Quantum Efficiency Research Articles

All-solution-processed perovskite-quantum-dot light-emitting diodes through effective synergistic combination of orthogonal solvent and electron transport material

Perovskite quantum dots (PQDs) have shown great promise for use in photovoltaic devices, due to their ability to offer advantages such as tunability of visible light and efficient light emission. This study demonstrates the successful utilization of a triazine-based PO-T2T (2,4,6-Tris[3(diphenylphosphenyl)phenyl]-1,3,5-triazine; PO-T2T) as the electron transport layer (ETL) through an all-solution process. To improve the structural and optical characterization of CsPbBr3 and CsPbI3 QDs, three organic solvents, namely chlorobenzene, methyl acetate, and ethyl acetate, were selected to find an effective orthogonal solvent for PO-T2T. The all-solution processed devices incorporating PO-T2T and Methyl acetate (MeOAc) demonstrated impressive external quantum efficiencies of 5.57% for CsPbBr3 and 1.60% for CsPbI3 QDs. Notably, these devices also achieved the highest maximum luminance among all-solution processed PQDs-LEDs, with values of 33334 cd m–2 for CsPbBr3 and 224 cd m–2 for CsPbI3 QDs.

Manipulating cationic ordering toward highly efficient and zero-thermal-quenching cyan photoluminescence

Developing effective design principle in crystalline materials for superior optical properties remains a critical challenge. Herein, we establish the cationic ordering strategy to build rigid framework and significantly improve phosphor performance. As a proof of concept, the NaHf2-xYx(PO4)3:Eu2+ (x = 0.05–0.2) phosphor series is constructed, which possesses absolutely cationic ordered structure and the linked outstanding photoluminescent properties. Structurally, heterovalent substitution in the lattice maintains the single-site occupancy of Na+ ions in NaHf2-xYx(PO4)3:Eu2+, as confirmed by Rietveld refinements and NMR spectroscopy. This cationic arrangement keeps the cation/vacancy ordered distribution that ensures high structural rigidity, with Debye temperature, as the indicator of rigidity, extracted from low temperature heat capacities exceeding 379 K. The resultant high structural rigidity, coupled with intrinsic defects, induces zero-thermal-quenching luminescence up to 150 °C. Moreover, the substitution of Y3+ at Hf4+ site facilitates effective Eu3+ to Eu2+ reduction, making them excellent cyan emitters with quantum efficiency exceeding 90 % and intense violet absorption. This work provides an impetus for the discovery of the currently state-of-the-art cyan phosphors for practical applications and gives insight into the structural factors influencing luminescent properties.

High External Quantum Efficiency and Dual-Band Emission of (C7H18N)3Sb2Cl9 for Sensitivity Temperature Sensing.

Organic-inorganic hybrid halides have gained attention for their ease of processing and remarkable optoelectronic properties. However, the relationship between the structure and optical properties requires further exploration. In this study, the butyltrimethylammonium cation (C7H18N+) was chosen, and seven compounds were synthesized: (C7H18N)3Sb2X9 (X = Cl, Br), (C7H18N)3Bi2X9 (X = Cl, Br, I), and (C7H18N)(C2H8N)MBr5 (M = Sb, Bi). Crystals with a single organic cation exhibit a zero-dimensional structure, while the introduction of dimethylamine ions increases the crystal dimensionality from zero-dimensional (C7H18N)3Sb2Br9 to one-dimensional (C7H18N)(C2H8N)SbBr5. Under 372 nm excitation, (C7H18N)3Sb2Cl9 showed broad orange-red single-band emission with a high photoluminescence quantum yield of 88.4% and an external quantum efficiency of up to 56.9%. A white light-emitting diode based on (C7H18N)3Sb2Cl9 achieved a high color rendering index of 96.3. Moreover, dual-band emission was observed in (C7H18N)3Sb2Cl9 under 308 nm excitation, which exhibits an absolute temperature sensitivity of 1.96 × 10-3 K-1 (320 K), and a flexible film was prepared by incorporating polydimethylsiloxane. This shows the promise of hybrid metal halides as photoluminescent materials and their possibilities for temperature sensing.

