All-inorganic perovskite nanocrystals (NCs) have emerged as a new generation of low-cost semiconducting luminescent system for optoelectronic applications. The room-temperature photoluminescence quantum yields (PLQYs) of these NCs in the green and red spectral range approach unity. However, their PLQYs in the violet are much lower, and an insightful understanding of such poor performance remains missing. We report a general strategy for the synthesis of all-inorganic violet-emitting perovskite NCs with near-unity PLQYs through engineering local order of the lattice by nickel ion doping. A broad range of experimental characterizations, including steady-state and time-resolved luminescence spectroscopy, X-ray absorption spectra, and magic angle spinning nuclear magnetic resonance spectra, reveal that the low PLQY in undoped NCs is associated with short-range disorder of the lattice induced by intrinsic defects such as halide vacancies and that Ni doping can substantially eliminate these defects and result in increased short-range order of the lattice. Density functional theory calculations reveal that Ni doping of perovskites causes an increase of defect formation energy and does not introduce deep trap states in the band gap, which is suggested to be the main reason for the improved local structural order and near-unity PLQY. Our ability to obtain violet-emitting perovskite NCs with near-perfect properties opens the door for a range of applications in violet-emitting perovskite-based devices such as light-emitting diodes, single-photon sources, lasers, and beyond.
Benzylamine is introduced as a surface passivation molecule that improves the moisture-resistance of the perovskites while simultaneously enhancing their electronic properties. Solar cells based on benzylamine-modified formamidinium lead iodide perovskite films exhibit a champion efficiency of 19.2% and an open-circuit voltage of 1.12 V. The modified FAPbI films exhibit no degradation after >2800 h air exposure.
Radiation detection, using materials to convert high-energy photons to low-energy photons (X-ray imaging) or electrical charges (X-ray detector), has become essential for a wide range of applications including medical diagnostic technologies, computed tomography, quality inspection and security, etc. Metal halide perovskite-based high-resolution scintillation-imaging screens or direct conversion detectors are promising candidates for such applications, because they have high absorption cross sections for X-rays due to their heavy atom (e.g., Pb2+, Bi3+, I–) compositions; moreover, these materials are solution-processable at low temperature, possessing tunable bandgaps, near-unity photoluminescence quantum yields, low trap density, high charge carrier mobility, and fast photoresponse. In this review, we explore and decipher the working mechanism of scintillators and direct conversion detectors as well as the key advantages of halide perovskites for both detection approaches. We further discuss the recent advancements in this promising research area, pointing out the remaining challenges and our perspective for future research directions toward perovskite-based X-ray applications.
Doping of lead halide perovskites (LHPs) with the targeted impurities has emerged as an additional lever, a dimension beyond structural perfection and compositional distinction, for the alteration of many properties of halide perovskites. The past several years has seen an explosive increase in our knowledge of doped halide perovskites, which exhibit distinct optical and electronic properties with respect to undoped counterparts and improve performance of perovskite optoelectronic devices. However, there are still a series of fundamental scientific issues unresolved in the domain of doped perovskites. In this review, we present a critical overview of recent advances in the synthesis, property, and functional applications of metal-doped halide perovskites. We lay a particular focus on three-dimensional LHPs and discuss the influence of doped metal ions on the properties of these perovskites, including main group metal cations, transition metal cations, and rare earth (RE) metal cations. We thoroughly summarize the synthesis methods used, doping-induced variation in optoelectronic properties, and benefit of doping engineering for optimization of device performance. We highlight the milestone achievements in this field and emphasize new properties arising from dopants in halide perovskites. We also address controversies encountered during the development of doped perovskites and examine the remaining challenges in this exciting field of science. Finally, we present our perspectives for further investigation of this star material by doping engineering.
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Wide bandgap (WB) organic-inorganic hybrid perovskites (OIHPs) with a bandgap ranging between 1.7 and 2.0 eV have shown great potential to improve the efficiency of single-junction silicon or thin-film solar cells by forming a tandem structure with one of these cells or with a narrow bandgap perovskite cell. However, WB-OIHPs suffer from a large opencircuit voltage (V oc ) deficit in photovoltaic devices, which is associated with the phase segregation of the materials under light illumination. In this work the photoinstability is demonstrated and V oc loss can be addressed by combining grain crystallization and grain boundary passivation, achieved simultaneously through tuning of perovskite precursor composition. Using FA 0.17 Cs 0.83 PbI 3-x Br x (x = 0.8, 1.2 1.5, and 1.8), with a varied bandgap from 1.72 to 1.93 eV, as the model system it is illustrated how precursor additive Pb(SCN) 2 should be matched with a proper ratio of FAX (I and Br) to realize large grains with defect-healed grain boundaries. The optimized WB-OIHPs show good photostability at both room-temperature and elevated temperature. Moreover, the corresponding solar cells exhibit excellent photovoltaic performances with the champion V oc /stabilized power output efficiency reaching 1.244 V/18.60%, 1.284 V/16.51%, 1.296 V/15.01%, and 1.312 V/14.35% for WB-OIHPs with x = 0.8, 1.2, 1.5, and 1.8, respectively.
Flexible copper halide films of 400 cm2 area were fabricated with outstanding mechanical stability, excellent film uniformity, nearly 100% photoluminescence quantum yields, and resistance to water and heat. The re-absorption-free X-ray imaging scintillators engineered based on these films exhibit superior scintillation performance with a detection limit as low as 48.6 nGy/s and 17 lp/mm X-ray imaging resolution, representing the highest imaging resolution for powder-based screens.
Solution‐processed perovskite solar cells have great potential for low‐cost roll‐to‐roll fabrication. However, the degradation of aged precursor solutions will become a critical obstacle to mass production. In this report, a small molecule (ITIC‐Th) is employed to stabilize the perovskite precursor solution containing mixed cations and halides. It is found that ITIC‐Th can effectively suppress the formation of yellow δ‐phase in the films made from aged precursor solutions. Consequently, the devices fabricated from the aged precursor solution with ITIC‐Th experience much less efficiency drop with the increase of the precursor aging time—from 19.20% (fresh) to 16.55% (39 d), compared with the devices made from conventional precursor solutions dropping from 18.07% (fresh) to 1.76% (39 d). The characterizations suggest that ITIC‐Th is beneficial for CH3NH3+ cations to be incorporated into the crystal structure, facilitating the formation of perovskite phase. Furthermore, the presence of ITIC‐Th in the perovskite thin film gives rise to additional photocurrent as well as improved fill factor due to the well‐matched energy levels, the passivation of defects, and the complementary absorption spectra, suggesting a new route toward future high‐efficiency solar cells—incorporating organic non‐fullerene acceptors and halide perovskite materials into the same active layer.
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