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1.
J Phys Chem Lett ; : 4138-4146, 2020 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-32370506

RESUMO

The phase instability of cesium lead halide perovskite is still a substantial challenge hindering its application. A 2D-3D all-inorganic Cs2PbI2Cl2-CsPbI2.5Br0.5 perovskite solar cell was successfully developed to address this issue. The 2D Cs2PbI2Cl2 phase distributed among the grain boundaries of the 3D CsPbI3-xBrx grains. The existence of Cs2PbI2Cl2 effectively facilitated the (100) preferential crystal orientation of the CsPbI2.5Br0.5 crystals, promoting the carrier transport. The smooth transition region between the (003)2D//(001)3D interface indicated the formation of a 2D-3D heterostructure. Due to the improved crystal quality, high uniformity, and repeatability, the efficiency of the solar cells with areas of 0.09, 1, and 2 cm2 significantly improved to 15.09%, 12.74%, and 10.01%, respectively. The power conversion efficiency (PCE) retained 95.3% of the initial efficiency after 60 days in a nitrogen atmosphere at room temperature and 80% of the initial efficiency at a humidity of 70 ± 10% relative humidity (RH) under continuous heating at 80 °C for 12 h.

2.
Nat Commun ; 11(1): 2304, 2020 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-32385231

RESUMO

The organic-inorganic hybrid lead halide perovskites have emerged as a series of star materials for solar cells, lasers and detectors. However, the issues raised by the toxic lead element and marginal stability due to the volatile organic components have severely limited their potential applications. In this work, we develop a nucleation-controlled solution method to grow large size high-quality Cs3Bi2I9 perovskite single crystals (PSCs). Using the technique, we harvest some centimeter-sized single crystals and achieved high device performance. We find that X-ray detectors based on PSCs exhibit high sensitivity of 1652.3 µC Gyair-1 cm-2 and very low detectable dose rate of 130 nGyair s-1, both desired in medical diagnostics. In addition, its outstanding thermal stability inspires us to develop a high temperature X-ray detector with stable response at up to 100 °C. Furthermore, PSCs exhibit high X-ray imaging capability thanks to its negligible signal drifting and extremely high stability.

3.
Small ; : e1907283, 2020 Apr 06.
Artigo em Inglês | MEDLINE | ID: mdl-32250013

RESUMO

Excellent power conversion efficiency (PCE) and stability are the primary forces that propel the all-inorganic cesium-based halide perovskite solar cells (PSCs) toward commercialization. However, the intrinsic high density of trap state and internal nonradiative recombination of CsPbIBr2 perovskite film are the barriers that limit its development. In the present study, a facile additive strategy is introduced to fabricate highly efficient CsPbIBr2 PSCs by incorporating sulfamic acid sodium salt (SAS) into the perovskite layer. The additive can control the crystallization behaviors and optimize morphology, as well as effectively passivate defects in the bulk perovskite film, thereby resulting in a high-quality perovskite. In addition, SAS in perovskite has possibly introduced an additional internal electric field effect that favors electron transport and injection due to inhomogeneous ion distribution. A champion PCE of 10.57% (steady-output efficiency is 9.99%) is achieved under 1 Sun illumination, which surpasses that of the contrast sample by 16.84%. The modified perovskite film also exhibits improved moisture stability. The unencapsulated device maintains over 80% initial PCE after aging for 198 h in air. The results provide a suitable additive for inorganic perovskite and introduce a new conjecture to explain the function of additives in PSCs more rationally.

4.
Artigo em Inglês | MEDLINE | ID: mdl-32293091

RESUMO

One-dimensional (1D) nanostructured oxides are proposed as excellent electron transport materials (ETMs) for perovskite solar cells (PSCs); however, experimental evidence is lacking. A facile hydrothermal approach was employed to grow highly oriented anatase TiO2 nanopyramid arrays and demonstrate their application in PSCs. The oriented TiO2 nanopyramid arrays afford sufficient contact area for electron extraction and increase light transmission. Moreover, the nanopyramid array/perovskite system exhibits an oriented electric field that can increase charge separation and accelerate charge transport, thereby suppressing charge recombination. The anatase TiO2 nanopyramid array-based PSCs deliver a champion power conversion efficiency of approximately 22.5 %, which is the highest power conversion efficiency reported to date for PSCs consisting of 1D ETMs. This work demonstrates that the rational design of 1D ETMs can achieve PSCs that perform as well as typical mesoscopic and planar PSCs.