Modified Synthesis of Cs4PbBr6 for Enhanced Purity and Quantum Yield and for Exploring Its Potential as a High Stokes Shift Material for Down‐Conversion in Solar Cells

Energy demands have kept increasing in recent years due to expanding human activity. Silicon solar cells offer an attractive renewable energy source while their external quantum efficiency (EQE) can still be enhanced; one way of doing this is by applying a photon energy downshifting layer. Herein, Cs4PbBr6 is applied as a downshifting layer; the Cs4PbBr6 is synthesized in the form of colloidal nanoparticles, and several modifications are introduced to the synthesis process, resulting in the enhancement of the photoluminescence quantum yield, improving the particle size distribution and reducing the CsBr impurities which appear as a side product during the synthesis of Cs4PbBr6. The application of the produced modified particles in the form of thin films on the top of Si solar cells shows an enhancement of the (EQE) of the solar cells when compared to the unmodified particles.

Efficient, Color-Stable, Pure-Blue Light-Emitting Diodes Based on Aromatic Ligand-Engineered Perovskite Nanoplatelets.

Perovskite nanoplatelets (NPLs) show great potential for high-color-purity light-emitting diodes (LEDs) due to their narrow line width and high exciton binding energy. However, the performance of perovskite NPL LEDs lags far behind perovskite quantum dot-/film-based LEDs, owing to their material instability and poor carrier transport. Here, we achieved efficient and stable pure blue-emitting CsPbBr3 NPLs with outstanding optical and electrical properties by using an aromatic ligand, 4-bromothiophene-2-carboxaldehyde (BTC). The BTC ligands with thiophene groups can guide two-dimensional growth and inhibit out-of-plane ripening of CsPbBr3 NPLs, which, meanwhile, increases their structural stability via strongly interacting with PbBr64- octahedra. Moreover, aromatic structures with delocalized π-bonds facilitate charge transport, diminish band tail states, and suppress Auger processes in CsPbBr3 NPLs. Consequently, the LEDs demonstrate efficient and color-stable blue emissions at 465 nm with a narrow emission line width of 17 nm and a maximum external quantum efficiency (EQE) of 5.4%, representing the state-of-the-art CsPbBr3 NPL LEDs.

Quantum barriers engineering toward radiative and stable perovskite photovoltaic devices

Efficient photovoltaic devices must be efficient light emitters to reach the thermodynamic efficiency limit. Here, we present a promising prospect of perovskite photovoltaics as bright emitters by harnessing the significant benefits of photon recycling, which can be practically achieved by suppressing interfacial quenching. We have achieved radiative and stable perovskite photovoltaic devices by the design of a multiple quantum well structure with long (∼3 nm) organic spacers with oleylammonium molecules at perovskite top interfaces. Our L-site exchange process (L: barrier molecule cation) enables the formation of stable interfacial structures with moderate conductivity despite the thick barriers. Compared to popular short (∼1 nm) Ls, our approach results in enhanced radiation efficiency through the recursive process of photon recycling. This leads to the realization of radiative perovskite photovoltaics with both high photovoltaic efficiency (in-lab 26.0%, certified to 25.2%) and electroluminescence quantum efficiency (19.7 % at peak, 17.8% at 1-sun equivalent condition). Furthermore, the stable crystallinity of oleylammonium-based quantum wells enables our devices to maintain high efficiencies for over 1000 h of operation and >2 years of storage.

Self-powered stable high-performance UV–Vis–NIR broadband photodetector based on PVP-Cobalt@Carbon nanofibers/n-GaAs heterojunction

The self-powered PVP-Co@C nanofibers/n-GaAs heterojunction photodetector (HJPD) was fabricated by electrospinning of the nanofibers onto GaAs. An excellent rectification ratio of 6.60 × 106 was obtained from I–V measurements of the device in the dark. The I–V measurements of the fabricated device under 365 nm, 395 nm and 850 nm lights, as well as I–V measurements in visible light depending on the light intensity, were performed. The HJPD demonstrated excellent photodetection performance in terms of a good responsivity of ∼225 mA W−1 (at −1.72 V) and at zero bias, an impressive detectivity of 6.28 × 1012 Jones, and a high on/off ratio of 8.38 × 105, all at 365 nm wavelength. In addition, the maximum external quantum efficiency and NPDR values were 3495% (V = −1.72 V) and 2.60 × 1010 W−1 (V = 0.0 V), respectively, while the minimum NEP value was ∼10−14 W.Hz−1/2 for 365 nm at V = 0.V volts. The HJPD also exhibited good long-term stability in air after 30 d without any encapsulation.

