Temperature-dependent Photoluminescence Research Articles

Evolved photovoltaic performance of MAPbI3 and FAPbI3-based perovskite solar cells in low-temperatures

Organic-inorganic hybrid perovskites have emerged as an up-and-coming contender for photovoltaic devices owing to their exceptional photovoltaic properties. However, current research predominantly concentrates on their performance under ambient conditions at room temperature. In this work, we delve into the novel territory by investigating MAPbI3-based and FAPbI3-based perovskite solar cells (PSCs) in the temperature range of 300 to 150 K. Remarkable efficiency enhancements of nearly 5% and 20% were obtained at 250 and 210 K, respectively. However, further decreasing the temperature impairs the photovoltaic performance. We propose an underlying mechanism influencing the performance change in perovskite devices at low temperatures by examining the temperature-dependent ultraviolet-visible and photoluminescence spectra results. At the beginning of the cooling process, from 300 to 250 K for MAPbI3 and from 300 to 210 K for FAPbI3, the performance enhancement stems primarily from the enhanced open-circuit voltage by the tuned band gap of the perovskite films. Further lowering the temperature would change the perovskite structure, impairing the performance of PSCs. FAPbI3-based PSCs show a better tolerance in low temperatures owing to the more stable perovskite crystal structure. The present findings offer valuable theoretical guidance for preparing outstanding PSCs for low-temperature applications.

Magnetic coupling interaction-related photoluminescence behaviors in all-inorganic manganese chloride perovskites

Manganese halides, as dilute magnetic semiconductor materials, have magnetic coupling interactions that play an essential role in their photoluminescence (PL); however, such interactions remain controversial. AMnCl3 (AMC, A = K, Rb, and Cs) and their hydrates AMnCl3·2H2O (AMCH, A = K, Rb, and Cs) are both in the ABX3 configuration but exhibit a wide variety of structures with different connectivity types and dimensions. Their magnetic coupling interaction has been demonstrated. However, few studies have systematically investigated the PL in conjunction with the magnetic coupling interaction over these chloride compounds. In this paper, the effect of the magnetic coupling interaction on AMC and AMCH PL is mainly revealed by temperature-dependent PL spectra and lifetimes. The MnX6 (X6 = Cl4(H2O)2 or Cl6) cluster connection types affect the Mn2+–Mn2+ distances. The magnetic coupling interaction between MnX6 octahedrons affects the radiative transitions of manganese chlorides, which is influenced by the Mn2+–Mn2+ distance, local symmetry, and water ligand. The Mn2+–Mn2+ distance and the magnetic coupling interaction also affect their lifetimes. Variations in magnetic coupling interactions can shift emission wavelength, especially dual-emissions and near-infrared (NIR) emission at lower temperatures while A+ = K+. This work helps researchers understand the optical process of Mn2+ ions in different manganese compounds and provides new insights into the design of tailored Mn2+ ion phosphors.

Probing multifunctional applications of LiCa2Mg2V3O12: Sm3+ phosphor using Judd-Ofelt analysis and dual mode non-contact optical thermometry

LiCa2Mg2V3O12:Sm3+ phosphors have been prepared by solid state method and analysed by X-ray diffraction, EDX-elemental mapping, UV–VIS-NIR spectroscopy, photoluminescence (PL) and temperature dependent photoluminescence (TDPL). The absorption spectra analysis using Judd-Ofelt theory provides the intensity parameters and manifest the covalent nature of Sm-O bond. The PL spectra monitored at 338 nm excitation exhibits emission peaks of Sm3+ at 567, 617 and 651 nm in addition to the broad band emission of LiCa2Mg2V3O12 host. The Commision Internationale deL’Eclairage (CIE) coordinates, correlated color temperature (CCT) and color rendering index (CRI) values elucidate the efficient yellow emission of phosphors. The radiative parameters are evaluated and have outrageous branching ratio and cross section that aids in visible laser applications. The optical thermometry of phosphor is carried out by utilizing FIR method through selecting spectral modes 6H5/2/VO43-, 6H7/2/VO43- and 6H9/2/ VO43-. The mode 6H9/2/ VO43- have higher absolute sensitivity (Sa) and relative sensitivity (Sr) values of 0.4418 K−1 and 1.6079% K−1. The temperature resolution of modes are 0.1633, 0.1677 and 0.1563 K respectively. The thermochromic study reveals the high chromaticity shift (Δs = 0.1869) of phosphor and the Sa(x) and Sr(x) values evaluated based on CIE coordinates are 0.0011 K−1 and 0.2407% K−1 respectively. The PL and TDPL characteristics of prepared phosphor suggest that it have multifunctional application in the fields of lasers, thermo-sensors, thermochromic displays and LEDs.

