Search Results (72)

We report an advanced passivation strategy for perovskite solar cells (PSCs) by introducing core–shell structured perovskite quantum dots (PQDs), composed of methylammonium lead bromide (MAPbBr₃) cores and tetraoctylammonium lead bromide (tetra-OAPbBr₃) shells, during the antisolvent-assisted crystallization step. The epitaxial compatibility between the PQDs and the host perovskite matrix enables effective passivation of grain boundaries and surface defects, thereby suppressing non-radiative recombination and facilitating more efficient charge transport. At an optimal PQD concentration of 15 mg/mL, the modified PSCs demonstrated a remarkable increase in power conversion efficiency (PCE) from 19.2% to 22.85%. This enhancement is accompanied by improved device metrics, including a rise in open-circuit voltage (Voc) from 1.120 V to 1.137 V, short-circuit current density (Jsc) from 24.5 mA/cm² to 26.1 mA/cm², and fill factor (FF) from 70.1% to 77%. Spectral response analysis via incident photon-to-current efficiency (IPCE) revealed enhanced photoresponse in the 400–750 nm wavelength range. Additionally, long-term stability assessments showed that PQD-passivated devices retained more than 92% of their initial PCE after 900 h under ambient conditions, outperforming control devices which retained ~80%. These findings underscore the potential of in situ integrated PQDs as a scalable and effective passivation strategy for next-generation high-efficiency and stable perovskite photovoltaics. Full article

Ionic liquids (ILs) can ideally reduce defects and improve the film stability of emissive metal halide perovskite films. In this work, we measure how the structure and emission of methylammonium lead tribromide (MAPbBr₃) perovskite films is modulated by long alkyl chain-containing pyridinium, imidazolium, or pyrrolidinium ILs. Two different film deposition methods are compared, with the resultant films characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), and photoluminescence (PL) spectroscopy. For the latter, the differences in PL intensity of the perovskite are quantified using photoluminescence quantum efficiency (PLQE) measurements. It is found that a spin coating method in conjunction with the use of an imidazolium-containing IL (for a given precursor concentration) produces the strongest emissive perovskite. This optimal enhancement is attributed to a function of accessible surface charges associated with the heterocyclic cation of a given IL and perovskite defect passivation by bromide, the latter elucidated with the help of density functional theory. Proof-of-concept device fabrication is demonstrated for the case of a light emitting diode (LED) with the IL present in the emissive perovskite layer. Full article

Metal halide perovskite (MHP) nanocrystals (NCs) offer great potential for high-efficiency optoelectronic devices; however, they suffer from structural softness and chemical instability. Doping MHP NCs can overcome this issue. In this work, we synthesize Mn-doped methylammonium lead bromide (MAPbBr₃) NCs using the ligand-assisted reprecipitation method and investigate their structural and optical stability. X-ray diffraction confirms Mn²⁺ substitution at Pb²⁺ sites and lattice contraction. Photoluminescence (PL) measurements show a blue shift, significant PL quantum yield enhancement, reaching 72% at 17% Mn²⁺ doping, and a 34% increase compared to undoped samples, attributed to effective defect passivation and reduced non-radiative recombination, supported by time-resolved PL data. Mn²⁺ doping also improves long-term stability under ambient conditions. Low-temperature PL reveals the crystal-phase transitions of perovskite NCs and Mn-doped NCs to be somewhat different than those of pure MAPbBr₃. Mn²⁺ incorporation into perovskite promotes self-assembly into superlattices with larger crystal sizes, better structural order, and stronger inter-NC coupling. These results demonstrate that Mn²⁺ doping enhances both optical performance and structural robustness, advancing the potential of MAPbBr₃ NCs for stable optoelectronic applications. Full article

Three-dimensional (3D) hybrid organic–inorganic perovskites (HOIPs) have attracted tremendous interest due to strong excitonic effects and large optical nonlinearities. Taking the advantages, 3D HOIPs show great potential for applications in excitonic and nonlinear devices. However, understanding the relevant mechanisms of exciton-associated nonlinear optical phenomena in 3D perovskites is still challenging. Here, we apply the quantum perturbation theory to calculate the exciton-associated degenerate 2PA spectra of 3D HOIPs. The calculated 2PA spectra of twelve 3D HOIPs are predicted to exhibit resonance peaks at both the sub-band and band edges. The exciton-resonance-associated 2PA coefficients are at least one order of magnitude larger than those of band-to-band transitions and are comparable to those of low-dimensional perovskites. To validate our model, we carried out measurements of the static light-intensity-dependent transmission on MAPbBr₃ single crystals. Enhancements of 2PA coefficients are predicted theoretically and observed experimentally with a resonant peak at 1100 nm, indicating intrinsic two-photon transitions to excitonic states in MAPbBr₃ single crystals. Full article