Pattern‐Matched Polymer Ligpands Toward Near‐Perfect Synergistic Passivation for High‐Performance and Stable Br/Cl Mixed Perovskite Light‐Emitting Diodes

Mixed Br/Cl perovskite nanocrystals (PeNCs) exhibit bright pure‐blue emission benefiting for fulfilling the Rec. 2100 standard. However, phase segregation remains a significant challenge that severely affects the stability and emission spectrum of perovskite light‐emitting diodes (PeLEDs). Here, we demonstrate the optimization of the spacing between polydentate functional groups of polymer ligands to match the surface pattern of CsPbBr1.8Cl1.2 PeNCs, resulting in effective synergistic passivation effect and significant improvements in PeLED performances. The block and alternating copolymers with different inter‐functional group spacing are facilely synthesized as ligands for PeNCs. Surprisingly, block copolymers with a higher functional group density do not match PeNCs, while alternating copolymers enable efficient PeNCs with the high photoluminescence intensity, low non‐radiative recombination rate and high exciton binding energy. Density functional theory calculations clearly confirm the almost perfect match between alternating copolymers and PeNCs. Finally, pure‐blue PeLEDs are achieved with the emission at 467 nm and Commission Internationale de l'Eclairage (CIE) coordinates of (0.131, 0.071), high external quantum efficiency (9.1%) and record spectral and operational stabilities (~ 80 mins) in mixed‐halide PeLEDs. Overall, this study contributes to designing the polymer ligands and promoting the development of high‐performance and stable pure‐color PeLEDs towards display applications.

Pattern-Matched Polymer Ligpands Toward Near-Perfect Synergistic Passivation for High-Performance and Stable Br/Cl Mixed Perovskite Light-Emitting Diodes.

Mixed Br/Cl perovskite nanocrystals (PeNCs) exhibit bright pure-blue emission benefiting for fulfilling the Rec. 2100 standard. However, phase segregation remains a significant challenge that severely affects the stability and emission spectrum of perovskite light-emitting diodes (PeLEDs). Here, we demonstrate the optimization of the spacing between polydentate functional groups of polymer ligands to match the surface pattern of CsPbBr1.8Cl1.2 PeNCs, resulting in effective synergistic passivation effect and significant improvements in PeLED performances. The block and alternating copolymers with different inter-functional group spacing are facilely synthesized as ligands for PeNCs. Surprisingly, block copolymers with a higher functional group density do not match PeNCs, while alternating copolymers enable efficient PeNCs with the high photoluminescence intensity, low non-radiative recombination rate and high exciton binding energy. Density functional theory calculations clearly confirm the almost perfect match between alternating copolymers and PeNCs. Finally, pure-blue PeLEDs are achieved with the emission at 467 nm and Commission Internationale de l'Eclairage (CIE) coordinates of (0.131, 0.071), high external quantum efficiency (9.1%) and record spectral and operational stabilities (~ 80 mins) in mixed-halide PeLEDs. Overall, this study contributes to designing the polymer ligands and promoting the development of high-performance and stable pure-color PeLEDs towards display applications.

Recent advances and prospects for GaN-based hybrid type ultraviolet photodetector

Abstract Solid-state UV photodetectors (PD) have received numerous attention because of the advantages of small size, absence of external cooling, high selectivity, and the ability to utilize the energy band structure semiconductor materials to achieve detection across various wavelengths. III-nitride thin films, as typical wide bandgap semiconductors with mature n-type and p-type doping capabilities, are ideal candidates for solid-state UV-PDs. However, a combination between III-nitride and other wide bandgap materials can either enrich the functionality of such devices such as spectrum-selective and broadband UV detection, or offers opportunities to enhance device performance, including high photoresponsivity, high external quantum efficiency, low dark current and fast response time. This topical review focuses on giving a thorough review of the III-nitride based hybrid-type UV photodetectors, their recent progress and future prospects. This review highlights different optical and electrical properties of various materials including GaN, Ga2O3, ZnO, perovskite etc. By carefully choosing the materials on two sides of the heterojunction and modulating the thickness and fermi levels and corresponding layers, p-i-n, Schottky, or MSM type photodetectors were successfully fabricated with outstanding device performances and novel spectral-selective properties. The advantages for future development of such hybrid-type PDs will be discussed, such as inherently formed p-n junction with large depletion region at the interface of two different materials, capability of bandgap engineering to tune the band offset of conduction band and valence band, thus enabling large barrier height for one type of carrier without influencing the other. The drawbacks in hybrid-type UV-PD due to poor interface quality and challenges in forming electrical contact in nanostructure hybrid UV-PD will also be discussed.

