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Sn-based halide perovskites are expected to be the best replacement for toxic lead-based counterparts, owing to their similar ionic radii and the optimal band gap for use in solar cells, as well as their versatile use in light-emitting diodes and photodetection applications. Concerns, however, exist about their stability under ambient conditions, an issue that is exacerbated in polycrystalline films because grain boundaries present large concentrations of defects and act as entrance points for oxygen and water, causing Sn oxidation. A current thriving research area in perovskite materials is the fabrication of perovskite single crystals, promising improved optoelectronic properties due to excellent uniformity, reduced defects, and the absence of grain boundaries. This review summarizes the most recent advances in the fabrication of single crystal Sn-based halide perovskites, with emphasis on synthesis methods, compositional engineering, and formation mechanisms, followed by a discussion of various challenges and appropriate strategies for improving their performance in optoelectronic applications.
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Among novel semiconductors, perovskites have gained significant attention due to their versatility, combining tunable optoelectronic properties with relatively easy fabrication processes. However, certain issues still hinder their widespread use, often related to the presence of defects and traps within the material. Beyond defect passivation in polycrystalline thin films, an alternative approach to enhancing material quality lies in the fabrication of single crystals. This review aims to provide an overview of the promising approaches explored to address specific challenges of perovskites that benefit from the single crystal nature, restricting our analysis to perovskite single crystal thin films (PSC-TF). We will discuss novel fabrication techniques and highlight recent achievements in devices, such as photodetectors, solar cells, and transistors. By examining the fundamental properties already discovered and showcasing the latest advancements, we aim to provide an overview of the perspectives and open challenges for PSC-TF in next-generation optoelectronic devices.
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Layered 2D perovskites are making inroads as materials for photovoltaics and light emitting diodes, but their photophysics is still lively debated. Although their large exciton binding energies should hinder charge separation, significant evidence has been uncovered for an abundance of free carriers among optical excitations. Several explanations have been proposed, like exciton dissociation at grain boundaries or polaron formation, without clarifying yet if excitons form and then dissociate, or if the formation is prevented by competing relaxation processes. Here we address exciton stability in layered Ruddlesden-Popper PEA2PbI4 (PEA stands for phenethylammonium) both in form of thin film and single crystal, by resonant injection of cold excitons, whose dissociation is then probed with femtosecond differential transmission. We show the intrinsic nature of exciton dissociation in 2D layered perovskites, demonstrating that both 2D and 3D perovskites are free carrier semiconductors and their photophysics is described by a unique and universal framework.
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There is increasing interest in the role of metal halide perovskites for heterogeneous catalysis. Here, we report a Ge-based 2D perovskite material that shows intrinsic water stability realized through organic cation engineering. Incorporating 4-phenylbenzilammonium (PhBz) we demonstrate, by means of extended experimental and computational results, that PhBz2GeBr4 and PhBz2GeI4 can achieve relevant air and water stability. The creation of composites embedding graphitic carbon nitride (g-C3N4) allows a proof of concept for light-induced hydrogen evolution in an aqueous environment by 2D Ge-based perovskites thanks to the effective charge transfer at the heterojunction between the two semiconductors.
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This publisher's note contains corrections to Opt. Lett.47, 6201 (2022)10.1364/OL.471241.
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Mixed-cation lead mixed-halide perovskites are the best candidates for perovskite-based photovoltaics, thanks to their higher efficiency and stability compared to the single-cation single-halide parent compounds. TripleMix (Cs0.05MA0.14FA0.81PbI2.55Br0.45 with FA = formamidinium and MA = methylammonium) is one of the most efficient and stable mixed perovskites for single-junction solar cells. The microscopic reasons why triple-cation perovskites perform so well are still under debate. In this work, we investigated the structure and dynamics of TripleMix by exploiting multinuclear solid-state nuclear magnetic resonance (SSNMR), which can provide this information at a level of detail not accessible by other techniques. 133Cs, 13C, 1H, and 207Pb SSNMR spectra confirmed the inclusion of all ions in the perovskite, without phase segregation. Complementary measurements showed a peculiar longitudinal relaxation behavior for the 1H and 207Pb nuclei in TripleMix with respect to single-cation single-halide perovskites, suggesting slower dynamics of both organic cations and halide anions, possibly related to the high photovoltaic performances.
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Manipulation by external pressure of the optical response of 2D Metal Halide Perovskites (MHPs) is a fascinating route to tune their properties and promote the emergence of novel features. We investigate here DA2PbI4 and DA2GeI4 (DA = decylammonium) perovskites in the pressure range up to â¼12 GPa by X-ray powder diffraction, absorption, and photoluminescence spectroscopy. Although the two systems share a similar structural evolution with pressure, the optical properties are rather different and influenced by Pb or Ge. DA2PbI4 shows a progressive red shift from 2.28 eV (P = 0 GPa) to 1.64 eV at 11.5 GPa, with a narrow PL emission, whereas DA2GeI4, changes from a non-PL system at ambient pressure to a clear broadband emitter centered around 730 nm with an intensity maximum at about 3.7 GPa. These results unveil the role of the central atom on the nature of emission under pressure in 2D MHPs containing a long alkyl chain.
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We demonstrate an integrated source of frequency-entangled photon pairs on a silicon photonics chip. The emitter has a coincidence-to-accidental ratio exceeding 103. We prove entanglement by showing two-photon frequency interference with a visibility of 94.6% ± 1.1%. This result opens the possibility of on-chip integration of frequency-bin sources with modulators and the other active and passive devices available in the silicon photonics platform.
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Efficient coupling to integrated high-quality-factor cavities is crucial for the employment of germanium quantum dot (QD) emitters in future monolithic silicon-based optoelectronic platforms. We report on strongly enhanced emission from single Ge QDs into L3 photonic crystal resonator (PCR) modes based on precise positioning of these dots at the maximum of the respective mode field energy density. Perfect site control of Ge QDs grown on prepatterned silicon-on-insulator substrates was exploited to fabricate in one processing run almost 300 PCRs containing single QDs in systematically varying positions within the cavities. Extensive photoluminescence studies on this cavity chip enable a direct evaluation of the position-dependent coupling efficiency between single dots and selected cavity modes. The experimental results demonstrate the great potential of the approach allowing CMOS-compatible parallel fabrication of arrays of spatially matched dot/cavity systems for group-IV-based data transfer or quantum optical systems in the telecom regime.
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Compact silicon integrated devices, such as micro-ring resonators, have recently been demonstrated as efficient sources of quantum correlated photon pairs. The mass production of integrated devices demands the implementation of fast and reliable techniques to monitor the device performances. In the case of time-energy correlations, this is particularly challenging, as it requires high spectral resolution that is not currently achievable in coincidence measurements. Here we reconstruct the joint spectral density of photons pairs generated by spontaneous four-wave mixing in a silicon ring resonator by studying the corresponding stimulated process, namely stimulated four wave mixing. We show that this approach, featuring high spectral resolution and short measurement times, allows one to discriminate between nearly-uncorrelated and highly-correlated photon pairs.