5.
Artigo em Inglês | MEDLINE | ID: mdl-32216332

RESUMO

Lead halide perovskites with good optoelectronic properties and high attenuation of high-energy radiation are great candidates for X-ray radiation detectors. Large area, dense, and thick films or wafers are a prerequisite for these applications. In this paper, a one-step heat-assisted high-pressure press method is developed to directly prepare a large (the largest has a diameter of 80 mm) and thickness- and shape-controlled phase-pure organic-inorganic hybrid CH3NH3PbI3 wafer of densely packed large microcrystals from raw powder materials. Meanwhile, this method uses no solvent to achieve essentially 100% material utilization. The obtained wafers show good ambipolar carrier mobilities of ∼20 cm2 V-1 s-1 and a µτ product as high as 3.84 × 10-4 cm2 V-1. Under an X-ray source using an acceleration voltage of 40 kV, the perovskite wafer-based X-ray detector shows an X-ray sensitivity as large as 1.22 × 105 µC Gyair-1 cm-2 under a 10 V bias, the highest reported for any perovskite material. The method provides a convenient strategy for producing large perovskite wafers with good optoelectronic properties, which will facilitate the development of large perovskite devices.

6.
Small ; 15(46): e1904387, 2019 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-31592578

RESUMO

All-inorganic perovskite solar cells have developed rapidly in the last two years due to their excellent thermal and light stability. However, low efficiency and moisture instability limit their future commercial application. The mixed-halide inorganic CsPbI2 Br perovskite with a suitable bandgap offers a good balance between phase stability and light harvesting. However, high defect density and low carrier lifetime in CsPbI2 Br perovskites limit the open-circuit voltage (Voc < 1.2 V), short-circuit current density (Jsc < 15 mA cm-2 ), and fill factor (FF < 75%) of CsPbI2 Br perovskite solar cells, resulting in an efficiency below 14%. For the first time, a CsPbI2 Br perovskite is doped by Eu(Ac)3 to obtain a high-quality inorganic perovskite film with a low defect density and long carrier lifetime. A high efficiency of 15.25% (average efficiency of 14.88%), a respectable Voc of 1.25 V, a reasonable Jsc of 15.44 mA cm-2 , and a high FF of 79.00% are realized for CsPbI2 Br solar cells. Moreover, the CsPbI2 Br solar cells with Eu(Ac)3 doping demonstrate excellent air stability and maintain more than 80% of their initial power conversion efficiency (PCE) values after aging in air (relative humidity: 35-40%) for 30 days.

7.
Adv Sci (Weinh) ; 6(18): 1901241, 2019 Sep 18.
Artigo em Inglês | MEDLINE | ID: mdl-31559138

RESUMO

A high-quality perovskite photoactive layer plays a crucial role in determining the device performance. An additive engineering strategy is introduced by utilizing different concentrations of N,1-diiodoformamidine (DIFA) in the perovskite precursor solution to essentially achieve high-quality monolayer-like perovskite films with enhanced crystallinity, hydrophobic property, smooth surface, and grain size up to nearly 3 µm, leading to significantly reduced grain boundaries, trap densities, and thus diminished hysteresis in the resultant perovskite solar cells (PSCs). The optimized devices with 2% DIFA additive show the best device performance with a significantly enhanced power conversion efficiency (PCE) of 21.22%, as compared to the control devices with the highest PCE of 19.07%. 2% DIFA modified devices show better stability than the control ones. Overall, the introduction of DIFA additive is demonstrated to be a facile approach to obtain high-efficiency, hysteresis-less, and simultaneously stable PSCs.

