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1.
Nature ; 624(7990): 69-73, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37938775

RESUMO

All-perovskite tandem solar cells hold great promise in surpassing the Shockley-Queisser limit for single-junction solar cells1-3. However, the practical use of these cells is currently hampered by the subpar performance and stability issues associated with mixed tin-lead (Sn-Pb) narrow-bandgap perovskite subcells in all-perovskite tandems4-7. In this study, we focus on the narrow-bandgap subcells and develop an all-in-one doping strategy for them. We introduce aspartate hydrochloride (AspCl) into both the bottom poly(3,4-ethylene dioxythiophene)-poly(styrene sulfonate) and bulk perovskite layers, followed by another AspCl posttreatment. We show that a single AspCl additive can effectively passivate defects, reduce Sn4+ impurities and shift the Fermi energy level. Additionally, the strong molecular bonding of AspCl-Sn/Pb iodide and AspCl-AspCl can strengthen the structure and thereby improve the stability of Sn-Pb perovskites. Ultimately, the implementation of AspCl doping in Sn-Pb perovskite solar cells yielded power conversion efficiencies of 22.46% for single-junction cells and 27.84% (27.62% stabilized and 27.34% certified) for tandems with 95% retention after being stored in an N2-filled glovebox for 2,000 h. These results suggest that all-in-one AspCl doping is a favourable strategy for enhancing the efficiency and stability of single-junction Sn-Pb perovskite solar cells and their tandems.

2.
J Am Chem Soc ; 143(18): 7069-7080, 2021 May 12.
Artigo em Inglês | MEDLINE | ID: mdl-33905231

RESUMO

Hybrid halide perovskites consisting of corner-sharing metal halide octahedra and small cuboctahedral cages filled with counter cations have proven to be prominent candidates for many high-performance optoelectronic devices. The stability limits of their three-dimensional perovskite framework are defined by the size range of the cations present in the cages of the structure. In some cases, the stability of the perovskite-type structure can be extended even when the counterions violate the size and shape requirements, as is the case in the so-called "hollow" perovskites. In this work, we engineered a new family of 3D highly defective yet crystalline "hollow" bromide perovskites with general formula (FA)1-x(en)x(Pb)1-0.7x(Br)3-0.4x (FA = formamidinium (FA+), en = ethylenediammonium (en2+), x = 0-0.44). Pair distribution function analysis shed light on the local structural coherence, revealing a wide distribution of Pb-Pb distances in the crystal structure as a consequence of the Pb/Br-deficient nature and en inclusion in the lattice. By manipulating the number of Pb/Br vacancies, we finely tune the optical properties of the pristine FAPbBr3 by blue shifting the band gap from 2.20 to 2.60 eV for the x = 0.42 en sample. A most unexpected outcome was that at x> 0.33 en incorporation, the material exhibits strong broad light emission (1% photoluminescence quantum yield (PLQY)) that is maintained after exposure to air for more than a year. This is the first example of strong broad light emission from a 3D hybrid halide perovskite, demonstrating that meticulous defect engineering is an excellent tool for customizing the optical properties of these semiconductors.

3.
J Am Chem Soc ; 142(35): 15049-15057, 2020 Sep 02.
Artigo em Inglês | MEDLINE | ID: mdl-32786780

RESUMO

The advent of the two-dimensional (2D) family of halide perovskites and their demonstration in 2D/three-dimensional (3D) hierarchical film structures broke new ground toward high device performance and good stability. The 2D Dion-Jacobson (DJ) phase halide perovskites are especially attractive in solar cells because of their superior charge transport properties. Here, we report on 2D DJ phase perovskites using a 3-(aminomethyl)piperidinium (3AMP) organic spacer for the fabrication of mixed Pb/Sn-based perovskites, exhibiting a narrow bandgap of 1.27 eV and a long carrier lifetime of 657.7 ns. Consequently, solar cells employing mixed 2D DJ 3AMP-based and 3D MA0.5FA0.5Pb0.5Sn0.5I3 (MA = methylammonium, FA = formamidinium) perovskite composites as light absorbers achieve enhanced efficiency and stability, giving a power conversion efficiency of 20.09% with a high open-circuit voltage of 0.88 V, a fill factor of 79.74%, and a short-circuit current density of 28.63 mA cm-2. The results provide an effective strategy to improve the performance of single-junction narrow-bandgap solar cells and, potentially, to give a highly efficient alternative to bottom solar cells in tandem devices.

