Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 80
Filtrar
Mais filtros










Base de dados
Intervalo de ano de publicação
1.
Artigo em Inglês | MEDLINE | ID: mdl-33146989

RESUMO

Although back-surface passivation plays an important role in high-efficiency photovoltaics, it has not yet been definitively demonstrated for CdTe. Here, we present a solution-based process, which achieves passivation and improved electrical performance when very small amounts of oxidized Al3+ species are deposited at the back surface of CdTe devices. The open circuit voltage (Voc) is increased and the fill factor (FF) and photoconversion efficiency (PCE) are optimized when the total amount added corresponds to ∼1 monolayer, suggesting that the passivation is surface specific. Addition of further Al3+ species, present in a sparse alumina-like layer, causes the FF and PCE to drop as the interface layer becomes blocking to current flow. The optimized deposit increases the average baseline PCE for both Cu-free devices and devices where Cu is present as a dopant. The greatest improvement is found when the Al3+ species are deposited prior to the CdCl2 activation step and Cu is employed. In this case, the best-cell efficiency was improved from 12.6 to 14.4%. Time-resolved photoluminescence measurements at the back surface and quantum efficiency measurements performed at the maximum power point indicate that the performance enhancement is due to a reduction in the interface recombination current at the back surface.

2.
J Am Chem Soc ; 2020 Aug 24.
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.

3.
J Chem Phys ; 152(6): 064705, 2020 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-32061228

RESUMO

Narrow bandgap mixed tin (Sn) + lead (Pb) perovskites are necessary for the bottom sub-cell absorber in high efficiency all-perovskite polycrystalline tandem solar cells. We report on the impact of mixed cation composition and atmospheric exposure of perovskite films on sub-gap absorption in films and performance of solar cells based on narrow bandgap mixed formamidinium (FA) + methylammonium (MA) and Sn + Pb halide perovskites, (FASnI3)x(MAPbI3)1-x. Structural and optical properties of 0.3 ≤ x ≤ 0.8 (FASnI3)x(MAPbI3)1-x perovskite thin film absorbers with bandgaps ranging from 1.25 eV (x = 0.6) to 1.34 eV (x = 0.3) are probed with and without atmospheric exposure. Urbach energy, which quantifies the amount of sub-gap absorption, is tracked for pristine perovskite films as a function of composition, with x = 0.6 and 0.3 demonstrating the lowest and highest Urbach energies of 23 meV and 36 meV, respectively. Films with x = 0.5 and 0.6 compositions show less degradation upon atmospheric exposure than higher or lower Sn-content films having greater sub-gap absorption. The corresponding solar cells based on the x = 0.6 absorber show the highest device performance. Despite having a low Urbach energy, higher Sn-content solar cells show reduced device performances as the amount of degradation via oxidation is the most substantial.

4.
Artigo em Inglês | MEDLINE | ID: mdl-32045195

RESUMO

The two-step solution-based process has demonstrated substantial success in fabricating high-efficiency perovskite solar cells in recent years. Despite the high performance, the underlying mechanisms that govern the formation of perovskite films and corresponding device performance are yet to be fully understood. Particularly, organic cation composition used in the two-step solution processing of mixed-cation lead halide perovskite solar cells plays a critical role in the perovskite film formation and the resultant device performance. However, little is understood about the impacts of organic cation composition on the current density-voltage (J-V) hysteretic behavior and stability of perovskite solar cells. To address this need, here, we study the effect of mixed organic cations, that is, the fraction of formamidinium (FA) and methylammonium (MA) contents, used for the two-step solution-processed perovskite thin films on solar cell performance, including efficiency, J-V hysteresis, and stability. In addition to the efficiency variations, we find that perovskite solar cells based on FA-rich and MA-rich stoichiometries show distinct characteristics in J-V hysteresis and stability. The origins of such a discrepancy are attributed to the thermodynamically driven conversion from lead iodide to perovskites, which is determined by the combination of organic cations. The perovskite solar cells based on the mixed cation FA0.6MA0.4PbI3 composition show a champion power conversion efficiency of over 21% and robust stability (retaining more than 90% of initial efficiency) under maximum power-point tracking in dry nitrogen for more than 500 h. Our work provides insights on understanding the formation of perovskite films in the two-step process, which may benefit further investigation on perovskite solar cells.

