Fluorescent carbon nanoparticles (F-CNPs) as a new kind of fluorescent nanoparticles, have recently attracted considerable research interest in a wide range of applications due to their low-cost and ...good biocompatibility. The fluorescent detection of metal ions is one of the most important applications. In this review, we first present the general detection mechanism of F-CNPs for the fluorescent detection of metal ions, including fluorescence turn-off, fluorescence turn-on, fluorescence resonance energy transfer (FRET) and ratiometric response. We then focus on the recent advances of F-CNPs in the fluorescent detection of metal ions, including Hg2+, Cu2+, Fe3+, and other metal ions. Further, we discuss the research trends and future prospects of F-CNPs. We envision that more novel F-CNPs-based nanosensors with more accuracy and robustness will be widely used to assay and remove various metal ions, and there will be more practical applications in coming years.
•Recent advances of F-CNPs-based fluorescent sensors for metal ions have been reviewed.•Simple and rapid detection of plenty of metal ions can be realized with F-CNPs.•The performance of F-CNPs for sensing metal ions has been compared.•The challenges and future prospects of F-CNPs for the fluorescent detection of metal ions have been discussed.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
The exciton binding energy in methylammonium lead iodide (MAPbI3) is about 10 meV, around 1/3 of the available thermal energy (k B T ∼ 26 meV) at room temperature. Thus, exciton populations are not ...stable at room temperature at moderate photoexcited carrier densities. However, excitonic resonances dominate the absorption onset. Furthermore, these resonances determine the transient absorbance and transient reflectance spectra. The exciton binding energy is a reflection of the Coulomb interaction energy between photoexcited electrons and holes. As such, it serves as a marker for the strength of electron/hole interactions and impacts a variety of phenomena, such as, absorption, radiative recombination, and Auger recombination. In this Perspective, we discuss the role of excitons and excitonic resonances in the optical properties of lead-halide perovskite semiconductors. Finally, we discuss how the strong light–matter interactions induce an optical stark effect splitting the doubly spin degenerate ground exciton states and are easily observed at room temperature.
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IJS, KILJ, NUK, PNG, UL, UM
Developing multijunction perovskite solar cells (PSCs) is an attractive route to boost PSC efficiencies to above the single-junction Shockley-Queisser limit. However, commonly used tin-based ...narrow-bandgap perovskites have shorter carrier diffusion lengths and lower absorption coefficient than lead-based perovskites, limiting the efficiency of perovskite-perovskite tandem solar cells. In this work, we discover that the charge collection efficiency in tin-based PSCs is limited by a short diffusion length of electrons. Adding 0.03 molar percent of cadmium ions into tin-perovskite precursors reduce the background free hole concentration and electron trap density, yielding a long electron diffusion length of 2.72 ± 0.15 µm. It increases the optimized thickness of narrow-bandgap perovskite films to 1000 nm, yielding exceptional stabilized efficiencies of 20.2 and 22.7% for single junction narrow-bandgap PSCs and monolithic perovskite-perovskite tandem cells, respectively. This work provides a promising method to enhance the optoelectronic properties of narrow-bandgap perovskites and unleash the potential of perovskite-perovskite tandem solar cells.
Metal halide perovskite semiconductors possess outstanding characteristics for optoelectronic applications including but not limited to photovoltaics. Low-dimensional and nanostructured motifs impart ...added functionality which can be exploited further. Moreover, wider cation composition tunability and tunable surface ligand properties of colloidal quantum dot (QD) perovskites now enable unprecedented device architectures which differ from thin-film perovskites fabricated from solvated molecular precursors. Here, using layer-by-layer deposition of perovskite QDs, we demonstrate solar cells with abrupt compositional changes throughout the perovskite film. We utilize this ability to abruptly control composition to create an internal heterojunction that facilitates charge separation at the internal interface leading to improved photocarrier harvesting. We show how the photovoltaic performance depends upon the heterojunction position, as well as the composition of each component, and we describe an architecture that greatly improves the performance of perovskite QD photovoltaics.
Metal–halide perovskite semiconductors have attracted attention for opto-spintronic applications where the manipulation of charge and spin degrees of freedom have the potential to lower power ...consumption and achieve faster switching times for electronic devices. Lower-dimensional perovskites are of particular interest since the lower degree of symmetry of the metal–halide connected octahedra and the large spin–orbit coupling can potentially lift the spin degeneracy. To achieve their full application potential, long spin-polarized lifetimes and an understanding of spin-relaxation in these systems are needed. Here, we report an intriguing spin-selective excitation of excitons in a series of 2D lead iodide perovskite (n = 1) single crystals by using time- and polarization-resolved transient reflection spectroscopy. Exciton spin relaxation times as long as ∼26 ps at low excitation densities and at room temperature were achieved for a system with small binding energy, 2D EOA2PbI4 (EOA = ethanolamine). By tuning the excitation density and the exciton binding energy, we identify the dominant mechanism as the D’yakonov–Perel (DP) mechanism at low exciton densities and the Bir–Aronov–Pikus (BAP) mechanism at high excitation densities. Together, these results provide new design principles to achieve long spin lifetimes in metal–halide perovskite semiconductors.
