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Register a new userOptical second harmonic generation in Yttrium Aluminum Borate single crystals (theoretical simulation and experiment)
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Experimental measurements of the second order susceptibilities for the second harmonic generation are reported for YAl3(BO3)4 (YAB) single crystals for the two principal tensor components xyz and yyy. First principles calculation of the linear and nonlinear optical susceptibilities for Yttrium Aluminum Borate YAl3(BO3)4 (YAB) crystal have been carried out within a framework of the full-potential linear augmented plane wave (FP-LAPW) method. Our calculations show a large anisotropy of the linear and nonlinear optical susceptibilities. The observed dependences of the second order susceptibilities for the static frequency limit and for the frequency may be a consequence of different contribution of electron-phonon interactions. The imaginary parts of the second order SHG susceptibility chi_{123}^{(2)}(omega), chi_{112}^{(2)}(omega), chi_{222}^{(2)}(omega), and chi_{213}^{(2)}(omega) are evaluated. We find that the 2(omega) inter-band and intra-band contributions to the real and imaginary parts of chi_{ijk}^{(2)}l(omega) show opposite signs. The calculated second order susceptibilities are in reasonably good agreement with the experimental measurements.
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A systematic {it ab initio} study of the second-order nonlinear optical properties of BN nanotubes within density functional theory in the local density approximation has been performed. Highly accurate full-potential projector augmented-wave method was used. Specifically, the second-harmonic generation ($chi_{abc}^{(2)}$) and linear electro-optical ($r_{abc}$) coefficients of a large number of the single-walled zigzag, armchair and chiral BN nanotubes (BN-NT) as well as the double-walled zigzag (12,0)@(20,0) BN nanotube and the single-walled zigzag (12,0) BN-NT bundle have been calculated. Importantly, unlike carbon nanotubes, both the zigzag and chiral BN-NTs are found to exhibit large second-order nonlinear optical behavior with the $chi_{abc}^{(2)}$ and $r_{abc}$ coefficients being up to thirty times larger than that of bulk BN in both zinc-blende and wurtzite structures, indicating that BN-NTs are promising materials for nonlinear optical and opto-electric applications. Though the interwall interaction in the double-walled BN-NTs is found to reduce the second-order nonlinear optical coefficients significantly, the interwall interaction in the single-walled BN-NT bundle has essentially no effect on the nonlinear optical properties. The prominant features in the spectra of $chi_{abc}^{(2)}(-2omega,omega,omega)$ of the BN-NTs are suscessfully correlated with the features in the linear optical dielectric function $epsilon (omega)$ in terms of single-photon and two-photon resonances.
We report the observation of optical second harmonic generation (SHG) in single-layer indium selenide (InSe). We measure a second harmonic signal of $>10^3$ $textrm{cts/s}$ under nonresonant excitation using a home-built confocal microscope and a standard pulsed pico-second laser. We demonstrate that polarization-resolved SHG serves as a fast, non-invasive tool to determine the crystal axes in single-layer InSe and to relate the sharp edges of the flake to the armchair and zigzag edges of the crystal structure. Our experiment determines these angles to an accuracy better than $pm$ $0.2^{circ}$. Treating the two-dimensional material as a nonlinear polarizable sheet, we determine a second-order nonlinear sheet polarizability $| chi_{textrm{sheet}}^{(2)}|=(17.9 pm 11.0)times 10^{-20}$ $textrm{m}^2 textrm{V}^{-1}$ for single-layer InSe, corresponding to an effective nonlinear susceptibility value of $| chi_textrm{eff}^{(2)}| approx (223 pm 138) times 10^{-12}$ $textrm{m} textrm{V}^{-1}$ accounting for the sheet thickness ($textrm{d} approx 0.8$ $textrm{nm}$). We demonstrate that the SHG technique can also be applied to encapsulated samples to probe their crystal orientations. The method is therefore suitable for creating high quality van der Waals heterostructures with control over the crystal directions.
Effect of L-threonine (LT) doping on crystalline perfection, second harmonic generation (SHG) efficiency, optical transparency and laser damage threshold (LDT) in potassium dihydrogen phosphate (KDP) crystals grown by slow evaporation solution technique (SEST) has been investigated. The influence of doping on growth rate and morphology of the grown crystals has also been studied. Powder X-ray diffraction data confirms the crystal structure of KDP and shows a systematic variation in intensity of diffraction peaks in correlation with morphology due to varying LT concentration. No extra phase formation was observed which is further confirmed by Fourier Transform (FT) Raman studies. High-resolution X-ray diffraction curves indicate that crystalline perfection has been improved to a great extent at low concentrations with a maximum perfection at 1 mol% doping. At higher concentrations (5 to 10 mol%), it is slightly reduced due to excess incorporation of dopants at the interstitial sites of the crystalline matrix. LDT has been increased considerably with increase in doping concentration, whereas SHG efficiency was found to be maximum at 1 mol% in correlation with crystalline. The optical transparency for doped crystals has been increased as compared to that of pure KDP with a maximum value at 1 mol% doping.
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.
We report the observations of unexpected layer-dependent, strong, and anisotropic second harmonic generations (SHGs) in atomically thin ReS2. Appreciable (negligible) SHGs are obtained from even (odd) numbers of ReS2 layers, which is opposite to the layer-dependence of SHGs in group VI transition metal dichalcogenides, such as MoS2 and WS2. The results are analyzed from ReS2s crystal structure, implying second harmonic polarizations generated from the interlayer coupling. Pumped by a telecomband laser, SHG from the bilayer ReS2 is almost one order of magnitude larger than that from the monolayer WS2. The estimated second-order nonlinear susceptibility of 900 pm/V is remarkably high among those reported in two-dimensional materials. The laser polarization dependence of ReS2s SHG is strongly anisotropic and indicates its distorted lattice structure with more unequal and non-zero second-order susceptibility elements.
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