8.
J Phys Chem Lett ; 10(19): 5687-5693, 2019 Oct 03.
Artigo em Inglês | MEDLINE | ID: mdl-31495169

RESUMO

Two-dimensional (2D) hybrid organic-inorganic metal halide perovskites (HOIPs) with considerably hydrophobic phenyl ethylammonium (PEA) organic cations have been used in highly efficient solar cells and LEDs, which are stable and enjoy a long lifetime, even when exposed to moisture. Different from other 2D HOIPs with alkyl amine cations, a benzene ring is present in the PEA cation. Until recently, an understanding of the effects of PEA on the structural, electronic, and optical properties of 2D HOIPs under pressure has remained limited. We find that there is a direct-indirect band gap transition at around 5.8 GPa and that the direct band gap recovers when the pressure is released. The stacking order of the benzene rings in the PEA cation plays a critical role in the mechanical and electronic properties. Our present work demonstrates that 2D HOIPs with organic cations containing benzene rings prove highly attractive for use in flexible optoelectronics.

9.
Adv Mater ; 31(42): e1903889, 2019 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-31475406

RESUMO

Layered Ruddlesden-Popper (RP) phase (2D) halide perovskites have attracted tremendous attention due to the wide tunability on their optoelectronic properties and excellent robustness in photovoltaic devices. However, charge extraction/transport and ultimate power conversion efficiency (PCE) in 2D perovskite solar cells (PSCs) are still limited by the non-eliminable quantum well effect. Here, a slow post-annealing (SPA) process is proposed for BA2 MA3 Pb4 I13 (n = 4) 2D PSCs by which a champion PCE of 17.26% is achieved with simultaneously enhanced open-circuit voltage, short-circuit current, and fill factor. Investigation with optical spectroscopy coupled with structural analyses indicates that enhanced crystal orientation and favorable alignment on the multiple perovskite phases (from the 2D phase near bottom to quasi-3D phase near top regions) is obtained with SPA treatment, which promotes carrier transport/extraction and suppresses Shockley-Read-Hall charge recombination in the solar cell. As far as it is known, the reported PCE is so far the highest efficiency in RP phase 2D PSCs based on butylamine (BA) spacers (n = 4). The SPA-processed devices exhibit a satisfactory stability with <4.5% degradation after 2000 h under N2 environment without encapsulation. The demonstrated process strategy offers a promising route to push forward the performance in 2D PSCs toward realistic photovoltaic applications.

10.
Adv Mater ; 31(44): e1903848, 2019 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-31523859

RESUMO

2D perovskites stabilized by alternating cations in the interlayer space (ACI) represent a very new entry as highly efficient semiconductors for solar cells approaching 15% power conversion efficiency (PCE). However, further improvements will require understanding of the nature of the films, e.g., the thickness distribution and charge-transfer characteristics of ACI quantum wells (QWs), which are currently unknown. Here, efficient control of the film quality of ACI 2D perovskite (GA)(MA)n Pbn I3 n +1 (〈n〉 = 3) QWs via incorporation of methylammonium chloride as an additive is demonstrated. The morphological and optoelectronic characterizations unambiguously demonstrate that the additive enables a larger grain size, a smoother surface, and a gradient distribution of QW thickness, which lead to enhanced photocurrent transport/extraction through efficient charge transfer between low-n and high-n QWs and suppressed nonradiative charge recombination. Therefore, the additive-treated ACI perovskite film delivers a champion PCE of 18.48%, far higher than the pristine one (15.79%) due to significant improvements in open-circuit voltage and fill factor. This PCE also stands as the highest value for all reported 2D perovskite solar cells based on the ACI, Ruddlesden-Popper, and Dion-Jacobson families. These findings establish the fundamental guidelines for the compositional control of 2D perovskites for efficient photovoltaics.

11.
Artigo em Inglês | MEDLINE | ID: mdl-31369195

RESUMO

In several photovoltaic (PV) technologies, the presence of electronic defects within the semiconductor band gap limit the efficiency, reproducibility, as well as lifetime. Metal halide perovskites (MHPs) have drawn great attention because of their excellent photovoltaic properties that can be achieved even without a very strict film-growth control processing. Much has been done theoretically in describing the different point defects in MHPs. Herein, we discuss the experimental challenges in thoroughly characterizing the defects in MHPs such as, experimental assignment of the type of defects, defects densities, and the energy positions within the band gap induced by these defects. The second topic of this Review is passivation strategies. Based on a literature survey, the different types of defects that are important to consider and need to be minimized are examined. A complete fundamental understanding of defect nature in MHPs is needed to further improve their optoelectronic functionalities.