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IJS, KILJ, NUK, PNG, UL, UM
The band edges of metal-halide perovskites with a general chemical structure of ABX
(A, usually a monovalent organic cation; B, a divalent cation; and X, a halide anion) are constructed mainly of the ...orbitals from B and X sites. Hence, the structural and compositional varieties of the inorganic B-X framework are primarily responsible for regulating their electronic properties, whereas A-site cations are thought to only help stabilize the lattice and not to directly contribute to near-edge states. We report a π-conjugation-induced extension of electronic states of A-site cations that affects perovskite frontier orbitals. The π-conjugated pyrene-containing A-site cations electronically contribute to the surface band edges and influence the carrier dynamics, with a properly tailored intercalation distance between layers of the inorganic framework. The ethylammonium pyrene increased hole mobilities, improved power conversion efficiencies relative to that of a reference perovskite, and enhanced device stability.
The performance of three-dimensional (3D) organic-inorganic halide perovskite solar cells (PSCs) can be enhanced through surface treatment with 2D layered perovskites that have efficient charge ...transport. We maximized hole transport across the layers of a metastable Dion-Jacobson (DJ) 2D perovskite that tuned the orientational arrangements of asymmetric bulky organic molecules. The reduced energy barrier for hole transport increased out-of-plane transport rates by a factor of 4 to 5, and the power conversion efficiency (PCE) for the 2D PSC was 4.9%. With the metastable DJ 2D surface layer, the PCE of three common 3D PSCs was enhanced by approximately 12 to 16% and could reach approximately 24.7%. For a triple-cation–mixed-halide PSC, 90% of the initial PCE was retained after 1000 hours of 1-sun operation at ~40°C in nitrogen.
Organic–inorganic halide perovskites incorporating two-dimensional (2D) structures have shown promise for enhancing the stability of perovskite solar cells (PSCs). However, the bulky spacer cations ...often limit charge transport. Here, we report on a simple approach based on molecular design of the organic spacer to improve the transport properties of 2D perovskites, and we use phenethylammonium (PEA) as an example. We demonstrate that by fluorine substitution on the para position in PEA to form 4-fluorophenethylammonium (F-PEA), the average phenyl ring centroid–centroid distances in the organic layer become shorter with better aligned stacking of perovskite sheets. The impact is enhanced orbital interactions and charge transport across adjacent inorganic layers as well as increased carrier lifetime and reduced trap density. Using a simple perovskite deposition at room temperature without using any additives, we obtained a power conversion efficiency of >13% for (F-PEA)2MA4Pb5I16-based PSCs. In addition, the thermal stability of 2D PSCs based on F-PEA is significantly enhanced compared to those based on PEA.
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Narrow‐bandgap (NBG) tin (Sn)–lead (Pb) perovskites generally have a high density of unintentional p‐type self‐doping, which reduces the charge‐carrier lifetimes, diffusion lengths, and device ...efficiencies. Here, a p–n homojunction across the Sn–Pb perovskite is demonstrated, which results from a gradient doping by barium ions (Ba2+). It is reported that 0.1 mol% Ba2+ can effectively compensate the p‐doping of Sn–Pb perovskites or even turns it to n‐type without changing its bandgap. Ba2+ cations are found to stay at the interstitial sites and work as shallow electron donor. In addition, Ba2+ cations show a unique heterogeneous distribution in perovskite film. Most of the barium ions stay in the top 600 nm region of the perovskite films and turn it into weakly n‐type, while the bottom portion of the film remains as p‐type. The gradient doping forms a homojunction from top to bottom of the perovskite films with a built‐in field that facilitates extraction of photogenerated carriers, resulting in an increased carrier extraction length. This strategy enhances the efficiency of Sn–Pb perovskite single‐junction solar cells to over 21.0% and boosts the efficiencies of monolithic perovskite–perovskite tandem solar cells to 25.3% and 24.1%, for active areas of 5.9 mm2 and 0.94 cm2, respectively.
Barium ions are reported to effectively n‐dope perovskites. Distribution of the barium ions and related n‐doping effect is in a gradient across the perovskite film, resulting in a homojunction, which facilitates the separation and transport of the photogenerated carriers. Carrier diffusion length >2 µm and boosted efficiencies of 21.2% for single‐junction cell and 25.3% for all‐perovskite tandem cell are achieved.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK