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High harmonic generation (HHG) in solids reflects the underlying nonperturbative nonlinear dynamics of electrons in a strong light field and is a powerful tool for ultrafast spectroscopy of electronic structures. Photo-carrier doping allows us to understand the carrier dynamics and the correlations between the carriers in the HHG process. Here, we study the effect of incoherent electron-hole pairs on HHG in an atomically thin semiconductor. The experimentally observed response to photo-carrier doping is successfully reproduced in numerical simulations incorporating the photo-excited carrier distribution, excitonic Coulomb interaction and electron-electron scattering effects. The simulation results reveal that the presence of photo-carriers enhances the intraband current that contributes to high harmonics below the absorption edge. We also clarify that the excitation-induced dephasing process rather than the phase-space filling effect is the dominant mechanism reducing the higher order harmonics above the absorption edge. Our work provides a deeper understanding of high harmonic spectroscopy and the optimum conditions for generating extreme ultraviolet light from solids.

Atomically thin one dimensional (1D) van der Waals wires of transition metal monochalocogenides (TMMs) have been anticipated as promising building blocks for integrated nanoelectronics. While reliable production of TMM nanowires has eluded scientists over the past few decades, we finally demonstrated a bottom up fabrication of MoTe nanowires inside carbon nanotubes (CNTs). Still, the current synthesis method is based on vacuum annealing of reactive MoTe2, and limits access to a variety of TMMs. Here we report an expanded framework for high yield synthesis of the 1D tellurides including WTe, an unprecedented family of TMMs. Experimental and theoretical analyses revealed that the choice of suitable metal oxides as a precursor provides useful yield for their characterization. These TMM nanowires exhibit a significant optical absorption in the visible light region. More important, electronic properties of CNTs can be tuned by encapsulating different TMM nanowires., Comment: accepted by Nanoscale

The Floquet state, which is a periodically and intensely light driven quantum state in solids, has been attracting attention as a novel state that is coherently controllable on an ultrafast time scale. An important issue has been to demonstrate experimentally novel electronic properties in the Floquet state. One technique to demonstrate them is the light scattering spectroscopy, which offers an important clue to clarifying the symmetries and energy structures of the states through symmetry analysis of the polarization selection rules. Here, we determine circular and linear polarization selection rules of light scattering in a mid-infrared-driven Floquet system in monolayer MoS2 and provide a comprehensive understanding in terms of the "dynamical symmetry" of the Floquet state.

We present measurements of temperature dependence of photoluminescence intensity from monolayer MoS2 encapsulated by hexagonal boron nitride (hBN) flakes. The obtained temperature dependence shows an opposite trend to that of previously observed in a monolayer MoS2 on a SiO2 substrate. Ab-initio bandstructure calculations have revealed that monolayer MoS2 encapsulated by hBN flakes have no longer a direct-gap semiconductor but an indirect-gap semiconductor. This is caused by orbital hybridization between MoS2 and hBN, which leads to upward shift of gamma-valley of MoS2. This work shows an important implication that the hBN-encapsulated structures used to address intrinsic properties of two-dimensional crystals can alter basic properties encapsulated materials.

We demonstrated nonperturbative high harmonics induced by intense mid-infrared light up to 18th order that well exceed the material bandgap in monolayer transition metal dichalcogenides. The intensities of the even-order high-harmonic radiation did not monotonically decrease as the harmonic order increased. By comparing the high harmonic spectra with the optical absorption spectra, we found that the enhancement in the even-order high harmonics could be attributed to the resonance to the band nesting energy. The symmetry analysis shows that the valley polarization and anisotropic band structure lead to polarization of the high-harmonic radiation under excitation with the polarization along the zigzag direction. We also examined the possible recombination pathways of electrons and holes by calculating their dynamics in real and momentum spaces based on three-step model in solids. It revealed that, by considering the electrons and holes generated at neighboring lattice sites, the electron-hole polarization driven to the band nesting region should contribute to the high harmonic radiation. Our findings open the way for attosecond science with monolayer materials having widely tunable electronic structures.

