuo a ɛne ne ho di nkitaho kɛseɛ sɛ wɔde toto control film no ho a (Supplementary Figure 7). Wɔde high-resolution transverse transmission electron microscopy (HR-TEM) dii dwuma de kyerɛɛ nsonsonoe a ɛda ade no ani fã no ntam. Sɛ yɛde toto control film (Mfonini 2c) ho a, wotumi hu ade a ɛyɛ tratraa a ɛyɛ pɛ na ɛyɛ den a ne kɛse bɛyɛ 10 nm no pefee wɔ LOS perovskite no atifi (Mfonini 2d). Sɛ wɔde high-angle annular dark-field scanning electron microscopy (HAADF-STEM) di dwuma de hwehwɛ nkitahodi a ɛda PbC2O4 ne FAPbI3 ntam a, wobetumi ahu pefee sɛ FAPbI3 mmeae a ɛyɛ ahwehwɛ ne PbC2O4 mmeae a ɛnyɛ nsɛ wɔ hɔ (Mfonini a Wɔde Ka Ho 8). Wɔde X-ray photoelectron spectroscopy (XPS) susudua kyerɛɛ perovskite no ani a ɛwɔ oxalic acid ayaresa akyi, sɛnea wɔakyerɛ wɔ Mfonini 2e–g mu no. Wɔ Mfonini 2e mu no, C 1s a ɛwɔ soro bɛyɛ 284.8 eV ne 288.5 eV no yɛ CC ne FA nsɛnkyerɛnne pɔtee no dea. Sɛ wɔde toto control membrane no ho a, LOS membrane no daa peak foforo adi wɔ 289.2 eV, a wɔkyerɛ sɛ efi C2O42-. O 1s spectrum a ɛwɔ LOS perovskite mu no da O 1s peaks abiɛsa a ɛsono nnuru adi wɔ 531.7 eV, 532.5 eV, ne 533.4 eV, a ɛne deprotonated COO, C=O a ɛwɔ oxalate akuw a enni dɛm 30 ne O atom a ɛwɔ OH fã no hyia (Mfonini 2e ). )). Wɔ control sample no fam no, wohuu O 1s peak ketewaa bi pɛ, a wobetumi aka sɛ efi oxygen chemisorbed wɔ soro. Control membrane su a ɛwɔ Pb 4f7/2 ne Pb 4f5/2 mu no wɔ 138.4 eV ne 143.3 eV, sɛnea ɛte biara. Yɛhunuu sɛ LOS perovskite no da nsakraeɛ a ɛba Pb peak no mu bɛyɛ 0.15 eV adi kɔ ahoɔden a ɛkorɔn a ɛkyekyere, a ɛkyerɛ sɛ nkitahodiɛ a emu yɛ den wɔ C2O42- ne Pb atom ntam ( Mfonini 2g ).
a SEM mfonini ahorow a ɛfa control ne b LOS perovskite sini ahorow ho, soro hwɛ. c High-resolution cross-sectional transmission electron microscopy (HR-TEM) a ɛfa control ne d LOS perovskite sini ahorow ho. XPS a ɛwɔ nsusuwii a ɛkorɔn a ɛyɛ e C 1s, f O 1s ne g Pb 4f perovskite sini ahorow. Wɔde Source data ma wɔ source data fael ahorow mu.
Sɛnea DFT aba no kyerɛ no, wɔhyɛ nkɔm wɔ nsusuwii mu sɛ VI sintɔ ne I atutra no ma ɛnyɛ den sɛ ɛde phase nsakrae fi α kɔ δ. Amanneɛbɔ a atwam ada no adi sɛ I2 fi PC-based perovskite films mu ntɛmntɛm wɔ photoimmersion bere a wɔde films no ahyɛ hann ne ɔhyew nhyɛso mu akyi31,32,33. Sɛnea ɛbɛyɛ na yɛasi tumi a lead oxalate nya wɔ perovskite α-fase so no so dua no, yɛde control ne LOS perovskite films no guu ahwehwɛ nkotoku a ɛyɛ mmerɛw a toluene wom mu, sɛnea ɛte biara, na afei yɛde owia hann 1 hyerɛn wɔn so h 24. Yɛsusuw sɛnea hann a ano yɛ den ne nea wotumi hu (UV-Vis) twetwe no. ) toluene solution, sɛnea wɔakyerɛ wɔ Mfonini 3a mu no. Sɛ wɔde toto control sample no ho a, wohuu I2 absorption ahoɔden a ɛba fam koraa wɔ LOS-perovskite asɛm no mu, a ɛkyerɛ sɛ compact LOS betumi asiw I2 a efi perovskite film no mu bere a wɔde hann ahyɛ mu no ano. Wɔakyerɛ mfonini ahorow a ɛkyerɛ mfe dodow a wɔde di dwuma ne LOS perovskite sini ahorow wɔ Mfonini 3b ne c mu nsɛm a wɔde ahyɛ mu no mu. LOS perovskite no da so ara yɛ tuntum, bere a control film no fã kɛse no ara adan kɔkɔɔ. UV–visible absorption spectra a ɛwɔ sini a wɔde ahyɛ mu no mu no wɔakyerɛ wɔ Figs. 3b, c. Yɛhunuu sɛ absorption a ɛne α hyia wɔ control film no mu no so tew pefee. Wɔyɛɛ X-ray susuw de kyerɛw sɛnea ahwehwɛ nhyehyɛe no dannan. Nnɔnhwerew 24 a wɔde hann hyerɛn akyi no, control perovskite no daa δ-phase sɛnkyerɛnne kɔkɔɔ a emu yɛ den adi (11.8°), bere a LOS perovskite no da so ara kura tuntum phase pa mu (Mfonini 3d).
