Natalia Yantara

Low-temperature solution-processed wavelength-tunable perovskites for lasing

Low-temperature solution-processed materials that show optical gain and can be embedded into a wide range of cavity resonators are attractive for the realization of on-chip coherent light sources. Organic semiconductors and colloidal quantum dots are considered the main candidates for this application. However, stumbling blocks in organic lasing include intrinsic losses from bimolecular annihilation and the conflicting requirements of high charge carrier mobility and large stimulated emission; whereas challenges pertaining to Auger losses and charge transport in quantum dots still remain. Herein, we reveal that solution-processed organic-inorganic halide perovskites (CH3NH3PbX3 where X = Cl, Br, I), which demonstrated huge potential in photovoltaics, also have promising optical gain. Their ultra-stable amplified spontaneous emission at strikingly low thresholds stems from their large absorption coefficients, ultralow bulk defect densities and slow Auger recombination. Straightforward visible spectral tunability (390-790 nm) is demonstrated. Importantly, in view of their balanced ambipolar charge transport characteristics, these materials may show electrically driven lasing.

High Efficiency Solid-State Sensitized Solar Cell-Based on Submicrometer Rutile TiO2 Nanorod and CH3NH3PbI3 Perovskite Sensitizer

We report a highly efficient solar cell based on a submicrometer (~0.6 μm) rutile TiO2 nanorod sensitized with CH3NH3PbI3 perovskite nanodots. Rutile nanorods were grown hydrothermally and their lengths were varied through the control of the reaction time. Infiltration of spiro-MeOTAD hole transport material into the perovskite-sensitized nanorod films demonstrated photocurrent density of 15.6 mA/cm(2), voltage of 955 mV, and fill factor of 0.63, leading to a power conversion efficiency (PCE) of 9.4% under the simulated AM 1.5G one sun illumination. Photovoltaic performance was significantly dependent on the length of the nanorods, where both photocurrent and voltage decreased with increasing nanorod lengths. A continuous drop of voltage with increasing nanorod length correlated with charge generation efficiency rather than recombination kinetics with impedance spectroscopic characterization displaying similar recombination regardless of the nanorod length.

Flexible, low-temperature, solution processed ZnO-based perovskite solid state solar cells

A ZnO compact layer formed by electrodeposition and ZnO nanorods grown by chemical bath deposition (CBD) allow the processing of low-temperature, solution based and flexible solid state perovskite CH3NH3PbI3 solar cells. Conversion efficiencies of 8.90% were achieved on rigid substrates while the flexible ones yielded 2.62%.

Perovskite Materials for Light-Emitting Diodes and Lasers

Organic-inorganic hybrid perovskites have cemented their position as an exceptional class of optoelectronic materials thanks to record photovoltaic efficiencies of 22.1%, as well as promising demonstrations of light-emitting diodes, lasers, and light-emitting transistors. Perovskite materials with photoluminescence quantum yields close to 100% and perovskite light-emitting diodes with external quantum efficiencies of 8% and current efficiencies of 43 cd A(-1) have been achieved. Although perovskite light-emitting devices are yet to become industrially relevant, in merely two years these devices have achieved the brightness and efficiencies that organic light-emitting diodes accomplished in two decades. Further advances will rely decisively on the multitude of compositional, structural variants that enable the formation of lower-dimensionality layered and three-dimensional perovskites, nanostructures, charge-transport materials, and device processing with architectural innovations. Here, the rapid advancements in perovskite light-emitting devices and lasers are reviewed. The key challenges in materials development, device fabrication, operational stability are addressed, and an outlook is presented that will address market viability of perovskite light-emitting devices.

Band-gap tuning of lead halide perovskites using a sequential deposition process

Band-gap tuning of mixed anion lead halide perovskites (MAPb(I1−xBrx)2 (0 ≤ x ≤ 1)) has been demonstrated by means of a sequential deposition process. The optical properties of perovskite hybrids can be flexibly modified by changing (mixing) the concentration of halogen precursors. The concentrations of precursor solution as well as the conversion time play an important role in determining the band-gap of perovskites. A systematic shift of the absorption band edge to shorter wavelengths is observed with increasing Br content in the perovskite films, which results in the decrement of the photocurrent. Nanorod like morphological features are also observed for perovskite films with an iodide to bromide molar ratio of <0.7.

