Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.459
Publication date: 18th December 2023
Lead halide perovskites (LHPs) constitute a vast and highly diverse library of emerging semiconductors, which can be tailored by their organic cation composition, halide alloying, dimensionality, or chiral ligands to the specific needs of contemporary optoelectronic devices. So far, to optimize material properties, the material science community mainly focused on changing the static design of the perovskite lattice by tuning the chemical composition or morphology. Meanwhile, the full potential for dynamic phonon-driven ultrafast material control, as successfully applied for oxide perovskites, has not been exploited yet. In the hunt for coherent control over the soft and anharmonic LHP lattice, a number of contemporary ultrafast experiments have been pioneered, e.g. employing the ultrafast optical Kerr effect. Nevertheless, the dynamic lattice responses was found to be buried under a complex nonlinear polarization response and its coherent control remained elusive. Here, we employ intense single-cycle THz fields exceeding 1.5 MV/cm to coherently drive octahedral twist modes, which act as a structural order parameter and modulate the optical bandgap. By confirming a nonlinear driving mechanism, we open the field of (nonlinear) phononics in LHPs and unlock related coherent control schemes.To investigate the impact of confinement and dimensionality on lattice dynamics and their coherences, we extend these studies to two-dimensional (2D) layered Ruddlesden-Popper (PEA) 2 MA n-1PbnI 3n+1 compounds with n=1,2,3 inorganic octahedra layers forming periodic multiple quantum wells, separated by phenethylamine (PEA) organic spacer molecules. Already at room temperature, we witness strikingly enhanced lattice coherences with a clear dependence on the quantum confinement. Eventually, we further reduce the dimensionality to chain-like (1D) hybrid metal halide structures given by α-Ethylbenzylamine lead bromide compounds, which additionally open our studies to chiral properties.
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