4.
J Am Chem Soc ; 142(19): 9028-9038, 2020 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-32283025

RESUMO

The optical and light emission properties of tin and lead halide perovskites are remarkable because of the robust room-temperature (RT) performance, broad wavelength tunability, high efficiency, and good quenching resistance to defects. These highly desirable attributes promise to transform current light-emitting devices, phosphors, and lasers. One disadvantage in most of these materials is the sensitivity to moisture. Here, we report a new air-stable one-dimensional (1D) hybrid lead-free halide material (DAO)Sn2I6 (DAO, 1,8-octyldiammonium) that is resistant to water for more than 15 h. The material exhibits a sharp optical absorption edge at 2.70 eV and a strong broad orange light emission centered at 634 nm, with a full width at half-maximum (fwhm) of 142 nm (0.44 eV). The emission has a long photoluminescence (PL) lifetime of 582 ns, while the intensity is constant over a very broad temperature range (145-415 K) with a photoluminescence quantum yield (PLQY) of at least 20.3% at RT. Above 415 K the material undergoes a structural phase transition from monoclinic (C2/c) to orthorhombic (Ibam) accompanied by a red shift in the band gap and a quench in the photoluminescence emission. Density functional theory calculations support the trend in the optical properties and the 1D electronic nature of the structure, where the calculated carrier effective masses along the inorganic chain are significantly lower than those perpendicular to the chain. Thin films of the compound readily fabricated from solutions exhibit the same optical properties, but with improved PLQY of 36%, for a 60 nm thick film, among the highest reported for lead-free low-dimensional 2D and 1D perovskites and metal halides.

5.
J Am Chem Soc ; 142(14): 6625-6637, 2020 Apr 08.
Artigo em Inglês | MEDLINE | ID: mdl-32176495

RESUMO

Large organic A cations cannot stabilize the 3D perovskite AMX3 structure because they cannot be accommodated in the cubo-octhedral cage (do not follow the Goldschmidt tolerance factor rule), and they generally template low-dimensional structures. Here we report that the large dication aminomethylpyridinium (AMPY) can template novel 3D structures which resemble conventional perovskites. They have the formula (xAMPY)M2I6 (x = 3 or 4, M = Sn2+ or Pb2+) which is double of the AMX3 formula. However, because of the steric requirement of the Goldschmidt tolerance factor rule, it is impossible for (xAMPY)M2I6 to form proper perovskite structures. Instead, a combination of corner-sharing and edge-sharing connectivity is adopted in these compounds leading to the new 3D structures. DFT calculations reveal that the compounds are indirect band gap semiconductors with direct band gaps presenting at slightly higher energies and dispersive electronic bands. The indirect band gaps of the Sn and Pb compounds are ∼1.7 and 2.0 eV, respectively, which is slightly higher than the corresponding AMI3 3D perovskites. The Raman spectra for the compounds are diffuse, with a broad rising central peak at very low frequencies around 0 cm-1, a feature that is characteristic of dynamical lattices, high anharmonicity, and dissipative vibrations very similar to the 3D AMX3 perovskites. Devices of (3AMPY)Pb2I6 crystals exhibit clear photoresponse under ambient light without applied bias, reflecting a high carrier mobility (µ) and long carrier lifetime (τ). The devices also exhibit sizable X-ray generated photocurrent with a high µτ product of ∼1.2 × 10-4 cm2 /V and an X-ray sensitivity of 207 µC·Gy-1·cm-2.

