https://absimage.aps.org/image/MAR14/MWS_MAR14-2014-020819.pdf

Van der Waals heterostructures

Black phosphorous (BP), the most thermodynamically stable allotrope of phosphorus, is a high-mobility layered semiconductor with direct band-gap determined by the number of layers from 0.3 eV (bulk) to 2.0 eV (single layer). Therefore, BP is considered as a natural candidate for broadband optical applications, particularly in the infrared (IR) and mid-IR part of the spectrum. The strong light-matter interaction, narrow direct band-gap, and wide range of tunable optical response make BP as a promising nonlinear optical material, particularly with great potentials for infrared and mid-infrared opto-electronics. Herein, we experimentally verified its broadband and enhanced saturable absorption of multi-layer BP (with a thickness of ~10 nm) by wide-band Z-scan measurement technique, and anticipated that multi-layer BPs could be developed as another new type of two-dimensional saturable absorber with operation bandwidth ranging from the visible (400 nm) towards mid-IR (at least 1930 nm). Our results might suggest that ultra-thin multi-layer BP films could be potentially developed as broadband ultra-fast photonics devices, such as passive Q-switcher, mode-locker, optical switcher etc.

Broadband nonlinear optical response in multi-layer black phosphorus: an emerging infrared and mid-infrared optical material

2D layered materials (2DLMs) are a subject of intense research for a wide variety of applications (e.g., electronics, photonics, and optoelectronics) due to their unique physical properties. Most recently, increasing research efforts on 2DLMs are projected toward the nonlinear optical properties of 2DLMs, which are not only fascinating from the fundamental science point of view but also intriguing for various potential applications. Here, the current state of the art in the field of nonlinear optics based on 2DLMs and their hybrid structures (e.g., mixed-dimensional heterostructures, plasmonic structures, and silicon/fiber integrated structures) is reviewed. Several potential perspectives and possible future research directions of these promising nanomaterials for nonlinear optics are also presented.

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Nonlinear Optics with 2D Layered Materials.

The properties and applications of molybdenum oxides are reviewed in depth. Molybdenum is found in various oxide stoichiometries, which have been employed for different high-value research and commercial applications. The great chemical and physical characteristics of molybdenum oxides make them versatile and highly tunable for incorporation in optical, electronic, catalytic, bio, and energy systems. Variations in the oxidation states allow manipulation of the crystal structure, morphology, oxygen vacancies, and dopants, to control and engineer electronic states. Despite this overwhelming functionality and potential, a definitive resource on molybdenum oxide is still unavailable. The aim here is to provide such a resource, while presenting an insightful outlook into future prospective applications for molybdenum oxides.

Molybdenum Oxides – From Fundamentals to Functionality

The discovery of graphene one decade ago has triggered enormous interest in developing two-dimensional materials (2DMs)—that is 2D allotropes of various elements or compounds (consisting of two or more covalently bonded elements) or molecular frameworks with periodic structures. At present, various synthesis strategies have been exploited to produce 2DMs, such as top-down exfoliation and bottom-up chemical vapor deposition and solution synthesis methods. In this review article, we will highlight the interfacial roles toward the controlled synthesis of inorganic and organic 2DMs with varied structural features. We will summarize the state-of-the-art progress on interfacial synthesis strategies and address their advancements in the structural, morphological, and crystalline control by the direction of the arrangement of the molecules or precursors at a confined 2D space. First, we will provide an overview of the interfaces and introduce their advantages and uniqueness for the synthesis of 2DMs, followed by ...

Interface-Assisted Synthesis of 2D Materials: Trend and Challenges

Strong optical nonlinearity of CVD-grown MoS 2 monolayer as probed by wavelength-dependent second-harmonic generation

In this study, we utilized picosecond pulses from an Nd:YAG laser to investigate the nonlinear optical characteristics of monolayer MoSe2. Two-step growth involving the selenization of pulsed-laser-deposited MoO3 film was employed to yield the MoSe2 monolayer on a SiO2/Si substrate. Raman scattering, photoluminescence (PL) spectroscopy, and atomic force microscopy verified the high optical quality of the monolayer. The second-order susceptibility χ(2) was calculated to be ∼50 pm V−1 at the second harmonic wavelength ∼810 nm, which is near the optical gap of the monolayer. Interestingly, our wavelength-dependent second harmonic scan can identify the bound excitonic states including negatively charged excitons much more efficiently, compared with the PL method at room temperature. Additionally, the MoSe2 monolayer exhibits a strong laser-induced damage threshold ∼16 GW cm−2 under picosecond-pulse excitation. Our findings suggest that monolayer MoSe2 can be considered as a promising candidate for high-power, thin-film-based nonlinear optical devices and applications.