Anisotropy of optical transitions in β-Ga2O3 investigated by polarized photoluminescence excitation spectroscopy

The monoclinic beta-phase of gallium oxide possesses an ultra-wide bandgap that surpasses other wide bandgap materials such as SiC and GaN, making it a promising candidate for power electronic device technologies. We investigate the first fundamental optical transitions in this material, which exhibit a strong directional dependence. To determine the energies and orientations of these transitions, temperature-dependent and angular resolved photoluminescence excitation spectroscopy is applied. We observe a distinct excitation channel located energetically between those of the first two optical transitions Γ1−1 and Γ1−2. While previous absorption edge and reflectance spectroscopy studies have assigned a transition in this spectral range to either the Γ1−1 or the Γ1−2 transition, our findings demonstrate no pronounced polarization dependence of this excitation channel within the (010) plane, an observation not reflected in calculations of the band-to-band transitions in β-Ga2O3.

Regulating photoluminescence through single-crystal-to-single-crystal transformation of solvent-containing zero-dimensional hybrid metal halide isomers

Regulating photoluminescence (PL) properties induced by single-crystal-to-single-crystal (SCSC) transformation has sparked significant interest in the research of zero-dimensional organic–inorganic metal halides (0-D OIMHs). To best of our knowledge, the SCSC transformation of solvent-containing 0-D OIMH isomers hasn’t been reported yet. In this work, we report the first example of SCSC transformation between two isomers containing lattice solvent molecules, namely α- and β-[EtPPh3]2[SbCl5]·MeCN (α- and β-1·MeCN; EtPPh3 = ethyltriphenylphosphonium; MeCN = acetonitrile). Differential scanning calorimetry (DSC) results show that the SCSC transformation from α- to β-1·MeCN is an exothermic process, implying that β-1·MeCN is a more stable phase than α-1·MeCN. Moreover, α- and β-1·MeCN exhibit bright orange (emission peak: 610 nm) and red (emission peak: 635 nm) emission under 360/365 nm excitation, respectively. DFT calculations suggest that the negligible self-absorption and a strong exciton confinement contribute to their effective PL emission. By analyzing temperature-dependent PL spectra, β-1·MeCN has been found to exhibit stronger electron-phonon coupling under excitation than α-1·MeCN. Thus, the broader emission with full width at half maximum (FWHM: 134 vs. 147 nm) and the higher photoluminescence quantum yield (PLQY: 40.37% vs. 70.50%) have been realized by SCSC transformation from α- to β-1·MeCN by heating at 92 °C. Benefitting from the regulation of PL performances brought by SCSC transformation, the white light-emitting-diode (LED) devices assembled by using β-1·MeCN as red phosphor could be optimized, and the CRI reaches as high as 95.3.

Effect of confinement on photoluminescence of MeLPPP/SBA-15 nanocomposite

Photoluminescence spectra and kinetics of methyl-substituted ladder-type poly(para-phenylene) (MeLPPP)/SBA-15 mesoporous silica (SBA-15) nanocomposite have been studied and compared with photoluminescence properties of the MELPPP film and solution. Relaxation processes of excited singlet states in the closed geometry of the nanocomposite and in the diluted solution compared to the film based on the temperature dependence of photoluminescence (5–220 K) were studied. It was shown that the nanocomposite has twice the photoluminescence lifetime and three times weaker temperature dependence of photoluminescence intensity in comparison with the film. These peculiarities are due to a decrease in the number of polymer chains in a low-dimensional structure and a reduced role of exciton diffusion.