Narrowband room temperature phosphorescence of closed-loop molecules through the multiple resonance effect

Luminescent materials with narrowband emission show great potential for diverse applications in optoelectronics. Purely organic phosphors with room-temperature phosphorescence (RTP) have made significant success in rationally manipulating quantum efficiency, lifetimes, and colour gamut in the past years, but there is limited attention on the purity of the RTP colours. Herein we report a series of closed-loop molecules with narrowband phosphorescence by multiple resonance effect, which significantly improves the colour purity of RTP. Phosphors show narrowband phosphorescence with full width at half maxima (FWHM) of 30 nm after doping into a rigid benzophenone matrix under ambient conditions, of which the RTP efficiency reaches 51.8%. At 77 K, the FWHM of phosphorescence is only 11 nm. Meanwhile, the colour of narrowband RTP can be tuned from sky blue to green with the modification of methyl groups. Additionally, the potential applications in X-ray imaging and display are demonstrated. This work not only outlines a design principle for developing narrowband RTP materials but also makes a major step forward extending the potential applications of narrowband luminescent materials in optoelectronics.

Intramolecular Hydrogen Bonding Rigidifying Flexible Bridge for Solution- and Vacuum-Processed TSCT-TADF Emitters.

To realize strong donor-acceptor face-to-face stacking for efficient through-space charge transfer-type thermally activated delayed fluorescence, a conceptually new design strategy is proposed to couple flexible bridges with adequate rigidity via built-in intramolecular hydrogen bonds (IHBs). The resulting emitter ACE-CN has a planarized benzyl methyl ether bridge self-anchored by the C-H···O IHB and shows a high photoluminescence quantum efficiency of 93%. The solution- and vacuum-processed devices exhibited high external quantum efficiencies of 11.8% and 24.7%, respectively.

Achieving Record External Quantum Efficiency of 11.5 % in Solution-Processable Deep-Blue Organic Light-Emitting Diodes Utilizing Hot Exciton Mechanism.

High performance solution-processable deep-blue emitters with a Commission International de l'Eclairage (CIE) coordinate of CIEy≤0.08 are highly desired in ultrahigh-definition display. Although, deep-blue materials with hybridized local and charge-transfer (HLCT) excited-state feature are promising candidates, their rigidity and planar molecular structures limit their application in solution-processing technique. Herein, four novel deep-blue solution-processable HLCT emitters were first proposed by attaching rigid imide aliphatic rings as functional units onto the HLCT emitting core. The functional units not only improve solubility, enhance thermal properties and morphological stability of the emitting core, but also promote photoluminescence efficiency, balance charge carrier transport, and inhibit aggregation-caused quenching effect due to the weak electron-withdrawing property as well as steric hindrance. The corresponding solution-processable organic light-emitting diodes (OLEDs) substantiate an unprecedented maximum external quantum efficiency (EQEmax) of 11.5 % with an emission peak at 456 nm and excellent colour purity (full width at half maximum=56 nm and CIEy=0.09). These efficiencies represent the state-of-the-art device performance among the solution-processable blue OLEDs based on the "hot exciton" mechanism. This simple strategy opens up a new avenue for designing highly efficient solution-processable deep-blue organic luminescent materials.