5.
J Phys Chem Lett ; 11(1): 121-128, 2020 Jan 02.
Artigo em Inglês | MEDLINE | ID: mdl-31820989

RESUMO

Temperature-dependent photoluminescence (PL) spectroscopy measurements have been performed over a range from 9 K to room temperature on polycrystalline methylammonium (MA)/formamidinium (FA) lead iodide (MA1-xFAxPbI3) perovskite thin films. Our low-temperature PL analysis reveals the existence of charge compensating defects in MAPbI3, which may explain the lower net free carrier concentration in MAPbI3 perovskite. More interestingly, we observe the suppression of the PL emission associated with the charged defects by appropriate FA inclusion. Furthermore, FA incorporation into MAPbI3 has been found to slow the phase transformation of MA1-xFAxPbI3 from orthorhombic to tetragonal phase, which occurs with increasing temperature. Our analyses of the FA concentration's impact on defect density and structural phase transformation provide beneficial insights that improve the understanding of the photovoltaic properties and application of organic-inorganic metal halide perovskites.

6.
Nat Commun ; 10(1): 5633, 2019 12 10.
Artigo em Inglês | MEDLINE | ID: mdl-31822670

RESUMO

The efficiencies of green and red perovskite light-emitting diodes (PeLEDs) have been increased close to their theoretical upper limit, while the efficiency of blue PeLEDs is lagging far behind. Here we report enhancing the efficiency of sky-blue PeLEDs by overcoming a major hurdle of low photoluminescence quantum efficiency in wide-bandgap perovskites. Blending phenylethylammonium chloride into cesium lead halide perovskites yields a mixture of two-dimensional and three-dimensional perovskites, which enhances photoluminescence quantum efficiency from 1.1% to 19.8%. Adding yttrium (III) chloride into the mixture further enhances photoluminescence quantum efficiency to 49.7%. Yttrium is found to incorporate into the three-dimensional perovskite grain, while it is still rich at grain boundaries and surfaces. The yttrium on grain surface increases the bandgap of grain shell, which confines the charge carriers inside grains for efficient radiative recombination. Record efficiencies of 11.0% and 4.8% were obtained in sky-blue and blue PeLEDs, respectively.

7.
J Phys Chem Lett ; 10(23): 7421-7425, 2019 Dec 05.
Artigo em Inglês | MEDLINE | ID: mdl-31735032

RESUMO

Dislocations are always observed during crystal growth, and it is usually desirable to reduce the dislocation density in high-quality crystals. Here, the annihilation process of the 30° Shockley partial dislocation pairs in CdTe is studied by first-principles calculations. We found that the dislocations can glide relatively easily due to the weak local bonding. Our systematic study of the slipping mechanism of the dislocations suggests that the energy barrier for the annihilation process is low. Band structure calculations reveal that the band bending caused by the charge transfer between the two dislocation cores depends on the core-core distance. A simple linear model is proposed to describe the mechanism of formation of the dislocation pair. More importantly, we demonstrate that hole injection can affect the core structure, increase the mobility, and eventually trigger a spontaneous mutual annihilation, which could be employed as a possible facile way to reduce the dislocation density.