Influence of Dy3+ ions on spectroscopic studies of thermally stable telluro zinc phosphate glasses for white light emitting devices

A transparent series of telluro zinc phosphate glasses with varying Dy3+ ion concentrations (BTZPDy) were synthesized using a melt-quenching procedure. The non-crystalline/amorphous form of the BTZPDy glass matrices has been demonstrated via an X-ray diffraction (XRD) profile. As a way of recognizing the proficient usage of the obtained BTZPDy glass matrices in the white light emitting devices, the spectroscopic characteristics such as optical absorption, photoluminescence excitation (PLE) and emission, as well as temperature-dependent photoluminescence (TDPL) were conducted and investigated in detail. The absorption spectrum was determined in the n-UV to NIR range for the as-prepared BTZPDy1.0 glass sample and the optical energy band gap has been assessed via utilizing Tauc’s plot. In the visible range, photoluminescence spectra demonstrate three distinct emission peaks under different n-UV excitations, among which an intense emission peak around 575 nm is related to the 4F9/2 → 6H13/2 transition in the prepared BTZPDy glasses. The color coordinates (x, y) for the prepared BTZPDy1.0 glass were situated in the white light zone of the CIE graph and adjacent to the standard white light region (0.33, 0.33). Furthermore, TDPL spectral studies suggest the excellent thermal stability of BTZPDy glass samples alongside a high value of activation energy. In view of the above results, as-prepared BTZPDy glasses can be utilized for the fabrication of thermally stable white light emitting devices.

Impact of Bright-Dark Exciton Thermal Population Mixing on the Brightness of CsPbBr3 Nanocrystals.

Understanding the interplay between bright and dark exciton states is crucial for deciphering the luminescence properties of low-dimensional materials. The origin of the outstanding brightness of lead halide perovskites remains elusive. Here, we analyze temperature-dependent time-resolved photoluminescence to investigate the population mixing between bright and dark exciton sublevels in individual CsPbBr3 nanocrystals in the intermediate confinement regime. We extract bright and dark exciton decay rates and show quantitatively that the decay dynamics can only be reproduced with second-order phonon transitions. Furthermore, we find that any exciton sublevel ordering is compatible with the most likely population transfer mechanism. The remarkable brightness of lead halide perovskite nanocrystals rather stems from a reduced asymmetry between bright-to-dark and dark-to-bright conversion originating from the peculiar second-order phonon-assisted transitions that freeze bright-dark conversion at low temperatures together with the very fast radiative recombination and favorable degeneracy of the bright exciton state.

Spectroscopic investigation and molecular docking analysis of an FRET probe: Trypsin from bovine pancreas@Coumarin 440 dye conjugate

Herein, a systematic investigation of energy transfer from bovine pancreas trypsin to coumarin 440 (C440) dye is presented with an aim to design a FRET probe, as trypsin is an important enzyme for absorption and digestion of nutrients in the small intestine. Conformational changes in trypsin upon interaction with C440 dye are studied by employing both spectroscopic and molecular docking techniques. Steady state and time resolved measurements validate the formation of trypsin-C440 complex via dynamic quenching, that confirms the role of C440 as an inhibitor to suppress the activity of trypsin. Spectral overlap integral, Förster's distance, rate and energy transfer efficiency are calculated from steady state measurements. The observed blue shift in fluorescence suggests conformational changes due to hydrophobicity that arises in trypsin structure on binding with C440 possibly due to their interaction through H-bond (SER195 and GLN192), hydrophobic (GLN192 and HIS57) and π-π stacking bonding (HIS57). The stability of trypsin@C440 bio-conjugate at higher temperature was established from temperature dependent PL studies and the thermodynamic parameters determined agree with second law of thermodynamics. The thermodynamic parameters such as change in enthalpy (ΔH=172.2Jmol−1), change in entropy (ΔS=15.3Jmol−1K−1) and the respective approximately same and unity values of Gibb's free energy (ΔG) and Hill coefficient (n), as well as binding affinities determined from temperature dependent fluorescence studies validate the hydrophobic, spontaneous, exothermic process engaged in trypsin@C440 bio-conjugate.