6.
J Am Chem Soc ; 141(21): 8627-8637, 2019 May 29.
Artigo em Inglês | MEDLINE | ID: mdl-31063361

RESUMO

The power conversion efficiency (PCE) of halide perovskite solar cells is now comparable to that of commercial solar cells. These solar cells are generally based on multication mixed-halide perovskite absorbers with nonideal band gaps of 1.5-1.6 eV. The PCE should be able to rise further if the solar cells could use narrower-band gap absorbers (1.2-1.4 eV). Reducing the Pb content of the semiconductors without sacrificing performance is also a significant driver in the perovskite solar cell research. Here, we demonstrate that mixed Pb/Sn-based perovskites containing the oversized ethylenediammonium ( en) dication, { en}FA0.5MA0.5Sn0.5Pb0.5I3 (FA = formamidinium, MA = methylammonium), can exhibit ideal band gaps of 1.27-1.38 eV, suitable for the assembly of single-junction solar cells with higher efficiencies. The use of en dication creates a three-dimensional (3D) hollow inorganic perovskite structure, which was verified through crystal density measurements and single-crystal X-ray diffraction structural analysis as well as nuclear magnetic resonance measurements. The { en}FA0.5MA0.5Sn0.5Pb0.5I3 structure has massive Pb/Sn vacancies and much higher chemical stability than the same structure without en and vacancies. This new property reduces the dark current and carrier trap density and increases the carrier lifetime of the Pb/Sn-based perovskite films. Therefore, solar cells using { en}FA0.5MA0.5Sn0.5Pb0.5I3 light absorbers have substantially enhanced air stability and around 20% improvement in efficiency. After overlaying a thin MABr top layer, we found that the {5% en}FA0.5MA0.5Sn0.5Pb0.5I3 material gives an optimized PCE of 17.04%. The results highlight the strong promise of 3D hollow mixed Pb/Sn perovskites in achieving ideal band gap materials with higher chemical stability and lower Pb content for high-performance single-junction solar cells or multijunction solar cells serving as bottom cells.

7.
J Am Chem Soc ; 141(13): 5518-5534, 2019 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-30827098

RESUMO

The unique hybrid nature of 2D Ruddlesden-Popper (R-P) perovskites has bestowed upon them not only tunability of their electronic properties but also high-performance electronic devices with improved environmental stability as compared to their 3D analogs. However, there is limited information about their inherent heat, light, and air stability and how different parameters such as the inorganic layer number and length of organic spacer molecule affect stability. To gain deeper understanding on the matter we have expanded the family of 2D R-P perovskites, by utilizing pentylamine (PA)2(MA) n-1Pb nI3 n+1 ( n = 1-5, PA = CH3(CH2)4NH3+, C5) and hexylamine (HA)2(MA) n-1Pb nI3 n+1 ( n = 1-4, HA = CH3(CH2)5NH3+, C6) as the organic spacer molecules between the inorganic slabs, creating two new series of layered materials, for up to n = 5 and 4 layers, respectively. The resulting compounds were extensively characterized through a combination of physical and spectroscopic methods, including single crystal X-ray analysis. High resolution powder X-ray diffraction studies using synchrotron radiation shed light for the first time to the phase transitions of the higher layer 2D R-P perovskites. The increase in the length of the organic spacer molecules did not affect their optical properties; however, it has a pronounced effect on the air, heat, and light stability of the fabricated thin films. An extensive study of heat, light, and air stability with and without encapsulation revealed that specific compounds can be air stable (relative humidity (RH) = 20-80% ± 5%) for more than 450 days, while heat and light stability in air can be exponentially increased by encapsulating the corresponding films. Evaluation of the out-of-plane mechanical properties of the corresponding materials showed that their soft and flexible nature can be compared to current commercially available polymer substrates (e.g., PMMA), rendering them suitable for fabricating flexible and wearable electronic devices.

