Cesium lead halide (CsPbX) perovskite nanocrystals (NCs) have demonstrated extremely excellent optical properties and great application potentials in various optoelectronic devices. However, because of the anion exchange, it is difficult to achieve white-light and multicolor emission for practical applications. Herein, we present the successful doping of various lanthanide ions (Ce, Sm, Eu, Tb, Dy, Er, and Yb) into the lattices of CsPbCl perovskite NCs through a modified hot-injection method. For the lanthanide ions doped perovskite NCs, high photoluminescence quantum yield (QY) and stable and widely tunable multicolor emissions spanning from visible to near-infrared (NIR) regions are successfully obtained. This work indicates that the doped perovskite NCs will inherit most of the unique optical properties of lanthanide ions and deliver them to the perovskite NC host, thus endowing the family of perovskite materials with excellent optical, electric, or magnetic properties.
Quantum cutting can realize the emission of multiple near-infrared photons for each ultraviolet/visible photon absorbed, and has potential to significantly improve the photoelectric conversion efficiency (PCE) of solar cells. However, due to the lack of an ideal downconversion material, it has merely served as a principle in the laboratory until now. Here, the fabrication of a novel type of quantum cutting material, CsPbCl Br :Yb , Ce nanocrystals is presented. Benefiting from the larger absorption cross-section, weaker electron-phonon coupling, and higher inner luminescent quantum yield (146%), the doped perovskite nanocrystals are successfully explored as a downconverter of commercial silicon solar cells (SSCs). Noticeably, the PCE of the SSCs is improved from 18.1% to 21.5%, with a relative enhancement of 18.8%. This work exhibits a cheap, convenient, and effective way to enhance the PCE of SSCs, which may be commercially popularized in the future.
A grand unified model (GUM) is developed to achieve fundamental understanding of rich structures of all 71 liganded gold clusters reported to date. Inspired by the quark model by which composite particles (for example, protons and neutrons) are formed by combining three quarks (or flavours), here gold atoms are assigned three ‘flavours' (namely, bottom, middle and top) to represent three possible valence states. The ‘composite particles' in GUM are categorized into two groups: variants of triangular elementary block Au3(2e) and tetrahedral elementary block Au4(2e), all satisfying the duet rule (2e) of the valence shell, akin to the octet rule in general chemistry. The elementary blocks, when packed together, form the cores of liganded gold clusters. With the GUM, structures of 71 liganded gold clusters and their growth mechanism can be deciphered altogether. Although GUM is a predictive heuristic and may not be necessarily reflective of the actual electronic structure, several highly stable liganded gold clusters are predicted, thereby offering GUM-guided synthesis of liganded gold clusters by design.
Intracellular pH sensing is of importance and can be used as an indicator for monitoring the evolution of various diseases and the health of cells. Here, we developed a new class of surface-functionalized MXene quantum dots (QDs), TiC, by the sonication cutting and hydrothermal approach and further explored their intracellular pH sensing. The functionalized TiC QDs exhibit bright excitation-dependent blue photoluminescence (PL) originating from the size effect and surface defects. Meanwhile, TiC QDs demonstrate a high PL response induced by the deprotonation of the surface defects. Furthermore, combining the highly pH sensitive TiC QDs with the pH insensitive [Ru(dpp)]Cl, we developed a ratiometric pH sensor to quantitatively monitor the intracellular pH values. These novel MXene quantum dots can serve as a promising platform for developing practical fluorescent nanosensors.
A 2D surface plasmon photonic crystal (SPPC) is achieved by implanting gold nanorods onto the periodic surface apertures of the poly(methyl methacrylate) (PMMA) opal photonic crystals. On the surface of the SPPC, the overall upconversion luminescence intensity of NaYF4 :Yb(3+) , Er(3+) under 980 nm excitation is improved more than 10(3) fold. The device is easily shifted to a transparent flexible substrate, applied to flexible displays.
Aggregation‐induced emission (AIE) provides an efficient strategy to synthesize highly luminescent metal nanoclusters (NCs), however, rational control of emission energy and intensity of metal NCs is still challenging. This communication reveals the impact of surface AuI‐thiolate motifs on the AIE properties of Au NCs, by employing a series of water‐soluble glutathione (GSH)‐coordinated Au complexes and NCs as a model ([Au10SR10], [Au15SR13], [Au18SR14], and [Au25SR18]−, SR=thiolate ligand). Spectroscopic investigations show that the emission wavelength of Au NCs is adjustable from visible to the near‐infrared II (NIR‐II) region by controlling the length of the AuI‐SR motifs on the NC surface. Decreasing the length of AuI‐SR motifs also changes the origin of cluster luminescence from AIE‐type phosphorescence to Au0‐core‐dictated fluorescence. This effect becomes more prominent when the degree of aggregation of Au NCs increases in solution.