Photoluminescence Enhancement in Silica-Confined Ligand-Free Perovskite Nanocrystals by Suppression of Silanol-Induced Traps and Phase Impurities.

The detriments of intrinsic silanol groups in mesoporous silica to the photoluminescence (PL) of lead halide perovskite nanocrystals (LHP NCs) confined in the template have never been determined and clearly elucidated. Here, we disclose that silanol-induced Cs+ and Br- deficiencies prompt the generation of traps and CsPb2Br5 impurities. The temperature-dependent PL spectra verify the higher energetic barrier of trap states in CsPbBr3 NCs confined in silanol-rich mesoporous silica. Femtosecond transient absorption spectra reveal the trapped state mediates a broadband photoinduced absorption and long-lived decay pathway of CsPbBr3 NCs in silanol-rich templates. A remarkable improvement (up to 160-fold) in PL quantum yields is realized by simple silanol elimination. This work demonstrates the detrimental effects of silanol sites on the PL properties of LHP NCs impregnated in mesoporous silica and provides a new perspective for the ligand-free synthesis of high-quality LHP NCs in mesoporous templates by facile impregnation for practical applications.

Positional isomerism engineering toward minimizing exciton binding energy in sulfone copolymers for enhanced uranyl photoreduction

Conjugated microporous polymers (CMPs) have emerged as promising platforms for photocatalytic separation and enrichment of radionuclides. However, the development of CMPs with efficient exciton dissociation and free charge generation is still highly hindered by their high exciton binding energy (Eb). Herein, for the first time, three sulfone-containing CMPs are fabricated to regulate Eb by position isomerism of altering linkage sites. Temperature-dependent photoluminescence spectra reveals that ECUT-3,7-SO with 3,7-site linkage achieves a diminished Eb of 40.1 meV. DFT calculation complementally demonstrate that the Eb is related to its strongly polarized electric field and large conjugation degree, which can be easily regulated via position isomerism of its building blocks. Among the three, ECUT-3,7-SO exhibits a completely conjugated structure and a large molecular dipole moment, thus significantly reducing the Eb. As a result, ECUT-3,7-SO exhibits the highest photoreduction uranium rate constant (k, T = 298.15 K) of 0.081 min−1, and the maximum uranium extraction capacity of 918.0 mg g−1 under visible-light irradiation. This work highlights the importance of positional isomerization to the development of low exciton binding energy photocatalyst for uranium resource field.

Manipulating the phase stability of a halide perovskite, CH3NH3PbI3 by high-pressure cycling

Methylammonium lead iodide perovskite, CH3NH3PbI3 (MAPbI3) is a highly promising photovoltaic material, whose structural and electronic properties are very sensitive to applied stresses. Here, we show that the phase stability of a MAPbI3 crystal can be controlled by structural defects and strains. We synthesized a single crystal of MAPbI3 and measured its electrical properties across two successive structural phase transitions under applied pressure up to 4–9 GPa under multiple high-pressure cycling. We revealed three types of effects of this high-pressure treatment. (i) An increasing the level of defects and strains in the crystal greatly delays the first reconstructive phase transition, conserving the ambient-pressure tetragonal phase up to a record pressure of ∼1.4 GPa, much higher compared to its typical stability range of up to 0.3–0.5 GPa only. (ii) A time exposure of the crystal at a fixed pressure corresponding to the beginning of the second phase transition to a “destabilized” structure eliminated some of defects and strains; it down-shifted the phase boundaries back. (iii) A recrystallization of the sample after pressure-induced amorphization enhanced its structural stability against amorphization upon subsequent pressurization cycle. We proposed that the most abundant defects and strains, which could appear in the pressure-cycled MAPbI3 crystals, were related to migration of iodine atoms from their regular sites to the MA interstices. Temperature-dependent photoluminescence measurements indicated that the sample recovered after the high-pressure cycling crystallized back into the initial tetragonal crystal structure. Whereas, its stability range expanded toward lower temperatures by 20 K and a band gap slightly increased, from 1.59 to 1.625 eV (at 290 K). Using this organic-inorganic perovskite as an example, we show how the phase stability of such materials can be manipulated by creation and elimination of structural defects and local strains.