8.
ACS Nano ; 13(10): 11800-11808, 2019 Oct 22.
Artigo em Inglês | MEDLINE | ID: mdl-31553178

RESUMO

Although Sn-Pb perovskites sensing near-ultraviolet-visible-near-infrared light could be an attractive alternative to silicon in photodiodes and imaging, there have been no clear studies on such devices constructed on metal/silicon substrates, hindering their direct integration with complementary metal-oxide semiconductor (CMOS) and silicon electronics. Typically, high surface roughness and severe pinholes of Sn-rich binary perovskites make it difficult for them to fulfill the requirements of efficient photodiodes and imaging. These issues cause inherently high dark current and poor (dark and photo-) current uniformity. Herein, we propose and demonstrate the room-temperature crystallization in the Sn-rich binary perovskite system to effectively control film crystallization kinetics. With experimental and theoretical studies of the crystallization mechanism, we successfully tune the density and location of nanocrystals in precursor films to achieve compact nanocrystals, which coalesce into high-quality (smooth, dense, and pinhole-free) perovskites with intensified preferred orientation and decreased trap density. The high-quality perovskites reduce dark current and improve (dark and photo-) current uniformity of perovskite photodiodes on CMOS-compatible metal/silicon substrates. Meanwhile, self-powered devices achieve a high responsivity of 0.2 A/W at 940 nm, a large dynamic range of 100 dB, and a fast fall time of 2.27 µs, exceeding those of most silicon-based imaging sensors. Finally, a 6 × 6 pixel integrated photodiode array is successfully demonstrated to realize the imaging application. The work contributes to understanding the fundamentals of the crystallization of Sn-rich binary perovskites and advancing perovskite integration with Si-based electronics.

9.
Angew Chem Int Ed Engl ; 58(39): 13717-13721, 2019 Sep 23.
Artigo em Inglês | MEDLINE | ID: mdl-31286608

RESUMO

Organic p-type semiconductors with tunable structures offer great opportunities for hybrid perovskite solar cells (PVSCs). We report herein two dithieno[3,2-b:2',3'-d]pyrrole (DTP) cored molecular semiconductors prepared through π-conjugation extension and an N-alkylation strategy. The as-prepared conjugated molecules exhibit a highest occupied molecular orbital (HOMO) level of -4.82 eV and a hole mobility up to 2.16×10-4  cm2 V-1 s-1 . Together with excellent film-forming and over 99 % photoluminescence quenching efficiency on perovskite, the DTP based semiconductors work efficiently as hole-transporting materials (HTMs) for n-i-p structured PVSCs. Their dopant-free MA0.7 FA0.3 PbI2.85 Br0.15 devices exhibit a power conversion efficiency over 20 %, representing one of the highest values for un-doped molecular HTMs based PVSCs. This work demonstrates the great potential of using a DTP core in designing efficient semiconductors for dopant-free PVSCs.

10.
Nanoscale ; 11(19): 9302-9309, 2019 May 16.
Artigo em Inglês | MEDLINE | ID: mdl-31062816

RESUMO

All-inorganic metal halide perovskites have attracted great interest in recent years due to their good device performance with higher thermal stability than that of their organic-inorganic perovskite counterparts. However, the all-inorganic perovskite polycrystalline films prepared by the conventional spin-coating method possess many pinholes, nonuniform surface with many small crystals, and irregular agglomerates, limiting their device performance. Herein, we introduced a monolayer nano-polystyrene (PS) sphere confined growth method for obtaining CsPbBr3 nanonet films (NFs) with ordered nanostructures grown in the preferred (110) orientation, which is beneficial for the charge carrier transport and the light-harvesting efficiency. The (110) peak intensity of CsPbBr3 NFs increased with the increase of the diameter of the monolayer sphere, while the (001) peak intensity was suppressed greatly, indicating the more preferred (110) oriented growth. The PDs based on (110)-orientation-preferred CsPbBr3 NFs prepared by using 850 nm PS spheres showed the best performance. The best performing device displayed the biggest linear dynamic range of up to 120 dB. In addition, a responsivity of 2.84 A W-1 and a detectivity of 5.47 × 1012 Jones were also achieved.

11.
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.

12.
Science ; 364(6439): 475-479, 2019 05 03.
Artigo em Inglês | MEDLINE | ID: mdl-31000592

RESUMO

All-perovskite-based polycrystalline thin-film tandem solar cells have the potential to deliver efficiencies of >30%. However, the performance of all-perovskite-based tandem devices has been limited by the lack of high-efficiency, low-band gap tin-lead (Sn-Pb) mixed-perovskite solar cells (PSCs). We found that the addition of guanidinium thiocyanate (GuaSCN) resulted in marked improvements in the structural and optoelectronic properties of Sn-Pb mixed, low-band gap (~1.25 electron volt) perovskite films. The films have defect densities that are lower by a factor of 10, leading to carrier lifetimes of greater than 1 microsecond and diffusion lengths of 2.5 micrometers. These improved properties enable our demonstration of >20% efficient low-band gap PSCs. When combined with wider-band gap PSCs, we achieve 25% efficient four-terminal and 23.1% efficient two-terminal all-perovskite-based polycrystalline thin-film tandem solar cells.

