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Register a new userInterlayer exciton mediated second harmonic generation in bilayer MoS2
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Second harmonic generation (SHG) is a non-linear optical process, where two photons coherently combine into one photon of twice their energy. Efficient SHG occurs for crystals with broken inversion symmetry, such as transition metal dichalcogenide monolayers. Here we show tuning of non-linear optical processes in an inversion symmetric crystal. This tunability is based on the unique properties of bilayer MoS2, that shows strong optical oscillator strength for the intra- but also inter-layer exciton resonances. As we tune the SHG signal onto these resonances by varying the laser energy, the SHG amplitude is enhanced by several orders of magnitude. In the resonant case the bilayer SHG signal reaches amplitudes comparable to the off-resonant signal from a monolayer. In applied electric fields the interlayer exciton energies can be tuned due to their in-built electric dipole via the Stark effect. As a result the interlayer exciton degeneracy is lifted and the bilayer SHG response is further enhanced by an additional two orders of magnitude, well reproduced by our model calculations.
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We show that the lack of inversion symmetry in monolayer MoS2 allows strong optical second harmonic generation. Second harmonic of an 810-nm pulse is generated in a mechanically exfoliated monolayer, with a nonlinear susceptibility on the order of 1E-7 m/V. The susceptibility reduces by a factor of seven in trilayers, and by about two orders of magnitude in even layers. A proof-of-principle second harmonic microscopy measurement is performed on samples grown by chemical vapor deposition, which illustrates potential applications of this effect in fast and non-invasive detection of crystalline orientation, thickness uniformity, layer stacking, and single-crystal domain size of atomically thin films of MoS2 and similar materials.
Coulomb bound electron-hole pairs, excitons, govern the optical properties of semi-conducting transition metal dichalcogenides like MoS$_2$ and WSe$_2$. We study optical transitions at the K-point for 2H homobilayer MoS$_2$ in Density Functional Theory (DFT) including excitonic effects and compare with reflectivity measurements in high quality samples encapsulated in hexagonal BN. In both calculated and measured spectra we find a strong interlayer exciton transition in energy between A and B intralayer excitons, observable for T$=4 -300$ K, whereas no such transition is observed for the monolayer in the same structure in this energy range. The interlayer excitons consist of an electron localized in one layer and a hole state delocalized over the bilayer, which results in the unusual combination of high oscillator strength and a static dipole moment. We also find signatures of interlayer excitons involving the second highest valence band (B) and compare absorption calculations for different bilayer stackings. For homotrilayer MoS$_2$ we also observe interlayer excitons and an energy splitting between different intralayer A-excitons originating from the middle and outer layers, respectively.
Nonreciprocal devices that allow the light propagation in only one direction are indispensable in photonic circuits and emerging quantum technologies. Contemporary optical isolators and circulators, however, require large size or strong magnetic fields because of the general weakness of magnetic light-matter interactions, which hinders their integration into photonic circuits. Aiming at stronger magneto-optical couplings, a promising approach is to utilize nonlinear optical processes. Here, we demonstrate nonreciprocal magnetoelectric second harmonic generation (SHG) in CuB2O4. SHG transmission changes by almost 100% in a magnetic-field reversal of just 10 mT. The observed nonreciprocity results from an interference between the magnetic-dipole- and electric-dipole-type SHG. Even though the former is usually notoriously smaller than the latter, it is found that a resonantly enhanced magnetic-dipole-transition has a comparable amplitude as non-resonant electric-dipole-transition, leading to the near-perfect nonreciprocity. This mechanism could form one of the fundamental bases of nonreciprocity in multiferroics, which is transferable to a plethora of magnetoelectric systems to realize future nonreciprocal and nonlinear-optical devices.
Strong second-harmonic generation has recently been experimentally observed from metamaterials consisting of periodic arrays of metal split ring resonators with an effective negative magnetic permeability [Science, 313, 502 (2006)]. To explore the underlying physical mechanism, a classical model derived from microscopic theory is employed here. The quasi-free electrons inside the metal are approximated as a classical Coulomb-interacting electron gas, and their motion under the excitation of an external electromagnetic field is described by the cold-plasma wave equations. Through numerical simulations, it is demonstrated that the microscopic theory includes the dominant physical mechanisms bothqualitatively and quantitatively.
Angle-resolved second harmonic generation (SHG) spectra of ZnO microwires show characteristic Fano resonances in the spectral vicinity of exciton-polariton modes. The output SHG spectra after SHG interacting with exciton polariton shows a resonant enhancement peak accompanied by a suppression dip originating from the constructive and destructive interference respectively. It is demonstrated that the Fano line shape, and thus the Fano asymmetry parameter q, can be tuned by the phase-shift of the two channels. The phase-dependent q was calculated and the model describes our experimental results well. In particular, the phase-to-q relation unveil the crucial information about the dynamics of the system, e.g., defining the line shape of output SHG spectra in a superposition of quantum states.
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