Achieving Record External Quantum Efficiency of 11.5 % in Solution‐Processable Deep‐Blue Organic Light‐Emitting Diodes Utilizing Hot Exciton Mechanism

AbstractHigh performance solution‐processable deep‐blue emitters with a Commission International de l′Eclairage (CIE) coordinate of CIEy≤0.08 are highly desired in ultrahigh‐definition display. Although, deep‐blue materials with hybridized local and charge‐transfer (HLCT) excited‐state feature are promising candidates, their rigidity and planar molecular structures limit their application in solution‐processing technique. Herein, four novel deep‐blue solution‐processable HLCT emitters were first proposed by attaching rigid imide aliphatic rings as functional units onto the HLCT emitting core. The functional units not only improve solubility, enhance thermal properties and morphological stability of the emitting core, but also promote photoluminescence efficiency, balance charge carrier transport, and inhibit aggregation‐caused quenching effect due to the weak electron‐withdrawing property as well as steric hindrance. The corresponding solution‐processable organic light‐emitting diodes (OLEDs) substantiate an unprecedented maximum external quantum efficiency (EQEmax) of 11.5 % with an emission peak at 456 nm and excellent colour purity (full width at half maximum=56 nm and CIEy=0.09). These efficiencies represent the state‐of‐the‐art device performance among the solution‐processable blue OLEDs based on the “hot exciton” mechanism. This simple strategy opens up a new avenue for designing highly efficient solution‐processable deep‐blue organic luminescent materials.

Enhanced photoluminescence characteristics in Mg doped Alq3: An insight into doping mechanism

The present paper deals with the investigations on the effect of Mg doping on the structural and photophysical properties of Alq3 thin films. Mg doped Alq3 powders, with varying Mg concentrations, are synthesized using co-precipitation method and their thin films are deposited using vacuum evaporation method. These films are subjected to different analytical analyses to study the effect of Mg doping on the structural and photophysical properties of Alq3. It has been observed that Mg is attached at the central part of the Alq3 molecules making bonds with Al, N and O atoms. In this process, Mg atoms transfer electrons to Alq3 molecules and increases the electron density in its highest occupied molecular orbital (HOMO). Increased HOMO electron density in Mg doped Alq3 results in the improvement in its photoluminescence characteristics. Highest photoluminescent characteristics are observed for Mg doped Alq3 having 1.5 % (by mole) Mg which shows almost 2-fold enhancement in photoluminescence quantum efficiency (PLQY) and 3-fold enhancement in radiative decay rate. The results obtained in this work suggest that Mg doped Alq3 films may be integrated in high performing organic light emitting devices.

Photodecarboxylative Ring Annulation of α‐ and β‐Functionalized Phthaloyl‐GABA Derivatives: Bioactive Pyrroloisoindolinones with High Quantum Efficiency

AbstractThe triplet‐sensitized (by the solvent acetone) as well as the direct (λex=300–320 nm) photochemical decarboxylation of N‐phthaloylated γ‐aminobutyric acid (GABA) derivatives are versatile and high‐yielding routes to benzopyrrolizidines via intramolecular electron transfer initiated decarboxylation followed by radical coupling. The ß‐mono‐ and ß,ß'‐disubstituted N‐phthaloyl GABA derivatives 7 a–7 g, respectively, were applied as substrates. Decarboxylative photocyclization yielded hydroxy benzopyrrolizidines 8 a–8 g in high chemical yields and with moderate diastereoselectivities from the ß‐monosubstituted substrates. The analogous α‐substituted GABA derivatives 11 a–11 c were also applied as potential substrates for memory of chirality effects. The reaction quantum yields of the photodecarboxylation reactions for the parent GABA derivative 13 and for the new substrates 7 h and 11 a were determined by the quantum yield determination system (QYDS) and showed a remarkable concentration dependency indicating aggregation at higher substrate concentrations. Inhibition studies on the atherogenic human serine hydrolase cholesterol esterase showed derivatives 8 a and 8 d to exhibit a hyperbolic mode of inhibition with moderate IC50 values of about 60–80 μM.

High-Efficiency Vertical-Chip Micro-Light-Emitting Diodes via p-GaN Optimization and Surface Passivation

Micro-LEDs have found widespread applications in modular large-screen TVs, automotive displays, and high-resolution-density augmented reality glasses. However, these micron-sized LEDs experience a significant efficiency reduction due to the defects originating from the dry etching process. By controlling the current distribution via engineering the electrode size, electrons will be less concentrated in the defect region. In this work, we propose a blue InGaN/GaN compound parabolic concentrator micro-LED with a metallic sidewall to boost efficiency by combining both an optical dipole cloud model and electrical TCAD (Technology Computer-Aided Design) model. By merely modifying the p-GaN contact size, the external quantum efficiency (EQE) can be improved by 15.6%. By further optimizing the passivation layer thickness, the EQE can be boosted by 52.1%, which helps enhance the display brightness or lower power consumption.

