Low-Dimensional Halide Perovskites and Their Advanced Optoelectronic Applications
Abstract
Metal halide perovskites are crystalline materials originally developed out of scientific curiosity. They have shown great potential as active materials in optoelectronic applications. In the last 6 years, their certified photovoltaic efficiencies have reached 22.1%. Compared to bulk halide perovskites, low-dimensional ones exhibited novel physical properties. The photoluminescence quantum yields of perovskite quantum dots are close to 100%. The external quantum efficiencies and current efficiencies of perovskite quantum dot light-emitting diodes have reached 8% and 43 cd A−1, respectively, and their nanowire lasers show ultralow-threshold room-temperature lasing with emission tunability and ease of synthesis. Perovskite nanowire photodetectors reached a responsivity of 10 A W−1 and a specific normalized detectivity of the order of 1012 Jones. Different from most reported reviews focusing on photovoltaic applications, we summarize the rapid progress in the study of low-dimensional perovskite materials, as well as their promising applications in optoelectronic devices. In particular, we review the wide tunability of fabrication methods and the state-of-the-art research outputs of low-dimensional perovskite optoelectronic devices. Finally, the anticipated challenges and potential for this exciting research are proposed.
Keywords
Metal halide perovskites Low-dimensional effect Synthesis Optoelectronic devices Versatility1 Introduction
Low-dimensional materials are nanocrystals with at least one dimension within the nanoscale range (1–100 nm). For the last few decades, they have been increasingly attracting interest as they exhibit unique properties. They are also referred to as artificial atoms because the density of their electronic states can be widely and easily tuned by adjusting the crystal composition, size, shape, and so on. A typical example of the effect of size on crystal properties is quantum dots (QDs), whose three dimensions are all in the nanoscale range. The bandgaps could be easily tuned by adjusting the dot size [1]. A variety of optoelectronic applications have been explored for low-dimensional perovskites such as photovoltaics, light sensors, light-emitting diodes (LEDs), owing to the strong light–matter interaction [2]. Unlike traditional semiconductor nanomaterials, low-dimensional halide perovskites can be prepared at low cost and by solution-processable techniques. They have demonstrated superior optical, magnetic, dielectric, electrical, and optoelectronic properties [3, 4, 5] and have been becoming a hot research topic in new semiconductor materials and optoelectronic devices.
Perovskite structure and solar cell efficiencies. a Perovskites possess the general crystal structure ABX3. The most prevalent perovskite in optoelectronic devices is MA lead trihalide, for which A = CH3NH3, B = Pb, and X = Cl, Br or I. b Best research cell efficiencies.
Adapted image reproduced from NREL [6]
In the 1990s, Mitzi [11] focused on layered organic–inorganic halide perovskites that featured strong excitonic characteristics and demonstrated applications in thin-film transistors and LEDs. After Miyasaka et al.’s pioneered work in sensitized solar cells, the hybrid perovskite began its debut in photovoltaics in 2006 [12]. In 2009, a power conversion efficiency (PCE) of 3.8% was achieved by replacing Br with I [13]. In 2011, Park and coworkers achieved an efficiency of 6.5% by employing perovskite QDs as the sensitizers [14]. Later, Snaith et al. reported an efficiency of 10.9% utilizing solid electrolyte as a hole transport layer (HTL) [15]. As the study progressed, the superior properties of perovskites unfolded. Ambipolar carrier transport enlightened and promised the intensive employment of planar heterojunction devices [16, 17, 18]. This sparked an enormous development in the hybrid lead perovskite solar cells, which obtained a record PCE up to 22.1% in just 6 years using a low-cost solution method (Fig. 1b). In addition to PV applications, low-dimensional perovskite crystals with specific morphologies and ultrasmall size evoked new research interest in optoelectronic applications.
Compared with the hot research into halide perovskite thin-film solar cells, the low-dimensional perovskites hold great potential and just open a small angle. Thus, the present review mainly focuses on low-dimensional halide perovskite to summarize their synthesis methods, optoelectronic applications, and development outlook. By analogy to the human lifetime, the present stage of research into low-dimensional halide perovskites is just in its infancy. The high quantum yield, narrow full-width-at-half-maximum (FWHM), and tunable emission color of low-dimensional perovskite materials make them bright prospects for novel optoelectronic devices. A variety of monochromatic LEDs have been fabricated at room temperature utilizing inorganic cesium lead halide perovskite QDs as the color conversion layer, which have exhibited the best perovskite LED performance so far. Simultaneously, a hybrid perovskite nanowire photodetector (PD) with a photoconductive gain approaching 1014 electrons per photon and a responsivity approaching 6.0 × 105 A W−1 has been developed. Single-crystal lead halide perovskite nanowire lasers exhibited ultralow lasing thresholds (220 nJ cm−2) and high quality factors (Q ∼ 3600) at a charge carrier density of ~1.5 × 1016 cm−3. As hybrid perovskite researchers investigate more deeply, many amazing properties are expected to be uncovered beyond photovoltaics.