The hot carrier multi-junction solar cell (HCMJC) is an advanced-concept solar cell with a theoretical efficiency greater than 65%. It combines the advantages of hot carrier solar cells and multi-junction solar cells with higher power conversion efficiency (PCE). The thermalization coefficient (Q_th) has been shown to slow down by an order of magnitude in low-dimensional structures, which will significantly improve PCE. However, there have been no studies calculating the Q_th of MAPbBr₃ quantum dots so far. In this work, the Q_th values of MAPbBr₃ quantum dots and after BABr addition were calculated based on power-dependent steady-state photoluminescence (PD-SSPL). Their peak positions in PD-SSPL increased from 2.37 to 2.71 eV after adding BABr. The fitting shows that, after adding BABr, the Q_th decreased from 2.64 ± 0.29 mW·K⁻¹·cm⁻² to 2.36 ± 0.25 mW·K⁻¹·cm⁻², indicating a lower relaxation rate. This is because BABr passivates surface defects, slowing down the carrier thermalization process. This work lays the foundation for the theoretical framework combining perovskite materials, which suggests that the appropriate passivation of BABr has the potential to further reduce Q_th and make MAPbBr₃ QDs with BABr modified more suitable as the top absorption layer of HCMJCs. Full article

The size-dependent photoluminescence (PL) blue shift in organometal halide perovskite nanoparticles has traditionally been attributed to quantum confinement effects (QCEs), irrespective of nanoparticle size. However, this interpretation lacks rigor for nanoparticles with diameters exceeding the exciton Bohr radius ($r_B$). To address this, we investigated the PL of MAPbBr₃ nanoparticles (MNPs) with diameters ranging from ~2 to 20 nm. By applying the Brus equation and Burstein–Moss theory to fit the PL and absorption blue shifts, we found that for MNPs larger than $r_B$, the blue shift is not predominantly governed by QCEs but aligns closely with the band filling effect. This was further corroborated by a pronounced excitation-density-dependent PL blue shift (Burstein−Moss shift) at high photoexcitation densities. Additionally, trap-state filling was also found to be not a negligible origin of the PL blue shift, especially for the smaller MNPs. The time-resolved PL spectra (TRPL) and excitation-density-dependent TRPL are collected to support the coexistence of both filling effects by the high initial carrier density (~10¹⁷–10¹⁸ cm⁻³) and the recombination dynamics of localized excitons and free carriers in the excited state. These findings underscore the combined role of the band filling and trap-state filling effects in the size-dependent PL blue shift for solution-prepared MNPs with diameters larger than $r_B$, offering new insights into the intrinsic PL blue shift in organometal halide perovskite nanoparticles. Full article

Semiconductor photodetectors can work only in specific material-dependent light wavelength ranges, connected with the bandgaps and absorption capabilities of the utilized semiconductors. This limitation has driven the development of hybrid devices that exceed the capabilities of individual materials. In this study, for the first time, a hybrid heterojunction photodetector based on methylammonium lead bromide (MAPbBr₃) polycrystalline film deposited on gallium arsenide (GaAs) was presented, along with comprehensive morphological, structural, optical, and photoelectrical investigations. The MAPbBr₃/GaAs heterojunction photodetector exhibited wide spectral responsivity, from 540 to 900 nm. The fabrication steps of the prototype device, including a new preparation recipe for the MAPbBr₃ solution and spinning, will be disclosed and discussed. It will be shown that extending the soaking time and refining the precursor solution’s stoichiometry may enhance surface coverage, adhesion to the GaAs, and film uniformity, as well as provide a new way to integrate MAPbBr₃ on GaAs. Compared to the pristine MAPbBr₃, the enhanced structural purity of the perovskite on GaAs was confirmed by X-ray Diffraction (XRD) upon optimization compared to the conventional glass substrate. Scanning Electron Microscopy (SEM) revealed the formation of microcube-like structures on the top of an otherwise continuous MAPbBr₃ polycrystalline film, with increased grain size and reduced grain boundary effects pointed by Energy-Dispersive Spectroscopy (EDS) and cathodoluminescence (CL). Enhanced absorption was demonstrated in the visible range and broadened photoluminescence (PL) emission at room temperature, with traces of reduction in the orthorhombic tilting revealed by temperature-dependent PL. A reduced average carrier lifetime was reduced to 13.8 ns, revealed by time-resolved PL (TRPL). The dark current was typically around 8.8 × 10⁻⁸ A. Broad photoresponsivity between 540 and 875 nm reached a maximum of 3 mA/W and 16 mA/W, corresponding to a detectivity of 6 × 10¹⁰ and 1 × 10¹¹ Jones at −1 V and 50 V, respectively. In case of on/off measurements, the rise and fall times were 0.40 s and 0.61 s or 0.62 s and 0.89 s for illumination, with 500 nm or 875 nm photons, respectively. A long-term stability test at room temperature in air confirmed the optical and structural stability of the proposed hybrid structure. This work provides insights into the physical mechanisms of new hybrid junctions for high-performance photodetectors. Full article

