Dimensional and Doping Engineering of Chiral Perovskites with Enhanced Spin Selectivity for Green Emissive Spin Light-Emitting Diodes.

Chiral perovskites play a pivotal role in spintronics and optoelectronic systems attributed to their chiral-induced spin selectivity (CISS) effect. Specifically, they allow for spin-polarized charge transport in spin light-emitting diodes (LEDs), yielding circularly polarized electroluminescence at room temperature without external magnetic fields. However, chiral lead bromide-based perovskites have yet to achieve high-performance green emissive spin-LEDs, owing to limited CISS effects and charge transport. Herein, we employ dimensional regulation and Sn2+-doping to optimize chiral bromide-based perovskite architecture for green emissive spin-LEDs. The optimized (PEA)x(S/R-PRDA)2-xSn0.1Pb0.9Br4 chiral perovskite film exhibits an enhanced CISS effect, higher hole mobility, and better energy level alignment with the emissive layer. These improvements allow us to fabricate green emissive spin-LEDs with an external quantum efficiency (EQE) of 5.7% and an asymmetry factor |gCP-EL| of 1.1 × 10-3. This work highlights the importance of tailored perovskite architectures and doping strategies in advancing spintronics for optoelectronic applications.

Surface heterojunction based on n-type low-dimensional perovskite film for highly efficient perovskite tandem solar cells.

Enhancing the quality of junctions is crucial for optimizing carrier extraction and suppressing recombination in semiconductor devices. In recent years, metal halide perovskite has emerged as the most promising next-generation material for optoelectronic devices. However, the construction of high-quality perovskite junctions, as well as characterization and understanding of their carrier polarity and density, remains a challenge. In this study, using combined electrical and spectroscopic characterization techniques, we investigate the doping characteristics of perovskite films by remote molecules, which is corroborated by our theoretical simulations indicating Schottky defects consisting of double ions as effective charge dopants. Through a post-treatment process involving a combination of biammonium and monoammonium molecules, we create a surface layer of n-type low-dimensional perovskite. This surface layer forms a heterojunction with the underlying 3D perovskite film, resulting in a favorable doping profile that enhances carrier extraction. The fabricated device exhibits an outstanding open-circuit voltage (VOC) up to 1.34 V and achieves a certified efficiency of 19.31% for single-junction wide-bandgap (1.77 eV) perovskite solar cells, together with significantly enhanced operational stability, thanks to the improved separation of carriers. Furthermore, we demonstrate the potential of this wide-bandgap device by achieving a certified efficiency of 27.04% and a VOC of 2.12 V in a perovskite/perovskite tandem solar cell configuration.

Stable and efficient pure blue quantum-dot LEDs enabled by inserting an anti-oxidation layer.

The efficiency and stability of red and green quantum-dot light-emitting diodes have already met the requirements for commercialization in displays. However, the poor stability of the blue ones, particularly pure blue color, is hindering the commercialization of full-color quantum-dot light-emitting diode technology. Severe hole accumulation at the blue quantum-dot/hole-transport layer interface makes the hole-transport layer prone to oxidation, limiting the device operational lifetime. Here, we propose inserting an anti-oxidation layer (poly(p-phenylene benzobisoxazole)) between this interface to take in some holes from the hole-transport layer, which mitigates the oxidation-induced device degradation, enabling a T50 (time for the luminance decreasing by 50%) of more than 41,000 h with an initial brightness of 100 cd m-2 in pure blue devices. Meanwhile, the inserted transition layer facilitates hole injection and helps reduce electron leakage, leading to a peak external quantum efficiency of 23%.

Enhanced Spin Polarization from Biaxially Strained Colloidal Quantum Dots.

Electron and hole spin polarization is crucial for quantum dots to be used in spin lasers and quantum information processing. However, the degree of spin polarization in II-VI and III-V semiconductor quantum dots is low because of the degenerated valence band. Here, we increase the light and heavy hole degeneracy by introducing biaxial strain into CdSe-based quantum dots, enabling the degree of spin polarization to be increased from 20% to 50% under photoexcitation. The optical gain threshold measurement further reveals that the increase in polarization helps to reduce the gain threshold.