In this review, we present a thorough treatment of the recent developments in the fundamental material properties of low-dimensional perovskites (QDs, nanowires, and nanosheets). We mainly focus on the synthesis, unique properties, and notable breakthroughs of perovskites, with optoelectronic applications in photovoltaics, LEDs, PDs, and lasers. Finally, the near-future challenges and the potential directions of this exciting research area are forecasted.
2 Crystal Structure and Tunability of Halide Perovskite
Perovskites, with general formula AMX3, are a well-known class of inorganic materials with widespread deployment in ferro- and piezoelectric, magnetoresistive, semiconducting, and catalysis applications. The rich diversity is attainable owing to the multitude of large bivalent cations occupying the A-site (e.g., Ca2+, Sr2+, Ba2+), the smaller tetravalent cations (e.g., Ti4+, Zr4+) at the M site, and oxygen anions located at the X-site. Halide perovskites are different from their classical chalcogenide counterparts with monovalent moieties introduced at the A-site, divalent metal cations at the M site, and typically halides at the X-site. The AMX3 hybrid perovskite structure is formed by a three-dimensional (3D) network, with A-site cations occupying the cavity between four adjacent corner-sharing MX6 metal halide octahedra (e.g., M = Pb2+, Sn2+, Ge2+, Cu2+, Eu2+, Co2+ and X = Cl−, Br−, I−). The probability of forming the perovskite structure can be estimated using the Goldschmidt tolerance factor (t) and the octahedral factor (µ) [12, 19, 20]. Here, t is based on the ionic radii (r) of the A, M, and X, constituenting in \(t = \left( {r_{A} + r_{X} } \right)/\sqrt 2 \cdot \left( {r_{M} + r_{X} } \right)\), and µ is defined as r M/r X . According to the tolerance factor, only the incorporation of small cations results in perovskite formation (t ~ 1) because it is empirically found that cubic perovskites can form from 0.80 < t < 0.90 and 0.40 < µ < 0.90 [12, 20, 21, 22]. This implies that the large ionic radii of Pb (1.19 Å) and the halides (e.g., iodide 2.20 Å) limit the ionic radius of the monovalent A cation to 2.9 Å. Therefore, only two or three C–C or C–N bonds or inorganic cations such as Cs+ (1.88 Å) are expected to fit in the 3D hybrid perovskite structure [22].
One of the major advantages over traditional inorganic oxide is the low energy barrier to halide perovskite formation. A crystalline phase can be readily obtained by merely mixing and grinding the precursor salts at room temperature. Although this method suffers from a lack of precise experimental control, it exemplifies the ease with which the cations can diffuse into the inorganic framework. Typically, halide perovskites are synthesized via wet-chemistry routes, allowing mixing at a molecular level, and resulting in materials with a pure phase. By carefully controlling the reaction conditions (e.g., temperature, solvent, ligands), halide perovskites of various morphologies (0D to 3D) and sizes (ranging over six orders of magnitude) can be prepared. For example, CH3NH3PbBr3 single crystals with a size of 5 × 5 × 2 mm3 are obtained within a growth period of several hours by exploiting its lower solubility in solvents at elevated temperatures [23]. CH3NH3PbBr3 nanoparticles (NPs) [24, 25, 26, 27], layered sheets [28, 29], and nanowires (NWs) [30, 31] could be prepared via tuning the synthesis strategy.
These examples briefly demonstrated the robust synthesis processes with which a wide scale of nanostructured perovskites can be synthesized. In recent years, nanomaterials have become more and more interesting, as the novel physical properties are only observed at the nanoscale range, in contrast to their larger-scale counterparts. Fine control over synthesis conditions (precursor concentration, reaction temperature, choice of ligands, etc.) could introduce new physical properties, such as quantum size effects [32] or anisotropic growth [33], to fulfill future application requirements.
3 Synthesis and Fundamental Properties of Low-Dimensional Halide Perovskites
3.1 Quantum Dots
QDs, combining unique optical and electrical properties and solution-processed advantages, have been studied intensively for decades. Here, we will cover the evolution of halide perovskite QDs and devices for light-emission applications. We will disclose the physical and chemical characteristics and analyze the rich diversity in composition and structure.
The PLQY of QDs was gradually optimized by reaction and ligand selection. Utilizing long-chain ammonium bromide ligands, colloidal CH3NH3PbX3 cubic NPs (~6 nm) produced using the LARP method [28] exhibited bright-green PL emission at 527 nm, with a PLQY of approximately 20%. The increased reaction temperatures (~120 °C) yielding equal quantum efficiencies and PL emission wavelengths [42] showcased the rigidity and high reproducibility of the above method. The synthesis was further optimized by increasing the organic/inorganic precursor ratios. This could narrow the PL emission (FWHM = 30 nm at 520 nm) and significantly improve PLQY values to a new record of 83% [25]. Quantization effects were observed for 1.8- to 3.6-nm-sized CH3NH3PbBr3 NPs [27, 43]. The highest PLQY ~93% was recorded from the supernatant phase of centrifugation [25, 28].