12.
Adv Mater ; 31(50): e1902037, 2019 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-31304651

RESUMO

Metal halide perovskite solar cells (PVSCs) have revolutionized photovoltaics since the first prototype in 2009, and up to now the highest efficiency has soared to 24.2%, which is on par with commercial thin film cells and not far from monocrystalline silicon solar cells. Optimizing device performance and improving stability have always been the research highlight of PVSCs. Metal cations are introduced into perovskites to further optimize the quality, and this strategy is showing a vigorous development trend. Here, the progress of research into metal cations for PVSCs is discussed by focusing on the position of the cations in perovskites, the modulation of the film quality, and the influence on the photovoltaic performance. Metal cations are considered in the order of alkali cations, alkaline earth cations, then metal cations in the ds and d regions, and ultimately trivalent cations (p- and f-block metal cations) according to the periodic table of elements. Finally, this work is summarized and some relevant issues are discussed.

13.
J Phys Chem Lett ; 10(16): 4587-4595, 2019 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-31359754

RESUMO

All-inorganic perovskite materials emerge to be potential promising candidates for photoelectric applications. However, their instability to moisture has seriously limited future applications. It is imperative to develop new fabrication methods to make the perovskite films moisture-tolerant. In this work, it is demonstrated that both crystallinity and photoelectronic performance of the CsPbI3-xBrx (x < 1) perovskite were enhanced with the existence of excess CsBr and employing moisture treatment. An intermediate product of CsI1-yBry/CsPbI3-xBrx was obtained by using an extra amount of CsBr, and the structural evolution toward a uniform CsPbI3-zBrz layer (as the Br- incorporation, the mole ratio increases from x to z) was initiated by moisture treatment, forming new (PbX6)4- octahedra with the bonding of CsI1-yBry to Pb2+. Attributed to the homogeneity of the stoichiometry and crystallinity, the photovoltaic performance of the moisture-treated perovskite films was improved, with the open-circuit voltage increased from 0.97 to 1.10 V and the power conversion efficiency from 10.89 to 13.09%.

14.
J Phys Chem Lett ; 10(13): 3670-3675, 2019 Jul 05.
Artigo em Inglês | MEDLINE | ID: mdl-31203625

RESUMO

Two-dimensional (2D) perovskites have attracted much attention in research for solar cell applications because of their increased stability. The versatile structures of 2D perovskites enable fine-tuning of their optoelectronic properties. Newly reported Dion-Jacobson (DJ) perovskites have shown superior out-of-plane charge transport properties and better stability than the Ruddlesden-Popper (RP)-type perovskites because of their freedom from weak van der Waals interactions between adjacent layers. Tunable band gaps of 2D AMX4 can be achieved by alternatively substituting the corresponding compositions at A, M, and X sites, and significantly enhanced stability is observed because of the two hydrogen bonds formed at both ends of the divalent organic cation. Enhanced interlayer charge transport properties are found in DJ perovskites because of the short apical I-I distance in AMX4 perovskites, especially for PDAPbI4 and PDASnI4 perovskites. These findings provide us effective ways to tune the stability and optoelectronic properties of 2D perovskites.

15.
Adv Sci (Weinh) ; 6(7): 1801704, 2019 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-30989024

RESUMO

Up to now, multijunction cell design is the only successful way demonstrated to overcome the Shockley-Quiesser limit for single solar cells. Perovskite materials have been attracting ever-increasing attention owing to their large absorption coefficient, tunable bandgap, low cost, and easy fabrication process. With their rapidly increased power conversion efficiency, organic-inorganic metal halide perovskite-based solar cells have demonstrated themselves as the most promising candidates for next-generation photovoltaic applications. In fact, it is a dream come true for researchers to finally find a perfect top-cell candidate in tandem device design in commercially developed solar cells like single-crystalline silicon and CIGS cells used as the bottom component cells. Here, the recent progress of multijunction solar cells is reviewed, including perovskite/silicon, perovskite/CIGS, perovskite/perovskite, and perovskite/polymer multijunction cells. In addition, some perspectives on using these solar cells in emerging markets such as in portable devices, Internet of Things, etc., as well as an outlook for perovskite-based multijunction solar cells are discussed.