UV-visible absorption spectra of toluene solutions a wɔde control film ne LOS film no guu mu wɔ owia hann 1 ase nnɔnhwerew 24. Inset no kyerɛ ahina bi a wɔde sini biara guu mu wɔ toluene dodow a ɛyɛ pɛ mu. b UV-Vis absorption spectra a ɛwɔ control film ne c LOS film ansa na ne akyi 24 h a wɔde ahyɛ mu wɔ owia hann 1 ase. Inset no kyerɛ sini a wɔasɔ ahwɛ no mfonini. d X-ray diffraction nhyehyeɛ a ɛfa control ne LOS films ho ansa na wɔde 24 h ahyɛ mu ne akyi. SEM mfonini ahorow a ɛkyerɛ control film e ne film f LOS wɔ nnɔnhwerew 24 a wɔde ahyɛ mu akyi. Wɔde Source data ma wɔ source data fael ahorow mu.
Yɛyɛɛ scanning electron microscopy (SEM) susuw de hwɛɛ microstructural nsakrae a ɛba perovskite film no mu wɔ nnɔnhwerew 24 a wɔde hann ahyɛ mu akyi, sɛnea wɔada no adi wɔ Mfonini 3e,f mu no. Wɔ control film no mu no, wɔsɛee aburow akɛse na wɔdanee no nnade nketewa, a ɛne δ-phase product FAPbI3 no nsɛso hyia (Mfonini 3e). Wɔ LOS sini ahorow mu no, perovskite nnua no da so ara wɔ tebea pa mu (Mfonini 3f). Nea efii mu bae no sii so dua sɛ I a ɛyera no ma nsakrae fi tuntum fã no mu kɔ kɔkɔɔ fã no mu kɛse, bere a PbC2O4 ma tuntum fã no gyina pintinn, na esiw I a ɛyera no ano. Esiane sɛ baabi a ɛda hɔ a ɛwɔ soro no dɔɔso sen aburow kɛse no nti,34 ɛda adi sɛ saa fã yi bɛba wɔ aburow no ani. bere koro mu no, ɛma iodine fi mu na ɛyɛ VI. Sɛnea DFT hyɛɛ nkɔm no, LOS betumi asiw VI sintɔ ahorow a ɛba no ano na asiw I ions a ɛbɛkɔ perovskite no ani no ano.
Bio nso, wɔyɛɛ nkɛntɛnso a PbC2O4 a ɛwɔ soro no nya wɔ perovskite films a ɛwɔ wim mframa mu (nsuo a ɛyɛ nwini 30-60%) no nsuo a ɛko tia no ho nhwehwɛmu. Sɛnea wɔada no adi wɔ Supplementary Figure 9 mu no, na LOS perovskite no da so ara yɛ tuntum wɔ nnafua 12 akyi, bere a control film no danee kɔkɔɔ. Wɔ XRD susudua mu no, control film no kyerɛ peak a ɛyɛ den wɔ 11.8° a ɛne δ phase a ɛwɔ FAPbI3 no hyia, bere a LOS perovskite no kura black α phase no yiye (Supplementary Figure 10).