Despite the high PLQY and colloidal stability of methylammonium halide NPs (>5 months of storage in air under dark conditions [25]), a major shortcoming arises from its instability in polar solvents. To overcome this limit, Vybronyi et al. synthesized CH3NH3PbX3 NPs without using polar solvents [44]. Although the precipitate displayed lower quantum efficiencies (25–50%) than previously reported CH3NH3PbBr3 NPs, it demonstrates an alternative synthesis route without the use of polar solvents. Other approaches involved the formation of PbS/CH3NH3PbX3 core–shell NPs via ligand-exchange reactions [45, 46]. Light emission associated with PbS/CdS NPs and PbS/CH3NH3PbI3−x Cl x core–shell NPs has also been reported [47].
Colloidal CsPbX3 perovskite NCs (X = Cl, Br, I) exhibit size- and composition-tunable bandgaps covering the entire visible spectral region with narrow and bright emission: a Colloidal solutions in toluene under UV lamp (λ = 365 nm) excitation. b Representative PL spectra. c Typical optical absorption and PL spectra. d Time-resolved PL decays for all samples shown in c except CsPbCl3.
Adapted image reproduced with permission of Ref. [37]
3.2 Nanowires
The high absorption coefficient enables it as an amazing absorber, which was first applied in dye-sensitized solar cells (DSSCs) to replace organic dye by Kojima et al. [13], Horvath et al. [49]. The further investigation shows that they not only play the role of the light absorbers, but also can be viewed both as electron- and hole-transporting media, owing to their ambipolar charge transport character [50]. In perovskite film synthesis, a nonporous homogenous perovskite film must be deposited in order to avoid shunting in planar devices. However, films produced by conventional spin coating methods were found to be comprised of large CH3NH3PbI3 microwhiskers and many uncovered void areas [51]. Dendrite crystal growth implies that organolead iodide perovskite (OIP) exhibits preferential growth. Inspired by that phenomenon, the synthesis of OIP nanowires (NWs) was investigated and implemented in our group [52]. In addition to our work, Swiss scientists Endre Horvá et al. pioneered the synthesis of OIP NWs by a simple slip coating method during a similar period [53]. The above two works opened the new research fields of halide perovskite NWs. The key synthesis methods and novel properties are summarized in chronological order.
3.2.1 One-Step Evaporation-Induced Self-Assembly (EISA) Growth
For the one-step method, the precursor solution (MAI and PbI2 in DMF) was cast on substrates, and then, the evaporation of the solvent resulted in supersaturated crystal growth with the c-axis parallel to the surface at room temperature [54]. The low symmetry (tetragonal I4/mcm) of OIP and strong intermolecular interactions may allow a preferred growth into NW morphology [55, 56]. For a high substrate temperature (>120 °C), it tended to grow homogeneously into NPs and suppress the preferential growth. Subsequent thermal annealing (~80 °C) can help to convert the NWs precursor into perovskite NWs.
One-step growth of perovskite NWs. a, b Slip coating fabrication process of filiform halide perovskite and their optical image. c, f Roll-to-roll printing for perovskite NWs thin film. d EISA method to fabricate aligned perovskite NWs. e Selective area deposition of perovskite NWs. g SEM image of NWs webs. f Transmittance spectra of NWs webs evolved with the precursor concentrations. Inset shows a photograph of semitransparent NWs networks from 30 wt% concentration. h Transmittance evolved with OTP precusor concentrations. i, j Full-inorganic CsPbBr3 NWs synthesized by one-step method and their typical optical absorption and PL spectra (j).
Adapted image reproduced with permission of Ref. [49, 52, 57, 58, 59]
Our further work created a network-like NW web, which could satisfy the cross-linking and uniform NW distribution requirements to overcome the obstacles to NW applications [52]. In contrast to our previous drop-casting style, we adopt a spin coating method with suitable rotary speed and an annealing technique to obtain perovskite NW webs (Fig. 4g). All the NWs welded to each other without opening the end. The transparency of NWs webs could be facilely tuned by the precursor concentrations (Fig. 4h). The low-temperature fabrication process and web geometry promise high application potential in transparent and flexible optoelectronics. The usual one-step growth methods often achieve large diameter NWs over 200 nm. Yang and coworkers added a surfactant solvent into the precursor to tune the NW crystallization kinetics [59] (Fig. 4i).
