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1.
J Am Chem Soc ; 145(51): 28156-28165, 2023 Dec 27.
Artigo em Inglês | MEDLINE | ID: mdl-38095593

RESUMO

Perovskite nanocrystals (PNCs) have attracted substantial attention due to their inspiring intrinsic merits such as low cost, high performance, and solution processability, but when it comes to the usage of blends of different colored PNCs with the purpose of covering the broadband spectrum field, the high degree of instability remains a major bottleneck. Herein, we report a family of dendritic ammonium ligands that act as stiff shell-encapsulating PNCs for improving their stability and suppressing ion permeability in mixed colloidal PNC solutions. The as-synthesized ligand-encapsulated PNCs notably achieve near-unity photoluminescence quantum yields (PLQYs) and strongly resist the unwanted ion exchange reaction under aggressive anion source attack. To fabricate self-powered white-emitting glass, the stabilized mixed colored PNCs were embedded into the laminated glass, which simultaneously acted as absorbers-emitters for luminescent solar concentrators (LSCs) and emitters for white light-emitting glass.

2.
Small ; 19(3): e2205976, 2023 01.
Artigo em Inglês | MEDLINE | ID: mdl-36408813

RESUMO

Highly sensitive broadband photodetectors are critical to numerous cutting-edge technologies such as biomedical imaging, environment monitoring, and night vision. Here, phototransistors based on mixed Sn/Pb perovskites are reported, which demonstrate ultrahigh responsivity, gain and specific detectivity in a broadband from ultraviolet to near-infrared region. The interface properties of the perovskite phototransistors are optimized by a special three-step cleaning-healing-cleaning treatment, leading to a high hole mobility in the channel. The highly sensitive performance of the mixed Sn/Pb perovskite phototransistors can be attributed to the vertical compositional heterojunction automatically formed during the film deposition, which is helpful for the separation of photocarriers thereby enhancing a photogating effect in the perovskite channel. This work demonstrates a convenient approach to achieving high-performance phototransistors through tuning compositional gradient in mixed-metal perovskite channels.


Assuntos
Chumbo , Estanho , Compostos de Cálcio , Monitoramento Ambiental
3.
Angew Chem Int Ed Engl ; 58(3): 806-810, 2019 Jan 14.
Artigo em Inglês | MEDLINE | ID: mdl-30499609

RESUMO

Tin-based perovskites with excellent optoelectronic properties and suitable band gaps are promising candidates for the preparation of efficient lead-free perovskite solar cells (PSCs). However, it is challenging to prepare highly stable and efficient tin-based PSCs because Sn2+ in perovskites can be easily oxidized to Sn4+ upon air exposure. Here we report the fabrication of air-stable FASnI3 solar cells by introducing hydroxybenzene sulfonic acid or its salt as an antioxidant additive into the perovskite precursor solution along with excess SnCl2 . The interaction between the sulfonate group and the Sn2+ ion enables the in situ encapsulation of the perovskite grains with a SnCl2 -additive complex layer, which results in greatly enhanced oxidation stability of the perovskite film. The corresponding PSCs are able to maintain 80 % of the efficiency over 500 h upon air exposure without encapsulation, which is over ten times longer than the best result reported previously. Our results suggest a possible strategy for the future design of efficient and stable tin-based PSCs.

4.
Adv Mater ; 35(6): e2207763, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36373546

RESUMO

Photodetectors (PDs) are the building block of various imaging and sensing applications. However, commercially available PDs based on crystalline inorganic semiconductors cannot meet the requirements of emerging wearable/implantable applications due to their rigidity and fragility, which creates the need for flexible devices. Here, a high-performance flexible PD is presented by gating an organic electrochemical transistor (OECT) with a perovskite solar cell. Due to the ultrahigh transconductance of the OECT, the device demonstrates a high gain of ≈106 , a fast response time of 67 µs and an ultrahigh detectivity of 6.7 × 1017 Jones to light signals under a low working voltage (≤0.6 V). Thanks to the ultrahigh sensitivity and fast response, the device can track photoplethysmogram signals and peripheral oxygen saturation under ambient light and even provide contactless remote sensing, offering a low-power and convenient way for continuous vital signs monitoring. This work offers a novel strategy for realizing high-performance flexible PDs that are promising for low-power, user-friendly and wearable optoelectronics.

5.
J Phys Chem Lett ; 14(8): 2047-2055, 2023 Mar 02.
Artigo em Inglês | MEDLINE | ID: mdl-36795606

RESUMO

Optical image encryption technology, in which the emission on/off can be controlled by using specially appointed wavelengths, is useful in information storage and protection. Herein, we report a family of sandwiched heterostructural nanosheets, consisting of three-layered (n = 3) perovskite (PSK) frameworks in center with two different polycyclic aromatic hydrocarbons [triphenylene (Tp) and pyrene (Py)] in periphery. Both heterostructural nanosheets (Tp-PSK and Py-PSK) exhibit blue emissions under UVA-I irradiation; however, different photoluminescent properties are observed under UVA-II. A bright emission of Tp-PSK is attributed to the fluorescence resonance energy transfer (FRET) from Tp-shield to PSK-core, whereas the observed photoquenching phenomenon in Py-PSK is due to the competitive absorption between Py-shield and PSK-core. We exploited the unique photophysical features (on/off emission) of the two nanosheets in a narrow UV window (320-340 nm) for optical image encrypting.