13.
Nat Commun ; 10(1): 665, 2019 02 08.
Artigo em Inglês | MEDLINE | ID: mdl-30737389

RESUMO

Quantum efficiencies of organic-inorganic hybrid lead halide perovskite light-emitting devices (LEDs) have increased significantly, but poor device operational stability still impedes their further development and application. All-inorganic perovskites show better stability than the hybrid counterparts, but the performance of their respective films used in LEDs is limited by the large perovskite grain sizes, which lowers the radiative recombination probability and results in grain boundary related trap states. We realize smooth and pinhole-free, small-grained inorganic perovskite films with improved photoluminescence quantum yield by introducing trifluoroacetate anions to effectively passivate surface defects and control the crystal growth. As a result, efficient green LEDs based on inorganic perovskite films achieve a high current efficiency of 32.0 cd A-1 corresponding to an external quantum efficiency of 10.5%. More importantly, our all-inorganic perovskite LEDs demonstrate a record operational lifetime, with a half-lifetime of over 250 h at an initial luminance of 100 cd m-2.

14.
J Am Chem Soc ; 141(8): 3515-3523, 2019 Feb 27.
Artigo em Inglês | MEDLINE | ID: mdl-30646682

RESUMO

Increasing the stability of perovskites is essential for their integration in commercial photovoltaic devices. Halide mixing is suggested as a powerful strategy toward stable perovskite materials. However, the stabilizing effect of the halides critically depends on their distribution in the mixed compound, a topic that is currently under intense debate. Here we successfully determine the exact location of the I and Cl anions in the  CH3NH3PbBr3- yI y and CH3NH3PbBr3- zCl z mixed halide perovskite lattices and correlate it with the enhanced stability we find for the latter. By combining scanning tunneling microscopy and density functional theory, we predict that, for low ratios, iodine and chlorine incorporation have different effects on the electronic properties and stability of the CH3NH3PbBr3 perovskite material. In addition, we determine the optimal Cl incorporation ratio for stability increase without detrimental band gap modification, providing an important direction for the fabrication of stable perovskite devices. The increased material stability induced by chlorine incorporation is verified by performing photoelectron spectroscopy on a half-cell device architecture. Our findings provide an answer to the current debate on halide incorporation and demonstrate their direct influence on device stability.

15.
J Phys Chem Lett ; 10(3): 501-506, 2019 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-30642179

RESUMO

Broadband emission is attributed to the formation of self-trapped excitons (STEs) due to the strong electron-phonon coupling. Interestingly, it has been observed in only certain three-dimensional and low-dimensional metal halide perovskites. Here, we show by density functional theory calculation that a low electronic dimensionality is a prerequisite for the formation of STE and, therefore, broadband emission. We further show that multiple STE structures exist in each perovskite exhibiting broadband emission. However, only the STE with Jahn-Teller-like octahedral distortion is mainly responsible for the observed broadband emission, though it may not be the lowest-energy structure. Our results provide important insights for designing perovskite materials for broadband emissions with preferred chromaticity coordinator or color temperature.

16.
Adv Mater ; 31(47): e1803792, 2019 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-30680809

RESUMO

Despite the exciting progress on power conversion efficiencies, the commercialization of the emerging lead (Pb) halide perovskite solar cell technology still faces significant challenges, one of which is the inclusion of toxic Pb. Searching for Pb-free perovskite solar cell absorbers is currently an attractive research direction. The approaches used for and the consequences of Pb replacement are reviewed herein. Reviews on the theoretical understanding of the electronic, optical, and defect properties of Pb and Pb-free halide perovskites and perovskite derivatives are provided, as well as the experimental results available in the literature. The theoretical understanding explains well why Pb halide perovskites exhibit superior photovoltaic properties, but Pb-free perovskites and perovskite derivatives do not.