Investigating the effect of Zn doping and temperature on the photoluminescence behaviour of CuLaSe2 quantum dots.

In this study, CuLaSe2 and ZnCuLaSe2 quantum dots (QDs) with a mean size of ~4nm were synthesized and characterized, and their temperature-dependent photoluminescence (PL) properties were studied in the temperature range from 90 to 300 K for the first time. The results show that the obtained QDs were spherical and revealed excitonic band gaps. The PL intensity for both types of materials decreased when increasing the temperature to 300 K, which was attributed to the nonradiative relaxation and thermal escape mechanisms. As the temperature was increased, the PL linewidths broadened, and PL peak energies were red shifted for both types of QDs due to the exciton-phonon coupling and lattice deformation potential mechanisms. In addition, we found that as the temperature was decreased, the PL spectrum of ZnCuLaSe2 QDs contained two extra components, which could be attributed to the shallow defect sites (low energy peak) and the crystal phase transition process (high energy peak). The spectrum of CuLaSe2 QDs contained one extra component, which could be attributed to the crystal phase transition process.

Investigating the use of Er3+ doped β-Ca2SiO4 phosphors derived from agricultural waste for thermal sensing and forensic applications

Leveraging agricultural waste, Erbium (Er3+) doped β-Ca2SiO4 phosphors (β-CS:Er3+) with concentrations ranging from 1 to 9 mol % were developed using the solid-state reaction method. These β-CS:Er3+ samples underwent extensive characterization to examine their crystalline structure, surface morphology, photoluminescence (PL) properties, and thermal sensing capabilities. The PL emission, excited at 378 nm, prominently displayed a peak at 549 nm, indicative of the green emission primarily due to the 4S3/2 → 4I15/2 transition. An optimal concentration of Er3+ at 5 mol% (β-CS:5Er3+) is identified, showing peak luminescence intensity, whereas, higher concentrations led to a decrease in intensity because of concentration quenching (CQ) effects. Temperature-dependent photoluminescence (TDPL) analysis revealed an increase in emission intensity at 523 nm, while the peak at 549 nm exhibited a decrease in intensity within the temperature range of 303–463 K. Nevertheless, the emission peak at 549 nm demonstrates remarkable thermal stability at elevated temperatures, maintaining 79.32% of its emission intensity at 423 K. The optimized β-CS:5Er3+ phosphor exhibited its chromaticity coordinates (0.3152, 0.6631) in the green region under 378 nm excitation, alongside promising temperature sensing capabilities with a relative sensitivity of 2.80 % K−1. The application of these phosphors in a powder dusting technique for revealing latent fingerprints (LFPs) and latent lip prints (LLPs) under 365 nm UV light uncovered detailed ridge and groove patterns on various substrates. This approach, highlighting the phosphor's exceptional fluorescence, dual adherence, and non-interfering background, showcased its potential for enhanced forensic analysis. The thorough examination of LFPs and LPs under various conditions, including aging, heat, and UV exposure, confirms the β-CS:Er3+ NPs' suitability for cutting-edge display technologies and forensic methodologies.

Superior Phonon-Limited Exciton Mobility in Lead-Free Two-Dimensional Perovskites.

