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Impact of Organic Spacers on the Carrier Dynamics in 2D Hybrid Lead-Halide Perovskites
摘要： We have carried out non-adiabatic molecular dynamics simulations combined with time-dependent density functional theory calculations to compare the properties of the two-dimensional (2D) (BA)2(MA)Pb2I7 and three-dimensional (3D) MAPbI3 (where MA = methylammonium and BA = butylammonium) materials. We evaluate the different impacts that the 2D-confined spacer layer of butylammonium cations and the 3D-confined methylammonium cations have on the charge carrier dynamics in the two systems. Our results indicate that while both the MA+ and BA+ cations play important roles in determining the carrier dynamics, the BA+ cations exhibit stronger non-adiabatic couplings with the 2D perovskite framework. The consequence is a faster hot-carrier decay rate in 2D (BA)2(MA)Pb2I7 than in 3D MAPbI3. Thus, tuning of the functional groups of the organic spacer cations in order to reduce the vibronic couplings between the cations and the Pb-I framework can offer the opportunity to slow down the hot-carrier relaxations and increase the carrier lifetimes in 2D lead-halide perovskites.
关键词： carrier dynamics,2D hybrid lead-halide perovskites,time-dependent density functional theory,non-adiabatic molecular dynamics,organic spacers
更新于2025-09-23 15:21:21
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Enhancing the performance of LARP-synthesized CsPbBr <sub/>3</sub> nanocrystal LEDs by employing a dual hole injection layer
摘要： Lead halide perovskites have been considered promising materials for optoelectronic applications owing to their superior properties. CsPbBr3 nanocrystals (NCs) with a narrow particle size distribution and a narrow emission spectrum are synthesized by ligand-assisted re-precipitation (LARP), a low-cost and facile process. In inverted CsPbBr3 NC LEDs, a dual hole injection layer (HIL) of 1,4,5,8,9,11-hexaazatriphenylene-hexacarbonitrile (HAT-CN)/MoO3 is introduced to enhance hole injection and transport, because HAT-CN can extract electrons easily from the hole transport layer and leave a large number of holes there. The current and power efficiencies of the optimized device with a dual HIL are 1.5- and 1.8-fold higher than those of the single HIL device. It is believed that the dual HAT-CN/MoO3 HIL effectively promotes hole injection and has promise for application in many other devices.
关键词： Ligand-assisted re-precipitation,Optoelectronic applications,Lead halide perovskites,CsPbBr3 nanocrystals,Dual hole injection layer,HAT-CN/MoO3
更新于2025-09-23 15:21:01
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Amplified and Multicolor Emission from Films and Interfacial Layers of Lead Halide Perovskite Nanocrystals
摘要： Lead halide perovskites are promising for energy harvesting and lighting applications. We show amplified emission from films of organic-inorganic or all inorganic lead halide perovskite nanocrystals. Also, multicolor emission is detected from interfacial layers of chloride and bromide perovskites. While amplified emission originates from spatial confinement of manifold charge carriers in films, multicolor emission emanates from interfacial ion exchanged layers. In a film, the amplified emission is averaged over a large number of nanocrystals, which prevents us from detecting any spectral narrowing. Conversely, amplified spontaneous emission (ASE) and spectral narrowing are detected from an isolated perovskite microcrystal. Interestingly, under low intensity excitation, a perovskite nanocrystal film shows unusually delayed emission, which becomes extremely fast and spatially confined at higher intensities of excitation light. By precisely detecting photoluminescence from an irradiated area and outside, we reveal the migration as well as confinement of photogenerated charge carriers in the film. The migration of charge carriers is more efficient in a film of organic-inorganic perovskites than all-inorganic perovskites.
关键词： spatial confinement,multicolor emission,interfacial ion exchange,amplified emission,Lead halide perovskites,charge carriers
更新于2025-09-23 15:21:01
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Review on recent advances of core-shell structured lead halide perovskites quantum dots
摘要： Lead halide perovskites have shown great potential in photovoltaic and optoelectronic devices due to their high brightness, defect tolerance, tunable emission wavelength, high color purity and near-unity luminescence quantum yield. Conversely, lead halide perovskites (LHP) show poor stability, which received strong criticism despite other promising characteristics. The poor stability attracted much research resulting in various modifications to enhance the stability and photoluminescence quantum yield (PLQY). The review outlines the basic structural and optical properties along with the conventional method of LHP synthesis and its drawbacks. Simultaneously discusses about factors responsible for instability like crystal structure, moisture, solvent, light and temperature. The review exclusively focuses on the recent research on core-shell LHP modification strategy to improve the stability and PLQY and its application in LED devices.
关键词： photoluminescence,Lead halide perovskites,stability,core-shell structure,quantum yield
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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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
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Light or Heat: What Is Killing Lead Halide Perovskites Under Solar Cell Operation Conditions?
摘要： We report the first systematic assessment of intrinsic photothermal stability of a large panel of complex lead halides APbX3 incorporating different univalent cations (A=CH3NH3+, [NH2CHNH2]+, Cs+) and halogen anions (X=Br, I) using a series of analytical techniques such as UV-vis and x-ray photoelectron spectroscopy, x-ray diffraction, EDX analysis, atomic force and scanning electron microscopy, ESR spectroscopy and mass spectrometry. We show that heat stress and light soaking induce a severe degradation of perovskite films even in the absence of oxygen and moisture. The stability of complex lead halides increases in the order MAPbBr3<MAPbI3<FAPbI3<FAPbBr3<CsPbI3<CsPbBr3, thus featuring all-inorganic perovskites as the most promising absorbers for stable perovskite solar cells. An important correlation was found between the stability of the complex lead halides and the volatility of univalent cation halides incorporated in their structure. The established relationship provides useful guidelines for designing new complex metal halides with immensely improved stability.
关键词： Plasmonics and Optoelectronics,Photothermal Stability,Solar Cell Operation Conditions,Energy Conversion and Storage,Lead Halide Perovskites
更新于2025-09-12 10:27:22
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High perovskite-to-manganese energy transfer efficiency in single-component white-emitting Mn-doped halide perovskite quantum dots
摘要： Taking advantages of negligible reabsorption and no phase separation, single-component white-emitting phosphors are believed as new promising color conversion materials for white light-emitting diodes. As a potential candidate, Mn-doped lead halide perovskites are studied intensively, but rare works can realize pure white emission with a single component due to the challenge for realizing sufficient energy transfer efficiency from perovskite to Mn at the desirable emission wavelengths. In this work, we reported the synthesis of single-component white light halide perovskite quantum dots (QDs) by doping Mn into the host of CsPb(Cl/Br)3@CsPb(Cl/Br)x core–amorphous shell (CAS). The small size of zero-dimensional core in CAS structure has a strong quantum confinement effect, which can enhance the energy transfer efficiency from halide perovskite to Mn impurity dramatically. Our result shows 19.3 times higher energy transfer efficiency for Mn-doped CAS than that of ordinary Mn-doped CsPb(Cl/Br)3 nanocubes. As a result, as-prepared Mn-doped CAS QDs give rise to a white light emission with Commission Internationale de l’Eclairage (CIE) color coordinates of (0.37, 0.33). After blending with polystyrene (PS), Mn-doped CAS QDs can be used as a single-component color conversion material for assembling white light LEDs.
关键词： energy transfer efficiency,white-emitting phosphors,white light LEDs,Mn-doped lead halide perovskites,quantum dots
更新于2025-09-12 10:27:22