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- ItemTowards low-temperature processing of efficient γ-CsPbI3 perovskite solar cells(London [u.a.] : RSC, 2023) Zhang, Zongbao; Ji, Ran; Hofstetter, Yvonne J.; Deconinck, Marielle; Brunner, Julius; Li, Yanxiu; An, Qingzhi; Vaynzof, YanaInorganic cesium lead iodide (CsPbI3) perovskite solar cells (PSCs) have attracted enormous attention due to their excellent thermal stability and optical bandgap (∼1.73 eV), well-suited for tandem device applications. However, achieving high-performance photovoltaic devices processed at low temperatures is still challenging. Here we reported a new method for the fabrication of high-efficiency and stable γ-CsPbI3 PSCs at lower temperatures than was previously possible by introducing the long-chain organic cation salt ethane-1,2-diammonium iodide (EDAI2) and regulating the content of lead acetate (Pb(OAc)2) in the perovskite precursor solution. We find that EDAI2 acts as an intermediate that can promote the formation of γ-CsPbI3, while excess Pb(OAc)2 can further stabilize the γ-phase of CsPbI3 perovskite. Consequently, improved crystallinity and morphology and reduced carrier recombination are observed in the CsPbI3 films fabricated by the new method. By optimizing the hole transport layer of CsPbI3 inverted architecture solar cells, we demonstrate efficiencies of up to 16.6%, surpassing previous reports examining γ-CsPbI3 in inverted PSCs. Notably, the encapsulated solar cells maintain 97% of their initial efficiency at room temperature and under dim light for 25 days, demonstrating the synergistic effect of EDAI2 and Pb(OAc)2 in stabilizing γ-CsPbI3 PSCs.
- ItemSub-cycle valleytronics: control of valley polarization using few-cycle linearly polarized pulses(Washington, DC : OSA, 2021) Jiménez-Galán, Álvaro; Silva, Rui E. F.; Smirnova, Olga; Ivanov, MishaSo far, it has been assumed that selective excitation of a desired valley in the Brillouin zone of a hexagonal two-dimensional material has to rely on using circularly polarized fields. We theoretically demonstrate a way to control the valley excitation in hexagonal 2D materials on a few-femtosecond timescale using a few-cycle, linearly polarized pulse with controlled carrier–envelope phase. The valley polarization is mapped onto the strength of the perpendicular harmonic signal of a weak, linearly polarized pulse, which allows to read this information all-optically without destroying the valley state and without relying on the Berry curvature, making our approach potentially applicable to inversion-symmetric materials. We show applicability of this method to hexagonal boron nitride and MoS2.
- ItemFew-cycle 65-µJ pulses at 11.4 µm for ultrafast nonlinear longwave-infrared spectroscopy(Washington, DC : Optical Society of America, OSA, 2022) Fuertjes, Pia; Bock, Martin; Grafenstein, Lorenz von; Ueberschaer, Dennis; Griebner, Uwe; Elsaesser, ThomasLow-energy excitations can provide insight into the basic ultrafast nonequilibrium dynamics of condensed matter. High-energy femtosecond pulses in the long-wavelength infrared are required to induce such processes, and can be generated in an optical parametric chirped pulse amplification (OPCPA) system comprising three GaSe stages. A femtosecond Cr:ZnS laser serves as the front-end, providing the seed for the 2.0-µm pump and the 2.4-µm signal pulses without nonlinear conversion processes. The OPCPA system is pumped at 2.05 µm by a picosecond Ho:YLF regenerative amplifier at a 1-kHz repetition rate. The recompressed idler pulses at 11.4 µm have a duration of 185 fs and an unprecedented energy of 65 µJ, corresponding to a pump-to-idler conversion efficiency of 1.2%. Nonlinear transmission experiments in the range of the L2 infrared band of liquid water demonstrate the potential of the pulses for nonlinear vibrational spectroscopy of liquids and solids.