Wɔde steady-state photoluminescence (PL) ne time-resolved photoluminescence (TRPL) dii dwuma de suaa passivation nkɛntɛnso a kɔbere oxalate nya wɔ perovskite ani. Wɔ Mfonini mu no Mfonini 4a kyerɛ sɛ LOS sini no ama PL ahoɔden akɔ soro. Wɔ PL map mfonini no mu no, LOS sini no ahoɔden wɔ beaeɛ a ɛyɛ 10 × 10 μm2 nyinaa so no korɔn sene deɛ ɛwɔ control film no so (Supplementary Figure 11), a ɛkyerɛ sɛ PbC2O4 ma perovskite film no yɛ adwuma pɛpɛɛpɛ. Wɔnam TRPL porɔwee no a wɔde bɛyɛ exponential function baako so na ɛkyerɛ carrier nkwa nna (Mfonini 4b). LOS film no carrier nkwa nna yɛ 5.2 μs, a ɛware sen control film a carrier nkwa nna yɛ 0.9 μs, a ɛkyerɛ sɛ surface nonradiative recombination so atew.
Steady-state PL ne b-spectra a ɛkyerɛ bere tiaa mu PL a perovskite sini ahorow wɔ ahwehwɛ substrates so. c SP curve a ɛwɔ afiri no mu (FTO/TiO2/SnO2/perovskite/spiro-OMeTAD/Au). d EQE spectrum ne Jsc EQE spectrum a wɔaka abom afiri afiri a ɛyɛ adwuma yie paa. d Hann ahoɔden a perovskite afiri bi gyina Voc mfonini no so. f MKRC nhwehwɛmu a wɔtaa yɛ a wɔde ITO/PEDOT:PSS/perovskite/PCBM/Au afiri a ɛho tew tokuru di dwuma. VTFL ne afiri a wɔde hyɛ mu ma a ɛsen biara. Yefi saa nsɛm yi mu buu afiri no dodow (Nt) ho akontaa. Wɔde Source data ma wɔ source data fael ahorow mu.
Sɛnea ɛbɛyɛ na wɔasua nkɛntɛnso a lead oxalate layer no nya wɔ mfiri no adwumayɛ so no, wɔde atetesɛm FTO/TiO2/SnO2/perovskite/spiro-OMeTAD/Au nkitahodi nhyehyɛe dii dwuma. Yɛde formamidine chloride (FACl) di dwuma sɛ ade a wɔde ka perovskite precursor no ho sen sɛ yɛde methylamine hydrochloride (MACl) bedi dwuma de anya mfiri no adwumayɛ a eye, efisɛ FACl betumi ama ahwehwɛ a eye na akwati FAPbI335 band gap (hwɛ Supplementary Figures 1 ne 2 ma ntotoho a ɛkɔ akyiri). ). 12-14 na ɛwɔ hɔ). Wɔpaw IPA sɛ antisolvent efisɛ ɛma crystal su pa ne orientation a wɔpɛ wɔ perovskite films mu sɛ wɔde toto diethyl ether (DE) anaa chlorrobenzene (CB)36 ho a (Supplementary Figures 15 ne 16). Wɔde ahwɛyiye yɛɛ PbC2O4 no mu duru yiye sɛnea ɛbɛyɛ a ɛbɛkari pɛ yiye wɔ sintɔ passivation ne charge transport denam nsakrae a wɔyɛe wɔ oxalic acid dodow mu (Supplementary Figure 17). Cross-sectional SEM mfonini a ɛfa optimized control ne LOS mfiri ho no wɔakyerɛ wɔ Supplementary Figure 18. Typical current density (CD) curves ma control ne LOS mfiri no wɔakyerɛ wɔ Mfonini 4c, na wɔde parameters a wɔayiyi no ama wɔ Supplementary Table 3. Maximum power conversion efficiency (PCE) control cells 23.43% (22.94%), Jsc 25.75 mA cm-2 (25.74 mA cm-2), Voc 1.16 V (1.16 V) ne akyi (anim) scan. Nneɛma a wɔde hyɛ mu (FF) yɛ 78.40% (76.69%). PCE LOS PSC a ɛkyɛn so yɛ 25.39% (24.79%), Jsc yɛ 25.77 mA cm-2, Voc yɛ 1.18 V, FF yɛ 83.50% (81.52%) fi akyi (kɔ anim Scan kɔ). LOS afiri no nyaa photovoltaic adwumayɛ a wɔagye atom a ɛyɛ 24.92% wɔ photovoltaic laboratory a ɛtɔ so mmiɛnsa a wɔgye di mu (Supplementary Figure 19). Abɔnten so quantum efficiency (EQE) no maa Jsc a wɔaka abom a ɛyɛ 24.90 mA cm-2 (control) ne 25.18 mA cm-2 (LOS PSC), sɛnea ɛte biara, a na ɛne Jsc a wɔsusuu wɔ standard AM 1.5 G spectrum mu no hyia yie (Mfonini .4d). ) . Akontaabu nkyekyɛmu a ɛfa PCE ahorow a wɔasusuw ho ama control ne LOS PSCs no wɔakyerɛ wɔ Supplementary Figure 20 mu.