6.
Nat Commun ; 14(1): 3216, 2023 Jun 03.
Artigo em Inglês | MEDLINE | ID: mdl-37270581

RESUMO

Although the power conversion efficiency values of perovskite solar cells continue to be refreshed, it is still far from the theoretical Shockley-Queisser limit. Two major issues need to be addressed, including disorder crystallization of perovskite and unbalanced interface charge extraction, which limit further improvements in device efficiency. Herein, we develop a thermally polymerized additive as the polymer template in the perovskite film, which can form monolithic perovskite grain and a unique "Mortise-Tenon" structure after spin-coating hole-transport layer. Importantly, the suppressed non-radiative recombination and balanced interface charge extraction benefit from high-quality perovskite crystals and Mortise-Tenon structure, resulting in enhanced open-circuit voltage and fill-factor of the device. The PSCs achieve certified efficiency of 24.55% and maintain >95% initial efficiency over 1100 h in accordance with the ISOS-L-2 protocol, as well as excellent endurance according to the ISOS-D-3 accelerated aging test.

7.
Adv Sci (Weinh) ; 9(18): e2200242, 2022 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-35460202

RESUMO

2D-3D mixed tin halide perovskites are outstanding candidate materials for lead-free perovskite solar cells (PSCs) due to their improved stability and decreased trap density in comparison with their pure 3D counterparts. However, the mixture of multiple phases may lead to poor charge transfer across the films and limit the device efficiency. Here, a stacked quasi-2D (down)-3D (top) double-layered structure in perovskite films prepared via vacuum treatment is demonstrated, which can result in a planar bilayer heterojunction. In addition, it is found that the introduction of guanidinium thiocyanate (GuaSCN) additive can improve the crystallinity and carrier mobility in the 2D perovskite layer and passivate defects in the whole film, leading to a long carrier lifetime (>140 ns) in photoluminescence measurements. As a result, the PSCs show a high open circuit voltage (VOC ) up to 1.01 V with a voltage loss of only 0.39 V, which represents the record values ever reported for tin-based PSCs. The champion device exhibits a power conversion efficiency (PCE) of 13.79% with decent stability, retaining 90% of the initial PCE for 1200 h storage in N2 -filled glovebox.

8.
Adv Mater ; 34(6): e2107729, 2022 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-34676933

RESUMO

Sn-Pb mixed perovskites with bandgaps in the range of 1.1-1.4 eV are ideal candidates for single-junction solar cells to approach the Shockley-Queisser limit. However, the efficiency and stability of Sn-Pb mixed-perovskite solar cells (PSCs) still lag far behind those of Pb-based counterparts due to the easy oxidation of Sn2+ . Here, a reducing agent 4-hydrazinobenzoic acid is introduced as an additive along with SnF2 to suppress the oxidation of Sn2+ . Meanwhile, a vertical Pb/Sn compositional gradient is formed spontaneously after an antisolvent treatment due to different solubility and crystallization kinetics of Sn- and Pb-based perovskites and it can be finely tuned by controlling the antisolvent temperature. Because the band structure of a perovskite is dependent on its composition, graded vertical heterojunctions are constructed in the perovskite films with a compositional gradient, which can enhance photocarrier separation and suppress carrier recombination in the resultant PSCs. Under optimal fabrication conditions, the Sn-Pb mixed PSCs show power conversion efficiency up to 22% along with excellent stability during light soaking.

9.
Adv Sci (Weinh) ; 8(11): e2004315, 2021 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-34105283

RESUMO

Tin (Sn)-based perovskites with favorable optoelectronic properties and ideal bandgaps have emerged as promising alternatives to toxic lead (Pb)-based perovskites for photovoltaic applications. However, it is challenging to obtain high-quality Sn-based perovskite films by solution process. Here, liquid-exfoliated 2D transition-metal dichalcogenides (i.e., MoS2 , WS2 , and WSe2 ) with smooth and defect-free surfaces are applied as growth templates for spin-coated FASnI3 perovskite films, leading to van der Waals epitaxial growth of perovskite grains with a growth orientation along (100). The authors find that WSe2 has better energy alignment with FASnI3 than MoS2 and WS2 and results in a cascade band structure in resultant perovskite solar cells (PSCs), which can facilitate hole extraction and suppress interfacial charge recombination in the devices. The WSe2 -modified PSCs show a power conversion efficiency up to 10.47%, which is among the highest efficiency of FASnI3 -based PSCs. The appealing solution phase epitaxial growth of FASnI3 perovskite on 2D WSe2 flakes is expected to find broad applications in optoelectronic devices.