Tin-based two-dimensional (2D) perovskites are emerging as lead-free alternatives in halide perovskite materials, yet their exciton dynamics and transport remain less understood due to defect scattering. Addressing this, we employed temperature-dependent transient photoluminescence (PL) microscopy to investigate intrinsic exciton transport in three structurally analogous Sn- and Pb-based 2D perovskites. Employing conjugated ligands, we synthesized high-quality crystals with enhanced phase stability at various temperatures. Our results revealed phonon-limited exciton transport in Sn perovskites, with diffusion constants increasing from 0.2 cm2 s-1 at room temperature to 0.6 cm2 s-1 at 40 K, and a narrowing PL line width. Notably, Sn-based perovskites exhibited greater exciton mobility than their Pb-based equivalents, which is attributed to lighter effective masses. Thermally activated optical phonon scattering was observed in Sn-based compounds but was absent in Pb-based materials. These findings, supported by molecular dynamics simulations, demonstrate that the phonon scattering mechanism in Sn-based halide perovskites can be distinct from their Pb counterparts.

Exploring potential of quantum dots for high power solid-state lighting protected by transparent ceramics

When quantum dot diffusion plates (QDDPs) are used as phosphor conversion materials for high-power lighting, transparent ceramics (TCs) can be used to prevent thermal damage of QDDPs. The spectral, suitable for diverse lighting environments, can be precisely calibrated by modifying their ratio. The temperature dependent photoluminescence spectra, fluorescence lifetime, Huang Rhys factor and activation energy of TCs were studied in detail. It was evident from the results that the intensity of TCs remained above 89% even at 423 K, while fluorescence lifetime remained stable, nearly 64 ns. Huang-Rhys factor and activation energy were consistently measured at 1.81 and 0.13 eV, respectively. The extraordinary luminescent stability of TCs revealed their integral role in providing reliable protection for QDDPs. The spectra of LEDs/LDs were successfully predicted using Monte Carlo ray tracing method. The service condition under high-energy laser was studied using finite element method. White light with Commission Internationale de l'Eclairage (CIE) of (0.38, 0.39) and (0.31, 0.34) and luminous efficiency of 58 and 150 lm/W were prepared by combining QDDPs/TCs with LEDs/LDs, and the Color Rendering Index (CRI) reached a remarkable 88.4 and 78.8. A detailed exploration of the proficient thermal management was accomplished using finite element analysis, with the simulated outcomes matching closely with the experimental results.

Simple hole transporting material based 2,7- carbazole for perovskite solar cells: Structural, photophysical, and theoretical studies

A simple carbazole-based hole transport material, termed HTM1, has been deposited as thin films. The samples were elaborated via a Physical Vapor Deposition to ensure the production of high-quality thin films. The study of the morphological and photophysical properties of the investigated compound was revealed through Scanning Electron Microscopy, Atomic Force Microscopy, Ultraviolet–Visible, and Photoluminescence spectroscopy. A flat surface with low roughness values was observed in the SEM and AFM images. Moreover, the obtained films revealed a higher absorption in the UV region. Optical parameters such as the energy gap (2.9 eV) and refractive index were determined using transmittance measurements. The temperature-dependent photoluminescence over a range of 77–300 K has also been investigated. It is found that, as the temperature decreases, a new emission band appears, which may be due to the formation of excimers. Added to that, theoretical investigation of the highest occupied molecular orbital, the lowest unoccupied molecular orbital, the density of states, and the optical energy gap were studied using density functional theory (DFT) with the hybrid B3LYP exchange-correlation function and the 6-311G (d,p) basis set. Absorption spectra was generated using the TD-DFT method. The absorption maximum obtained (398 nm) for HTM1 closely matched with the experimental value (393 nm). Following these characterizations, simulation studies on the photovoltaic performances of the HTM1 for perovskite solar cells have been done. This cell provided a maximum PCE of 21.31%.

