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Martin Vacha

Publications and source records attributed to Martin Vacha.

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Engineering in-plane anisotropy in 2D materials via surface-bound ligands

2D materials exhibiting in-plane anisotropy enable novel functionality in electronic, optoelectronic, and photonic devices, yet their availability is generally limited to naturally-occurring low-symmetry van der Waals compounds. Here, we demonstrate an approach to structural engineering in a family of blue-emitting 2D silver phenylchalcogenide semiconductors based on steric interactions among surface-bound organic molecular ligands. By strategically halogenating specific sites of phenyl ligands, we demonstrate dramatic changes to the inorganic AgSe plane in mithrene (silver phenylselenolate, AgSePh). Density functional theory revealed pronounced in-plane electronic anisotropy for direct-gap fluorinated derivatives, while a chlorinated variant exhibited a direct-to-indirect bandgap transition. Furthermore, some fluorinated variants displayed strongly polarized absorption and luminescence, accompanied by a 10x enhancement in photoluminescence quantum yield. This work establishes a versatile approach for tailoring optoelectronic properties in hybrid semiconductors that is difficult or impossible to achieve in all-inorganic materials alone, offering new opportunities in advanced material design.

cond-mat.mtrl-sci

Room Temperature Collective Blinking and Photon Bunching from CsPbBr3 Quantum Dot Superlattice

Development of quantum light sources and search for quantum systems capable of supporting collective many-body states are crucial for further progress of modern quantum technologies. Metal halide perovskite quantum dots (QDs) have emerged as a promising candidate for quantum light sources, as individual QDs are reliable single photon emitters even at room temperature. However, photon bunching, a key signature of collective many-body states, has been so far largely observed at cryogenic temperatures in perovskite materials, limiting their applications under ambient conditions. Here, we report the observation of collective blinking and photon bunching in perovskite QD superlattices at room temperature. Sub-wavelength-sized (100 - 500 nm) CsPbBr3 QD superlattices, fabricated via a self-assembly process, exhibit an unusual two-level blinking behavior similar to that of single QDs, and demonstrate photon bunching with a degree of up to 2.75. Time-resolved photoluminescence (PL) measurements and super-resolution imaging reveal that the superlattices have a significantly longer PL lifetime than individual QDs and that their emission is spatially confined to regions tens of nanometers in size. These observations suggest long-range exciton migration to a localized energy trap within the superlattice. Excitation power dependent degree of bunching and analysis of the bunching dynamics indicate that the photon bunching originates from exciton-biexciton cascade emission, a key mechanism for generating entangled photons. These findings establish perovskite QD superlattices as a promising platform for room-temperature collective optical phenomena and quantum light generation, advancing scalable quantum photonic technologies.

physics.optics

Microscopic Intricacies of Self-Healing in Halide Perovskite-Charge Transport Layer Heterostructures

The stability and performance of halide perovskite photovoltaic devices are critically limited by progressive defect generation and associated local non-radiative losses during operation. Self-healing of defects provides a promising pathway to prolong device functionality, yet the underlying microscopic mechanisms remain poorly understood, particularly the role of interfacial chemistry on trap dynamics and healing kinetics. Here, we elucidate self-healing and defect evolution in triple-cation mixed halide (TCMH) perovskite films and their device-relevant charge transport layer heterostructures subjected to photo-induced damage. Using correlation clustering imaging (CLIM), our recently developed local functional imaging tool, we map spatiotemporal photoluminescence heterogeneity to track defect dynamics in pristine and heterostructure films. The defect healing follows bi-phasic kinetics, with an initial electronic relaxation (tens of minutes) and a subsequent slower phase (~ hours) associated to ionic and lattice rearrangement. Most importantly, our results demonstrate that the chemical nature of charge-transport layers modulates trap activity, healing kinetics, and halide redistribution, with heterostructures exhibiting faster recovery than pristine films, a boon for device resilience. These findings provide new insights into the dynamic interaction between defects, interfaces, and ion migration, and establish a framework for rational design of durable, next-generation perovskite optoelectronic devices.

cond-mat.mtrl-sci