Sɛnea wɔakyerɛ wɔ Mfonini 4e mu no, wɔbuu abusuabɔ a ɛda Voc ne hann ahoɔden ntam de suaa nkɛntɛnso a PbC2O4 nya wɔ afiri a ɛboa soro a wɔsan ka bom no so. Ntrɛwmu a wɔde hyɛ LOS afiri no mu no yɛ 1.16 kBT/sq, a ɛba fam sen nhama a wɔde ahyɛ mu ma afiri a wɔde di dwuma no kwan (1.31 kBT/sq), a ɛkyerɛ sɛ LOS ho wɔ mfaso ma decoys a wɔde siw ɔfasuo a wɔsan ka bom no ano. Yɛde space charge current limiting (SCLC) mfiridwuma di dwuma de susuw perovskite film mu sintɔ density dodow denam susuw IV su a ɛyɛ sum a ɛwɔ tokuru afiri (ITO/PEDOT:PSS/perovskite/spiro-OMeTAD/Au) mu sɛnea wɔakyerɛ wɔ mfonini no mu no so. 4f Kyerɛw. Wɔde fomula Nt = 2ε0εVTFL/eL2 na ɛbu afiri no dodoɔ, a ε yɛ perovskite film no dielectric constant a ɛfa ho, ε0 yɛ dielectric constant a ɛwɔ vacuum mu, VTFL yɛ limiting voltage a wɔde hyɛ afiri no ma, e yɛ charge, L yɛ perovskite film no mu duru (650 nm). Wɔabu VOC afiri no sintɔ dodoɔ sɛ ɛyɛ 1.450 × 1015 cm–3, a ɛba fam sene afiri a wɔde di dwuma no sintɔ dodoɔ a ɛyɛ 1.795 × 1015 cm–3.
Wɔsɔɔ afiri a wɔankyekyere no hwɛe wɔ tumi a ɛkyɛn so (MPP) wɔ awia hann a edi mũ ase wɔ nitrogen ase de hwehwɛɛ sɛnea ɛyɛ adwuma bere tenten (Mfonini 5a). Nnɔnhwerew 550 akyi no, LOS afiri no da so ara kura ne adwumayɛ a ɛsen biara no mu 92%, bere a na afiri a wɔde di dwuma no adwumayɛ akɔ fam akodu ne mfitiase adwumayɛ no 60%. Wɔde bere-a-tun a ɛto so abien ion mass spectrometry (ToF-SIMS) susuw nneɛma a ɛwɔ afiri dedaw no mu no kyekyɛ (Mfonini 5b, c). Wobetumi ahu iodine a aboaboa ano kɛse wɔ beae a wɔde sika kɔkɔɔ di dwuma wɔ soro no. Tebea horow a mframa a ɛnyɛ adwuma ahobammɔ wom no yi nneɛma a ɛsɛe nneɛma a atwa yɛn ho ahyia te sɛ nsu ne oxygen fi mu, na ɛkyerɛ sɛ emu akwan (kyerɛ sɛ, ion a ɛkɔ baabi foforo) na ɛde ba. Sɛnea ToF-SIMS aba kyerɛ no, wohuu I- ne AuI2- ions wɔ Au electrode no mu, a ɛkyerɛ sɛ I trɛw fi perovskite no mu kɔ Au mu. Nsɛnkyerɛnneɛ ahoɔden a ɛwɔ I- ne AuI2- ions a ɛwɔ control device no mu no boro VOC nhwɛsoɔ no so bɛyɛ mpɛn 10. Amanneɛbɔ a atwam no ada no adi sɛ ion a ɛkɔ mu no betumi ama spiro-OMeTAD tokuru no mu nsuo a ɛkɔ mu no so atew ntɛmntɛm na nnuru a ɛwɔ soro electrode layer no asɛe, na ɛnam so ama interfacial contact a ɛwɔ afiri no mu no asɛe Wɔyii Au electrode no na wɔde chlorbenzene solution tew spiro-OMeTAD layer no ho fii substrate no mu. Afei yɛde grazing incidence X-ray diffraction (GIXRD) (Mfonini 5d) yɛɛ sini no su. Nea efii mu bae no kyerɛ sɛ control film no wɔ diffraction peak a ɛda adi pefee wɔ 11.8°, bere a diffraction peak foforo biara mpue wɔ LOS nhwɛsode no mu. Nea efii mu bae no kyerɛ sɛ I ions a wɔhwere kɛse wɔ control film no mu no ma δ phase no ba, bere a wɔ LOS film no mu no, ɛda adi pefee sɛ wosiw saa adeyɛ yi ano.