The application of low-dimensional NWs needs large-scale growth to meet the wide application fields. The blade coating method enables the synthesis of aligned single-crystalline OIP microwire (MW) arrays in terms of high yield and wafer size capability. Thus, Jie et al. first applied the doctor blade coating technique for large-scale and aligned NW growth [60]. It is well known that the highest efficiency deposition technique is printing. The low deposition temperature and one-step solution method promise potential applicability by printing methods. Recently, Yang et al. developed a large-scale roll-to-roll microgravure printing technique for perovskite NWs synthesis [61] (Fig. 4f). By systematic deposition recipe optimization, perovskite NW thin film was deposited on PET substrates (Fig. 4c).
3.2.2 Two-Step Method Growth
Two-step method for perovskite NW growth. a SEM images of vertically aligned CsPbBr3 NWs with a rectangular cross section. b HRTEM and FFT images of a CsPbBr3 NWs. c Fluorescence decay kinetics of MAPbI3 NWs. d Conductivity improvement in the in-plane perovskite NWs. e SEM image of CH3NH3PbBr3 nanorod array. f, g Typical absorption and PL spectra of CH3NH3PbBr3 nanorod arrays.
Similarly, Yang’s group replaced the second spin coating step with immersion in CH3NH3Br IPA solution [30]. The lead acetate substrate could support vertical perovskite nanorod arrays (Fig. 5e). The NW absorption onset was at approximately 530 nm with a bandgap of 2.3 eV [64] (Fig. 5f). The room-temperature PL of the CH3NH3PbBr3 NWs peaked at 534 nm with a narrow FWHM of 26 nm under 325-nm HeCd laser excitation (Fig. 5g). The temperature-dependent phases of the CH3NH3PbBr3 NWs underwent multiple phase transitions at 236.3 (to a tetragonal phase), 154.0 (to another tetragonal phase), and 148.8 K (to an orthorhombic phase), which may account for the observed redshift [65]. In comparison with bulk crystal PL, the CH3NH3PbBr3 nanorod arrays had a 13% contribution of the fast component to the steady-state PL, which indicated the high quality of the single-crystalline nanorods.
3.2.3 Chemical Vapor Transport (CVT) Method
This instrument is the same as a tube furnace for traditional chemical vapor deposition [66]. The reaction sources of PbX2 and CsX (X = Cl, Br, or I) powders were placed inside a quartz tube reactor [66]. The Si substrate was positioned at a distance from the source. The temperatures of the powder sources and Si substrate were set at 570–600 and 350–380 °C, respectively. The inert carrier gas was utilized to transport the source vapor for deposition on the Si substrate (Fig. 5a, b). Apart from the above-mentioned research, Yi-bing Cheng et al. also utilized the CVT method to synthesize perovskite MWs [67].
3.2.4 Template Method
Template method for perovskite NWs: Pb-containing precursor template a method for perovskite NWs (b, c). AAO template for perovskite NWs. d Photograph of a ~9 × 9 cm2 NW arrays. e Cross-sectional SEM images of perovskite NWs. Scale bar is 500 nm. f Average τ c for different diameter NWs. g Extension of carrier lifetime as the decrease in NW diameter. h, i Nanofluidic channel template growth.
Adapted image reproduced with permission of Ref. [68, 70, 71]
The traditional universal templates, anodized aluminum oxide (AAO) templates, were also applied for the synthesis of perovskite NWs [70]. Oriented cylindrical nanopores constructed the uniform vertical perovskite nanowire array templates. This method combined the AAO template and perovskite one-step solution method. Perovskite precursor DMF solution filled into the pores of AAO. The following thermal annealing led to perovskite recrystallization and NW formation at the bottoms of the pores (Fig. 6d, e). The advantage of the present AAO template method is the fine-tuning of the NW dimensions (diameter and length) by controlling the AAO anodizing recipes [66, 72, 73, 74].
Different from the vertical templates, traditional planar electronic fabrication techniques such as photolithography, electron beam lithography could help to fabricate the 1D channel as the planar growth template. The perovskite NWs were fabricated with the assistance of open nanofluidic channel templates [30] (Fig. 6h, i). The synthesis could be guided and visualized in real time and underwent a metastable solvatomorph formation in polar aprotic solvents. The superior advantages were the precise controlling of sizes, cross-sectional shapes, aspect ratios, and orientations, which had not been achieved by other deposition methods.
