Wenpeng Han

Valley-selective circular dichroism of monolayer molybdenum disulphide

A two-dimensional honeycomb lattice harbors a pair of inequivalent valleys in the k-space electronic structure, in the vicinities of the vertices of a hexagonal Brillouin zone, K±. It is particularly appealing to exploit this emergent degree of freedom of charge carriers, in what is termed “valleytronics”, if charge carrier imbalance between the valleys can be achieved. The physics of valley polarization will make possible electronic devices such as valley filter and valley valve, and optoelectronic Hall devices, all very promising for next-generation electronic and optoelectronic applications. The key challenge lies with achieving valley imbalance, of which a convincing demonstration in a two-dimensional honeycomb structure remains evasive, while there are only a handful of examples for other materials. We show here, using first principles calculations, that monolayer MoS2, a novel two-dimensional semiconductor with a 1.8 eV direct band gap, is an ideal material for valleytronics by valley-selective circular dichroism, with ensuing valley polarization and valley Hall effect.

The shear mode of multilayer graphene

The quest for materials capable of realizing the next generation of electronic and photonic devices continues to fuel research on the electronic, optical and vibrational properties of graphene. Few-layer graphene (FLG) flakes with less than ten layers each show a distinctive band structure. Thus, there is an increasing interest in the physics and applications of FLGs. Raman spectroscopy is one of the most useful and versatile tools to probe graphene samples. Here, we uncover the interlayer shear mode of FLGs, ranging from bilayer graphene (BLG) to bulk graphite, and suggest that the corresponding Raman peak measures the interlayer coupling. This peak scales from ~43 cm(-1) in bulk graphite to ~31 cm(-1) in BLG. Its low energy makes it sensitive to near-Dirac point quasiparticles. Similar shear modes are expected in all layered materials, providing a direct probe of interlayer interactions.

Raman spectroscopy of shear and layer breathing modes in multilayer MoS2

We study by Raman scattering the shear and layer breathing modes in multilayer MoS2. These are identified by polarization measurements and symmetry analysis. Their positions change significantly with the number of layers, with different scaling for odd and even layers. A chain model can explain the results, with general applicability to any layered material, allowing a reliable diagnostic of their thickness.

Robust optical emission polarization in MoS2 monolayers through selective valley excitation

We report polarization resolved photoluminescence from monolayer MoS2, a two-dimensional, noncentrosymmetric crystal with direct energy gaps at two different valleys in momentum space. The inherent chiral optical selectivity allows exciting one of these valleys, and close to 90% polarized emission at 4 K is observed with 40% polarization remaining at 300 K. The high polarization degree of the emission remains unchanged in transverse magnetic fields up to 9 T indicating robust, selective valley excitation.

Resonant Raman spectroscopy of twisted multilayer graphene

Graphene and other two-dimensional crystals can be combined to form various hybrids and heterostructures, creating materials on demand, in which the interlayer coupling at the interface leads to modified physical properties as compared to their constituents. Here, by measuring Raman spectra of shear modes, we probe the coupling at the interface between two artificially-stacked few-layer graphenes rotated with respect to each other. The strength of interlayer coupling between the two interface layers is found to be only 20% of that between Bernal-stacked layers. Nevertheless, this weak coupling manifests itself in a Davydov splitting of the shear mode frequencies in systems consisting of two equivalent graphene multilayers, and in the intensity enhancement of shear modes due to the optical resonance with several optically allowed electronic transitions between conduction and valence bands in the band structures. This study paves way for fundamental understanding into the interface coupling of two-dimensional hybrids and heterostructures.Graphene and other two-dimensional crystals can be combined to form various hybrids and heterostructures, creating materials on demand with properties determined by the interlayer interaction. This is the case even for a single material, where multilayer stacks with different relative orientation have different optical and electronic properties. Probing and understanding the interface coupling is thus of primary importance for fundamental science and applications. Here we study twisted multilayer graphene flakes with multi-wavelength Raman spectroscopy. We find a significant intensity enhancement of the interlayer coupling modes (C peaks) due to resonance with new optically allowed electronic transitions, determined by the relative orientation of the layers. The interlayer coupling results in a Davydov splitting of the C peak in systems consisting of two equivalent graphene multilayers. This allows us to directly quantify the interlayer interaction, which is much smaller compared with Bernal-stacked interfaces. This paves the way to the use of Raman spectroscopy to uncover the interface coupling of two-dimensional hybrids and heterostructures.

Interface Coupling in Twisted Multilayer Graphene by Resonant Raman Spectroscopy of Layer Breathing Modes

Raman spectroscopy is the prime nondestructive characterization tool for graphene and related layered materials. The shear (C) and layer breathing modes (LBMs) are due to relative motions of the planes, either perpendicular or parallel to their normal. This allows one to directly probe the interlayer interactions in multilayer samples. Graphene and other two-dimensional (2d) crystals can be combined to form various hybrids and heterostructures, creating materials on demand with properties determined by the interlayer interaction. This is the case even for a single material, where multilayer stacks with different relative orientations have different optical and electronic properties. In twisted multilayer graphene there is a significant enhancement of the C modes due to resonance with new optically allowed electronic transitions, determined by the relative orientation of the layers. Here we show that this applies also to the LBMs, which can be now directly measured at room temperature. We find that twisting has a small effect on LBMs, quite different from the case of the C modes. This implies that the periodicity mismatch between two twisted layers mostly affects shear interactions. Our work shows that ultralow-frequency Raman spectroscopy is an ideal tool to uncover the interface coupling of 2d hybrids and heterostructures.

Diluted ferromagnetic semiconductor Li(Zn,Mn)P with decoupled charge and spin doping

We report the discovery of a diluted magnetic semiconductor, Li(Zn,Mn)P, in which charge and spin are introduced independently via lithium off-stoichiometry and the isovalent substitution of Mn2+ for Zn2+, respectively. Isostructural to (Ga,Mn)As, Li(Zn, Mn) P was found to be a p-type ferromagnetic semiconductor with excess lithium providing charge doping. First-principles calculations indicate that excess Li is favored to partially occupy the Zn site, leading to hole doping. Ferromagnetism with Curie temperature up to 34 K is achieved while the system still shows semiconducting transport behavior.

(La1-xBax)(Zn1-xMnx)AsO: A two-dimensional 1111-type diluted magnetic semiconductor in bulk form

We employ NMR techniques to investigate the nature of Mn spins in the I-II-V diluted magnetic semiconductor Li(Zn1−xMnx)P (x = 0.1, Curie temperature Tc = 25 K). We successfully identify the Li NMR signals arising from the Li sites adjacent to Mn, and probe the static and dynamic properties of Mn spins. From the NMR spin-lattice relaxation data, we show that the Mn spin-spin interactions extend over many unit cells.

Ultralow-frequency shear modes of 2-4 layer graphene observed in scroll structures at edges

The in-plane shear modes between neighbor-layers of 2-4 layer graphenes (LGs) and the corresponding graphene scrolls rolled up by 2-4LGs were investigated by Raman scattering. In contrast to that just one shear mode was observed in 3-4LGs, all the shear modes of 3-4LGs were observed in 3-4 layer scrolls (LSs), whose frequencies agree well with the theoretical predication by both a force-constant model and a linear chain model. In comparison to the broad width (about 12cm

(Ca,Na)(Zn,Mn)2As2: A new spin and charge doping decoupled diluted ferromagnetic semiconductor

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