Halide perovskite has shown great potential in photocatalysis owing to its diversity, suitable energy band alignment, rapid charge transfer, and excellent optical properties. However, poor stability, especially under humid conditions, hinders their practical application in photocatalysis. In this work, we report the encapsulation of inorganic–organic hybrid perovskite QDs into MIL-101(Cr) through an in situ growth strategy to prepare a series of MAPbBr₃@MIL-101(Cr) (MA = CH₃NH₃⁺) composites. The perovskite precursors, i.e., MABr and PbBr₂, were successively introduced into the pores of MOF, where the perovskite quantum dots were self-assembled in the confined environment. In photocatalytic CO₂ reduction, 11%MAPbBr₃@MIL-101(Cr) composite displayed the best performance among the composites with a total CO and CH₄ yield of 875 μmol g⁻¹ in 9 h, which was 8 times higher than that of the pure MAPbBr₃. Such high gas production efficiency could be maintained for 78 h at least without structural and morphologic decomposition. The remarkable stability and catalytic activity of composites are mainly due to the synergistic effect and improved electron transfer between MAPbBr₃ and MIL-101(Cr). Moreover, these composites revealed a novel mechanism, showing switched CH₄ selectivity with the controlling of the perovskite location and contents. Those with perovskites encapsulated in the mesopores of MIL-101(Cr) were more preferential for CO production, while those with perovskites encapsulated in both meso- and micropores could produce CH₄ dominantly. Full article

Organic–inorganic hybrid perovskite quantum dots (QDs) have garnered significant research interest owing to their unique structure and optoelectronic properties. However, their poor optical performance in ambient air remains a significant limitation, hindering their advancement and practical applications. Herein, three amino acids (valine, threonine and cysteine) were chosen as surface ligands to successfully prepare highly luminescent CH₃NH₃PbBr₃ (MAPbBr₃) QDs. The morphology and XRD results suggest that the inclusion of the amino acid ligands enhances the octahedral structure of the QD solutions. Moreover, the observed blue-shifted phenomenon in the photoluminescence (PL) aligns closely with the blue-shifted phenomenon observed in the ultraviolet–visible (UV-Vis) absorption spectra, attributed to the quantum confinement effect. The time-resolved spectra indicated that the introduction of the amino acid ligands successfully suppressed non-radiative recombination, consequently extending the fluorescence lifetime of the MAPbBr₃ QDs. The photoluminescence quantum yields (PLQYs) of the amino acid-treated MAPbBr₃ QDs are increased by 94.8%. The color rendering index (CRI) of the produced white light-emitting diode (WLED) is 85.3, with a correlated color temperature (CCT) of 5453 K. Our study presents a novel approach to enhancing the performance of perovskite QDs by employing specially designed surface ligands for surface passivation. Full article

Organic/inorganic hybrid perovskite materials, such as CH₃NH₃PbX₃ (X = I, Br), have attracted the attention of the scientific community due to their excellent properties such as a widely tunable bandgap, high optical absorption coefficient, excellent power conversion efficiency, etc. The exposure of perovskite solar cells and photovoltaic devices to heat can significantly degrade their performance. Therefore, elucidating their temperature-dependent optical properties is essential for performance optimization of perovskite solar cells. We synthesized CH₃NH₃PbBr₃ (MAPbBr₃) single crystals through the polymer-controlled nucleation route and investigated the optical properties and molecular structure evolution of them with temperature. Through temperature evolution photoluminescence (PL) spectroscopy, we found that the fluorescence intensity was greatly affected by increasing the temperature, with an asymmetric PL profile suggesting that more captured excitons undergo radiative complexation. The optical photographs showed that the color of MAPbBr₃ single crystals faded. Raman spectroscopy revealed that during the heating process, the structure of MAPbBr₃ was still preserved at 90 °C since all of the Raman bands were very clear. When the temperature increased to 120 °C, the Raman bands of the internal modes became very weak. On further heating, the inorganic framework on sample’s surface started to disintegrate above 210 °C. During the heating process, the PL spectra exhibited significant changes in spectral intensity, peak position and Full Width Half Maximum (FWHM). The PL spectral intensity decreased abruptly with increasing temperature. The peak position was blue shifted with increasing temperature, and the peak shape showed an obvious asymmetry. The FMWH of the PL spectra was gradually broadened with the increase in the temperature, and there was a sharp increase from 270 °C to 300 °C. These variations in the PL spectra with temperature indicate that the optical properties of MAPbBr₃ are greatly affected by temperature, which in turn affects the application of MAPbBr₃ in fields such as optical devices. These results may be instructive for the application of MAPbBr₃. Full article