Nnɔnhwerew 575 a wɔde MPP di akyi a ɛkɔ so wɔ afiri a wɔantoto mu wɔ nitrogen wim ne owia hann 1 a UV filter nni mu. ToF-SIMS kyekyɛ b I- ne c AuI2- ions wɔ LOS MPP control device ne onyin mfiri. Nsuo a ɛyɛ kɔkɔɔ, ahabammono ne borɔdɔma no ne Au, Spiro-OMeTAD ne perovskite hyia. d GIXRD a ɛwɔ perovskite film mu wɔ MPP sɔhwɛ akyi. Wɔde Source data ma wɔ source data fael ahorow mu.
Wɔsusuu ɔhyew-gyina conductivity de sii so dua sɛ PbC2O4 betumi asiw ion migration (Supplementary Figure 21). Wɔnam nsakrae a ɛba wɔ conductivity (σ) a ɛwɔ FAPbI3 film no mu wɔ ɔhyew ahorow (T) mu ne Nernst-Einstein abusuabɔ a wɔde di dwuma so na ɛkyerɛ ion migration no activation ahoɔden (Ea), a σ0 yɛ constant, kB yɛ Boltzmann constant. Yɛnya Ea boɔ no firi ln(σT) a ɛkɔ fam no mu kyerɛ 1/T, a ɛyɛ 0.283 eV ma control no ne 0.419 eV ma LOS device no.
Sɛ yɛbɛbɔ no mua a, yɛde nsusuwii nhyehyɛe a yɛde bɛkyerɛ ɔkwan a FAPbI3 perovskite no sɛe ne nkɛntɛnso a sintɔ ahorow nya wɔ ahoɔden akwanside a ɛwɔ α-δ fase nsakrae no so ma. Wɔ saa sintɔ ahorow yi mu no, wɔahyɛ nkɔm wɔ nsusuwii mu sɛ VI sintɔ ahorow no bɛma ɛnyɛ den sɛ ɛbɛma phase nsakrae afi α akɔ δ. Wɔde PbC2O4 a ɛyɛ den a nsu ntumi nkɔ mu na ɛyɛ den wɔ nnuru mu ba de ma FAPbI3 α-fase no gyina denam I mmeae a ɛda hɔ a ɛba ne I ions a ɛkɔ baabi foforo a wobesiw ano no so. Saa nhyehyeɛ yi brɛ interfacial non-radiative recombination no ase kɛseɛ, ɛma owia nkwammoaa no ahoɔden kɔ soro kɔduru 25.39%, na ɛma adwumayɛ no gyina pintinn. Yɛn aba no ma akwankyerɛ a yɛde benya formamidine PSCs a etu mpɔn na ɛyɛ den denam α kɔ δ phase nsakrae a sintɔ de ba no a wobesiw ano no so.
Wɔtɔɔ titanium(IV) isopropoxide (TTIP, 99.999%) fii Sigma-Aldrich hɔ. Wɔtɔɔ hydrochloric acid (HCl, 35.0–37.0%) ne ethanol (a nsu nnim) fii Guangzhou Nnuruyɛ Nnwumakuw hɔ. Wɔtɔɔ SnO2 (15 wt% tin(IV) oxide colloidal dispersion) fii Alfa Aesar hɔ. Wɔtɔɔ kɔbere(II) iodide (PbI2, 99.99%) fii TCI Shanghai (China). Ɔde ne nsa kyerɛɛ ne so, na ɔde ne nsa kyerɛɛ ne so bio. ≥99.5%), wɔtɔɔ lithium bis (trifluoromethane)sulfonylimide (Li-TFSI, 99.95%), 4-tert -butylpyridine (tBP, 96%) fii Xi’an Polymer Hann Mfiridwuma Adwumakuw (China) hɔ. N,N-dimethylformamide (DMF, 99.8%), dimethyl sulfoxide (DMSO, 99.9%), isopropyl nsa (IPA, 99.8%), klorobenzene (CB, 99.8%), acetonitrile (ACN) a wɔde di dwuma wɔ ɔkwan a ɛyɛ mmerɛw so. Wɔtɔɔ fii Sigma-Aldrich hɔ. Wɔtɔɔ oxalic acid (H2C2O4, 99.9%) fii Macklin hɔ. Wɔde nnuru no nyinaa dii dwuma sɛnea wonyae no a wɔanyɛ nsakrae foforo biara.
