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Area-selective atomic layer deposition is a key technology for modern microelectronics as it eliminates alignment errors inherent to conventional approaches by enabling material deposition only in specific areas. Typically, the selectivity originates from surface modifications of the substrate that allow or block precursor adsorption. The control of the deposition process currently remains a major challenge as the selectivity of the no-growth areas is lost quickly. Here, we show that surface modifications of the substrate strongly manipulate surface diffusion. The selective deposition of TiO

Tip-induced optical spectroscopy overcomes the inherent resolution limits of conventional optical techniques enabling studies of sub-nm sized objects due to the tip's near-field antenna action. This statement is true for individual molecules on surfaces or in the gas phase, but does not hold without restrictions for spatially extended samples. The reason is that the perturbations caused by the tip extend into the sample volume. The tip may induce strain, heating or hot-carrier injection locally in the material. These effects add additional degrees of complexity by changing near-field and far-field optical response. The far-field response varies because strain relaxation, heat and carrier diffusion possess areas of influence exceeding the sample area influenced by the short-range near-field effects. Tip-in spectra are not simply enhanced compared to tip-out spectra, they will also vary in spectral appearance, i.e., peak positions, relative peak intensities, and linewidths. Detailed studies of MoS2 samples ranging from a single layer to bulk-like multi-layer MoS2 also reveal that the spectra are sensitive to variations of phonon and band structure with increasing layer number. These variations have a direct impact on the signals detected, but also clearly modify the relative magnitudes of the contributions of the tip-induced effects to the tip-in spectra. In addition, the optical response is affected by the kind of tip and substrate used. Hence, the presented results provide further insight into the underlying microscopic mechanisms of tip-enhanced spectroscopy and demonstrate that 2D materials are an ideal playground for obtaining a fundamental understanding of these spectroscopic techniques.

The physicochemical properties of thin metal oxide layers strongly depend on the layer thickness and thus differ significantly from their bulk counterpart. In this work, we present the growth of de...

Multinary organic-inorganic metal halide materials beyond the perovskite motif can help to address both fundamental aspects such as the electronic interactions between different metalate building units and practical issues like stability and ease of preparation in this new field of research. However, such multinary compounds have remained quite rare for the halogenido pentelates, as the formation of simpler side phases can be a significant hindrance. Here, we report a family of four new multinary iodido pentelates [PPh4]2[ECu2I7(nitrile)] (E = Sb, Bi; nitrile = acetonitile or propionitrile), including the first metalate with a Cu-I-Sb unit. The compounds can be obtained by facile solution or mechanochemical methods and display good stability up to 160 °C. A comparison with compounds containing binary anions [EI6]3- reveals that, unexpectedly, the addition of the iodido cuprate unit causes a blue-shift in the absorption of the antimonates but a red-shift in the bismuthates. Photoluminescence investigations at 10 K show that the compounds display broad luminescence bands that correspond well with the trend in their onset of absorption. Overall, the work highlights that multinary, non-perovskite halogenido metalates can be a valuable expansion of the chemistry of metal halide perovskites.

Low-dimensional organic-inorganic perovskites synergize the virtues of two unique classes of materials featuring intriguing possibilities for next-generation optoelectronics: they offer tailorable building blocks for atomically thin, layered materials while providing the enhanced light-harvesting and emitting capabilities of hybrid perovskites. This work goes beyond the paradigm that atomically thin materials require in-plane covalent bonding and reports single layers of the 1D organic-inorganic perovskite [C7 H10 N]3 [BiCl5 ]Cl. Its unique 1D-2D structure enables single layers and the formation of self-trapped excitons, which show white-light emission. The thickness dependence of the exciton self-trapping causes an extremely strong shift of the emission energy. Thus, such 2D perovskites demonstrate that already 1D covalent interactions suffice to realize atomically thin materials and provide access to unique exciton physics. These findings enable a much more general construction principle for tailoring and identifying 2D materials that are no longer limited to covalently bonded 2D sheets.