Nonlinear optical characteristics of monolayer MoSe2

We have investigated strong optical nonlinearity of monolayer MoS2(1–x)Se2x across the exciton resonance, which is directly tunable by Se doping. The quality of monolayer alloys prepared by chemical vapor deposition is verified by atomic force microscopy, Raman spectroscopy, and photoluminescence analysis. The crystal symmetry of all of our alloys is essentially D3h, as confirmed by polarization-dependent second-harmonic generation (SHG). The spectral structure of the exciton resonance is sampled by wavelength-dependent SHG (λ = 1000–1800 nm), where the SHG resonance red-shifts in accordance with the corresponding optical gap. Surprisingly, the effect of compositional variation turns out to be much more dramatic owing to the unexpected increase of B-exciton-induced SHG, which indeed dominates over the A-exciton resonance for x ≥ 0.3. The overall effect is therefore stronger and broader SHG resonance where the latter arises from different degrees of red-shift for the two exciton states. We report the corre...

Impact of Selenium Doping on Resonant Second-Harmonic Generation in Monolayer MoS2

The covalently bonded in-plane heterostructure (HS) of monolayer transition-metal dichalcogenides (TMDCs) possesses huge potential for high-speed electronic devices in terms of valleytronics. In this study, high-quality monolayer MoSe2-WSe2 lateral HSs are grown by pulsed-laser-deposition-assisted selenization method. The sharp interface of the lateral HS is verified by morphological and optical characterizations. Intriguingly, photoluminescence spectra acquired from the interface show rather clear signatures of pristine MoSe2 and WSe2 with no intermediate energy peak related to intralayer excitonic matter or formation of MoxW(1–x)Se2 alloys, thereby confirming the sharp interface. Furthermore, the discrete nature of laterally attached TMDC monolayers, each with doubly degenerated but nonequivalent energy valleys marked by (KM, K′M) for MoSe2 and (KW, K′W) for WSe2 in k space, allows simultaneous control of the four valleys within the excitation area without any crosstalk effect over the interface. As an ...

Growth and Simultaneous Valleys Manipulation of Two-Dimensional MoSe2-WSe2 Lateral Heterostructure

In this work, the friction characteristics of single-layer MoS2 prepared with chemical vapor deposition (CVD) at three different temperatures were quantitatively investigated and compared to those of single-layer MoS2 prepared using mechanical exfoliation. The surface and crystalline qualities of the MoS2 specimens were characterized using an optical microscope, atomic force microscope (AFM), and Raman spectroscopy. The surfaces of the MoS2 specimens were generally flat and smooth. However, the Raman data showed that the crystalline qualities of CVD-grown single-layer MoS2 at 800 °C and 850 °C were relatively similar to those of mechanically exfoliated MoS2 whereas the crystalline quality of the CVD-grown single-layer MoS2 at 900 °C was lower. The CVD-grown single-layer MoS2 exhibited higher friction than mechanically exfoliated single-layer MoS2, which might be related to the crystalline imperfections in the CVD-grown MoS2. In addition, the friction of CVD-grown single-layer MoS2 increased as the CVD growth temperature increased. In terms of tribological properties, 800 °C was the optimal temperature for the CVD process used in this work. Furthermore, it was observed that the friction at the grain boundary was significantly larger than that at the grain, potentially due to defects at the grain boundary. This result indicates that the temperature used during CVD should be optimized considering the grain size to achieve low friction characteristics. The outcomes of this work will be useful for understanding the intrinsic friction characteristics of single-layer MoS2 and elucidating the feasibility of single-layer MoS2 as protective or lubricant layers for micro- and nano-devices.

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Chinh Tam Le

Papers

Strong optical nonlinearity of CVD-grown MoS 2 monolayer as probed by wavelength-dependent second-harmonic generation

Nonlinear optical characteristics of monolayer MoSe2

Impact of Selenium Doping on Resonant Second-Harmonic Generation in Monolayer MoS2

Growth and Simultaneous Valleys Manipulation of Two-Dimensional MoSe2-WSe2 Lateral Heterostructure

Friction characteristics of mechanically exfoliated and CVD-grown single-layer MoS2