8.
J Am Chem Soc ; 141(32): 12880-12890, 2019 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-31313919

RESUMO

Two-dimensional (2D) halide perovskites have extraordinary optoelectronic properties and structural tunability. Among them, the Dion-Jacobson phases with the inorganic layers stacking exactly on top of each other are less explored. Herein, we present the new series of 2D Dion-Jacobson halide perovskites, which adopt the general formula of A'An-1PbnI3n+1 (A' = 4-(aminomethyl)pyridinium (4AMPY), A = methylammonium (MA), n = 1-4). By modifying the position of the CH2NH3+ group from 4AMPY to 3AMPY (3AMPY = 3-(aminomethyl)pyridinium), the stacking of the inorganic layers changes from exactly eclipsed to slightly offset. The perovskite octahedra tilts are also different between the two series, with the 3AMPY series exhibiting smaller bandgaps than the 4AMPY series. Compared to the aliphatic cation of the same size (AMP = (aminomethyl)piperidinium), the aromatic spacers increase the rigidity of the cation, reduce the interlayer spacing, and decrease the dielectric mismatch between inorganic layer and the organic spacer, showing the indirect but powerful influence of the organic cations on the structure and consequently on the optical properties of the perovskite materials. All A'An-1PbnI3n+1 compounds exhibit strong photoluminescence (PL) at room temperature. Preliminary solar cell devices based on the n = 4 perovskites as absorbers of both series exhibit promising performances, with a champion power conversion efficiency (PCE) of 9.20% for (3AMPY)(MA)3Pb4I13-based devices, which is higher than the (4AMPY)(MA)3Pb4I13 and the corresponding aliphatic analogue (3AMP)(MA)3Pb4I13-based ones.

9.
J Am Chem Soc ; 141(6): 2684-2694, 2019 Feb 13.
Artigo em Inglês | MEDLINE | ID: mdl-30648861

RESUMO

The two-dimensional (2D) perovskites stabilized by alternating cations in the interlayer space (ACI) define a new type of structure with different physical properties than the more common Ruddlesden-Popper counterparts. However, there is a lack of understanding of material crystallization in films and its influence on the morphological/optoelectronic properties and the final photovoltaic devices. Herein, we undertake in situ studies of the solidification process for ACI 2D perovskite (GA)(MA) nPb nI3 n+1 (⟨ n⟩ = 3) from ink to solid-state semiconductor, using solvent mixture of DMSO:DMF (1:10 v/v) as the solvent and link this behavior to solar cell devices. The in situ grazing-incidence X-ray scattering (GIWAXS) analysis reveals a complex journey through disordered sol-gel precursors, intermediate phases, and ultimately to ACI perovskites. The intermediate phases, including a crystalline solvate compound and the 2D GA2PbI4 perovskite, provide a scaffold for the growth of the ACI perovskites during thermal annealing. We identify 2D GA2PbI4 to be the key intermediate phase, which is strongly influenced by the deposition technique and determines the formation of the 1D GAPbI3 byproducts and the distribution of various n phases of ACI perovskites in the final films. We also confirm the presence of internal charge transfer between different n phases through transient absorption spectroscopy. The high quality ACI perovskite films deposited from solvent mixture of DMSO:DMF (1:10 v/v) deliver a record power conversion efficiency of 14.7% in planar solar cells and significantly enhanced long-term stability of devices in contrast to the 3D MAPbI3 counterpart.

10.
J Am Chem Soc ; 140(17): 5728-5742, 2018 05 02.
Artigo em Inglês | MEDLINE | ID: mdl-29617127

RESUMO

The newly introduced class of 3D halide perovskites, termed "hollow" perovskites, has been recently demonstrated as light absorbing semiconductor materials for fabricating lead-free perovskite solar cells with enhanced efficiency and superior stability. Hollow perovskites derive from three-dimensional (3D) AMX3 perovskites ( A = methylammonium (MA), formamidinium (FA); M = Sn, Pb; X = Cl, Br, I), where small molecules such as ethylenediammonium cations ( en) can be incorporated as the dication without altering the structure dimensionality. We present in this work the inherent structural properties of the hollow perovskites and expand this class of materials to the Pb-based analogues. Through a combination of physical and spectroscopic methods (XRD, gas pycnometry, 1H NMR, TGA, SEM/EDX), we have assigned the general formula (A)1- x( en) x(M)1-0.7 x(X)3-0.4 x to the hollow perovskites. The incorporation of en in the 3D perovskite structure leads to massive M and X vacancies in the 3D [ MX3] framework, thus the term hollow. The resulting materials are semiconductors with significantly blue-shifted direct band gaps from 1.25 to 1.51 eV for Sn-based perovskites and from 1.53 to 2.1 eV for the Pb-based analogues. The increased structural disorder and hollow nature were validated by single crystal X-ray diffraction analysis as well as pair distribution function (PDF) analysis. Density functional theory (DFT) calculations support the experimental trends and suggest that the observed widening of the band gap is attributed to the massive M and X vacancies, which create a less connected 3D hollow structure. The resulting materials have superior air stability, where in the case of Sn-based hollow perovskites it exceeds two orders of temporal magnitude compared to the conventional full perovskites of MASnI3 and FASnI3. The hollow perovskite compounds pose as a new platform of promising light absorbers that can be utilized in single junction or tandem solar cells.