ITO anaa FTO substrates (1.5 × 1.5 cm2) na ultrasonically tew ne detergent, acetone, ne ethanol ma 10 min, sɛnea ɛte biara, na afei wee wɔ nitrogen asuten ase. Wɔde TiO2 akwanside a ɛyɛ den guu FTO substrate so denam titanium diisopropoxybis(acetylacetonate) a wɔde ahyɛ ethanol (1/25, v/v) a wɔde ahyɛ 500 °C mu simma 60 mu. Wɔde nsu a wɔayi ion afi mu no guu SnO2 colloidal dispersion no mu wɔ dodow a ɛyɛ 1:5 mu. Wɔ substrate a ɛho tew a wɔde UV ozone ayɛ ho adwuma simma 20 so no, wɔde SnO2 nanoparticles a ɛyɛ tratraa guu 4000 rpm so simma 30 na afei wɔde dii kan yɛɛ hyew wɔ 150 °C simma 30. Wɔ perovskite precursor solution no ho no, wɔde 275.2 mg FAI, 737.6 mg PbI2 ne FACl (20 mol%) guu DMF/DMSO (15/1) afrafra aduru mu. Wɔnam centrifuging 40 μL perovskite precursor solution so na ɛyɛɛ perovskite layer no denam UV-ozone-treated SnO2 layer no atifi wɔ 5000 rpm wɔ ambient air mu 25 s. Wɔ bere a etwa to no akyi sikani 5 no, wɔde MACl IPA aduru 50 μL (4 mg/mL) guu substrate no so ntɛmntɛm sɛ ade a ɛko tia aduru. Afei, wɔde sini ahorow a wɔasiesie no foforo no yɛɛ annealed wɔ 150°C simma 20 na afei wɔ 100°C simma 10. Bere a wɔama perovskite film no ayɛ nwini akodu dan mu hyew akyi no, wɔde H2C2O4 aduru (1, 2, 4 mg a wɔapete wɔ 1 mL IPA mu) centrifuged wɔ 4000 rpm s 30 de yɛɛ perovskite no ani. Wɔde spiro-OMeTAD aduru a wɔasiesie denam 72.3 mg spiro-OMeTAD, 1 ml CB, 27 μl tBP ne 17.5 μl Li-TFSI (520 mg wɔ 1 ml acetonitrile mu) a wɔde frafrae so wɔ sini no so wɔ 4000 rpm mu wɔ s 30 mu. Awiei koraa no, wɔde Au a ne kɛse yɛ 100 nm yɛɛ hyew wɔ vacuum mu wɔ ahoɔhare a ɛyɛ 0.05 nm/s (0~1 nm), 0.1 nm/s (2~15 nm) ne 0.5 nm/s (16~100 nm) . ).
Wɔde Keithley mita 2400 wɔ owia simulator hann (SS-X50) ase wɔ hann a ano yɛ den 100 mW/cm2 mu na ɛsusuu perovskite owia nkwammoaa no SC adwumayɛ na wɔde calibrated standard silicon solar cells dii ho adanseɛ. Gye sɛ wɔakyerɛ sɛ ɛnte saa, wɔsusuu SP curves wɔ glove box a nitrogen ahyɛ mu ma mu wɔ dan mu hyew (~25°C) mu wɔ anim ne akyi scan modes (voltage step 20 mV, delay time 10 ms). Wɔde sunsuma akatasoɔ dii dwuma de kyerɛɛ beaeɛ a ɛtu mpɔn a ɛyɛ 0.067 cm2 maa PSC a wɔsusuu no. Wɔde PVE300-IVT210 nhyehyɛe (Industrial Vision Technology(s) Pte Ltd) a hann a ɛyɛ kɔla biako na ɛtwe adwene si afiri no so na ɛyɛɛ EQE susuw wɔ mframa a atwa yɛn ho ahyia mu. Sɛnea ɛbɛyɛ a mfiri no betumi agyina pintinn no, wɔyɛɛ owia nkwammoaa a wɔmfa nhyɛ mu ho sɔhwɛ wɔ nitrogen nsateaa adaka mu wɔ 100 mW/cm2 nhyɛso a UV filter nni mu. Wɔde PHI nanoTOFII bere a wɔde tu kwan SIMS na ɛsusuw ToF-SIMS. Wɔde 4 kV Ar ion tuo a ne kɛse yɛ 400×400 μm na ɛyɛɛ depth profiling.