3.3 Two-Dimensional Perovskite
Two-dimensional (2D) perovskites such as nanosheets, nanoplatelets, and microdisks (MDs) have recently shown high PLQY [75, 76, 77]. These 2D perovskites are promising candidates for a variety of applications in nanoelectronics, nanophotonics, and photovoltaics [32, 78]. For instance, Zhao and Zhu [79] prepared MAPbI2Br nanosheets with a 1.8-eV bandgap through a thermal decomposition process from a precursor containing PbI2, MABr, and MACl. The planar solar cells based on the compact layer of MAPbI2Br nanosheets achieved a PCE of ~10%.
a Single-crystalline organometal halide perovskite nanoplatelets were synthesized by a one-pot method. Inset is the photograph of the achieved colloidal perovskite nanoplatelet solution. b TEM images and selected area diffraction pattern of MAPbBr3 nanoplatelets. c X-ray diffraction of MAPbBr3 nanoplatelet film. d PL spectra of MAPbBr3 nanoplatelets in toluene solution and solid state. Inset, the optical images of MAPbBr3 nanoplatelets in toluene solution and in solid-state thin film under ambient light (left) and UV irradiation (right). e Schematic drawing of the nanoplatelet synthesis setup using a home-built vapor transport system.
Adapted image reproduced with permission of Ref. [76]
Chemical vapor-deposited methylammonium lead halide perovskite nanoplatelets. a Schematic figure of crystal structures of CH3NH3PbI3−a X a (X = I, Br, Cl). Morphological and electronic band edge characterizations of CH3NH3PbI3 (b), CH3NH3PbI3−a Br a (c), and CH3NH3PbI3−a Cl a (d) nanoplatelets.
Adapted image reproduced with permission of Ref. [24]
Recently, Liao et al. [81] fabricated single-crystalline CH3NH3PbBr3 square MDs-based microlasers by using a one-step solution self-assembly method. That approach was similar to anti-solvent vapor-assisted crystallization method [82]. The obtained square MDs had smooth outer surfaces and sharp edges and displayed an absorption peak at 535 nm and an emission peak at 545 nm. Their four side faces constituted a built-in whispering-gallery mode microresonator with a quality factor as high as 430. By partial replacement of Br with Cl, the lasing wavelength can be effectively tuned in the green-light range from 525 to 557 nm.
Reaction temperature influence on colloidal CsPbBr3 synthesis. 8- to 10-nm nanocubes were formed at 150 °C (a), 20-nm nanoplates from 130 °C (b) reaction and 90 °C, c reaction yielded several hundred nanometer scale lamellar nanostructures. Scale bar is 50 nm. d Absorption (solid lines) and emission (dashed lines) spectra of NPLs and nanocubes for comparison. e Colloidal solution of anion-exchanged NPLs in hexane under UV illumination (λ = 365 nm). f Inorganic perovskite PL peaks evolved with their anions.
Adapted image reproduced with permission of Ref. [75]
It is interesting to note that perovskite nanosheets were surprisingly obtained from electrospraying the precursor solution into a mixed bath of toluene (as anti-solvent) and oleylamine (for intercalation) [88]. Recently, single crystals of OIP nanoplates with well-defined facets were grown via a dissolution–recrystallization path from PbI2 (or PbAc2) films [89]. These 2D perovskite nanostructures displayed strong room-temperature PL and long carrier lifetime.
4 Low-Dimensional Perovskite Optoelectronic Applications
4.1 Light-Emitting Diodes
a–c Emissions of QLED devices utilizing different QD sizes. d The EL (solid line) and the PL spectra (dashed line) of samples shown in (a–c). e CIE coordinates of the three color QLEDs (circular) compared to the NTSC color standards (star).
Adapted image reproduced with permission of Ref. [90]
Device characteristics of visible PeLEDs. a Absorption (black), normalized EL (solid line in green), and PL (dashed line in green) spectra of CH3NH3PbBr3 perovskite. EL spectrum of mixed halide perovskite is shown in red. b Luminance (black) and current density (red) versus voltage characteristics of the green PeLED. c EQE versus voltage characteristics of the green PeLED. d EQE versus current density of the green PeLED.
Adapted image reproduced with permission of Ref. [96]. (Color figure online)
Illustration of multilayer PeLED device. a Device structure. b Cross-sectional TEM image of multiple layers with distinct contrast. Scale bar is 50 nm. c Flat-band energy level diagram.