Van der Waals epitaxy of CsPbBr3/WSe2 heterostructure and dynamics study of exciton recombination

Van der Waals heterostructures formed by inorganic perovskites and transition metal dichalcogenides (TMDCs) have promising applications in photonics and optoelectronics. However, there are few studies on the properties of CsPbBr3/TMDC at low temperatures. Here, we demonstrate van der Waals epitaxy of CsPbBr3 nanowires (NWs), nanoplates (NPs) and nanocones (NCs) on monolayer (ML) WSe2, and investigate the lattice dynamics of the heterostructure at low temperatures using temperature-dependent Raman spectroscopy. In addition, temperature-dependent photoluminescence (PL) spectroscopy shows that the type II band alignment between CsPbBr3 and ML WSe2 leads to a broad emission peak at the low-energy side of the ML WSe2 emission at low temperatures. Meanwhile, a high-energy peak appears near the CsPbBr3 emission below 133 K, which may be related to the phase transition of CsPbBr3 from the cubic to the orthorhombic phase. These findings are important for the development of van der Waals heterostructure based self-powered photodetector with high performance.

Photoluminescence Enhancement in Silica‐Confined Ligand‐Free Perovskite Nanocrystals by Suppression of Silanol‐Induced Traps and Phase Impurities

AbstractThe detriments of intrinsic silanol groups in mesoporous silica to the photoluminescence (PL) of lead halide perovskite nanocrystals (LHP NCs) confined in the template have never been determined and clearly elucidated. Here, we disclose that silanol‐induced Cs+ and Br− deficiencies prompt the generation of traps and CsPb2Br5 impurities. The temperature‐dependent PL spectra verify the higher energetic barrier of trap states in CsPbBr3 NCs confined in silanol‐rich mesoporous silica. Femtosecond transient absorption spectra reveal the trapped state mediates a broadband photoinduced absorption and long‐lived decay pathway of CsPbBr3 NCs in silanol‐rich templates. A remarkable improvement (up to 160‐fold) in PL quantum yields is realized by simple silanol elimination. This work demonstrates the detrimental effects of silanol sites on the PL properties of LHP NCs impregnated in mesoporous silica and provides a new perspective for the ligand‐free synthesis of high‐quality LHP NCs in mesoporous templates by facile impregnation for practical applications.

Ag-CsPbI3 nanocomposite structure in glasses boosts photoluminescence for efficient light emitting diodes

Nanocomposite structures based on perovskite nanocrystals (NCs) and metal nanostructures within transparent monolithic media hold promise for a wide range of applications in optoelectronics. However, the microstructure of such nanocomposites and the reason for enhanced emissions remain incompletely understood. In this work, we present the successful creation of Ag-CsPbI3 nanocomposite within a highly transparent borosilicate glass (Ag-CsPbI3 NCs@glass). We reveal that Ag and CsPbI3 NCs form after thermal treatment of the glass, either in the form of Ag-CsPbI3 heterostructures or of separate Ag and CsPbI3 NCs. Based on combined characterization of Mott-Schottky and steady-state photoluminescence (PL) of the products, we attribute the enhanced PL in the nanocomposite of Ag-CsPbI3 to the regulation of CsPbI3 lattice by Ag ions and/or the plasmonic effect of Ag NCs. Temperature-dependent time-resolved PL decay measurements suggest that Ag NCs could play an important role in the relaxation process of excited carriers by increasing the radiative recombination. Moreover, the Ag-CsPbI3 nanocomposite structure within the glass matrix curtails PL quenching caused by water molecules and high temperature. Using the Ag-CsPbI3 nanocomposite, we achieve high-performance white light-emitting diodes with a color rendering index of 83.9 and luminous efficiency of 58.07 lmW−1. This work elucidates the underlying mechanism on the enhanced PL in nanocomposites containing perovskite NCs and metal nanostructures, and aids in the rational design of glass-based perovskite nanocomposites for a diversity of optoelectronic applications.