11.
J Am Chem Soc ; 140(38): 12226-12238, 2018 09 26.
Artigo em Inglês | MEDLINE | ID: mdl-30169031

RESUMO

Low-dimensional halide perovskites have recently attracted intense interest as alternatives to the three-dimensional (3D) perovskites because of their greater tunability and higher environmental stability. Herein, we present the new homologous 2D series (NH3C mH2 mNH3)(CH3NH3) n-1Pb nI3 n+1 ( m = 4-9; n = 1-4), where m represents the carbon-chain number and n equals layer-thickness number. Multilayer ( n > 1) 2D perovskites incorporating diammonium cations were successfully synthesized by the solid-state grinding method for m = 4 and 6 and by the solution method for m = 7-9. Structural characterization by single-crystal X-ray diffraction for the m = 8 and m = 9 series ( n = 1-4) reveals that these compounds adopt the Cc space group for even n members and Pc for odd n members. The optical bandgaps are 2.15 eV for two-layer ( n = 2), 2.01 eV for three-layer ( n = 3), and 1.90 eV for four-layer ( n = 4). The materials exhibit excellent solution processability, and casting thin-films of the n = 3 members was successfully accomplished. The films show a clear tendency for the higher- m members to have preferred orientation on the glass substrate, with m = 8 exhibiting almost perfect vertical layer orientation and m = 9 displaying both vertical and parallel layer orientation, as confirmed by grazing-incidence wide-angle X-ray scattering (GIWAXS) measurements. The vertical layer orientation for the (NH3C8H16NH3)(CH3NH3)2Pb3I10 member results in the best thermal, light, and air stability within this series, thus showing excellent potential for solar cell applications.

12.
J Am Chem Soc ; 140(10): 3775-3783, 2018 03 14.
Artigo em Inglês | MEDLINE | ID: mdl-29465246

RESUMO

The three-dimensional hybrid organic-inorganic perovskites have shown huge potential for use in solar cells and other optoelectronic devices. Although these materials are under intense investigation, derivative materials with lower dimensionality are emerging, offering higher tunability of physical properties and new capabilities. Here, we present two new series of hybrid two-dimensional (2D) perovskites that adopt the Dion-Jacobson (DJ) structure type, which are the first complete homologous series reported in halide perovskite chemistry. Lead iodide DJ perovskites adopt a general formula A'A n-1Pb nI3 n+1 (A' = 3-(aminomethyl)piperidinium (3AMP) or 4-(aminomethyl)piperidinium (4AMP), A = methylammonium (MA)). These materials have layered structures where the stacking of inorganic layers is unique as they lay exactly on top of another. With a slightly different position of the functional group in the templating cation 3AMP and 4AMP, the as-formed DJ perovskites show different optical properties, with the 3AMP series having smaller band gaps than the 4AMP series. Analysis on the crystal structures and density functional theory (DFT) calculations suggest that the origin of the systematic band gap shift is the strong but indirect influence of the organic cation on the inorganic framework. Fabrication of photovoltaic devices utilizing these materials as light absorbers reveals that (3AMP)(MA)3Pb4I13 has the best power conversion efficiency (PCE) of 7.32%, which is much higher than that of the corresponding (4AMP)(MA)3Pb4I13.