Adapted image reproduced with permission of Ref. [90]
Perovskite emitter | Morphology | Device architecture | EQE (%) | CE (cd A2) | Lmax (cd m−2) | Vr (V) | Publication date (month-year) |
---|---|---|---|---|---|---|---|
CH3NH3PbBr3 | Thin film | ITO/PEDOT:PSS/Pe/F8/Ca/Ag | 0.1 | 0.3 | 364 | 3.3 | 08-2014 |
CH3NH3PbBr3 | Thin film | ITO/Buf HIL/Pe/TPBI/LiF/Al | 0.125 | 0.57 | 417 | ~4 | 11-2014 |
CH3NH3PbBr3 | Thin film | ITO/PEDOT:PSS/TPD/Pe/Ag | 6.5 × 10−3 | ~1.8 × 10−2 | 21 | 4 | 01-2015 |
CH3NH3Pb3−x Br x | Thin film | ITO/PEDOT:PSS/TPD/Pe/Ag | 1.1 × 10−3 | n.r | n.r | n.r | 01-2015 |
CH3NH3PbBr3 | Thin film | ITO/PEDOT:PSS/Pe/ZnO/Ca/Ag | n.r. | ~21 | ~550 | 2 | 02-2015 |
CH3NH3PbBr3 | Thin film | ITO/PEDOT:PSS/Pe-PIP/F8/Ca/Ag | 1.2 | n.r | 200 | n.r | 04-2015 |
CH3NH3PbBr3 | Thin film | ITO/ZnO-PEI/Pe/TFB/MoO x /Au | 0.8 | n.r | 20,000 | 2.8 | 04-2015 |
CH3NH3Pb3−x Cl x (red) | Thin film | ITO/ZnO-PEI/Pe/TFB/MoO x /Au | 3.5 | n.r | n.r | 2.2 | 05-2015 |
CH3NH3Pb3−x Cl x (red) | Thin film | FTO/TiO2/Pe/Spiro-MeTAD/Au | 0.48 | n.r | n.r | 1.5 | 05-2015 |
CH3NH3PbBr3 | Thin film | ITO/c-TiO2/EA/Pe/SPB-02T/MoO x /Au | 0.051 | 0.22 | 545 | n.r | 07-2015 |
CH3NH3Pb3−x Cl x | Thin film | ITO/Mg-ZnO/Pe/CBP/MoO x /Au | 0.1 | n.r | n.r | 2.2 | 08-2015 |
CH3NH3PbBr3 | Thin film | ITO/Pe-PEO/In-Ga | 0.083 | 0.38 | 4064 | 2.9 | 10-2015 |
CsPbBr3 | QD | ITO/PEDOT:PSS/PVK/Pe/TPBI/LiF-Al | 0.12 | 0.43 | 946 | 4.2 | 10-2015 |
CsPbBr3 | Thin film | ITO/PEDOT:PSS/Pe/F8/Ca/Ag | 0.008 | 0.035 | 407 | 3 | 11-2015 |
CH3NH3PbBr3 | Thin film | ITO/PEDOT:PSS/Pe/SPB-02T/LiF/Al | 0.1 | 0.43 | 3490 | 2.4 | 11-2015 |
CH3NH3PbBr3 | NPLs | ITO/PEDOT:PSS/Pe/PVK:PBD/BCP/LiF/Al | 0.48 | n.r | 10590 | 3.8 | 11-2015 |
CH3NH3PbBr3 | Thin film | ITO/PEDOT:PSS/Pe(6%HBr)/SPB-02T/LiF/Ag | 0.2 | 0.43 | 3490 | 4.3 | 11-2015 |
CH3NH3PbBr3 | Thin film | Glass/SOCP/Pe/TPBI/LiF-Al | 8.53 | 42.9 | ~15,000 | 4 | 12-2015 |
CH3NH3PbBr3 | Printed thin film | ITO/Pe-PEO/Ag NWs | 1.1 | 4.91 | 21,014 | 2.6 | 12-2015 |
4.2 Solar Cells
Perovskite NW solar cells: a, b SEM image of NWs from a one-step method and its corresponding J–V curve. Two-step-method-grown NWs and corresponding device performances. c, d Top-view and cross section of NWs films. e, f J–V and IPCE curves of NW solar cells. The scale bar is 1 μm.
There are many reviews discussing about halide perovskite thin-film solar cells. Thus, we only list the key breakthroughs in chronological order. Miyasaka and coworkers were the first to report CH3NH3PbBr3 solar cells with a PCE of 2.2% in 2006 [98]. In 2009, they improved the PCE to 3.8% by replacing bromine with iodine. Subsequently, Park and colleagues optimized a titania surface and substituted DMF solvent by γ-butyrolactone, yielding an efficiency of triiodide cells to 6.5% in 2011 [14]. Unfortunately, the device stability had not significantly improved. Until 2012, Kanatzidis and coworkers utilized the p-type solution-processable perovskite fluorine-doped CsSnI3 as a solid HTL in a solid-state DSSC [99]. This was the first time that a perovskite material has been used as the HTL with efficiencies up to 10.2%. The real breakthrough of perovskite stability was obtained by the Gratzel and Park groups [5]. They utilized MAPbI3 as a light harvester combined with the solid hole conductor 2,2′,7,7′, tetrakis(N,N-dimethoxy-phenyl-amine)-9,9′-spirobifluorene (spiro-MeOTAD) on mesoporous TiO2 leading to a PCE of 9.7% and dramatically improving the device stability compared to CH3NH3PbI3-sensitized liquid junction cells. From the above-mentioned research [5, 99], it can be concluded that OIP had the excellent capability to achieve ambipolar charge transport. At the same time, a significant study reported by Seok, M. Gratzel, and coworkers [100] boosted the PCE to 12%.
