The high conversion efficiency has made metal halide perovskite solar cells a real breakthrough in thin film photovoltaic technology in recent years. Here, we introduce a straightforward strategy to reduce the level of electronic defects present at the interface between the perovskite film and the hole transport layer by treating the perovskite surface with different types of ammonium salts, namely ethylammonium, imidazolium and guanidinium iodide. We use a triple cation perovskite formulation containing primarily formamidinium and small amounts of cesium and methylammonium. We find that this treatment boosts the power conversion efficiency from 20.5% for the control to 22.3%, 22.1%, and 21.0% for the devices treated with ethylammonium, imidazolium and guanidinium iodide, respectively. Best performing devices showed a loss in efficiency of only 5% under full sunlight intensity with maximum power tracking for 550 h. We apply 2D- solid-state NMR to unravel the atomic-level mechanism of this passivation effect.
Chemical doping of inorganic–organic hybrid perovskites is an effective way of improving the performance and operational stability of perovskite solar cells (PSCs). Here we use 5-ammonium valeric acid iodide (AVAI) to chemically stabilize the structure of α-FAPbI3. Using solid-state MAS NMR, we demonstrate the atomic-level interaction between the molecular modulator and the perovskite lattice and propose a structural model of the stabilized three-dimensional structure, further aided by density functional theory (DFT) calculations. We find that one-step deposition of the perovskite in the presence of AVAI produces highly crystalline films with large, micrometer-sized grains and enhanced charge-carrier lifetimes, as probed by transient absorption spectroscopy. As a result, we achieve greatly enhanced solar cell performance for the optimized AVA-based devices with a maximum power conversion efficiency (PCE) of 18.94%. The devices retain 90% of the initial efficiency after 300 h under continuous white light illumination and maximum-power point-tracking measurement.
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...
Colloidal quantum dot solar cells (CQDSCs) are attracting growing attention owing to significant improvements in efficiency. However, even the best depleted-heterojunction CQDSCs currently display open-circuit voltages (VOCs) at least 0.5 V below the voltage corresponding to the bandgap. We find that the tail of states in the conduction band of the metal oxide layer can limit the achievable device efficiency. By continuously tuning the zinc oxide conduction band position via magnesium doping, we probe this critical loss pathway in ZnO–PbSe CQDSCs and optimize the energetic position of the tail of states, thereby increasing both the VOC (from 408 mV to 608 mV) and the device efficiency.
A droop-free nitride light-emitting diode (LED) with the capacity to operate beyond the "green gap" has been a subject of intense scientific and engineering interest. While several properties of nanowires on silicon make them promising for use in LED development, the high aspect ratio of individual nanowires and their laterally discontinuous features limit phonon transport and device performance. Here, we report on the monolithic integration of metal heat-sink and droop-free InGaN/GaN quantum-disks-in-nanowire LEDs emitting at ∼710 nm. The reliable operation of our uncooled nanowire-LEDs (NW-LEDs) epitaxially grown on molybdenum was evident in the constant-current soft burn-in performed on a 380 μm × 380 μm LED. The square LED sustained 600 mA electrical stress over an 8 h period, providing stable light output at maturity without catastrophic failure. The absence of carrier and phonon transport barriers in NW-LEDs was further inferred from current-dependent Raman measurements (up to 700 mA), which revealed the low self-heating. The radiative recombination rates of NW-LEDs between room temperature and 40 °C was not limited by Shockley-Read-Hall recombination, Auger recombination, or carrier leakage mechanisms, thus realizing droop-free operation. The discovery of reliable, droop-free devices constitutes significant progress toward the development of nanowires for practical applications. Our monolithic approach realized a high-performance device that will revolutionize the way high power, low-junction-temperature LED lamps are manufactured for solid-state lighting and for applications in high-temperature harsh environment.
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