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Hybrid organic-inorganic semiconductors with strong electron-phonon interactions provide a programmable platform for developing a variety of electronic, optoelectronic, and quantum materials by controlling these interactions. However, in current hybrid semiconductors, such as halide perovskites, anharmonic vibrations with rapid dephasing hinder the ability to coherently manipulate phonons. Here, we report the observation of long-lived coherent phonons in lead organic chalcogenides (LOCs), a new family of hybrid two-dimensional semiconductors. These materials feature harmonic phonon dynamics despite distorted lattices, combining long phonon dephasing times with tunable semiconducting properties. Dephasing time as long as 75 ps at 10 K, with up to 500 cycles of phonon oscillation between scattering events, was observed, corresponding to a dimensionless harmonicity parameter more than an order of magnitude larger than that of halide perovskites. The phonon dephasing time is significantly influenced by anharmonicity and centrosymmetry, both of which can be tuned through the design of the organic ligands thanks to the direct bonding between the organic and inorganic motifs. This research opens new opportunities for the manipulation of electronic properties with coherent phonons in hybrid semiconductors.

Moir\'e superlattices have emerged as a new platform for studying strongly correlated quantum phenomena, but these systems have been largely limited to van der Waals layer two-dimensional (2D) materials. Here we introduce moir\'e superlattices leveraging ultra-thin, ligand-free halide perovskites, facilitated by ionic interactions. Square moir\'e superlattices with varying periodic lengths are clearly visualized through high-resolution transmission electron microscopy. Twist-angle-dependent transient photoluminescence microscopy and electrical characterizations indicate the emergence of localized bright excitons and trapped charge carriers near a twist angle of ~10{\deg}. The localized excitons are accompanied by enhanced exciton emission, attributed to an increased oscillator strength by a theoretically forecasted flat band. This work illustrates the potential of extended ionic interaction in realizing moir\'e physics at room temperature, broadening the horizon for future investigations.

The vertical stacking of two-dimensional materials into heterostructures gives rise to a plethora of intriguing optoelectronic properties and presents an unprecedented potential for technological development. While much progress has been made combining different monolayers of transition metal dichalgonenides (TMDs), little is known about TMD-based heterostructures including organic layers of molecules. Here, we present a joint theory-experiment study on a TMD/tetracene heterostructure demonstrating clear signatures of spatially separated interlayer excitons in low temperature photoluminescence spectra. Here, the Coulomb-bound electrons and holes are localized either in the TMD or in the molecule layer, respectively. In particular, we reveal both in theory and experiment signatures of the entire intra- and interlayer exciton landscape in the photoluminescence spectra. In particular, we find both in theory and experiment a pronounced transfer of intensity from the intralayer TMD exciton to a series of energetically lower interlayer excitons with decreasing temperature. In addition, we find signatures phonon-sidebands stemming from these interlayer exciton states. Our findings shed light on the microscopic nature of interlayer excitons in TMD/molecule heterostructures and could have important implications for technological applications of these materials.

Manipulating materials with atomic-scale precision is essential for the development of next-generation material design toolbox. Tremendous efforts have been made to advance the compositional, structural, and spatial accuracy of material deposition and patterning. The family of 2D materials provides an ideal platform to realize atomic-level material architectures. The wide and rich physics of these materials have led to fabrication of heterostructures, superlattices, and twisted structures with breakthrough discoveries and applications. Here, we report a novel atomic-scale material design tool that selectively breaks and forms chemical bonds of 2D materials at room temperature, called atomic-layer substitution (ALS), through which we can substitute the top layer chalcogen atoms within the 3-atom-thick transition-metal dichalcogenides using arbitrary patterns. Flipping the layer via transfer allows us to perform the same procedure on the other side, yielding programmable in-plane multi-heterostructures with different out-of-plane crystal symmetry and electric polarization. First-principle calculations elucidate how the ALS process is overall exothermic in energy and only has a small reaction barrier, facilitating the reaction to occur at room temperature. Optical characterizations confirm the fidelity of this design approach, while TEM shows the direct evidence of Janus structure and suggests the atomic transition at the interface of designed heterostructure. Finally, transport and Kelvin probe measurements on MoXY (X,Y=S,Se; X and Y corresponding to the bottom and top layers) lateral multi-heterostructures reveal the surface potential and dipole orientation of each region, and the barrier height between them. Our approach for designing artificial 2D landscape down to a single layer of atoms can lead to unique electronic, photonic and mechanical properties previously not found in nature.