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A Study of Eu Doping in Nanolayers of CsPbBr <sub/>3</sub> using Ab Initio Calculations to Understand <i>fa??f</i> Transitions in Eu <sup>3+</sup> -Doped Nanocrystals for Light-Emitting Diodes
摘要： Recent experiments on Eu doped nanocrystals of CsPbX3 (X = Cl, Br) show that Eu exists in 3+ oxidation state even though it substitutes Pb which is in 2+ state in these perovskites. Therefore, the question arises, what is it that leads to the formation of Eu3+ in nanocrystals of these materials? In order to understand this, we have studied the doping of Eu in a slab (~1.8 nm thick) of CsPbBr3 from ab initio calculations and explored various possibilities that could lead to the formation of Eu3+ and the occurrence of f-f transitions. These include: 1) the presence of a Cs vacancy, 2) the existence of H or OH due to moisture, 3) substitution of O at a surface halogen site, and 4) the possibility of excess halogen around Eu. It is found that the presence of surface oxygen is the most likely reason for the observation of Eu3+ in these nanolayers. Our results show the presence of partially occupied spin-up f states and 6.48 μB magnetic moment on Eu that could lead to the possibility of f-f transition in these doped systems. A similar result has also been obtained for Eu doped in CsPbCl3 nanolayers. The calculated change in energy when defects/impurities are present gives favourable indication of finding H, OH, and Br as interstitials and O as substitutional entities, but Cs vacancy is unlikely. Additionally, we find that the doping of Eu in nanolayers does not affect the atomic structure and the cost of doping is also very small making these perovskites very promising materials for light emitting diodes and other solid-state lighting applications.
关键词： Two-dimensional systems,Light emitting diodes,Solid state lighting,Density functional theory,Metal-halide perovskites,Nanolayers,Defects,f-f transitions
更新于2025-09-23 15:19:57
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Multifunctional Phosphorusa??Containing Lewis Acid and Base Passivation Enabling Efficient and Moisturea??Stable Perovskite Solar Cells
摘要： Multiple-cation lead mixed-halide perovskites (MLMPs) have been recognized as ideal candidates in perovskite solar cells in terms of high efficiency and stability due to decreased open-circuit voltage loss and suppressed yellow phase formation. However, they still suffer from an unsatisfactory long-term moisture stability. In this study, phosphorus-containing Lewis acid and base molecules are employed to improve device efficiency and stability based on their multifunction including recombination reduction, phase segregation suppression, and moisture resistance. The strong fluorine-containing Lewis acid treatment can achieve a champion PCE of 22.02%. Unencapsulated and encapsulated devices retain 63% and 80% of the initial efficiency after 14 days of aging under 75% and 85% relative humidity, respectively. The better passivation of Lewis acid implies more halide defects than Pb defects at the MLMP surface. This unbalanced defect type results from phase segregation that is the synergistic effect of Cs and halide ion migrations. Identifying defect type based on different passivation effects is beneficial to not only choose suitable passivators to boost the efficiency and slow down the moisture degradation of MLMP solar cells, but also to understand the mechanism of defect-assisted moisture degradation.
关键词： lewis acids,trap passivation,moisture stable solar cells,multiple-cation lead mixed-halide perovskites,phase segregation,lewis bases
更新于2025-09-23 15:19:57
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Effect of temperature on the performance of perovskite solar cells
摘要： The poor stability of perovskite solar cells is a crucial obstacle for its commercial applications. Here, we investigate the thermal stability of the mixed cation organic–inorganic lead halide perovskites (FAPbI3)1?xMAPb(Br3?yCly)x films and devices in air atmosphere. The results show that with the increase of heat treatment from 25 to 250 °C, the MA-perovskite decomposed into PbI2 firstly and the efficiency of corresponding solar cells reduced linearly. For the perovskite film, the increased heat treatment temperature can bring the redshift of the absorption edge leading to the decrease of band gap from 1.569 to 1.508 eV and increase of defect density from 3.87 × 1017 cm?3 to 9.03 × 1017 cm?3. However, a proper heat treatment time (10 min) at certain temperature (85 °C) can passivate defects effectively and improve the efficiency to 16.50%, realizing a 15% relative improvement of average efficiency. This work reveals a detailed thermal decomposition behavior of perovskite material and solar cells, which may provide insights into the stability of perovskite solar cells.