We have investigated atomic and electronic structure of grain boundaries in monolayer MoS2, where relative angles between two different grains are 0 and 60 degree. The grain boundaries with specific relative angle have been formed with chemical vapor deposition growth on graphite and hexagonal boron nitride flakes; van der Waals interlayer interaction between MoS2 and the flakes restricts the relative angle. Through scanning tunneling microscopy and spectroscopy measurements, we have found that the perfectly stitched structure between two different grains of MoS2 was realized in the case of the 0 degree grain boundary. We also found that even with the perfectly stitched structure, valence band maximum and conduction band minimum shows significant blue shift, which probably arise from lattice strain at the boundary.

Property by design is one appealing idea in material synthesis but hard to achieve in practice. A recent successful example is the demonstration of van der Waals (vdW) heterostructures,1-3 in which atomic layers are stacked on each other and different ingredients can be combined beyond symmetry and lattice matching. This concept, usually described as a nanoscale Lego blocks, allows to build sophisticated structures layer by layer. However, this concept has been so far limited in two dimensional (2D) materials. Here we show a class of new material where different layers are coaxially (instead of planarly) stacked. As the structure is in one dimensional (1D) form, we name it "1D vdW heterostructures". We demonstrate a 5 nm diameter nanotube consisting of three different materials: an inner conductive carbon nanotube (CNT), a middle insulating hexagonal boron nitride nanotube (BNNT) and an outside semiconducting MoS2 nanotube. As the technique is highly applicable to other materials in the current 2D libraries,4-6 we anticipate our strategy to be a starting point for discovering a class of new semiconducting nanotube materials. A plethora of function-designable 1D heterostructures will appear after the combination of CNTs, BNNTs and semiconducting nanotubes.

The electronic states in isolated single-wall carbon nanotubes (SWCNTs) have been considered as an ideal realization of a Tomonaga-Luttinger liquid (TLL). However, it remains unclear whether one-dimensional correlated states are realized under local environmental effects such as the formation of a bundle structure. Intertube effects originating from other adjacent SWCNTs within a bundle may drastically alter the one-dimensional correlated state. In order to test the validity of the TLL model in bundled SWCNTs, low-energy spin excitation is investigated by nuclear magnetic resonance (NMR). The NMR relaxation rate in bundled mixtures of metallic and semiconducting SWCNTs shows a power-law temperature dependence with a theoretically predicted exponent. This demonstrates that a TLL state with the same strength as that for effective Coulomb interactions is realized in a bundled sample, as in isolated SWCNTs. In bundled metallic SWCNTs, we found a power-law temperature dependence of the relaxation rate, but the magnitude of the relaxation rate is one order of magnitude smaller than that predicted by theory. Furthermore, we found an almost doubled magnitude of the Luttinger parameter. These results indicate suppressed spin excitations with reduced Coulomb interactions in bundled metallic SWCNTs, which are attributable to intertube interactions originating from adjacent metallic SWCNTs within a bundle. Our findings give direct evidence that bundling reduces the effective Coulomb interactions via intertube interactions within bundled metallic SWCNTs., Comment: 6 pages, 3 figures

We report the observation of the intrinsic magnetic susceptibility of highly purified SWCNT samples prepared by a combination of acid treatment and density gradient ultracentrifugation (DGU). We observed that the diamagnetic susceptibility of SWCNTs increases linearly with increasing nanotube diameter. We found that the magnetic susceptibility divided by the diameter is a universal function of the scaled temperature. Furthermore, the estimated magnetic susceptibilities of pure semiconducting and pure metallic SWCNT samples suggest that they respond differently to changes in carrier density, which is consistent with theory. These findings provide experimental verification of the theoretically predicted diameter, temperature, and metallicity dependence of the magnetic susceptibility., Comment: 5 pages