Despite the exciting progress on power conversion efficiencies, the commercialization of the emerging lead (Pb) halide perovskite solar cell technology still faces significant challenges, one of which is the inclusion of toxic Pb. Searching for Pb-free perovskite solar cell absorbers is currently an attractive research direction. The approaches used for and the consequences of Pb replacement are reviewed herein. Reviews on the theoretical understanding of the electronic, optical, and defect properties of Pb and Pb-free halide perovskites and perovskite derivatives are provided, as well as the experimental results available in the literature. The theoretical understanding explains well why Pb halide perovskites exhibit superior photovoltaic properties, but Pb-free perovskites and perovskite derivatives do not.

From Lead Halide Perovskites to Lead-Free Metal Halide Perovskites and Perovskite Derivatives

Laser excitation of nanometer-sized atomic and molecular clusters offers various opportunities to explore and control ultrafast many-particle dynamics. Whereas weak laser fields allow the analysis of photoionization, excited-state relaxation, and structural modifications on these finite quantum systems, large-amplitude collective electron motion and Coulomb explosion can be induced with intense laser pulses. This review provides an overview of key phenomena arising from laser-cluster interactions with focus on nonlinear optical excitations and discusses the underlying processes according to the current understanding. A general survey covers basic cluster properties and excitation mechanisms relevant for laser-driven cluster dynamics. Then, after an excursion in theoretical and experimental methods, results for single-photon and multiphoton excitations are reviewed with emphasis on signatures from time- and angular-resolved photoemission. A key issue of this review is the broad spectrum of phenomena arising from clusters exposed to strong fields, where the interaction with the laser pulse creates short-lived and dense nanoplasmas. The implications for technical developments such as the controlled generation of ion, electron, and radiation pulses will be addressed along with corresponding examples. Finally, future prospects of laser-cluster research as well as experimental and theoretical challenges are discussed.

Laser-driven nonlinear cluster dynamics

Cluster beams in the super-intense femtosecond laser pulse

Rational Design of Halide Double Perovskites for Optoelectronic Applications

The organic-inorganic hybrid lead halide perovskites have emerged as a series of star materials for solar cells, lasers and detectors. However, the issues raised by the toxic lead element and marginal stability due to the volatile organic components have severely limited their potential applications. In this work, we develop a nucleation-controlled solution method to grow large size high-quality Cs3Bi2I9 perovskite single crystals (PSCs). Using the technique, we harvest some centimeter-sized single crystals and achieved high device performance. We find that X-ray detectors based on PSCs exhibit high sensitivity of 1652.3 μC Gyair−1 cm−2 and very low detectable dose rate of 130 nGyair s−1, both desired in medical diagnostics. In addition, its outstanding thermal stability inspires us to develop a high temperature X-ray detector with stable response at up to 100 °C. Furthermore, PSCs exhibit high X-ray imaging capability thanks to its negligible signal drifting and extremely high stability. Organic-inorganic hybrid halide perovskites have been emerged as promising candidates for X-ray detectors while toxicity and instability are known issues. Here, Zhang et al. grow large size lead-free single crystals for high performance X-ray detection and imaging devices that can operate at 100 °C.

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Nucleation-controlled growth of superior lead-free perovskite Cs3Bi2I9 single-crystals for high-performance X-ray detection.

Lead (Pb) halide perovskites have attracted tremendous attention in recent years because of their rich optoelectronic properties, which have resulted in more than 22% power conversion efficient photovoltaics (PVs). Nevertheless, Pb-metal toxicity remains a huge hurdle for extensive applications of these compounds. Thus, alternative compounds with similar optoelectronic properties need to be developed. Bismuth possesses electronic structure similar to that of lead with the presence of ns2 electrons that exhibit rich structural variety as well as interesting optical and electronic properties. Herein, we critically assess Cs3Bi2I9 as a candidate for thin-film solar cell absorber. Despite a reasonable optical band gap (∼2 eV) and absorption coefficient, the power conversion efficiency of the Cs3Bi2I9 mesoscopic solar cells was found to be severely lacking, limited by the poor photocurrent density. The efficiency of the Cs3Bi2I9 solar cell can be slightly improved by changing the stoichiometry of the precursor...

Limitations of Cs3Bi2I9 as Lead-Free Photovoltaic Absorber Materials.

Bismuth-based halide perovskite derivatives have now attracted huge attention for photovoltaic (PV) applications after the unparalleled success of lead-based halide perovskites. However, the performances of PV devices based on these compounds are poor, despite theoretical predictions. In this Article, we have investigated the electronic structure and defect formation energies of Cs3Bi2I9 using density functional theory (DFT) calculations. The calculated electronic bandstructure indicates an indirect bandgap and high carrier effective masses. Our calculations reveal a large stability region for this compound; however, deep level defects are quite prominent. Even the varying chemical potentials from the stoichiometric region do not eliminate the presence of deep defects, ultimately limiting photovoltaic efficiencies.

Poor Photovoltaic Performance of Cs3Bi2I9: An Insight through First-Principles Calculations

Superior Performance of Silver Bismuth Iodide Photovoltaics Fabricated via Dynamic Hot‐Casting Method under Ambient Conditions

We present the deformation pathway of critically charged glycol and water droplets from the onset of the Rayleigh instability and compare it to numerical results, obtained for perfectly conducting inviscid droplets. In this simple model presented here, the time evolution of the droplet shape is given by the velocity potential equation. The Laplace equation for the velocity potential is solved by expanding the potential onto harmonic functions. For the part of the pathway dominated by electrostatic pressure, the calculations reproduce the experimental data nicely, obtained for both, glycol and water microdroplets. We find that the droplet shape and in particular the tips, just before charge emission, are well fitted by a lemon shape. We stress that the tip is tangent to a cone of 39° and thus significantly narrower than a Taylor cone.

Shape deformations of surface-charged microdroplets.

This paper proposes the preparation and formula analysis of anti-biofouling Titania–polyurea (TiO2–SPUA) spray coating, which uses nano-scale antibacterial and photocatalytic agents, titanium dioxide, to construct regularly hydrophobic surface texture on the polyurea coating system. Through formulating analysis of anti-biofouling performance, it is found the causal factors include antibacterial TiO2, surface wettability and morphology in order of their importance. The most optimized formula group is able to obtain uniform surface textures, high contact angle (91.5°), low surface energy (32.5 mJ/m2), and strong hardness (74 A). Moreover, this newly fabricated coating can effectively prevent Pseudomonas aeruginosa and biofilm from enriching on the surface, and there is no toxins release from the coating itself, which makes it eco-friendly, even after long-time exposure. These studies provide insights to the relative importance of physiochemical properties of Titania–polyurea spray coatings for further use in marine, as well as bio medical engineering.

Claude Guet

Papers

Limitations of Cs3Bi2I9 as Lead-Free Photovoltaic Absorber Materials.

Poor Photovoltaic Performance of Cs3Bi2I9: An Insight through First-Principles Calculations

Superior Performance of Silver Bismuth Iodide Photovoltaics Fabricated via Dynamic Hot‐Casting Method under Ambient Conditions

Shape deformations of surface-charged microdroplets.

Preparation and Formula Analysis of Anti-Biofouling Titania–Polyurea Spray Coating with Nano/Micro-Structure