13.
J Am Chem Soc ; 140(1): 388-393, 2018 01 10.
Artigo em Inglês | MEDLINE | ID: mdl-29211458

RESUMO

Developing dopant-free hole transporting layers (HTLs) is critical in achieving high-performance and robust state-of-the-art perovskite photovoltaics, especially for the air-sensitive tin-based perovskite systems. The commonly used HTLs require hygroscopic dopants and additives for optimal performance, which adds extra cost to manufacturing and limits long-term device stability. Here we demonstrate the use of a novel tetrakis-triphenylamine (TPE) small molecule prepared by a facile synthetic route as a superior dopant-free HTL for lead-free tin-based perovskite solar cells. The best-performing tin iodide perovskite cells employing the novel mixed-cation ethylenediammonium/formamidinium with the dopant-free TPE HTL achieve a power conversion efficiency as high as 7.23%, ascribed to the HTL's suitable band alignment and excellent hole extraction/collection properties. This efficiency is one of the highest reported so far for tin halide perovskite systems, highlighting potential application of TPE HTL material in low-cost high-performance tin-based perovskite solar cells.

14.
J Am Chem Soc ; 139(41): 14800-14806, 2017 10 18.
Artigo em Inglês | MEDLINE | ID: mdl-28953381

RESUMO

Tin-based perovskites have very comparable electronic properties to lead-based perovskites and are regarded as possible lower toxicity alternates for solar cell applications. However, the efficiency of tin-based perovskite solar cells is still low and they exhibit poor air stability. Here, we report lead-free tin-based solar cells with greatly enhanced performance and stability using so-called "hollow" ethylenediammonium and methylammonium tin iodide ({en}MASnI3) perovskite as absorbers. Our results show that en can improve the film morphology and most importantly can serve as a new cation to be incorporated into the 3D MASnI3 lattice. When the cation of en becomes part of the 3D structure, a high density of SnI2 vacancies is created resulting in larger band gap, larger unit cell volume, lower trap-state density, and much longer carrier lifetime compared to classical MASnI3. The best-performing {en}MASnI3 solar cell has achieved a high efficiency of 6.63% with an open circuit voltage of 428.67 mV, a short-circuit current density of 24.28 mA cm-2, and a fill factor of 63.72%. Moreover, the {en}MASnI3 device shows much better air stability than the neat MASnI3 device. Comparable performance is also achieved for cesium tin iodide solar cells with en loading, demonstrating the broad scope of this approach.

15.
Small ; 13(2)2017 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-28060468

RESUMO

Despite the rapid increase of efficiency, perovskite solar cells (PSCs) still face some challenges, one of which is the current-voltage hysteresis. Herein, it is reported that yttrium-doped tin dioxide (Y-SnO2 ) electron selective layer (ESL) synthesized by an in situ hydrothermal growth process at 95 °C can significantly reduce the hysteresis and improve the performance of PSCs. Comparison studies reveal two main effects of Y doping of SnO2 ESLs: (1) it promotes the formation of well-aligned and more homogeneous distribution of SnO2 nanosheet arrays (NSAs), which allows better perovskite infiltration, better contacts of perovskite with SnO2 nanosheets, and improves electron transfer from perovskite to ESL; (2) it enlarges the band gap and upshifts the band energy levels, resulting in better energy level alignment with perovskite and reduced charge recombination at NSA/perovskite interfaces. As a result, PSCs using Y-SnO2 NSA ESLs exhibit much less hysteresis and better performance compared with the cells using pristine SnO2 NSA ESLs. The champion cell using Y-SnO2 NSA ESL achieves a photovoltaic conversion efficiency of 17.29% (16.97%) when measured under reverse (forward) voltage scanning and a steady-state efficiency of 16.25%. The results suggest that low-temperature hydrothermal-synthesized Y-SnO2 NSA is a promising ESL for fabricating efficient and hysteresis-less PSC.