Efficient All-Perovskite Tandem Solar Cells with Low-Optical-Loss Carbazolyl Interconnecting Layers.

Combining wide-band gap (WBG) and narrow-band gap (NBG) perovskites with interconnecting layers (ICLs) to construct monolithic all-perovskite tandem solar cell is an effective way to achieve high power conversion efficiency (PCE). However, optical losses from ICLs need to be further reduced to leverage the full potential of all-perovskite tandem solar cells. Here, metal oxide nanocrystal layers anchored with carbazolyl hole-selective-molecules (CHs), which exhibit much lower optical loss, is employed to replace poly(3,4-ethylenedioxythiophene) polystyrenesulfonate (PEDOT : PSS) as the hole transporting layers (HTLs) in lead-tin (Pb-Sn) perovskite sub-cells and ICLs in all-perovskite tandem solar cells. Optically transparent indium tin oxide nanocrystals (ITO NCs) layers are employed to enhance anchoring of CHs, while a mixture of two CHs is adopted to tune the surface energy-levels of ITO NCs. The optimized mixed Pb-Sn NBG perovskite solar cells demonstrate a high PCE of 23.2 %, with a high short-circuit current density (Jsc ) of 33.5 mA cm-2 . A high PCE of 28.1 % is further obtained in all-perovskite tandem solar cells, with the highest Jsc of 16.7 mA cm-2 to date. Encapsulated tandem solar cells maintain 90 % of their reference point after 500 h of operation at the maximum power point (MPP) under 1-Sun illumination.

Minimizing heat generation in quantum dot light-emitting diodes by increasing quasi-Fermi-level splitting.

Minimizing heat accumulation is essential to prolonging the operational lifetime of quantum dot light-emitting diodes (QD-LEDs). Reducing heat generation at the source is the ideal solution, which requires high brightness and quantum efficiency at low driving voltages. Here we propose to enhance the brightness of QD-LEDs at low driving voltages by using a monolayer of large QDs to reduce the packing number in the emitting layer. This strategy allows us to achieve a higher charge population per QD for a given number of charges without charge leakage, enabling enhanced quasi-Fermi-level splitting and brightness at low driving voltage. Due to the minimized heat generation, these LEDs show a high power conversion efficiency of 23% and a T95 operation lifetime (the time for the luminance to decrease to 95% of the initial value) of more than 48,000 h at 1,000 cd m-2.

All-perovskite tandem solar cells with 3D/3D bilayer perovskite heterojunction.

All-perovskite tandem solar cells promise higher power-conversion efficiency (PCE) than single-junction perovskite solar cells (PSCs) while maintaining a low fabrication cost1-3. However, their performance is still largely constrained by the subpar performance of mixed lead-tin (Pb-Sn) narrow-bandgap (NBG) perovskite subcells, mainly because of a high trap density on the perovskite film surface4-6. Although heterojunctions with intermixed 2D/3D perovskites could reduce surface recombination, this common strategy induces transport losses and thereby limits device fill factors (FFs)7-9. Here we develop an immiscible 3D/3D bilayer perovskite heterojunction (PHJ) with type II band structure at the Pb-Sn perovskite-electron-transport layer (ETL) interface to suppress the interfacial non-radiative recombination and facilitate charge extraction. The bilayer PHJ is formed by depositing a layer of lead-halide wide-bandgap (WBG) perovskite on top of the mixed Pb-Sn NBG perovskite through a hybrid evaporation-solution-processing method. This heterostructure allows us to increase the PCE of Pb-Sn PSCs having a 1.2-µm-thick absorber to 23.8%, together with a high open-circuit voltage (Voc) of 0.873 V and a high FF of 82.6%. We thereby demonstrate a record-high PCE of 28.5% (certified 28.0%) in all-perovskite tandem solar cells. The encapsulated tandem devices retain more than 90% of their initial performance after 600 h of continuous operation under simulated one-sun illumination.

