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Register a new userUltrafast photocarrier recombination dynamics in black phosphorus-molybdenum disulfide (BP/MoS2) heterostructure
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Van der Waals (vdW) heterostructures constructed with two-dimensional (2D) materials have attracted great interests, due to their fascinating properties and potential for novel applications. While earlier efforts have advanced the understanding of the ultrafast cross-layer charge transfer process in 2D heterostructures, mechanisms for the interfacial photocarrier recombination remain, to a large extent, unclear. Here, we investigate a heterostructure comprised of black phosphorus (BP) and molybdenum disulfide (MoS2), with a type-II band alignment. Interestingly, it is found that the photo-generated electrons in MoS2 (transferred from BP) exhibit an ultrafast lifetime of about 5 ps, significantly shorter than those of the constituent materials. By corroborating with the relaxation of photo-excited holes in BP, it is revealed that the ultrafast time constant is as a result of efficient Langevin recombination, where the high hole mobility of BP facilitates a large recombination coefficient (approximately 2x10^-10 m^2/s). In addition, broadband transient absorption spectroscopy confirms that the hot electrons transferred to MoS2 distribute over a broad energy range following an ultrafast thermalization. The rate of the interlayer Langevin recombination is found to exhibit no energy level dependence. Our findings provide essential insights into the fundamental photo-physics in type-II 2D heterostructures, and also provide useful guidelines for customizing photocarrier lifetimes of BP for high-speed photo-sensitive devices.
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Single layer molybdenum disulfide (SLMoS2), a semiconductor possesses intrinsic bandgap and high electron mobility, has attracted great attention due to its unique electronic, optical, mechanical and thermal properties. Although thermal conductivity of SLMoS2 has been widely investigated recently, less studies focus on molybdenum disulfide nanotube (MoS2NT). Here, the comprehensive temperature, size and strain effect on thermal conductivity of MoS2NT are investigated. A chirality-dependent strain effect is identified in thermal conductivity of zigzag nanotube, in which the phonon group velocity can be significantly reduced by strain. Besides, results show that thermal conductivity has a ~T-1 and a ~Lb{eta} relation with temperature from 200 to 400 K and length from 10 to 320 nm, respectively. This work not only provides feasible strategies to modulate the thermal conductivity of MoS2NT, but also offers useful insights into the fundamental mechanisms that govern the thermal conductivity, which can be used for the thermal management of low dimensional materials in optical, electronic and thermoelectrical devices. Introduction.
The band structure of MoS$_2$ strongly depends on the number of layers, and a transition from indirect to direct-gap semiconductor has been observed recently for a single layer of MoS$_2$. Single-layer MoS$_2$ therefore becomes an efficient emitter of photoluminescence even at room temperature. Here, we report on scanning Raman and on temperature-dependent, as well as time-resolved photoluminescence measurements on single-layer MoS$_2$ flakes prepared by exfoliation. We observe the emergence of two distinct photoluminescence peaks at low temperatures. The photocarrier recombination at low temperatures occurs on the few-picosecond timescale, but with increasing temperatures, a biexponential photoluminescence decay with a longer-lived component is observed.
Black phosphorus (bP) has been recently investigated for next generation nanoelectronic multifunctional devices. However, the intrinsic instability of exfoliated bP (the bP nanoflakes) towards both moisture and air has so far overshadowed its practical implementation. In order to contribute to fill this gap, we report here the preparation of new hybrid polymer-based materials where bP nanoflakes exhibit a significantly improved stability. The new materials have been prepared by different synthetic paths including: i) the mixing of conventionally liquid-phase exfoliated bP (in DMSO) with PMMA solution; ii) the direct exfoliation of bP in a polymeric solution; iii) the in situ radical polymerization after exfoliating bP in the liquid monomer (methyl methacrylate, MMA). This last methodology concerns the preparation of stable suspensions of bPn-MMA by sonication-assisted liquid phase exfoliation (LPE) of bP in the presence of MMA followed by radical polymerization. The hybrids characteristics have been compared in order to evaluate the bP dispersion and the effectiveness of the bPn interfacial interactions with polymer chains aimed at their long-term environmental stabilization. The passivation of bPn results particularly effective when the hybrid material is prepared by in situ polymerization. By using this synthetic methodology, the nanoflakes, even if with a gradient of dispersion (size of aggregates), preserve their chemical structure from oxidation (as proved by both Raman and 31P-Solid State NMR studies) and are particularly stable to air and UV light exposure.
The interface between two-dimensional semiconductors and metal contacts is an important topic of research of nanoelectronic devices based on two-dimensional semiconducting materials such as molybdenum disulfide (MoS2). We report transport properties of thin MoS2 flakes in a field-effect transistor geometry with Ti/Au and Al contacts. In contrast to widely used Ti/Au contacts, the conductance of flakes with Al contacts exhibits a smaller gate-voltage dependence, which is consistent with a substantial electron doping effect of the Al contacts. The temperature dependence of two-terminal conductance for the Al contacts is also considerably smaller than for the Ti/Au contacts, in which thermionic emission and thermally assisted tunneling play a dominant role. This result is explained in terms of the assumption that the carrier injection mechanism at an Al contact is dominated by tunneling that is not thermally activated.
The current state of the chemical functionalization of three types of single sheet 2D materials, namely, graphene, molybdenum disulfide (MoS2), and black phosphorus (BP) is summarized. Such 2D sheet polymers represent currently an emerging field at the interface of synthetic chemistry, physics, and materials science. Both covalent and non-covalent functionalization of sheet architectures allows for a systematic modification of their properties, i.e. an improvement of solubility and processability, the prevention of re-aggregation or a band gap tuning. Next to successful functionalization concepts also fundamental challenges are addressed. These include the insolubility and polydispersity of most 2D sheet polymers, the development of suitable characterization tools, the identification of effective binding strategies, the chemical activation of the usually rather unreactive basal planes for covalent addend binding, and the regioselectivity of plane addition reactions. Although a number of these questions remain elusive in this review, the first promising concepts to overcome such hurdles have been listed.
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