Inorganic Halide Perovskites for Efficient Light-Emitting Diodes

Lead-halide perovskites have transcended photovoltaics. Perovskite light-emitting diodes (PeLEDs) emerge as a new field to leverage on these fascinating semiconductors. Here, we report the first use of completely inorganic CsPbBr3 thin films for enhanced light emission through controlled modulation of the trap density by varying the CsBr-PbBr2 precursor concentration. Although pure CsPbBr3 films can be deposited from equimolar CsBr-PbBr2 and CsBr-rich solutions, strikingly narrow emission line (17 nm), accompanied by elongated radiative lifetimes (3.9 ns) and increased photoluminescence quantum yield (16%), was achieved with the latter. This is translated into the enhanced performance of the resulting PeLED devices, with lower turn-on voltage (3 V), narrow electroluminescence spectra (18 nm) and higher electroluminescence intensity (407 Cd/m(2)) achieved from the CsBr-rich solutions.

High efficiency electrospun TiO2 nanofiber based hybrid organic–inorganic perovskite solar cell

The good electrical and morphological characteristics of TiO₂ nanofibers and the high extinction coefficient of CH₃NH₃PbI₃ perovskite are combined to obtain a solar cell with a power conversion efficiency of 9.8%. The increase of the film thickness dramatically diminishes the performance due to the reduction in porosity of the TiO₂ nanofiber framework. The optimum device (∼413 nm film thickness) is compared to a planar device, where the latter produces higher V(oc) but lower J(sc), and consequently lower efficiency at all measured light intensities.

Interfacial Electron Transfer Barrier at Compact TiO2/CH3NH3PbI3 Heterojunction

Low-temperature solution-processed CH3 NH3 PbI3 interfaced with TiO2 has recently been demonstrated as a highly successful type-II light harvesting heterojunction with ≈20% efficiency. Therefore, an efficient ultrafast photoexcited electron transfer from CH3 NH3 PbI3 to TiO2 is expected. However, by probing the photoexcited charge carrier dynamics in CH3 NH3 PbI3 /quartz, CH3 NH3 PbI3 /TiO2 (compact), and CH3 NH3 PbI3 /PCBM in a comparative study, an electron transfer potential barrier between CH3 NH3 PbI3 and the compact TiO2 (prepared with the spray pyrolysis method) formed by surface states is uncovered. Consequently, the CH3 NH3 PbI3 photoluminescence intensity and lifetime is enhanced when interfaced to compact TiO2 . The electron accumulation within CH3 NH3 PbI3 needed to overcome this interfacial potential barrier results in the undesirable large current-voltage hysteresis observed for CH3 NH3 PbI3 /TiO2 planar heterojunctions. The findings in this study indicate that careful surface engineering to reduce this potential barrier is key to pushing perovskite solar cell efficiencies toward the theoretical limit.

Formamidinium tin-based perovskite with low Eg for photovoltaic applications

A lead-free low bandgap organic–inorganic hybrid perovskite, formamidinium tin iodide, is utilized as a light absorbing layer in photovoltaics. This material has a bandgap of 1.41 eV which allows light harvesting from the near infrared region, making high photocurrents achievable. A power conversion efficiency of 2.10% was accomplished upon incorporating SnF2.

Slow cooling and highly efficient extraction of hot carriers in colloidal perovskite nanocrystals

Hot-carrier solar cells can overcome the Shockley-Queisser limit by harvesting excess energy from hot carriers. Inorganic semiconductor nanocrystals are considered prime candidates. However, hot-carrier harvesting is compromised by competitive relaxation pathways (for example, intraband Auger process and defects) that overwhelm their phonon bottlenecks. Here we show colloidal halide perovskite nanocrystals transcend these limitations and exhibit around two orders slower hot-carrier cooling times and around four times larger hot-carrier temperatures than their bulk-film counterparts. Under low pump excitation, hot-carrier cooling mediated by a phonon bottleneck is surprisingly slower in smaller nanocrystals (contrasting with conventional nanocrystals). At high pump fluence, Auger heating dominates hot-carrier cooling, which is slower in larger nanocrystals (hitherto unobserved in conventional nanocrystals). Importantly, we demonstrate efficient room temperature hot-electrons extraction (up to ∼83%) by an energy-selective electron acceptor layer within 1 ps from surface-treated perovskite NCs thin films. These insights enable fresh approaches for extremely thin absorber and concentrator-type hot-carrier solar cells.