关键词： defect passivation,heat treatment,perovskite solar cells,thermal stability,mixed cation organic–inorganic lead halide perovskites
更新于2025-09-23 15:19:57
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Ambient-Processed, Additive-Assisted CsPbBr3 Perovskite Light-Emitting Diodes with Colloidal NiOx Nanoparticles for Efficient Hole Transporting
摘要： In this study, the electrically driven perovskite light-emitting diodes (PeLEDs) were investigated by hybridizing the organic polyethylene oxide, 1,3,5-tris (N-phenylbenzimiazole-2-yl) benzene (TPBi), and bis(3,5-di?uoro-2-(2-pyridyl)phenyl-(2-carboxypyridyl) iridium III (FIrpic) with CsPbBr3 in the emission layer and adopting the colloidal NiOx nanoparticle (NP) hole transport layer. The synthesized NiOx NPs, having an average size of ~5 nm, can be spin-coated to become a smooth and close-packed ?lm on the indium–tin–oxide anode. The NiOx NP layer possesses an overall transmittance of ~80% at 520 nm, which is about the peak position of electroluminescence (EL) spectra of CsPbBr3 emission layer. The coating procedures of NiOx NP and CsPbBr3 layers were carried out in ambient air. The novel PeLED turned on at 2.4 V and emitted bright EL of 4456 cd/m2 at 7 V, indicating the remarkable nonradiative-related defect elimination by organic additive addition and signi?cant charge balance achieved by the NiOx NP layer.
关键词： colloidal NiOx nanoparticles,organic additives,ambient-process,perovskite light-emitting diodes (PeLEDs),inorganic lead halide perovskites
更新于2025-09-23 15:19:57
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Size- and Composition-Dependent Exciton Spin Relaxation in Lead Halide Perovskite Quantum Dots
摘要： The strong spin-orbital coupling in lead halide perovskites allows for facile spin injection for spintronics applications, but on the other hand also limits the lifetime of the injected spins. Full-dimensional confinement of the carriers using quantum dots (QDs) has been envisioned as an effective means to prolong the spin relaxation lifetime and has been explored for II-VI and III-V group QDs. Here we applied this idea to colloidal lead halide perovskite QDs and measured the exciton spin dynamics of QDs of varying sizes and compositions using circularly polarized transient absorption spectroscopy at room temperature. Interestingly, the spin lifetimes of CsPbI3 and CsPbBr3 QDs were prolonged and shortened, respectively, as compared to their bulk counterparts. Both CsPbI3 and CsPbBr3 QDs showed decreasing spin lifetime with decreasing QD size. Possible spin relaxation mechanisms, including those that are unique to these quantum-confined systems, were proposed, with important ramifications for the use of these perovskite QDs in spin-related applications.
关键词： lead halide perovskites,spin-orbital coupling,exciton spin dynamics,circularly polarized transient absorption spectroscopy,quantum dots
更新于2025-09-23 15:19:57
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Efficient and accurate calculation of band gaps of halide perovskites with the Tran-Blaha modified Becke-Johnson potential
摘要： We report on a reoptimization of the Tran-Blaha modified Becke-Johnson (TB-mBJ) potential dedicated to the prediction of the band gaps of three-dimensional (3D) and layered hybrid organic-inorganic perovskites (HOPs) within pseudopotential-based density functional theory methods. These materials hold promise for future photovoltaic and optoelectronic applications. We begin by determining a set of parameters for 3D HOPs optimized over a large range of materials. Then we consider the case of layered HOPs. We design an empirical relationship that facilitates the prediction of band gaps of layered HOPs with arbitrary interlayer molecular spacers with a computational cost considerably lower than that of more advanced methods like hybrid functionals or GW. Our study also shows that substituting interlayer molecular chains of layered HOPs with Cs atoms is an appealing and cost-effective route to band gap calculations. Finally, we discuss the pitfalls and limitations of TB-mBJ for HOPs, notably its tendency to overestimate the effective masses due to the narrowing of the band dispersions. We expect our results to extend the use of TB-mBJ for other low-dimensional materials.
关键词： Tran-Blaha modified Becke-Johnson potential,halide perovskites,computational methods,band gaps,density functional theory,hybrid organic-inorganic perovskites,pseudopotential
更新于2025-09-19 17:15:36
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Indirect tail states formation by thermal-induced polar fluctuations in halide perovskites
摘要： Halide perovskites possess enormous potential for various optoelectronic applications. Presently, a clear understanding of the interplay between the lattice and electronic effects is still elusive. Specifically, the weakly absorbing tail states and dual emission from perovskites are not satisfactorily described by existing theories based on the Urbach tail and reabsorption effect. Herein, through temperature-dependent and time-resolved spectroscopy on metal halide perovskite single crystals with organic or inorganic A-site cations, we confirm the existence of indirect tail states below the direct transition edge to arise from a dynamical Rashba splitting effect, caused by the PbBr6 octahedral thermal polar distortions at elevated temperatures. This dynamic effect is distinct from the static Rashba splitting effect, caused by non-spherical A-site cations or surface induced lattice distortions. Our findings shed fresh perspectives on the electronic-lattice relations paramount for the design and optimization of emergent perovskites, revealing broad implications for light harvesting/photo-detection and light emission/lasing applications.
