Manipulating properties of matter at the nanoscale is the essence of nanotechnology, which has enabled the realization of quantum dots, nanotubes, metamaterials, and two-dimensional materials with tailored electronic and optical properties. Two-dimensional semiconductors have revealed promising perspectives in nanotechnology. However, the tunability of their physical properties is challenging for semiconductors studied until now. Here we show the ability of morphological manipulation strategies, such as nanotexturing or, at the limit, important surface roughness, to enhance light absorption and the luminescent response of atomically thin indium selenide nanosheets. Besides, quantum-size confinement effects make this two-dimensional semiconductor to exhibit one of the largest band gap tunability ranges observed in a two-dimensional semiconductor: from infrared, in bulk material, to visible wavelengths, at the single layer. These results are relevant for the design of new optoelectronic devices, including heterostructures of two-dimensional materials with optimized band gap functionalities and in-plane heterojunctions with minimal junction defect density.
Van der Waals materials offer a wide range of atomic layers with unique properties that can be easily combined to engineer novel electronic and photonic devices. A missing ingredient of the van der Waals platform is a two-dimensional crystal with naturally occurring out-of-plane luminescent dipole orientation. Here we measure the far-field photoluminescence intensity distribution of bulk InSe and two-dimensional InSe, WSe 2 and MoSe 2 . We demonstrate, with the support of ab-initio calculations, that layered InSe flakes sustain luminescent excitons with an intrinsic out-of-plane orientation, in contrast with the in-plane orientation of dipoles we find in two-dimensional WSe 2 and MoSe 2 at room-temperature. These results, combined with the high tunability of the optical response and outstanding transport properties, position layered InSe as a promising semiconductor for novel optoelectronic devices, in particular for hybrid integrated photonic chips which exploit the out-of-plane dipole orientation.
Gallium selenide is one of the most promising candidates to extend the window of band gap values provided by existing two-dimensional semiconductors deep into the visible potentially reaching the ultraviolet. However, the tunability of its band gap by means of quantum confinement effects is still unknown, probably due to poor nanosheet stability. Here, we demonstrate that the optical band gap band of GaSe nanosheets can be tuned by ∼120 meV from bulk to 8 nm thick. The luminescent response of very thin nanosheets (<8 nm) is strongly quenched due to early oxidation. Oxidation favors the emergence of sharp material nanospikes at the surface attributable to strain relaxation. Simultaneously, incorporated oxygen progressively replaces selenium giving rise to GaO with a residual presence of GaSe that tends to desorb. These results are relevant for the development and design of visible/ultraviolet electronics and optoelectronics with tunable functionalities based on atomically thin GaSe.
The successful integration of few-layer thick hexagonal boron nitride (hBN) into devices based on two-dimensional materials requires fast and non-destructive techniques to quantify their thickness. Optical contrast methods and Raman spectroscopy have been widely used to estimate the thickness of two-dimensional semiconductors and semi-metals. However, they have so far not been applied to two-dimensional insulators. In this work, we demonstrate the ability of optical contrast techniques to estimate the thickness of few-layer hBN on SiO2/Si substrates, which was also measured by atomic force microscopy. Optical contrast of hBN on SiO2/Si substrates exhibits a linear trend with the number of hBN monolayers in the few-layer thickness range. We also used bandpass filters (500–650 nm) to improve the effectiveness of the optical contrast methods for thickness estimations. We also investigated the thickness dependence of the high frequency in-plane E2g phonon mode of atomically thin hBN on SiO2/Si substrates by micro-Raman spectroscopy, which exhibits a weak thickness-dependence attributable to the in-plane vibration character of this mode. Ab initio calculations of the Raman active phonon modes of atomically thin free-standing crystals support these results, even if the substrate can reduce the frequency shift of the E2g phonon mode by reducing the hBN thickness. Therefore, the optical contrast method arises as the most suitable and fast technique to estimate the thickness of hBN nanosheets.
The particular optical and electronic properties recently reported for 2D InSe depict this 2D material as being very versatile for future electronic and optoelectronic devices with tunable and optimized functionalities. For its fundamental study and the development of practical applications, rapid and accurate identification methods of atomically thin InSe are essential. Here, we demonstrate an enhancement of the optical contrast between InSe nanosheets and the underlying SiO/Si substrate by illuminating with a 40 nm wide bandpass filter centered at 500 nm. Moreover, we study the optical contrast of 2D InSe on transparent substrates. Our results suggest that a good optical contrast is achieved for transparent substrates with low real refractive indices such as LiF or a viscoelastic polydimethylsiloxane stamp. In this case, an optimum optical contrast would be achieved by using a bandpass filter centered at 450 nm. These results can be very useful for speeding up the continuously growing research on 2D InSe and its applications.
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