Self-Assembled and Wavelength-Tunable Quantum Dot Whispering-Gallery-Mode Lasers for Backlight Displays.

Thanks to the narrow line width and high brightness, colloidal quantum dot (CQD) lasers show promising applications in next-generation displays. However, CQD laser-based displays have yet to be demonstrated because of two challenges in integrating red, green, and blue (RGB) lasers: absorption from red CQDs deteriorates the optical gain of blue and green CQDs, and imbalanced white spectra lack blue lasing due to the high lasing threshold of blue CQDs. Herein, we introduce a facile surfactant-free self-assembly method to assemble RGB CQDs into high-quality whispering-gallery-mode (WGM) RGB lasers with close lasing thresholds among them. Moreover, these RGB lasers can lase nearly independently even when they are closely integrated, and they can construct an ultrawide color space whose color gamut is 105% of that of the BT.2020 standard. These combined strategies allow us to demonstrate the first full-color liquid crystal displays using CQD lasers as the backlight source.

A library of polytypic copper-based quaternary sulfide nanocrystals enables efficient solar-to-hydrogen conversion.

Designing polytypic homojunction is an efficient way to regulate photogenerated electrons and holes, thereafter bringing desired physical and chemical properties and being attractive photocatalysts for solar-to-hydrogen conversion. However, the high-yield and controllable synthesis of well-defined polytypes especially for multinary chalcogenide - the fundamental factor favoring highly efficient solar-to-hydrogen conversion - has yet to be achieved. Here, we report a general colloidal method to construct a library of polytypic copper-based quaternary sulfide nanocrystals, including Cu2ZnSnS4, Cu2CdSnS4, Cu2CoSnS4, Cu2MnSnS4, Cu2FeSnS4, Cu3InSnS5 and Cu3GaSnS5, which can be synthesized by selective epitaxial growth of kesterite phase on wurtzite structure. Besides, this colloidal method allows the precise controlling of the homojunction number corresponding to the photocatalytic performance. The single-homojunction and double-homojunction polytypic Cu2ZnSnS4 nanocrystal photocatalysts show 2.8-fold and 3.9-fold improvement in photocatalytic hydrogen evolution rates relative to the kesterite nanocrystals, respectively. This homojunction existed in the polytypic structure opens another way to engineer photocatalysts.

Biomimetic non-classical crystallization drives hierarchical structuring of efficient circularly polarized phosphors.

Hierarchically structured chiral luminescent materials hold promise for achieving efficient circularly polarized luminescence. However, a feasible chemical route to fabricate hierarchically structured chiral luminescent polycrystals is still elusive because of their complex structures and complicated formation process. We here report a biomimetic non-classical crystallization (BNCC) strategy for preparing efficient hierarchically structured chiral luminescent polycrystals using well-designed highly luminescent homochiral copper(I)-iodide hybrid clusters as basic units for non-classical crystallization. By monitoring the crystallization process, we unravel the BNCC mechanism, which involves crystal nucleation, nanoparticles aggregation, oriented attachment, and mesoscopic transformation processes. We finally obtain the circularly polarized phosphors with both high luminescent efficiency of 32% and high luminescent dissymmetry factor of 1.5 × 10-2, achieving the demonstration of a circularly polarized phosphor converted light emitting diode with a polarization degree of 1.84% at room temperature. Our designed BNCC strategy provides a simple, reliable, and large-scale synthetic route for preparing bright circularly polarized phosphors.

Enhanced emission directivity from asymmetrically strained colloidal quantum dots.

Current state-of-the-art quantum dot light-emitting diodes have reached close to unity internal quantum efficiency. Further improvement in external quantum efficiency requires more efficient photon out-coupling. Improving the directivity of the photon emission is considered to be the most feasible approach. Here, we report improved emission directivity from colloidal quantum dot films. By growing an asymmetric compressive shell, we are able to lift their band-edge state degeneracy, which leads to an overwhelming population of exciton with in-plane dipole moment, as desired for high-efficiency photon out-coupling. The in-plane dipole proportion determined by back-focal plane imaging method is 88%, remarkably higher than 70% obtained from conventional hydrostatically strained colloidal quantum dots. Enhanced emission directivity obtained here opens a path to increasing the external quantum efficiencies notably.

Evaluating Lead Halide Perovskite Nanocrystals as a Spin Laser Gain Medium.

Spin-polarized charge endows conventional lasers with not only new functionalities but also reduced lasing thresholds thanks to the lifting of spin degeneracy. II-VI and III-V semiconductors have been extensively investigated as spin laser gain mediums; however, the degree of polarization is limited by the light hole and heavy hole degeneracy. Herein, we evaluate the potential of CsPbBr3 nanocrystals─ones that are featured with low band-edge degeneracy and therefore a high degree of polarization as a result of inverted band structure and large spin-orbit coupling─as a gain medium for spin lasers. Our experiment and numerical modeling results reveal that, within the spin relaxation lifetime, the optical gain threshold can be depressed by polarizing the charge using circularly polarized photoexcitation. However, prolonging the spin relaxation lifetime is required to realize a spin laser.

Optical-Gain-based Sensing Using Inorganic-Ligand-Passivated Colloidal Quantum Dots.

Thanks to their extremely large surface-to-volume ratio, colloidal quantum dots are potential high-performance sensing materials. However, previous sensing works using their spontaneous emission suffer from low sensitivities. The absence of an amplification process and the presence of the steric hindrance of long-chain organic ligands are two possible causations. Herein we propose that these two issues can be circumvented by using the amplified spontaneous emission of colloidal quantum dots capped by short-chain inorganic ligands. To exemplify this concept, we performed humidity sensing and observed a ∼31 times enhancement in sensitivity. Meanwhile, we found that the amplified spontaneous emission threshold power was reduced by 34% in a high humidity environment. On the basis of our transient absorption measurements, we attribute these observations to the mitigation of ultrafast subpicosecond trapping processes, which are enabled by the absorption of water molecules.

Bulk-like ZnSe Quantum Dots Enabling Efficient Ultranarrow Blue Light-Emitting Diodes.

Blue-emitting heavy-metal free QDs simultaneously exhibiting photoluminescence quantum yield close to unity and narrow emission line widths are essential for next-generation electroluminescence displays, yet their synthesis is highly challenging. Herein, we develop the synthesis of blue-emitting QDs by growing a thin shell of ZnS on ZnSe cores with their size larger than bulk Bohr diameter. The bulk-like size of ZnSe cores enables the emission to locate in the blue region with a narrow emission width close to its intrinsic peak width. The obtained bulk-like ZnSe/ZnS core/shell QDs display high quantum yield of 95% and extremely narrow emission width of ∼9.6 nm. Moreover, the bulk-like size of ZnSe cores reduces the energy level difference between QDs and adjacent layers in LEDs and improves charge transport. The LEDs fabricated with these high-quality QDs show bright pure blue emission with an external quantum efficiency of 12.2% and a relatively long operating lifetime.

One-Dimensional Superlattice Heterostructure Library.

Axially, epitaxially organizing nano-objects of distinct compositions and structures into superlattice nanowires enables full utilization of sunlight, readily engineered band structures, and tunable geometric parameters to fit carrier transport, thus holding great promise for optoelectronics and solar-to-fuel conversion. To maximize their efficiency, the general and high-precision synthesis of colloidal axial superlattice nanowires (ASLNWs) with programmable compositions and structures is the prerequisite; however, it remains challenging. Here, we report an axial encoding methodology toward the ASLNW library with precise control over their compositions, dimensions, crystal phases, interfaces, and periodicity. Using a predesigned, editable nanoparticle framework that offers the synthetic selectivity, we are able to chemically decouple adjacent sub-objects in ASLNWs and thus craft them in a controlled approach, yielding a library of distinct ASLNWs. We integrate therein plasmonic, metallic, or near-infrared-active chalcogenides, which hold great potential in solar energy conversion. Such synthetic capability enables a performance boost in target applications, as we report order-of-magnitude enhanced photocatalytic hydrogen production rates using optimized ASLNWs compared to corresponding solo objects. Furthermore, it is expected that such unique superlattice nanowires could bring out new phenomena.

Single crystalline quaternary sulfide nanobelts for efficient solar-to-hydrogen conversion.

Although solar-driven water splitting on semiconductor photocatalysts is an attractive route for hydrogen generation, there is a lack of excellent photocatalysts with high visible light activity. Due to their tunable bandgaps suitable for superior visible-light absorption, copper-based quaternary sulfides have been the important candidates. Here, we first assessed the preferred facet of wurtzite Cu-Zn-In-S for photocatalytic hydrogen evolution reaction using the relevant Gibbs free energies determined by first principle calculation. We then developed a colloidal method to synthesize single crystalline wurtzite Cu-Zn-In-S nanobelts (NBs) exposing (0001) facet with the lowest reaction Gibbs energy, as well as Cu-Zn-Ga-S NBs exposing (0001) facet. The obtained single crystalline Cu-Zn-In-S and Cu-Zn-Ga-S NBs exhibit superior hydrogen production activities under visible-light irradiation, which is composition-dependent. Our protocol represents an alternative surface engineering approach to realize efficient solar-to-chemical conversion of single crystalline copper-based multinary chalcogenides.

Quantum Dot-Plasmon Lasing with Controlled Polarization Patterns.

The tailored spatial polarization of coherent light beams is important for applications ranging from microscopy to biophysics to quantum optics. Miniaturized light sources are needed for integrated, on-chip photonic devices with desired vector beams; however, this issue is unresolved because most lasers rely on bulky optical elements to achieve such polarization control. Here, we report on quantum dot-plasmon lasers with engineered polarization patterns controllable by near-field coupling of colloidal quantum dots to metal nanoparticles. Conformal coating of CdSe-CdS core-shell quantum dot films on Ag nanoparticle lattices enables the formation of hybrid waveguide-surface lattice resonance (W-SLR) modes. The sidebands of these hybrid modes at nonzero wavevectors facilitate directional lasing emission with either radial or azimuthal polarization depending on the thickness of the quantum dot film.

Highly Luminescent Copper Iodide Cluster Based Inks with Photoluminescence Quantum Efficiency Exceeding 98.

Highly luminescent inks are desirable for various applications such as decorative coating, art painting, and anticounterfeiting, to name a few. However, present inks display low photoluminescent efficiency requiring a strong excitation light to make them glow. Here, we report a highly luminescent ink based on the copper-iodide/1-Propyl-1,4-diazabicyclo[2.2.2]octan-1-ium (Cu4I6(pr-ted)2) hybrid cluster with a quantum efficiency exceeding 98%. Under the interaction between the Cu4I6(pr-ted)2 hybrid cluster and polyvinylpyrrolidone (PVP), the highly luminescent Cu4I6(pr-ted)2/PVP ink can be facilely prepared via the one-pot solution synthesis. The obtained ink exhibits strong green light emission that originates from the efficient phosphorescence of Cu4I6(pr-ted)2 nanocrystals. Attractively, the ink displays high conversion efficiency for the ultraviolet light to bright green light emission due to its wide Stokes shift, implying great potential for anticounterfeiting and luminescent solar concentrator coating.

Engineering Directionality in Quantum Dot Shell Lasing Using Plasmonic Lattices.

We report how the direction of quantum dot (QD) lasing can be engineered by exploiting high-symmetry points in plasmonic nanoparticle (NP) lattices. The nanolaser architecture consists of CdSe-CdS core-shell QD layers conformally coated on two-dimensional square arrays of Ag NPs. Using waveguide-surface lattice resonances (W-SLRs) near the Δ point in the Brillouin zone as optical feedback, we achieved lasing from the gain in CdS shells at off-normal emission angles. Changing the periodicity of the plasmonic lattices enables other high-symmetry points (Γ or M) of the lattice to overlap with the QD shell emission, which facilitates tuning of the lasing direction. We also increased the thickness of the QD layer to introduce higher-order W-SLR modes with additional avoided crossings in the band structure, which expands the selection of cavity modes for any desired lasing emission angle.