Metal halide perovskites are of great interest for various high-performance optoelectronic applications. The ability to tune the perovskite bandgap continuously by modifying the chemical composition opens up applications for perovskites as coloured emitters, in building-integrated photovoltaics, and as components of tandem photovoltaics to increase the power conversion efficiency. Nevertheless, performance is limited by non-radiative losses, with luminescence yields in state-of-the-art perovskite solar cells still far from 100 per cent under standard solar illumination conditions. Furthermore, in mixed halide perovskite systems designed for continuous bandgap tunability (bandgaps of approximately 1.7 to 1.9 electronvolts), photoinduced ion segregation leads to bandgap instabilities. Here we demonstrate substantial mitigation of both non-radiative losses and photoinduced ion migration in perovskite films and interfaces by decorating the surfaces and grain boundaries with passivating potassium halide layers. We demonstrate external photoluminescence quantum yields of 66 per cent, which translate to internal yields that exceed 95 per cent. The high luminescence yields are achieved while maintaining high mobilities of more than 40 square centimetres per volt per second, providing the elusive combination of both high luminescence and excellent charge transport. When interfaced with electrodes in a solar cell device stack, the external luminescence yield-a quantity that must be maximized to obtain high efficiency-remains as high as 15 per cent, indicating very clean interfaces. We also demonstrate the inhibition of transient photoinduced ion-migration processes across a wide range of mixed halide perovskite bandgaps in materials that exhibit bandgap instabilities when unpassivated. We validate these results in fully operating solar cells. Our work represents an important advance in the construction of tunable metal halide perovskite films and interfaces that can approach the efficiency limits in tandem solar cells, coloured-light-emitting diodes and other optoelectronic applications.
We control the electronic structure of the silicon-vacancy (SiV) color-center in diamond by changing its static strain environment with a nano-electro-mechanical system. This allows deterministic and local tuning of SiV optical and spin transition frequencies over a wide range, an essential step towards multi-qubit networks. In the process, we infer the strain Hamiltonian of the SiV revealing large strain susceptibilities of order 1 PHz/strain for the electronic orbital states. We identify regimes where the spin-orbit interaction results in a large strain suseptibility of order 100 THz/strain for spin transitions, and propose an experiment where the SiV spin is strongly coupled to a nanomechanical resonator.arXiv:1801.09833v2 [quant-ph]
The uncontrolled interaction of a quantum system with its environment is detrimental for quantum coherence. For quantum bits in the solid state, decoherence from thermal vibrations of the surrounding lattice can typically only be suppressed by lowering the temperature of operation. Here, we use a nano-electro-mechanical system to mitigate the effect of thermal phonons on a spin qubit – the silicon-vacancy colour centre in diamond – without changing the system temperature. By controlling the strain environment of the colour centre, we tune its electronic levels to probe, control, and eventually suppress the interaction of its spin with the thermal bath. Strain control provides both large tunability of the optical transitions and significantly improved spin coherence. Finally, our findings indicate the possibility to achieve strong coupling between the silicon-vacancy spin and single phonons, which can lead to the realisation of phonon-mediated quantum gates and nonlinear quantum phononics.
toward the optimization of perovskite thin film growth from simple precursors have improved the efficiency and stability of devices to a high quality standard and low cost, placing them on the verge of commercialization. [1][2][3][4][5][6] Nevertheless, a better understanding of what influences their crystalline structure is needed in order to achieve phase purity, manage defects, and ultimately achieve optimal device performances.The dramatic gain in solar cell device efficiency since 2012 is only one of the features making perovskites stand out among other photovoltaic materials. With a Young's modulus around 20 GPa, [7][8][9][10] perovskites are mechanically softer than most other PV materials such as silicon (>160 GPa), [11,12] GaAs (≈85 GPa), [13] CIGS (≈80 GPa), [14,15] and CdTe (≈40 GPa), [16,17] and their structure has been reported to be prone to light-induced, electric-fieldinduced, and temperature-dependent rearrangements. [18][19][20][21][22][23] The workhorse system studied to date, methylammonium lead iodide (MAPbI 3 ), is in a tetragonal phase (TP) at room temperature, but undergoes a transition to a cubic phase at high temperature (≈330 K) and an orthorhombic phase (OP) at low temperature (≈150 K). Recently, we and others [24][25][26] have reported that the structural rearrangement from TP to OP causes a distinct hysteretic change in optical and transport properties as well as device behavior between heating and cooling cycles. This hysteresis could be reduced by scraping the film from the substrate and instead measuring randomly oriented powder samples. [24] These results provide hints that the thermal stability [27] and phase transition can be influenced by the local environment of the film due to interactions between the material and substrate as well as within the bulk film itself. Unless understood and mitigated, such hysteretic changes at low temperature may limit the use of perovskite solar cells in some specific applications, for example, aerospace applications, which require operation at extremely low temperatures [28] (<200 K).State-of-the-art perovskite films are polycrystalline, which leads to microscale inhomogeneities in a number of properties such as morphology and defect distributions [29][30][31][32] and, in turn, to local variations in the electronic environment for charge carriers. Generally, increasing grain sizes in MAPbI 3 films has resulted in improvements in critical performance parameters, such as an increase in carrier mobility and charge collection efficiency, [33,34] along with smaller bandgaps, longer lifetimes, Grain size in polycrystalline halide perovskite films is known to have an impact on the optoelectronic properties of the films, but its influence on their soft structural properties and phase transitions is unclear. Here, temperature-dependent X-ray diffraction, absorption, and macro-and microphotoluminescence measurements are used to investigate the tetragonal to orthorhombic phase transition in thin methylammonium lead iodide films with grain sizes ranging fr...
Perovskite solar cells and light-emission devices are yet to achieve their full potential owing in part to spatially heterogeneous non-radiative loss pathways that are both on, and buried beneath, the surfaces of films and crystals.
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