SEM, J–V, and EQE measurements for perovskite solar cells. a Cross-sectional SEM image of the device. The comparison of SEM surface images of FAPbI3-based layer formed on mp-TiO2 by IEP (b) and conventional method (c). d J–V curves of best device measured in reverse and forward modes, and e EQE spectra for best device and integrated J SC.
Adapted image reproduced with permission of Ref. [101]
4.3 Photodetectors
Perovskite NW photodetectors: slip coating-based NWs PDs. a Dark and laser-illuminated I–V curves. b Time-resolved photoresponse. EISA method-based device performances. c I–t curves. d High-resolution scan to one cycle of I–t curves. Doctor blading-based NW PDs. e Wavelength-dependent photoresponsivity of the CH3NH3PbI3 MW array-based photodetectors. f Photocurrent versus light intensity curves. g Variation of dark current/photocurrent with day of photodetector based on OTP MW arrays. h Perovskite MW PD arrays for light source mapping. NW web-based PDs for imaging. i–j Flexibility performances. k–m NW network PD arrays for imaging. n, o Encapsulation could help to improve the device stability.
Adapted image reproduced with permission of Ref. [49, 52, 60]
Materials | Configuration | Responsivity (A W−1) | Detectivity (Jones) | Response time | Report year |
---|---|---|---|---|---|
CH3NH3PbI3/TiO2 film | Photodetector | 0.49 × 10−6 | – | 0.02 s | 2014 |
CH3NH3PbI3 film | Photodetector | 3.49 | – | <0.2 s | 2014 |
CH3NH3PbI3−x CI x film | Photodetector | 5 × 10−3 | 1014 | 160 ns | 2014 |
CH3NH3PbI3 nanowires | Phototransistor | 14.5 | – | <500 µs | 2015 |
CH3NH3PbI3 film | Photodetector | 180 | – | 0.2 µs | 2015 |
Graphene-CH3NH3PbI3 composites | Phototransistor | 242 | 109 | 87 ms | 2015 |
CH3NH3PbI3 film | Photodetector | – | – | 5.7 ± 1.0 µs | 2015 |
CH3NH3PbI3 film | Photodiode | – | 3 × 1012 | <5 µs | 2015 |
CH3NH3PbI3 film | Photodetector | – | 7.4 × 1012 | 120 ns | 2015 |
CH3NH3PbI3 film | Optocoupler | 1.0 | – | 20 µs | 2015 |
CH3NH3PbI3 nanowires | Photodetector | 1.3 | 2.5 × 1012 | 0.3 ms | 2015 |
4.4 Lasing
Perovskite NWs lasers. a–f SEM image and nanolaser performances from MAPbX3 NWs. g A set of dark-field images of a IOP MW waveguide. Scale bar is 10 µm. h, i FAPbX3 NW laser performances. j–l Full-inorganic halide perovskite NW lasers.
Adapted image reproduced with permission of Ref. [67, 119, 128, 129]
Considering the photo- and thermal stabilities of MAPbX3 NW lasers, Song Jin et al. reported a low-temperature solution growth of single-crystal NWs of formamidinium lead halide perovskites (FAPbX3) that feature redshifted emission and better thermal stability compared to MAPbX3 [129]. They demonstrated optically pumped room-temperature near-infrared (∼820 nm) and green lasing (∼560 nm) from FAPbI3 and FAPbBr3 NWs with low lasing thresholds of several microjoules per square centimeter and high quality factors of approximately 1500–2300. More remarkably, the FAPbI3 and MABr-stabilized FAPbI3 NWs displayed durable room-temperature lasing under ∼108 shots of sustained illumination, greatly exceeding the stability of MAPbI3 (∼107 laser shots). They also demonstrated tunable NWs lasers in a wider wavelength region from FA-based lead halide perovskite alloys through cation and anion exchange (Fig. 17h–i).