17.
J Am Chem Soc ; 138(45): 14998-15003, 2016 11 16.
Artigo em Inglês | MEDLINE | ID: mdl-27776416

RESUMO

Achieving high open-circuit voltage (Voc) for tin-based perovskite solar cells is challenging. Here, we demonstrate that a ZnS interfacial layer can improve the Voc and photovoltaic performance of formamidinium tin iodide (FASnI3) perovskite solar cells. The TiO2-ZnS electron transporting layer (ETL) with cascade conduction band structure can effectively reduce the interfacial charge recombination and facilitate electron transfer. Our best-performing FASnI3 perovskite solar cell using the cascaded TiO2-ZnS ETL has achieved a power conversion efficiency of 5.27%, with a higher Voc of 0.380 V, a short-circuit current density of 23.09 mA cm-2, and a fill factor of 60.01%. The cascade structure is further validated with a TiO2-CdS ETL. Our results suggest a new approach for further improving the performance of tin-based perovskite solar cells with a higher Voc.

18.
Phys Chem Chem Phys ; 18(24): 16436-43, 2016 Jun 28.
Artigo em Inglês | MEDLINE | ID: mdl-27264190

RESUMO

Efficient planar antimony sulfide (Sb2S3) heterojunction solar cells have been made using chemical bath deposited (CBD) Sb2S3 as the absorber, low-temperature solution-processed tin oxide (SnO2) as the electron conductor and poly (3-hexylthiophene) (P3HT) as the hole conductor. A solar conversion efficiency of 2.8% was obtained at 1 sun illumination using a planar device consisting of F-doped SnO2 substrate/SnO2/CBD-Sb2S3/P3HT/Au, whereas the solar cells based on a titanium dioxide (TiO2) electron conductor exhibited a power conversion efficiency of 1.9%. Compared with conventional Sb2S3 sensitized solar cells, the high-temperature processed mesoscopic TiO2 scaffold is no longer needed. More importantly, a low-temperature solution-processed SnO2 layer was introduced for electron transportation to substitute the high-temperature sintered dense blocking TiO2 layer. Our planar solar cells not only have simple geometry with fewer steps to fabricate but also show enhanced performance. The higher efficiency of planar Sb2S3 solar cell devices based on a SnO2 electron conductor is attributed to their high transparency, uniform surface, efficient electron transport properties of SnO2, suitable energy band alignment, and reduced recombination at the interface of SnO2/Sb2S3.

19.
J Am Chem Soc ; 137(21): 6730-3, 2015 Jun 03.
Artigo em Inglês | MEDLINE | ID: mdl-25987132

RESUMO

Lead halide perovskite solar cells with the high efficiencies typically use high-temperature processed TiO2 as the electron transporting layers (ETLs). Here, we demonstrate that low-temperature solution-processed nanocrystalline SnO2 can be an excellent alternative ETL material for efficient perovskite solar cells. Our best-performing planar cell using such a SnO2 ETL has achieved an average efficiency of 16.02%, obtained from efficiencies measured from both reverse and forward voltage scans. The outstanding performance of SnO2 ETLs is attributed to the excellent properties of nanocrystalline SnO2 films, such as good antireflection, suitable band edge positions, and high electron mobility. The simple low-temperature process is compatible with the roll-to-roll manufacturing of low-cost perovskite solar cells on flexible substrates.

20.
ACS Nano ; 18(8): 6095-6110, 2024 Feb 27.
Artigo em Inglês | MEDLINE | ID: mdl-38372495

RESUMO

Halide perovskites have emerged as highly promising materials for ionizing radiation detection due to their exceptional characteristics, including a large mobility-lifetime product, strong stopping power, tunable band gap, and cost-effective crystal growth via solution processes. Semiconductor-type X-ray detectors employing various micro/nano perovskite materials have shown impressive progress in achieving heightened sensitivity and lower detection limits. Here, we present a comprehensive review of the applications of micro/nano perovskite materials for direct type X-ray detection, with a focus on the requirements for micro/nano crystal assembly and device properties in advanced X-ray detectors. We explore diverse processing techniques and optoelectronic considerations applied to perovskite X-ray detectors. Additionally, this review highlights the challenges and promising opportunities for perovskite X-ray detector arrays in real-world applications, potentially necessitating further research efforts.

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