The influence of the atom source operating parameters on the structural and optical properties of In xGa 1 − xN/GaN nanowires (NWs) grown by plasma-assisted molecular beam epitaxy is investigated. Electron microscopy and photoluminescence spectroscopy reveal a change of the NW tip morphology and an enhancement of the local indium incorporation with increasing nitrogen flux. Tuning the density ratio of atomic-to-excited molecular nitrogen to lower values minimizes the point defect density, which results in a decrease of the non-radiative recombination rate as demonstrated by a combination of continuous wave and time-resolved photoluminescence spectroscopy.The influence of the atom source operating parameters on the structural and optical properties of In xGa 1 − xN/GaN nanowires (NWs) grown by plasma-assisted molecular beam epitaxy is investigated. Electron microscopy and photoluminescence spectroscopy reveal a change of the NW tip morphology and an enhancement of the local indium incorporation with increasing nitrogen flux. Tuning the density ratio of atomic-to-excited molecular nitrogen to lower values minimizes the point defect density, which results in a decrease of the non-radiative recombination rate as demonstrated by a combination of continuous wave and time-resolved photoluminescence spectroscopy.

Two-dimensional (2D) materials, such as graphene1, boron nitride2, and transition metal dichalcogenides (TMDs)3-5, have sparked wide interest in both device physics and technological applications at the atomic monolayer limit. These 2D monolayers can be stacked together with precise control to form novel van der Waals heterostructures for new functionalities2,6-9. One highly coveted but yet to be realized heterostructure is that of differing monolayer TMDs with type II band alignment10-12. Their application potential hinges on the fabrication, understanding, and control of bonded monolayers, with bound electrons and holes localized in individual monolayers, i.e. interlayer excitons. Here, we report the first observation of interlayer excitons in monolayer MoSe2-WSe2 heterostructures by both photoluminescence and photoluminescence excitation spectroscopy. The energy and luminescence intensity of interlayer excitons are highly tunable by an applied vertical gate voltage, implying electrical control of the heterojunction band-alignment. Using time resolved photoluminescence, we find that the interlayer exciton is long-lived with a lifetime of about 1.8 ns, an order of magnitude longer than intralayer excitons13-16. Our work demonstrates the ability to optically pump interlayer electric polarization and provokes the immediate exploration of interlayer excitons for condensation phenomena, as well as new applications in 2D light-emitting diodes, lasers, and photovoltaic devices., With Supplementary Materials

Light-emitting diodes are of importance for lighting, displays, optical interconnects, logic and sensors. Hence the development of new systems that allow improvements in their efficiency, spectral properties, compactness and integrability could have significant ramifications. Monolayer transition metal dichalcogenides have recently emerged as interesting candidates for optoelectronic applications due to their unique optical properties. Electroluminescence has already been observed from monolayer MoS2 devices. However, the electroluminescence efficiency was low and the linewidth broad due both to the poor optical quality of MoS2 and to ineffective contacts. Here, we report electroluminescence from lateral p-n junctions in monolayer WSe2 induced electrostatically using a thin boron nitride support as a dielectric layer with multiple metal gates beneath. This structure allows effective injection of electrons and holes, and combined with the high optical quality of WSe2 it yields bright electroluminescence with 1000 times smaller injection current and 10 times smaller linewidth than in MoS2. Furthermore, by increasing the injection bias we can tune the electroluminescence between regimes of impurity-bound, charged, and neutral excitons. This system has the required ingredients for new kinds of optoelectronic devices such as spin- and valley-polarized light-emitting diodes, on-chip lasers, and two-dimensional electro-optic modulators., Comment: 13 pages main text with 4 figures + 4 pages upplemental materials

Coupling degrees of freedom of distinct nature plays a critical role in numerous physical phenomena. The recent emergence of layered materials provides a laboratory for studying the interplay between internal quantum degrees of freedom of electrons. Here, we report experimental signatures of new coupling phenomena connecting real spin with layer pseudospins in bilayer WSe2. In polarization-resolved photoluminescence measurements, we observe large spin orientation of neutral and charged excitons generated by both circularly and linearly polarized light, with a splitting of the trion spectrum into a doublet at large vertical electrical field. These observations can be explained by locking of spin and layer pseudospin in a given valley. Because up and down spin states are localized in opposite layers, spin relaxation is substantially suppressed, while the doublet emerges as a manifestation of electrically induced spin splitting resulting from the interlayer bias. The observed distinctive behavior of the trion doublet under circularly and linearly polarized light excitation further provides spectroscopic evidence of interlayer and intralayer trion species, a promising step toward optical manipulation in van der Waals heterostructures through the control of interlayer excitons., Comment: Original submitted version. To appear in Nature Physics