Materials (X = CI−,Br−,or I−) | Morphology | Pump source | S.E wavelengths (nm) | Modal gain coefficient | Threshold (ASE or lasing) | Cavity type | Publication date |
---|---|---|---|---|---|---|---|
CH3NH3PbX3 | Thin film | 600 nm, 150 fs | 500–790 | 40 | 12 (ASE) | N.A | 03-2014 |
CH3NH3PbI3 | Thin film | 530 nm, 4 ns | 780 | – | 10 (ASE) | N.A | 08-2015 |
CH3NH3PbI3−x Cl x | Thin film | 532 nm, 400 ps | 760 | – | 120 (ASE) 0.2 µJ per pulse (lasing) | N.A Vertical microcavity | 04-2014 |
CH3NH3PbI3 | Thin film | 355 nm, 2 ns | 775 | 125 | 65 (ASE) 75 (lasing) | N.A Spherical WGM | 10-2014 |
CH3NH3PbI3 | Thin film | 532,1 ns | 780 | – | 0.32 (lasing) | DFB | 12-2015 |
CH3NH3PbBr3 | Square microdisk | 400 nm, 120 fs | 550 | – | 4 (lasing) | Planar WGM | 04-2015 |
CH3NH3PbI3−x Cl x | Microplatelet | 400 nm, 50 fs | 760 | – | 40 (lasing) | Planar WGM | 08-2014 |
CH3NH3PbI3 | Microcrystal networks | 355 nm, 0.8 ns | 765 | – | 200 (lasing) | Random lasing | 10-2014 |
CH3NH3PbX3 | NWs | 402 nm, 150 fs | 500–780 | – | 0.2 (lasing) | Fabry–Perot cavity | 03-2015 |
CsPbX3 | NPs | 400 nm, 100 fs | 470–620 | 98 | 22 (ASE) 11 × 103 (lasing) | N.A ring WGM | 10-2015 |
CsPbX3 | NPs | 400 nm, 100 fs | 470–640 | 450 | 5–22 (ASE) N.A (lasing) | N.A Spherical WGM Random lasing | 07-2015 |
CsPbBr3 | NPs | 800 nm, 35 fs | 520 | – | 12 × 103 (ASE) | N.A | 12-2015 |
CsPbBr3 | NWs | 400 nm, 150 fs | 530 | – | 10 (lasing) | Fabry–Perot cavity | 02-2016 |
5 Summary and Outlook
Perovskite | Passivation materials | Method | Report time |
---|---|---|---|
CsPbX3 | The incorporation of poly(maleic anhydride-alt-l-octadecene) (PMA) | Tightening the ligand binding | 2016 |
CsPbX3 | A polyhedral oligomeric silsesquioxane (POSS) | Surface protection | 2016 |
CsPbX3 | (3-aminopropyl)triethoxysilane (APTES) | A silica matrix | 2016 |
CsPbX3 | – | X-ray illumination | 2016 |
CsPbX3 | – | Intermolecular C = C bonding | 2016 |
CH3NH3PbBr3 | SiO2 | Coupling with perovskites | 2016 |
FAPbBr3 | Hydrophobic association | Capping nanocrystals | 2016 |
CsPbX3 | Chloride | Chloride doping | 2016 |
For low-dimensional halide perovskite synthesis, the perovskite formation processes play a paramount role in determining their final device performances. They can be prepared by a variety of techniques via the competition between in situ transformation and dissolution–crystallization mechanisms. Moreover, the use of capping ligands and solvent engineering can help to tailor the shape of perovskite crystals. Emerging applications of these randomly distributed perovskite units require the achievement of controllable alignment in order to match the planar microelectronic fabrication techniques.
Beyond PV applications, low-dimensional perovskite materials with high crystallinity, emission efficiency, and benign defects enable the fabrication of LEDs, lasers, PDs, and other optoelectronic/microelectronic devices. Furthermore, their high atomic number and high density may find applicability to high-energy radiation detection. Additionally, perovskites exhibit interesting ferroelectric properties, potentially due to the free rotation of the polar organic species, which further bolsters their potential for switchable electronics and memory devices. Despite the novel properties of low-dimensional perovskites, several crucial challenges, including toxicity and instability, limit wide industrial application. Limited success has been reported for the replacement of Pb with environmental friendly elements. Nontoxic Sn shares relatively similar properties to Pb in hybrid perovskites and is theoretically expected to yield more efficient performances. However, Sn-based perovskite solar cells experience more serious instability due to the naturally favorable oxidation of Sn(II), which inevitably requires advanced encapsulation techniques. Apart from the toxicity, Pb-based perovskites experience inherent instability under long-term operation, which is even more urgent to address. The degradation mechanisms of perovskites upon exposure to thermal, moisture, UV, and mechanical conditions require a reliable strategy in order to improve material stability. Encouraging results have been demonstrated through interface modifications between transport materials and electrodes [121]. Optimized devices have realized stable working times over 1000 h. However, considering the durability requirements of 20 years operation for solar cells, there is still much work required to improve the intrinsic properties of halide perovskites and more stable device structures. From an academic research perspective, there have been great success for the synthesis and applications of halide perovskites. Further research efforts are expected to focus on: (1) deep understanding of the structure–property relationships of the entire hybrid material system to guide the rational design and careful manipulation of the optoelectronic properties and (2) introducing new ideas to break the trade-off between the halide perovskite novelties and the working stability. Under the intensely driven research, the future development of environmentally friendly and reliably working perovskite devices is hopeful.
Notes
Acknowledgements
This work is supported by the Doctoral Program of Higher Education (20130142120075), the Fundamental Research Funds for the Central Universities (HUST:2016YXMS032) and National Key Research and Development Program of China (Grant No. 2016YFB0700702). The authors also thank Testing Center of HUST and the Center for Nanoscale Characterization and Devices, Wuhan National Laboratory for Optoelectronics (WNLO) for facility access.
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