Atomically thin nanowires (NWs) can be synthesized inside single-walled carbon nanotubes (SWCNTs) and feature unique crystal structures. Here we show that HgTe nanowires formed inside small-diameter (<1 nm) SWCNTs can advantageously alter the optical and electronic properties of the SWCNTs. Metallic purification of the filled SWCNTs was achieved by a gel column chromatography method, leading to an efficient extraction of the semiconducting and metallic portions with known chiralities. Electron microscopic imaging revealed that zigzag HgTe chains were the dominant NW geometry in both the semiconducting and metallic species. Equilibrium-state and ultrafast spectroscopy demonstrated that the coupled electron–phonon system was modified by the encapsulated HgTe NWs, in a way that varied with the chirality. For semiconducting SWCNTs with HgTe NWs, Auger relaxation processes were suppressed, leading to enhanced photoluminescence emission. In contrast, HgTe NWs enhanced the Auger relaxation rate of metallic SWCNTs and created faster phonon relaxation, providing experimental evidence that encapsulated atomic chains can suppress hot carrier effects and therefore boost electronic transport.
Metrics & MoreArticle Recommendations CONSPECTUS: Due to the spatial confinement, two-dimensional metal chalcogenides display an extraordinary optical response and carrier transport ability. Solution-based synthesis techniques such as colloidal hot injection and ion exchange provide a cost-effective way to fabricate such low-dimensional semiconducting nanocrystals. Over the years, developments in colloidal chemistry made it possible to synthesize various kinds of ultrathin colloidal nanoplatelets, including wurtzite-and zinc blende-type CdSe, rock salt PbS, black phosphorus-like SnX (X = S or Se), hexagonal copper sulfides, selenides, and even transition metal dichalcogenides like MoS 2 . By altering experimental conditions and applying capping ligands with specific functional groups, it is possible to accurately tune the dimensionality, geometry, and consequently the optical properties of these colloidal metal chalcogenide crystals.Here, we review recent progress in the syntheses of twodimensional colloidal metal chalcogenides (CMCs) and property characterizations based on optical spectroscopy or device-related measurements. The discoveries shine a light on their huge prospect for applications in areas such as photovoltaics, optoelectronics, and spintronics. In specific, the formation mechanisms of two-dimensional CMCs are discussed. The growth of colloidal nanocrystals into a two-dimensional shape is found to require either an intrinsic structural asymmetry or the assist of coexisted ligand molecules, which act as lamellar double-layer templates or "facet" the crystals via selective adsorption. By performing optical characterizations and especially ultrafast spectroscopic measurements on these two-dimensional CMCs, their unique electronic and excitonic features are revealed. A strong dependence of optical transition energies linked to both interband and inter-subband processes on the crystal geometry can be verified, highlighting a tremendous confinement effect in such nanocrystals. With the selfassembly of two-dimensional nanocrystals or coupling of different phases by growing heterostructures, unconventional optical performances such as charge transfer state generation or efficient Forster resonance energy transfer are discovered. The growth of large-scale individualized PbS and SnS nanosheets can be realized by facile hot injection techniques, which gives the opportunity to investigate the charge carrier behavior within a single nanocrystal. According to the results of the device-based measurements on these individualized crystals, structure asymmetry-induced anisotropic electrical responses and Rashba effects caused by a splitting of spin-resolved bands in the momentum space due to strong spin−orbit-coupling are demonstrated. It is foreseen that such geometrycontrolled, large-scale two-dimensional CMCs can be the ideal materials used for designing high-efficiency photonics and electronics.
Studying the optical performance of carbon nanotubes (CNTs) filled with guest materials can reveal the fundamental photochemical nature of ultrathin one-dimensional (1D) nanosystems, which are attractive for applications including photocatalysis. Here, we report comprehensive spectroscopic studies of how infiltrated HgTe nanowires (NWs) alter the optical properties of small-diameter (d t < 1 nm) single-walled carbon nanotubes (SWCNTs) in different environments: isolated in solution, suspended in a gelatin matrix, and heavily bundled in network-like thin films. Temperature-dependent Raman and photoluminescence measurements revealed that the HgTe NW filling can alter the stiffness of SWCNTs and therefore modify their vibrational and optical modes. Results from optical absorption and X-ray photoelectron spectroscopy demonstrated that the semiconducting HgTe NWs did not provide substantial charge transfer to or from the SWCNTs. Transient absorption spectroscopy further highlighted that the fillinginduced nanotube distortion can alter the temporal evolution of excitons and their transient spectra. In contrast to previous studies on functionalized CNTs, where electronic or chemical doping often drove changes to the optical spectra, we highlight structural distortion as playing an important role.
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