16.
Angew Chem Int Ed Engl ; 58(44): 15596-15618, 2019 Oct 28.
Artigo em Inglês | MEDLINE | ID: mdl-30861267

RESUMO

Recently, lead halide-based perovskites have become one of the hottest topics in photovoltaic research because of their excellent optoelectronic properties. Among them, organic-inorganic hybrid perovskite solar cells (PSCs) have made very rapid progress with their power conversion efficiency (PCE) now at 23.7 %. However, the intrinsically unstable nature of these materials, particularly to moisture and heat, may be a problem for their long-term stability. Replacing the fragile organic group with more robust inorganic Cs+ cations forms the cesium lead halide system (CsPbX3 , X is halide) as all-inorganic perovskites which are much more thermally stable and often more stable to other factors. From the first report in 2015 to now, the PCE of CsPbX3 -based PSCs has abruptly increased from 2.9 % to 17.1 % with much enhanced stability. In this Review, we summarize the field up to now, propose solutions in terms of development bottlenecks, and attempt to boost further research in CsPbX3 PSCs.

17.
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.

18.
Angew Chem Int Ed Engl ; 58(14): 4466-4483, 2019 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-30332522

RESUMO

Flexible perovskite solar cells have attracted widespread research effort because of their potential in portable electronics. The efficiency has exceeded 18 % owing to the high-quality perovskite film achieved by various low-temperature fabrication methods and matching of the interface and electrode materials. This Review focuses on recent progress in flexible perovskite solar cells concerning low-temperature fabrication methods to improve the properties of perovskite films, such as full coverage, uniform morphology, and good crystallinity; demonstrated interface layers used in flexible perovskite solar cells, considering key figures-of-merit such as high transmittance, high carrier mobility, suitable band gap, and easy fabrication via low-temperature methods; flexible transparent electrode materials developed to enhance the mechanical stability of the devices; mechanical and long-term environmental stability; an outlook of flexible perovskite solar cells in portable electronic devices; and perspectives of commercialization for flexible perovskite solar cells based on cost.

19.
ACS Appl Mater Interfaces ; 11(1): 634-639, 2019 Jan 09.
Artigo em Inglês | MEDLINE | ID: mdl-30560655

RESUMO

The development of Cu2ZnSn(S,Se)4 (CZTSSe) solar cells determines the prospect of thin-film photovoltaic devices because of some of their strengths. However, the usual solution fabrication processes of CZTSSe absorbing layers are either too tedious or highly toxic. Here, we have developed an alternative strategy to prepare kesterite CZTSSe absorber films with a simple and low-toxicity solution process by replacing the commonly employed thiol-based compounds using the glycolic acid aqueous solution, which significantly reduces the environment pollution and toxicity, providing a possibility toward the green solvent process. The power conversion efficiency of 6.81% has been acquired based the aqueous solution-processed CZTSSe thin film via optimizing the fabrication technology.

20.
Adv Sci (Weinh) ; 5(12): 1801123, 2018 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-30581708

RESUMO

Recently, inorganic CsPbI2Br perovskite is attracting ever-increasing attention for its outstanding optoelectronic properties and ambient phase stability. Here, an efficient CsPbI2Br perovskite solar cell (PSC) is developed by: 1) using a dimension-grading heterojunction based on a quantum dots (QDs)/bulk film structure, and 2) post-treatment of the CsPbI2Br QDs/film with organic iodine salt to form an ultrathin iodine-ion-enriched perovskite layer on the top of the perovskite film. It is found that the above procedures generate proper band edge bending for improved carrier collection, resulting in effectively decreased recombination loss and improved hole extraction efficiency. Meanwhile, the organic capping layer from the iodine salt also surrounds the QDs and tunes the surface chemistry for further improved charge transport at the interface. As a result, the champion device achieves long-term stabilized power conversion efficiency beyond 14%.

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