Perovskite single crystals have garnered significant interest in photodetector applications due to their exceptional optoelectronic properties. The outstanding crystalline quality of these materials further enhances their potential for efficient charge transport, making them promising candidates for next-generation photodetector devices. This article reports the synthesis of methyl ammonium lead bromide (MAPbBr₃) perovskite single crystal (SC) via the inverse-temperature crystallization method. To further improve the performance of the photodetector, Zn-porphyrin (Zn-PP) was used as a passivating agent during the growth of SC. The optical characterization confirmed the enhancement of optical properties with Zn-PP passivation. On single-crystal surfaces, integrated photodetectors are fabricated, and their photodetection performances are evaluated. The results show that the single-crystalline photodetector passivated with 0.05% Zn-PP enhanced photodetection properties and rapid response speed. The photoelectric performance of the device, including its responsivity (R), external quantum efficiency (EQE), detective nature (D), and noise-equivalent power (NEP), showed an enhancement of the un-passivated devices. This development introduces a new potential to employ high-quality perovskite single-crystal-based devices for more advanced optoelectronics. Full article

High-quality perovskite films (PFs) are crucial for achieving high-performance perovskite solar cells (PSCs). Herein, we report a dual-modification strategy via incorporating CsPbBr₃ QDs into MAPbI₃ perovskite bulk and capping the interface of the perovskite/hole transport layer (HTL) with phenylethylamine iodide (PEAI) to improve perovskite crystallinity and interface contact properties to acquire high-quality PFs with fewer defects. CsPbBr₃ QDs promoted perovskite grain growth and reduced bulk defects, while PEAI surface modification passivated interfaces, improved hydrophobic properties, and prevented carrier recombination at the perovskite/HTL interface. Benefiting from growth control and the effective suppression of both bulk and interface carrier recombination, the resulting devices show a greatly improved photoelectric conversion efficiency (PCE) from 17.21% of the reference cells to 21.04% with a champion Voc of 1.15 V, Jsc of 23.30 mA/cm², and fill factor (FF) of 78.6%. Furthermore, the dual-modification strategy endows PFs with promoted moisture tolerance, and the nonencapsulated PSCs retain 75% of their initial efficiency after aging for 30 days at 40% relative humidity and room temperature, which is significantly higher than the 59% value of the original PSCs. Good operational stability and the maintained efficiency of the target device over time suggest the potential for future commercialization. Full article

Perovskite thin films directly impact solar cell properties, making defect reduction crucial in perovskite solar cell research. In our study, we used perovskite quantum dots in the anti-solvent to act as nucleation centers in MAPbI3 thin films. These centers had lower nucleation barriers than homogeneous nucleation, improving perovskite crystallinity, reducing defects, and extending carrier lifetime. Fine-tuning the energy band also enhanced carrier transport. The most effective results were obtained using CsPb(Br_0.5 I_0.5)₃ perovskite quantum dots. The resulting device, ITO/SnO₂/MAPbI₃ (300 nm)/spiro-OMeTAD (200 nm)/Ag (100 nm), achieved a 12.88% power conversion efficiency, a 16% increase from the standard element. The modified device maintained approximately 95% of its efficiency over 100 h in a 70% humidity environment. Full article

To produce highly efficient and repeatable perovskite solar cells (PSCs), comprehending interfacial loss and developing approaches to ameliorate interfacial features is essential. Nonradiative recombination at the SnO₂–perovskite interface in SnO₂-based perovskite solar cells (PSCs) leads to significant potential loss and variability in device performance. To improve the quality of the SnO₂ electron transport layer, a novel polymer-doped SnO₂ matrix, specifically using polyacrylic acid, was developed. This matrix is formed by spin-coating a SnO₂ colloidal solution that includes polymers. The polymer aids in dispersing nanoparticles within the substrate and is evenly distributed in the SnO₂ solution. As a result of the polymer addition, the density and wetting properties of the SnO₂ layer substantially improved. Subsequently, perovskite-based photovoltaic devices comprising SnO₂ and Spiro-OMeTAD layers and using (FAPbI₃)_0.97(MAPbBr₃)_0.03 perovskite are constructed. These optimized devices exhibited an increased efficiency of 17.2% when compared to the 15.7% power conversion efficiency of the control device. The incorporation of polymers in the electron transport layer potentially enables even better performance in planar perovskite solar cells. Full article