10.
Nat Commun ; 12(1): 4815, 2021 Aug 10.
Artigo em Inglês | MEDLINE | ID: mdl-34376697

RESUMO

Graded bulk-heterojunction (G-BHJ) with well-defined vertical phase separation has potential to surpass classical BHJ in organic solar cells (OSCs). In this work, an effective G-BHJ strategy via nonhalogenated solvent sequential deposition is demonstrated using nonfullerene acceptor (NFA) OSCs. Spin-coated G-BHJ OSCs deliver an outstanding 17.48% power conversion efficiency (PCE). Depth-profiling X-ray photoelectron spectroscopy (DP-XPS) and angle-dependent grazing incidence X-ray diffraction (GI-XRD) techniques enable the visualization of polymer/NFA composition and crystallinity gradient distributions, which benefit charge transport, and enable outstanding thick OSC PCEs (16.25% for 300 nm, 14.37% for 500 nm), which are among the highest reported. Moreover, the nonhalogenated solvent enabled G-BHJ OSC via open-air blade coating and achieved a record 16.77% PCE. The blade-coated G-BHJ has drastically different D-A crystallization kinetics, which suppresses the excessive aggregation induced unfavorable phase separation in BHJ. All these make G-BHJ a feasible and promising strategy towards highly efficient, eco- and manufacture friendly OSCs.

11.
Light Sci Appl ; 10(1): 68, 2021 Mar 31.
Artigo em Inglês | MEDLINE | ID: mdl-33790230

RESUMO

Grain boundaries in organic-inorganic halide perovskite solar cells (PSCs) have been found to be detrimental to the photovoltaic performance of devices. Here, we develop a unique approach to overcome this problem by modifying the edges of perovskite grain boundaries with flakes of high-mobility two-dimensional (2D) materials via a convenient solution process. A synergistic effect between the 2D flakes and perovskite grain boundaries is observed for the first time, which can significantly enhance the performance of PSCs. We find that the 2D flakes can conduct holes from the grain boundaries to the hole transport layers in PSCs, thereby making hole channels in the grain boundaries of the devices. Hence, 2D flakes with high carrier mobilities and short distances to grain boundaries can induce a more pronounced performance enhancement of the devices. This work presents a cost-effective strategy for improving the performance of PSCs by using high-mobility 2D materials.

12.
Adv Sci (Weinh) ; 7(14): 2000776, 2020 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-32714769

RESUMO

2D Ruddlesden-Popper perovskites have attracted wide attention recently because of tunable optoelectronic properties and have been used as alternatives to their 3D counterparts in various optoelectronic devices. Here, a series of (PEA)2(MA) n -1Pb n I3 n +1 perovskite thin films is designed and fabricated by a convenient hot-casting method to obtain gradient n in the films, which leads to the formation of vertical heterojunctions that can enhance charge separation in the films under light illumination. Based on a single gradient perovskite film, a highly sensitive and stable photodetector with a responsivity up to 149 AW-1 and a specific detectivity of 2 × 1012 Jones is obtained. This work paves a way to realizing high-performance optoelectronic devices with enhanced charge separation by introducing compositional gradient in a perovskite film.

13.
Adv Mater ; 31(24): e1807689, 2019 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-31033074

RESUMO

The quality of perovskite films is critical to the performance of perovskite solar cells. However, it is challenging to control the crystallinity and orientation of solution-processed perovskite films. Here, solution-phase van der Waals epitaxy growth of MAPbI3 perovskite films on MoS2 flakes is reported. Under transmission electron microscopy, in-plane coupling between the perovskite and the MoS2 crystal lattices is observed, leading to perovskite films with larger grain size, lower trap density, and preferential growth orientation along (110) normal to the MoS2 surface. In perovskite solar cells, when perovskite active layers are grown on MoS2 flakes coated on hole-transport layers, the power conversion efficiency is substantially enhanced for 15%, relatively, due to the increased crystallinity of the perovskite layer and the improved hole extraction and transfer rate at the interface. This work paves a way for preparing high-performance perovskite solar cells and other optoelectronic devices by introducing 2D materials as interfacial layers.

14.
J Colloid Interface Sci ; 498: 223-228, 2017 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-28334660

RESUMO

The present study reports a new type of quantum dot sensitized solar cells (QDSSCs) using the zinc tin mixed metal oxides (MMO) as the anode materials, which were obtained from the layered double hydroxide (LDH) precursor. The successive ionic layer adsorption and reaction (SILAR) method is applied to deposit CdS quantum dots. The effects of sensitizing cycles on the performance of CdS QDSSC are studied. Scanning electron microscopy (SEM), Transmission electron microscope (TEM) and X-ray diffraction (XRD) are used to identify the surface profile and crystal structure of the mixed metal oxides anode. The photovoltaic performance of the QDSSC is studied by the electrochemical method. The new CdS QDSSC exhibits power conversion efficiency (PCE) up to 0.48% when the anode was sensitized for eight cycles.

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