Wɔyɛɛ X-ray photoelectron spectroscopy (XPS) susudua wɔ Thermo-VG Nyansahu nhyehyɛe (ESCALAB 250) a wɔde monochromatized Al Kα (ma XPS mode) dii dwuma wɔ nhyɛso a ɛyɛ 5.0 × 10–7 Pa. Wɔyɛɛ scanning electron microscopy (SEM) wɔ JEOL-JSM-6330F nhyehyɛe so. Wɔde atom force microscopy (AFM) (Bruker Dimension FastScan) na ɛsusuu sɛnea perovskite sini ahorow no ani te ne sɛnea ɛyɛ mmerɛw. Wɔyɛ STEM ne HAADF-STEM wɔ FEI Titan Themis STEM. Wɔde UV-3600Plus (Shimadzu Corporation) na ɛsusuu UV–Vis absorption spectra. Wɔkyerɛw ahunmu charge limiting current (SCLC) wɔ Keithley mita 2400 so. Wɔde FLS 1000 photoluminescence spectrometer susuw photoluminescence a ɛwɔ tebea a ɛyɛ gyinabea (PL) ne bere a wɔasiesie photoluminescence (TRPL) a ɛfa carrier nkwa nna mu porɔw ho. Wɔde Horiba LabRam Raman nhyehyɛe HR Evolution na ɛsusuu PL map mfonini ahorow. Wɔde Thermo-Fisher Nicolet NXR 9650 nhyehyɛe na ɛyɛɛ Fourier transform infrared spectroscopy (FTIR).
Wɔ saa adwuma yi mu no, yɛde SSW kwan nhwɛsoɔ kwan no di dwuma de sua fase nsakraeɛ kwan a ɛfiri α-fase kɔ δ-fase so. Wɔ SSW kwan no mu no, wɔde random soft mode (second derivative) no kwankyerɛ na ɛkyerɛ sɛnea ahoɔden a ebetumi aba no ani no kankan, a ɛma wotumi yɛ ahoɔden a ebetumi aba no ani ho adesua a ɛkɔ akyiri na ɛyɛ botae. Wɔ saa adwuma yi mu no, wɔyɛ akwan nhwɛsoɔ wɔ atom 72 supercell so, na wɔboaboa mfitiaseɛ/awieɛ tebea (IS/FS) mmienu bɛboro 100 ano wɔ DFT gyinabea. Wogyina IS/FS pairwise data set so no, wobetumi de atom ahorow ntam nkitahodi akyerɛ ɔkwan a ɛka mfitiase nhyehyɛe no ne nhyehyɛe a etwa to no bom, na afei wɔde akwan abien a ɛkɔ variable unit surface no so no di dwuma de kyerɛ nsakrae tebea kwan no yiye. (VK-DESV) na ɛyɛ adwuma. Sɛ wɔhwehwɛ nsakrae tebea no wie a, wobetumi ahu ɔkwan a akwanside a ɛba fam sen biara wɔ no denam ahoɔden akwanside ahorow no a wɔde besisi hɔ no so.
Wɔde VASP (version 5.3.5) na ɛyɛɛ DFT akontabuo nyinaa, baabi a wɔde projected amplified wave (PAW) nhyehyɛeɛ gyina hɔ ma electron–ion nkitahodiɛ a ɛwɔ C, N, H, Pb, ne I atoms mu. Wɔde generalized gradient approximation a ɛwɔ Perdue-Burke-Ernzerhoff parametrization mu na ɛkyerɛkyerɛ nsakraeɛ nkitahodi dwumadie no mu. Wɔde ahoɔden anohyeto a ɛwɔ hɔ ma wimhyɛn asorɔkye no sii hɔ sɛ 400 eV. Monkhorst–Pack k-point grid no kɛseɛ yɛ (2 × 2 × 1). Wɔ nhyehyɛe nyinaa mu no, wɔyɛɛ lattice ne atom gyinabea ahorow no yiye koraa kosii sɛ nhyɛso fã a ɛsen biara no baa fam sen 0.1 GPa na ahoɔden fã a ɛsen biara no kɔɔ fam 0.02 eV/Å. Wɔ soro nhwɛsoɔ no mu no, FAPbI3 ani wɔ ntoatoasoɔ 4, ase ntoatoasoɔ no wɔ atom a ɛyɛ pintinn a ɛyɛ FAPbI3 nipadua no ho mfonini, na ntoatoasoɔ mmiɛnsa a ɛwɔ soro no tumi tu fa ahofadie mu wɔ optimization nhyehyɛeɛ no mu. PbC2O4 layer no mu duru yɛ 1 ML na ɛwɔ FAPbI3 I-terminal surface, baabi a Pb kyekyere 1 I ne 4 O.
Sɛ wopɛ adesua nhyehyɛe no ho nsɛm pii a, hwɛ Natural Portfolio Report Abstract a ɛbata asɛm yi ho no.
Wɔde nsɛm a wonyae anaa wɔhwehwɛɛ mu wɔ adesua yi mu nyinaa ka asɛm a wɔatintim no ho, ne nsɛm a ɛfoa so ne data fael ahorow a wɔanhyehyɛ no yiye no nso. Raw data a wɔde ama wɔ nhwehwɛmu yi mu no wɔ https://doi.org/10.6084/m9.figshare.2410016440. Wɔde Source data ama ama asɛm yi.
