Abstract:into their structure-property relationships. [2] The factors of spacer cations (e.g., structure of anchoring group and chain length) are of key importance in advancing the quality and use of 2D halide perovskites for applications in many optoelectronic fields. [2d,3] Concretely, it is necessary to design the structure of the head amino anchoring group with an appropriate size that matches the inorganic layer pockets. [4] For instance, primary ammonium spacer cations are easier to penetrate into the inorganic… Show more
“…As a result of GTMACl treatment, the defects at the OHP/ETL interface were effectively passivated; hence, the carrier lifetime was prolonged by suppression of the non-radiative recombination of photogenerated carriers. [42,62] The passivation effect is also verified by steady-state photoluminescence (PL) spectra. The reduced PL intensity for OHP/SnO 2 /FTO sample than bare OHP/FTO sample reveals the effect of non-radiative recombination induced by defect located at interface between the OHP and SnO 2 (Figure S2, Supporting Information).…”
Organometal halide perovskites (OHPs) have become potential candidates for high‐efficiency photoelectrodes for use in photoelectrochemical (PEC) water splitting. However, undesired losses, such as the non‐radiative recombination of photogenerated carriers and sluggish reaction kinetics of PEC water splitting, are the main limitations to achieving maximum efficiency for OHP‐based photoelectrodes. Herein, high‐efficiency OHP‐based photoanodes with a rational design that suppresses the undesired losses is reported. As a rational design for OHP‐based photoanodes, the defect‐passivated electron transport layers effectively suppress the undesired recombination of photogenerated carriers from the OHP layers. In addition, Fe‐doped Ni3S2 with a high catalytic activity promotes the reaction kinetics of PEC water oxidation, thereby suppressing the undesired losses at the interface between the OHP photoanodes and electrolytes. The fabricated Fe‐doped Ni3S2/Ni foil/OHP photoanodes exhibit a remarkable applied bias photon‐to‐current efficiency of 12.79%, which is the highest of the previously reported OHP‐based photoanodes by suppressing undesired losses. The strategies for achieving high‐efficiency OHP‐based photoanodes provide insights into the rational design of photoelectrodes based on OHPs.
“…As a result of GTMACl treatment, the defects at the OHP/ETL interface were effectively passivated; hence, the carrier lifetime was prolonged by suppression of the non-radiative recombination of photogenerated carriers. [42,62] The passivation effect is also verified by steady-state photoluminescence (PL) spectra. The reduced PL intensity for OHP/SnO 2 /FTO sample than bare OHP/FTO sample reveals the effect of non-radiative recombination induced by defect located at interface between the OHP and SnO 2 (Figure S2, Supporting Information).…”
Organometal halide perovskites (OHPs) have become potential candidates for high‐efficiency photoelectrodes for use in photoelectrochemical (PEC) water splitting. However, undesired losses, such as the non‐radiative recombination of photogenerated carriers and sluggish reaction kinetics of PEC water splitting, are the main limitations to achieving maximum efficiency for OHP‐based photoelectrodes. Herein, high‐efficiency OHP‐based photoanodes with a rational design that suppresses the undesired losses is reported. As a rational design for OHP‐based photoanodes, the defect‐passivated electron transport layers effectively suppress the undesired recombination of photogenerated carriers from the OHP layers. In addition, Fe‐doped Ni3S2 with a high catalytic activity promotes the reaction kinetics of PEC water oxidation, thereby suppressing the undesired losses at the interface between the OHP photoanodes and electrolytes. The fabricated Fe‐doped Ni3S2/Ni foil/OHP photoanodes exhibit a remarkable applied bias photon‐to‐current efficiency of 12.79%, which is the highest of the previously reported OHP‐based photoanodes by suppressing undesired losses. The strategies for achieving high‐efficiency OHP‐based photoanodes provide insights into the rational design of photoelectrodes based on OHPs.
“…[101] Lu et al prepared perovskite nanosheets with alloyed chiral and achiral spacer cations and investigated the effect of composition on their chiroptical properties. [102] With the introduction of achiral cation phenylethylammonium (PEA) in chiral (R/S-MBA) 2 PbBr 4 , the alloyed (R-MBA 1−x PEA x ) 2 PbBr 4 nanosheets exhibited better thermal stability, reduced bandgap (60 meV) as well as red-shifted PL peak (409 to 416 nm), as illustrated in Figure 7a. In virtue of the stronger binding ability of PEA cations with the inorganic framework and the inhibition of the formation of impure 1D R-MBAPbBr 3 phases, the (R/S-MBA 1−x PEA x ) 2 PbBr 4 nanosheets displayed enhanced chiroptical activity (Figure 7b).…”
Section: Modulation Of Chiralitymentioning
confidence: 99%
“…Meanwhile, with the increase of the concentration of achiral PEA cations, the g abs decreased gradually and its sign reversed, which can be explained by the fact that the introduction of achiral cations may change the long-range orientation of chiral cations and lead to the inversion of CD signals. [102] Figure 6. a) Schematic illustrations of chiral mono-, bi-, and tri-layer (1, 2, and 3 ML) CsPbBr 3 nanoplatelets.…”
Section: Modulation Of Chiralitymentioning
confidence: 99%
“…Reproduced with permission. [102] Copyright 2023, Wiley-VCH. c) CD spectra of chiral CsPbBr 3 PeNCs treated with different amounts of S-PEAI (upper) and S-PEACl (bottom).…”
Section: Nonlinear Opticsmentioning
confidence: 99%
“…Figure 7. a) UV-vis absorption (left) and PL (right) spectra of (R-MBA1−xPEAx)2PbBr4 nanosheet solution with different x. b) CD spectra (left) and corresponding g abs at maximum CD peak (right).Reproduced with permission [102]. Copyright 2023, Wiley-VCH.…”
Lead halide perovskite nanocrystals (PeNCs) have attracted intense interest by virtue of their numerous remarkable optoelectronic properties, which render them promising for various optoelectronic applications. Over the past few years, substantial progress has been made in the study of chiral PeNCs, from the sample preparation, spectroscopic characterization to practical applications. In this review, the state‐of‐the‐art progress of the construction strategies and photophysical properties of chiral PeNCs has been summarized. The focus is placed on emerging developments in terms of synthetic methods, chiroptical properties, nonlinear optics, and chiral spintronics in chiral PeNCs. In the end, there is a discussion on the current challenges and future prospects in this versatile, rapidly evolving field.
Chiral hybrid organic–inorganic perovskites (HOIPs) have garnered considerable research interest in the field of optoelectronics, owing to their ability to integrate outstanding optoelectronic characteristics with distinct chiral or spin‐related properties. Although recent years have witnessed the rapid development of chiral perovskites, methods for producing perovskites with high absorption dissymmetry factors (gCD) enabling polarization‐resolved chiroptical applications are still lacking. This study introduces a strategic combination of dual spacer cations, i.e., achiral hexane‐1,6‐diammonium (HDA) and chiral 1‐(chlorophenyl)ethylammonium (ClPEA), for boosting the chiroptical performance of 2D lead iodide HOIPs. Interestingly, ortho‐ClPEA, incapable of forming 2D HOIPs independently, successfully creates 2D structures in collaboration with HDA, exhibiting CD signals aligned with the absorption characteristics of 2D HOIPs. This significant milestone leads to an outstanding gCD value of 0.018, positioning it among the top performers in the field of lead‐based HOIPs. Furthermore, this study demonstrates the fabrication of circularly polarized light (CPL) detectors with a photocurrent dissymmetry factor (gIph) of 0.12, utilizing the HOIPs with enhanced chiroptical activity.
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