17.
Nature ; 563(7732): 541-545, 2018 11.
Artigo em Inglês | MEDLINE | ID: mdl-30405238

RESUMO

Lighting accounts for one-fifth of global electricity consumption1. Single materials with efficient and stable white-light emission are ideal for lighting applications, but photon emission covering the entire visible spectrum is difficult to achieve using a single material. Metal halide perovskites have outstanding emission properties2,3; however, the best-performing materials of this type contain lead and have unsatisfactory stability. Here we report a lead-free double perovskite that exhibits efficient and stable white-light emission via self-trapped excitons that originate from the Jahn-Teller distortion of the AgCl6 octahedron in the excited state. By alloying sodium cations into Cs2AgInCl6, we break the dark transition (the inversion-symmetry-induced parity-forbidden transition) by manipulating the parity of the wavefunction of the self-trapped exciton and reduce the electronic dimensionality of the semiconductor4. This leads to an increase in photoluminescence efficiency by three orders of magnitude compared to pure Cs2AgInCl6. The optimally alloyed Cs2(Ag0.60Na0.40)InCl6 with 0.04 per cent bismuth doping emits warm-white light with 86 ± 5 per cent quantum efficiency and works for over 1,000 hours. We anticipate that these results will stimulate research on single-emitter-based white-light-emitting phosphors and diodes for next-generation lighting and display technologies.

18.
Nat Commun ; 9(1): 4981, 2018 11 26.
Artigo em Inglês | MEDLINE | ID: mdl-30478392

RESUMO

Identifying the origin of intrinsic instability for organic-inorganic halide perovskites (OIHPs) is crucial for their application in electronic devices, including solar cells, photodetectors, radiation detectors, and light-emitting diodes, as their efficiencies or sensitivities have already been demonstrated to be competitive with commercial available devices. Here we show that free charges in OIHPs, whether generated by incident light or by current-injection from electrodes, can reduce their stability, while efficient charge extraction effectively stabilizes the perovskite materials. The excess of both holes and electrons reduce the activation energy for ion migration within OIHPs, accelerating the degradation of OIHPs, while the excess holes and electrons facilitate the migration of cations or anions, respectively. OIHP solar cells capable of efficient charge-carrier extraction show improved light stability under regular operation conditions compared to an open-circuit condition where the photo-generated charges are confined in the perovskite layers.

19.
iScience ; 1: 55-71, 2018 Mar 23.
Artigo em Inglês | MEDLINE | ID: mdl-30227957

RESUMO

Electrodeposition (ED) technology is a low-cost industrial candidate for solar cell fabrication. However, the practical aspects of controlling deposit morphology and composition have not been significantly addressed because of the complex co-plating variables that still need to be understood for multinary alloy ED. This work addresses these practical aspects on how to control composition and deposit morphology using co-electrodeposited kesterite alloy precursors as a case study. The alloy precursors co-plated under the optimized conditions from a mixed thiosulfate-sulfite electrolyte bath show uniform, smooth, and compact film morphology as well as uniform distribution of composition, well suited for efficient kesterite absorbers, finally delivering a Cu2ZnSnS4 (CZTS) thin-film solar cell with 7.4% efficiency based on a configuration Mo/CZTS/CdS/ZnO/aluminum-doped ZnO. This work underscores that alloy ED, with the advantage of controllable composition and morphology, holds promise for low-cost industrial manufacture of thin-film solar cells.

20.
J Phys Chem Lett ; 9(16): 4714-4719, 2018 Aug 16.
Artigo em Inglês | MEDLINE | ID: mdl-30066567

RESUMO

Owing to their low trap-state density, high carrier mobility, and high thermal stability, CsPbBr3 perovskite microcrystals (MCs) have attracted significant attention for applications as photodetectors (PDs). However, solution synthesis processes lead to MC films with high void density, seriously limiting the performance of the PDs. Here, a pressure-assisted annealing strategy is introduced to significantly reduce the void density and decrease the surface roughness. The resulting self-powered all-inorganic CsPbBr3 perovskite MC thick-film PDs show improved performance characteristics, with responsivities and detectivities of up to 0.206 A W-1 and 7.23 × 1012 Jones, respectively. Moreover, the on/off ratios of the devices are up to 106, and the highest linear dynamic range reaches 123.5 dB. These improved results indicate that the pressure-assisted annealing method is an effective strategy to enhance the performance of solution-synthesized perovskite MC PDs.

SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA