Perovskite light-emitting diodes based on solution-processed self-organized multiple quantum wells, Nature Photonics, 2016. 10(11) Encouraging performance metrics of light-emitting diodes (LEDs) based on 3Dperovskites, such as low turn-on voltages and external quantum efficiencies (EQEs) of up to 3.5% at high current densities, have been demonstrated 9 . However, the EL quantum efficiency is far behind the limit predicated by ~70% PLQE of the 3D perovskites, mainly due to the existence of current losses caused by incomplete surface coverage of the perovskite films and the fact that the high PLQE can only be obtained at high excitations 8,9 . By using thick (>300 nm) perovskite films, Cho et al.obtained LEDs with over 8% EQE 10 . However, for this device, the turn-on voltage is high and the power efficiency is low, which may result from the thick perovskite layer used. In order to further enhance the performance of 3D perovskite-based LEDs, it is 3 essential to obtain perovskite thin films with both complete surface coverage and high PLQE [8][9][10] . Moreover, device stability, which was proven to be a vital issue in organic-inorganic halide perovskite-based photovoltaics 11 , has not been addressed in perovskite LEDs.The 3D perovskites are actually an extreme case of layered organometal halide perovskites with a general formula of L2(SMX3)n-1MX4, where M, X, L, and S are a divalent metal cation, a halide, and organic cations with long and short chains, respectively ( Fig. 1a) [12][13][14] . Here n is the number of semiconducting MX4 monolayer sheets within the two organic insulating layers (cation L), with n=∞ corresponding to the structure of a 3D perovskite SMX3. With smaller numbers of MX4 layers, quantum confinement effects, such as an increase in bandgap and exciton energy, become important 6,15 . In consequence, the layered perovskites naturally form quantum-well structures. At the opposite extreme, when n=1, the layered perovskites form a monolayer structure of a two-dimensional (2D) perovskite L2MX4. The 2D L2MX4 perovskites generally have good film-formation properties 13 . Nevertheless, the PLQEs of the 2D perovskites are rather low at room temperature, owing to fast exciton quenching rates 6,7 . LEDs based on the 2D perovskites have been attempted, while the devices are either very low in efficiency or only operational at cryogenic temperatures [16][17][18] . Here we demonstrate very efficient (up to 11.7% EQE) and high-brightness EL achievable at room temperature by using solution-processed perovskite multiple quantum wells (MQWs) with an energy cascade, which can combine the advantages of 2D and 3D perovskites. We note, a relevant perovskite LED work 19 which shows a peak EQE of 8.8% has been published online during the revision of this paper.A precursor solution of 1-naphthylmethylamine iodide (NMAI), formamidinium iodide (FAI), and PbI2 with a molar ratio of 2:1:2 dissolved in N,N-dimethylformamide (DMF) was used to deposit perovskite films (see Methods for details), which are abbreviated as NFPI...
Perovskite-based optoelectronic devices have gained significant attention due to their remarkable performance and low processing cost, particularly for solar cells. However, for perovskite light-emitting diodes (LEDs), non-radiative charge carrier recombination has limited electroluminescence (EL) efficiency. Here we demonstrate perovskite-polymer bulk heterostructure LEDs exhibiting record-high external quantum efficiencies (EQEs) exceeding 20%, and an EL half-life of 46 hours under continuous operation. This performance is achieved with an emissive layer comprising quasi-2D and 3D perovskites and an insulating polymer. Transient optical spectroscopy reveals that photogenerated excitations at the quasi-2D perovskite component migrate to lower-energy sites within 1 ps. The dominant component of the photoluminescence (PL) is primarily bimolecular and is characteristic of the 3D regions. From PL quantum efficiency and transient kinetics of the emissive layer with/without charge-transport contacts, we find non-radiative recombination pathways to be effectively eliminated. Light outcoupling from planar LEDs, as used in OLED displays, generally limits EQE to 20-30%, and we model our reported EL efficiency of over 20% in the forward direction to indicate the internal quantum efficiency (IQE) to be close to 100%. Together with the low drive voltages needed to achieve useful photon fluxes (2-3 V for 0.1-1 mA cm -2 ), these results establish that perovskite-based LEDs have significant potential for light-emission applications.
Organic LEDs promise highly efficient lighting and display technologies. We introduce a new class of linear donor-bridge-acceptor light-emitting molecules, which enable solution-processed LEDs with near-100% internal quantum efficiency at high brightness. Key to this performance is their rapid and efficient utilization of triplet states. Using time-resolved spectroscopy, we establish that luminescence via triplets occurs within 350 ns at ambient temperature, after reverse intersystem crossing to singlets. We find that molecular geometries exist at which the singlet-triplet energy gap (exchange energy) is close to zero, such that rapid interconversion is possible. Calculations indicate that exchange energy is tuned by relative rotation of donor and acceptor moieties about the bridge. Unlike other low exchange energy systems, substantial oscillator strength is sustained at the singlet-triplet degeneracy point
The increasing prevalence of infectious diseases in recent decades has posed a serious threat to public health. Routes of transmission differ, but the respiratory droplet or airborne route has the greatest potential to disrupt social intercourse, while being amenable to prevention by the humble face mask. Different types of masks give different levels of protection to the user. The ongoing COVID-19 pandemic has even resulted in a global shortage of face masks and the raw materials that go into them, driving individuals to self-produce masks from household items. At the same time, research has been accelerated towards improving the quality and performance of face masks, e.g., by introducing properties such as antimicrobial activity and superhydrophobicity. This review will cover mask-wearing from the public health perspective, the technical details of commercial and home-made masks, and recent advances in mask engineering, disinfection, and materials and discuss the sustainability of mask-wearing and mask production into the future.
Human behaviors are extremely sophisticated, relying on the adaptive, plastic and event-driven network of sensory neurons. Such neuronal system analyzes multiple sensory cues efficiently to establish accurate depiction of the environment. Here, we develop a bimodal artificial sensory neuron to implement the sensory fusion processes. Such a bimodal artificial sensory neuron collects optic and pressure information from the photodetector and pressure sensors respectively, transmits the bimodal information through an ionic cable, and integrates them into post-synaptic currents by a synaptic transistor. The sensory neuron can be excited in multiple levels by synchronizing the two sensory cues, which enables the manipulating of skeletal myotubes and a robotic hand. Furthermore, enhanced recognition capability achieved on fused visual/haptic cues is confirmed by simulation of a multi-transparency pattern recognition task. Our biomimetic design has the potential to advance technologies in cyborg and neuromorphic systems by endowing them with supramodal perceptual capabilities.
Singlet fission offers the potential to overcome thermodynamic limits in solar cells by converting the energy of a single absorbed photon into two distinct triplet excitons. However, progress is limited by the small family of suitable materials, and new chromophore design principles are needed. Here, we experimentally vindicate the design concept of diradical stabilization in a tunable family of functionalized zethrenes. All molecules in the series exhibit rapid formation of a bound, spin-entangled triplet-pair state TT. It can be dissociated by thermally activated triplet hopping and exhibits surprisingly strong emission for an optically "dark" state, further enhanced with increasing diradical character. We find that the TT excited-state absorption spectral shape correlates with the binding energy between constituent triplets, providing a new tool to understand this unusual state. Our results reveal a versatile new family of tunable materials with excellent optical and photochemical properties for exploitation in singlet fission devices.
probability of a triplet pair forming a singlet) in solution is >60%, much higher than the spin-statistical prediction of 25% (one pair of triplets collides to form one of the four states: one singlet S 1 and three triplets T 1 , assuming higher triplet and quintet states are inaccessible). Practical application of solar energy conversion requires the TTA-UC material to be in solid state rather than in solution phase. However, the TTA-UC quantum yield of solidstate systems remains low, typically below 5%, [10] and is moderately high (about 10%) in only one example. [19] To achieve high efficiencies, high excitation intensities (200 mW cm −2 or above) are commonly required. These imply that in solid state, the experimentally observed reaction efficiency of TTA-UC was up to about 20%, below the 25% spin-statistical limit.To achieve highly efficient triplet fusion (TTA-UC) in OLEDs and other TTA upconverters, we consider four criteria for the selection of emitters: (1) high fluorescence quantum yield, (2) short singlet lifetime, (3) long triplet lifetime, and (4) the energy of two triplet excitons, 2E(T 1 ) lies slightly above that of the singlet exciton, E(S 1 ), but below the second triplet state, E(T 2 ) (and also the energies of any spin-quintet states) (E(S 1 ) ≲ 2E(T 1 ) < E(T 2 )). The first and second criteria are prerequisites for efficient fluorescence. The third criterion is essential for the accumulation of a sufficiently high triplet population density required for rapid triplet-triplet collision processes. The fourth criterion ensures that higher-lying triplet or quintet states do not provide loss channels. The spin states of the triplet excitons give in principle nine spin configurations for the interacting triplet exciton pair, five associated with a quintet, three with a triplet, and one with the singlet state. It is generally considered that the quintet is always higher in energy than the initial triplet pair, so is neglected. If there are no energetically accessible higher-lying triplet states at E(T 2 ), we expect only the S 1 and T 1 excitons to form. Triplets produced from this reaction can be recycled and participate in a further fusion reaction. [7] The basic working principle of a triplet fusion LED (FuLED) is illustrated in Figure 1a. The initial stage (Stage I) of the device operation includes charge injection and exciton formation. Exciton formation on the emissive molecules may occur directly or indirectly through an additional exciton transfer step from a host material. If a host material is present, the S 1 and T 1 of the host are required to be higher than that of the emitter to allow efficient host-emitter energy transfer and to ensure long triplet lifetime of the emitter (Criterion 3 discussed above). The 25% singlet population can be converted to light emission (and nonradiative losses) from the singlet channel immediately, resulting in prompt electroluminescence (EL). The 75% triplet excitons remain nonemissive, but the population of triplets is When an organic light-emitting dio...
on mononuclear silver. [7] Indeed, OLED devices based on 2nd row metals in general are remarkably rare and characterized by low efficiency. [8] Here, we report silver complexes with sub-microsecond radiative triplet lifetimes and high performance in both solution and vacuum-deposited OLED devices.Complexes 1 and 2 were readily obtained from ( Ad L)AgCl [3] and carbazole/NaO t Bu as off-white (1) or yellow (2) solids (Figure 1). The compounds are stable for long periods of time both in air and in solution in nonprotic organic solvents. Unlike many silver complexes, they are not sensitive to ambient light. Thermogravimetric analysis gives decomposition temperatures (5% weight loss) of 264.8 (1) and 263.6 °C (2). The observation of the 13 C(carbene) NMR signal (δ C 263) as two sharp 13 C 109 Ag and 13 C 107 Ag coupled doublets (J AgC = 219 and 189 Hz, respectively) confirmed that the complexes do not undergo carbene ligand exchange. [9] Single crystal X-ray diffraction of 1 and 2 confirmed the mononuclear two-coordinate geometry and the absence of significant intermolecular contacts. The C1(CAAC)···N2(Cz) distance is of prime importance since it is directly related to the highest occupied molecular orbital (HOMO)-lowest unoccupied molecular orbital (LUMO) overlap, which impacts on the radiative rate and exchange energy of (carbene)metal amides; this distance is slightly longer for 1 (4.152 Å) than for 2 (4.125 Å).Both 1 and 2 show a quasi-reversible one-electron metalcentered reduction process (tetrahydrofuran (THF) solution, [ n Bu 4 N]PF 6 as supporting electrolyte; Figures S2 and S3 and Table S1, Supporting Information). The estimated LUMO energies (1: −2.86 eV; 2: −2.83 eV) compare well with those for the Au (−2.79 eV) and Cu analogs (−2.66 eV) [5] and are only marginally affected by the nature of the metal. The peak-to-peak separation ΔE p is smaller for 2 (124 mV) than for 1 (185 mV), indicating higher stability of the reduced species of 2, potentially making it a more robust emitter under electrical excitation. The HOMO levels based on the onset of the first oxidation potentials are at −5.51 and −5.29 eV for 1 and 2, respectively. These values guide the identification of host materials for OLED fabrication. [10] The electronic structure of 1 and 2 has been evaluated using density-functional theory (DFT) for the ground state and timedependent DFT (TD-DFT) [11] calculations for the excited states using the MN15 functional by Truhlar and co-workers [12] in combination with def2-TZVP basis set by Ahlrichs and Carbene metal amides are a new class of highly efficient light-emitting molecules based on a linear donor-metal-acceptor geometry. Here the synthesis, structure, and photo-and electroluminescence of carbene silver carbazolato complexes, ( Ad L)Ag(Cz) [ Ad L = adamantyl-substituted cyclic (alkyl)(amino) carbene; Cz = carbazolate (1) and 3,6-t Bu 2 Cz (2)], are reported. They display green emission with photoluminescence quantum yields of up to 74%. Efficient mixing of triplet and singlet excited states is o...
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