Recently, various lanthanide ions (Ln 3+ ) have been successfully doped into perovskite quantum dots (PQDs), and the quantum-cutting emission of 2 F 5/2 − 2 F 7/2 for Yb 3+ with a measurable inner efficiency of more than 100% has been discovered and applied as the luminescent converter of solar cells, which has opened a new branch for the application of PQDs. In this work, to further improve the quantum-cutting efficiency of Yb 3+ , the codoping and tridoping methods were used to improve the quantum-cutting emission of PQDs. The Yb 3+ −Ln 3+ (Ln = Nd, Dy, Tb, Pr, Ce) pair-doped CsPbCl x Br y I 3−x−y PQDs were fabricated, with all displaying excitonic emission, narrowband emission of Ln 3+ ions, and quantum-cutting emission of Yb 3+ ions. It was interesting that Yb 3+ −Pr 3+ as well as Yb 3+ −Ce 3+ pairs could effectively sensitize the emission of Yb 3+ , owing to Pr 3+ and Ce 3+ ions offering intermediate energy states close to the exciton transition energy of the PQDs. After host composition optimization and tridoping investigation, overall emissions with a 173% photoluminescence quantum yield (PLQY) were obtained in the Yb 3+ −Pr 3+ −Ce 3+ -tridoped CsPbClBr 2 PQDs. Then, the tridoped PQDs were designed as the down-converter for CuIn 1−x Ga x Se 2 (CIGS) as well as the silicon solar cells, which leads to an enhancement of the power conversion efficiency (PCE) of as high as ∼20%. The modified CIGS was further employed to charge the smart mobile phone, which could largely shorten the charging time from 180 to 150 min. This finding is of great significant for expanding the application fields of the impurity-doped PQDs.
Conspectus Understanding special stability of numerous ligand-protected gold nanoclusters has always been an active area of research. In the past few decades, several theoretical models, including the polyhedral skeletal electron pair theory (PSEPT), superatom complex (SAC), and superatom network (SAN), among others, have been developed for better understanding the stabilities and structures of selected ligand-protected gold nanoclusters. This Account overviews the recently proposed grand unified model (GUM) to offer some new insights into the structures and growth mechanism of nearly all crystallized and predicted ligand-protected gold nanoclusters. The main conceptual advancement of the GUM is identification of the duet and octet rules on the basis of the “big data” of 70+ reported ligand-protected gold nanoclusters. According to the two empirical rules, the cores of the gold nanoclusters can be regarded as being composed of two kinds of elementary blocks (namely, triangle Au3 and tetrahedron Au4), each having 2e closed-shell valence electrons (referred as Au3(2e) and Au4(2e)), as well as the secondary block (icosahedron Au13) with 8e closed-shell valence electrons (referred as Au13(8e)). The two elementary blocks (Au3(2e) and Au4(2e)) and the secondary block (Au13(8e)), from electron counting point of view, can be regarded as an analogy of the highly stable noble-gas atoms of He and Ne, respectively. In each elementary block, the Au atoms exhibit three different valence-electron states (i.e., 1e, 0.5e, and 0e), depending on the type of ligands bonded with these Au atoms. Such three valence-electron states are coined as three “flavors” of gold (namely, bottom, middle, and top “flavor”), a term borrowed from the quark model in the particle physics. Upon application of the duet and octet rules with accounting the three valence states of gold atoms, the Au3(2e), Au4(2e), and Au13(8e) blocks can exhibit 10 (denoted as Δ1–Δ10), 15 (denoted as T1–T15), and 91 (denoted as I1–I91) variants of valence states, respectively. When packing these blocks (with distinct electronic states) together, it forms the gold core of ligand-protected gold nanocluster. As such, the special stabilities of the ligand-protected gold nanoclusters are explained based on the local stability of each block. With GUM, rich and complex structures of ligand-protected gold nanoclusters have been analyzed through structure anatomy. Moreover, the growth of these clusters can be simply viewed as sequential addition of the blocks, rather than as addition of the gold atoms. Another useful application of the GUM is to analyze the structural isomerism. The three types of isomerism for the gold nanoclusters, i.e., core, staple, and complex isomerism, can be considered as an analogy of chain, point, and functional isomerism (known in organic chemistry), respectively. GUM can be applied to predict new clusters, thereby guiding experimental synthesis. Indeed, a number of ligand-protected gold nanoclusters with high stabilities were rationally designed based on...
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