2022, Belitsch, Martin, Dirin, Dmitry N., Kovalenko, Maksym V., Pichler, Kevin, Rotter, Stefan, Ghalgaoui, Ahmed, Ditlbacher, Harald, Hohenau, Andreas, Krenn, Joachim R.

Colloidal semiconducting nanocrystals are efficient, stable and spectrally tunable emitters, but achievable optical gain is often limited by fast nonradiative processes. These processes are strongly suppressed in slab-shaped nanocrystals (nanoplatelets), due to relaxed exciton Coulomb interaction. Here, we show that CdSe/CdS nanoplatelets can be engineered into (sub)microscopic stripe waveguides that achieve lasing without further components for feedback, i.e., just relying on the stripe end reflection. We find a remarkably high gain factor for the CdSe/CdS nanoplatelets of 1630 cm−1. In addition, by comparison with numerical simulations we assign a distinct emission peak broadening above laser threshold to emission pulse shortening. Our results illustrate the feasibility of geometrically simple monolithic microscale nanoplatelet lasers as an attractive option for a variety of photonic applications.

2023, Gallop, Nathaniel. P., Maslennikov, Dmitry R., Mondal, Navendu, Goetz, Katelyn P., Dai, Zhenbang, Schankler, Aaron M., Sung, Woongmo, Nihonyanagi, Satoshi, Tahara, Tahei, Bodnarchuk, Maryna I., Kovalenko, Maksym V., Vaynzof, Yana, Rappe, Andrew M., Bakulin, Artem A.

Vibrational control (VC) of photochemistry through the optical stimulation of structural dynamics is a nascent concept only recently demonstrated for model molecules in solution. Extending VC to state-of-the-art materials may lead to new applications and improved performance for optoelectronic devices. Metal halide perovskites are promising targets for VC due to their mechanical softness and the rich array of vibrational motions of both their inorganic and organic sublattices. Here, we demonstrate the ultrafast VC of FAPbBr3 perovskite solar cells via intramolecular vibrations of the formamidinium cation using spectroscopic techniques based on vibrationally promoted electronic resonance. The observed short (~300 fs) time window of VC highlights the fast dynamics of coupling between the cation and inorganic sublattice. First-principles modelling reveals that this coupling is mediated by hydrogen bonds that modulate both lead halide lattice and electronic states. Cation dynamics modulating this coupling may suppress non-radiative recombination in perovskites, leading to photovoltaics with reduced voltage losses.