Green, M. ne afoforo. Owia Nkwammoaa a Wɔde Di Dwuma Yiye Ho Nkyerɛwde (57th ed.). dwumadi no. photoelectric a ɛma anyinam ahoɔden. ade a wɔde yɛ adwuma. abisadeɛ. 29, 3–15 (2021) na ɔkyerɛwee.
Parker J. ne afoforo. Perovskite layers nyin a wɔde alkyl ammonium chlorides a ɛyɛ hyew di dwuma. Abɔdeɛ 616, 724-730 (2023).
Zhao Y. ne afoforo. Inactive (PbI2)2RbCl ma perovskite sini ahorow no gyina pintinn ma owia nkwammoaa a ɛyɛ adwuma yiye. Nyansahu 377, 531-534 (2022).
Tan, K. ne afoforo. Perovskite owia nkwammoaa a wɔadan no a wɔde dimethylacridinyl dopant di dwuma. Abɔdeɛ, 620, 545-551 (2023).
Han, K. ne afoforo. Single crystalline formamidine lead iodide (FAPbI3): nhumu a ɛfa nhyehyɛe, aniwa ne anyinam ahoɔden su ho. ɔkyerɛfoɔ. Mat. 28, 2253–2258 (2016) Nsɛm a wɔahyehyɛ.
Massey, S. ne afoforo. Perovskite tuntum fã no a ɛma ɛyɛ den wɔ FAPbI3 ne CsPbI3 mu. AKS Ahoɔden Nkitahodi. 5, 1974–1985 (2020) Nsɛm a wɔka kyerɛ.
Wo, JJ, ne afoforo. Perovskite owia nkwammoaa a etu mpɔn denam nneɛma a wɔde fa so a wɔhwɛ so yiye so. Abɔdeɛ 590, 587-593 (2021).
Saliba M. ne afoforo. Rubidium cations a wɔde ka perovskite owia nkwammoaa mu no ma photovoltaic adwumayɛ tu mpɔn. Nyansahu 354, 206-209 (2016).
Saliba M. ne afoforo. Triple-cation perovskite cesium owia nkwammoaa: nkɔso a ɛma ɛyɛ den, ɛtumi san yɛ bio na ɛyɛ adwuma yie. ahoɔden a atwa yɛn ho ahyia. nyansahu no. 9, 1989–1997 (2016) Nsɛm a wɔka kyerɛ.
Cui X. ne afoforo. Nnansa yi nkɔso a aba wɔ FAPbI3 phase stabilization mu wɔ perovskite owia nkwammoaa a ɛyɛ adwuma yiye mu Sol. RRL 6, 2200497 (2022) na ɔkyerɛwee.
Delagetta S. ne afoforo. Rationalized photoinduced phase mpaapaemu a afrafra halide organic-inorganic perovskites. Nat. nkutahodie. 8, 200 (2017) na ɔkyerɛwee.
Slotcavage, D. J. ne afoforo. Hann-a ɛma phase mpaapaemu wɔ halide perovskite absorbers. AKS Ahoɔden Nkitahodi. 1, 1199–1205 (2016) Nsɛm a wɔahyehyɛ.
Chen, L. ne afoforo. Intrinsic phase stability ne intrinsic bandgap a formamidine kɔbere triiodide perovskite ahwehwɛ biako. Anjiva na ɔkyerɛwee. Nnuru a wɔde yɛ nneɛma. amanaman ntam nkitahodi. Ed. 61. e202212700 (2022) na ɛyɛ adwuma.
Duinsti, EA etc. Te methylenediammonium a ɛporɔw ne dwuma a edi wɔ lead triiodide formamidine phase stabilization mu ase. J. Chem. Bitch a ɔyɛ ɔbarima. 18, 10275–10284 (2023) Nsɛm a wɔahyehyɛ.
Lu, HZ ne afoforo. Nsuo a ɛyɛ adwuma yie na ɛyɛ pintinn a ɛyɛ tuntum perovskite owia nkwammoaa FAPbI3. Nyansahu 370, 74 (2020).
Doherty, TAS ne nea ɛkeka ho Stable tilted octahedral halide perovskites siw localized formation of phases a anohyeto su. Nyansahu 374, 1598-1605 (2021).
Ho, K. ne afoforo. Akwan a wɔfa so dannan na ɛsɛe formamidine aburow ne cesium ne lead iodide perovskites wɔ nsu ne hann nkɛntɛnso ase. AKS Ahoɔden Nkitahodi. 6, 934–940 (2021) Nsɛm a wɔahyehyɛ.
Zheng J. ne afoforo. Nkɔsoɔ a ɛfa pseudohalide anions ho ma α-FAPbI3 perovskite owia nkwammoaa. Abɔdeɛ 592, 381-385 (2021).