关键词： thermal fluctuations,halide perovskites,Rashba effect,optoelectronics,tail states
更新于2025-09-19 17:15:36
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DFT study of electronic structure and optical properties of layered two-dimensional CH <sub/>3</sub> NH <sub/>3</sub> PbX <sub/>3</sub> (X=Cl, Br, I)
摘要： Two-dimensional (2D) organic–inorganic hybrid halide perovskites (OIHPs) have been considered by researchers in the field of solar cells due to their high-temperature stability. In this paper, the electronic and optical properties of single-layer (SL) and multilayer (ML) structures of MAPbX3 (X = Cl, Br, I and MA = CH3NH3) have been studied by density functional theory (DFT) in order to predict its photovoltaic capabilities. The results have shown that SL- and ML-MAPbX3 have a direct band gap in the range of 1.76–2.70 eV. The calculation of dielectric constants has depicted that the static dielectric constants (SDCs) of SL-MAPbX3 are smaller than SDCs of ML-MAPbX3. However, as we expected, the reaction of the structures to in-plane (║) and out-of-plane (┴) polarizations was different; therefore, the SL- and ML-MAPbX3 (X = Cl, Br, I) were optically anisotropic. In addition, the intensity of the optical absorption spectrum for ML-MAPbX3 structures is approximately three times higher than that of SL-MAPbX3 structures. By increasing the radius of halogens (RCl<RBr<RI), surface area under the absorption curve increases and absorbs more. Furthermore, our results have shown that the electronic and optical behavior of 2D-MAPbX3 is suitable for photovoltaic applications and makes them useful for OIHP solar cells.
关键词： optical properties,DFT,2D-MAPbX3,organic–inorganic hybrid halide perovskites,solar cell
更新于2025-09-19 17:15:36
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Halide perovskites for resistive random-access memories
摘要： Halide perovskite based resistive random-access memory (ReRAM) devices are emerging as a new class of revolutionary data storage devices because their switching material—halide perovskite—has received considerable attention in recent years. Among the electrical characteristics of the material, its current–voltage (I–V) hysteresis, which may occur due to defect formation and migration, means that ReRAM can employ halide perovskites as a resistive switching material. Many studies have been conducted on resistive switching materials; however, the investigation of halide perovskites for ReRAM devices is still in the early research stages; therefore, the application of halide perovskites in ReRAM devices is a topic worth studying. Herein, we introduce halide perovskites and their operating mechanism within a ReRAM device. Moreover, recent notable achievements along with future challenges have been reviewed.
关键词： Halide perovskites,ion migration,hysteresis,resistive random-access memories,switching materials,ReRAM
更新于2025-09-19 17:15:36
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Dynamic Screening and Slow Cooling of Hot Carriers in Lead Halide Perovskites
摘要： Among the exceptional properties of lead halide perovskites (LHPs) is the ultraslow cooling of hot carriers. Carrier densities below the Mott density for large polarons (≤ ≈1018 cm?3) are focused on here. As in other semiconductors, a nascent hot electron distribution initially cools down via emission of longitudinal optical (LO) phonons on the 10?14–10?13 s timescale. What distinguishes LHPs from conventional semiconductors is the exceptionally efficient screening in the former. The dielectric screening in LHPs on the 10?13 s timescale results in an order-of-magnitude reduction in the Coulomb potential upon the formation of a large polaron, likely with ferroelectric-like local ordering. Further LO-phonon emission is inhibited, and this leads to partial retention of hot electron energy on the 10?12 s timescale, more so in hybrid LHPs than in their all-inorganic counterparts. Further cooling of hot polarons occurs on the 10?10 s timescale, and this can be attributed to the slow diffusion of heat out of the large polaron volume due to the low thermal conductivity of LHPs. Like other carrier properties, slow hot carrier cooling in LHPs can be intimately related to efficient screening in a soft, anharmonic, and dynamically disordered lattice.
关键词： dielectric function,lead halide perovskites,screening,hot electrons,large polarons
更新于2025-09-19 17:15:36