Constructing Multi‐Functional Polymeric‐Termination Surface Enables High‐Performance Flexible Perovskite LEDs

AbstractFlexible perovskite light‐emitting diodes (f‐PeLEDs) have attracted increasing interest to realize true‐color, low‐cost, and light‐weight wearable optoelectronic and flexible display applications. However, their external quantum efficiency (EQE) and mechanical stability lag far behind because of the inherent surface and brittle issues of polycrystalline perovskite films. In this work, a multi‐functional polymeric‐termination surface of perovskite film is constructed for achieving efficient and mechanically stable f‐PeLEDs. It takes the roles to not only reduce defects through equipping coordination groups to improve emission properties, but also optimize film morphology and eliminate pinholes to solve the long‐standing issue of leakage current. Meanwhile, the polymeric‐termination surface with anchoring points and polymeric soft chains on perovskites demonstrates synergetic effects beyond the corresponding functional group‐only or polymer‐only strategies in reducing the Young's modulus and improving the mechanical flexibility. Ultimately, the record EQE of 22.1% and significantly enhanced mechanical stability of maintaining 82% of the initial performance after 2000 bending cycles with radius of 5 mm are achieved in pure‐green f‐PeLEDs. The work paves the way for the development of high‐performance flexible optoelectronic devices.

Phosphonic Chloride Assisted Fabrication of Highly Emissive Mixed Halide Perovskite Films in Ambient Air for Blue Light-Emitting Diodes.

Blue perovskite light-emitting diodes (LEDs) have emerged as promising candidates for full-color display and lighting applications. However, the fabrication of blue-emitting perovskite films typically requires an inert environment, leading to increased complexity and cost in the manufacturing process, which is undesirable for applications of perovskite LEDs. Herein, we report a strategy to fabricate bright blue-emitting perovskite films in ambient air by incorporating phosphonic chlorides in a perovskite precursor solution. We used two different phosphonic chlorides, diphenylphosphonic chloride (DPPC) and phenylphosphonic dichloride (PPDC), and comparatively studied their effects on the properties of perovskite films and the blue LEDs. It is found that PPDC possesses a stronger chlorination ability due to higher hydrolysis reactivity; meanwhile, it has a stronger interaction with the perovskite compared to DPPC, resulting in an improved film quality and enhanced blue emission with a photoluminescence quantum yield of 45%, which represents the record value for the air-processed blue perovskite films. Blue perovskite LEDs are fabricated, and the emission wavelengths are effectively tuned by controlling the concentration of phosphonic chlorides. Benefiting from the optimized perovskite films with reduced nonradiative recombination and promoted charge injection and transport, the PPDC-derived blue perovskite LEDs exhibit improved performance with an external quantum efficiency of 3.3% and 1.2% for the 490 and 480 nm emission wavelength, respectively.

Mesoporous Pt/N−TiO2/Ti Photocatalytic Plate for Highly Efficient Hydrogen Production

AbstractMonolithic plate‐type photocatalyst with excellent light absorption, abundant active sites and strong mechanical adhesion is the growing trend of photocatalysis application, as referring to a photovoltaic panel. In this study, we report a large‐scale Pt/N−TiO2/Ti photocatalytic plate with granular and mesoporous structure, which shows a superior photocatalytic performance and adhesion than nanowires and nanosheets photocatalysts. The outstanding photocatalytic performance of Pt/N−TiO2/Ti is attributed to the large exposed surface area, enhanced light absorption, high separation efficiency of photogenerated carriers and excellent surface activity induced by single Pt atom cocatalyst. The best Pt/N−TiO2/Ti sample could exhibit an outstanding photocatalytic hydrogen production activity of 72547.9 μmol ⋅ h−1 ⋅ g−1, and a high apparent quantum efficiency of 47.07 % under a 350 nm light irradiation. It can be anticipated that the proposed method and insights would pave a solid way on the development and application of superior TiO2 based photocatalytic plate.