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Register a new userHigh order harmonic generation in semiconductors driven at near- and mid-IR wavelengths
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David Freeman
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We study high order harmonics generation (HHG) in crystalline silicon and diamond subjected to near and mid-infrared laser pulses. We employ time-dependent density functional theory and solve the time-dependent Kohn-Sham equation in the single-cell geometry. We demonstrate that clear and clean HHG spectra can be generated with careful selection of the pulse duration. In addition, we implement dephasing effects through a displacement of atomic positions in a silicon large super-cell prepared by a molecular dynamics simulation. We compare our results with the previous calculations by Floss et al. [arXiv:1705.10707] [Phys. Rev. A 97, 011401(R) (2018)] on Diamond at 800 nm and by Tancogne-Dejean et al. [arXiv:1609.09298] [Phys. Rev. Lett. 118, 087403 (2017)] on Si at 2000 nm.
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Two types of optical metamaterials operating at near-IR and mid-IR frequencies, respectively, have been designed, fabricated by nanoimprint lithography (NIL), and characterized by laser spectroscopic ellipsometry. The structure for the near-IR range was a metal/dielectric/metal stack fishnet structure that demonstrated negative permittivity and permeability in the same frequency region and hence exhibited a negative refractive index at a wavelength near 1.7 um. In the mid-IR range, the metamaterial was an ordered array of four-fold symmetric L-shaped resonators (LSRs) that showed both a dipole plasmon resonance resulting in negative permittivity and a magnetic resonance with negative permeability near wavelengths of 3.7 um and 5.25 um, respectively. The optical properties of both metamaterials are in agreement with theoretical predictions. This work demonstrates the feasibility of designing various optical negative-index metamaterials and fabricating them using the nanoimprint lithography as a low-cost, high-throughput fabrication approach.
High harmonic generation (HHG) has unleashed the power of strong laser physics in solids. Here we investigate HHG from a large system, solid C$_{60}$, with 240 valence electrons engaging harmonic generation at each crystal momentum, the first of this kind. We employ the density functional theory and the time-dependent Liouville equation of the density matrix to compute HHG signals. We find that under a moderately strong laser pulse, HHG signals reach 15th order, consistent with the experimental results from C$_{60}$ plasma. The helicity dependence in solid C$_{60}$ is weak, due to the high symmetry. In contrast to the general belief, HHG is unsuitable for band structure mapping in C$_{60}$. However, we find a window of opportunity using a long wavelength, where harmonics are generated through multiple-photon excitation. In particular, the 5th order harmonic energies closely follow the transition energy dispersion between the valence and conduction bands. This finding is expected to motivate future experimental investigations.
We investigate high-order harmonic generation (HHG) in graphene with a quantum master equation approach. The simulations reproduce the observed enhancement in HHG in graphene under elliptically polarized light [N. Yoshikawa et al, Science 356, 736 (2017)]. On the basis of a microscopic decomposition of the emitted high-order harmonics, we find that the enhancement in HHG originates from an intricate nonlinear coupling between the intraband and interband transitions that are respectively induced by perpendicular electric field components of the elliptically polarized light. Furthermore, we reveal that contributions from different excitation channels destructively interfere with each other. This finding suggests a path to potentially enhance the HHG by blocking a part of the channels and canceling the destructive interference through band-gap or chemical potential manipulation.
A first-principles study of the birefringence and the frequency dependent second harmonic generation (SHG) coefficients of the ternary pnictide semiconductors with formula ABC$_2$ (A = Zn, Cd; B = Si, Ge; C = As, P) with the chalcopyrite structures was carried out. We show that a simple empirical observation that a smaller value of the gap is correlated with larger value of SHG is qualitatively true. However, simple inverse power scaling laws between gaps and SHG were not found. Instead, the real value of the nonlinear response is a result of a very delicate balance between different intraband and interband terms.
We theoretically investigate detuning-dependent properties of high-order harmonic generation (HHG) in monolayer transition metal dichalcogenides (TMDCs). In contrast to HHG in conventional materials, TMDCs show both parallel and perpendicular emissions with respect to the incident electric field. We find that such an anomalous emission can be artificially controlled by the frequency detuning of the incident electric fields, i.e., the parallel and perpendicular HHG can be strongly enhanced by multiphoton resonances. This peculiar phenomenon would provide a way for controlling HHG in TMDCs and stimulate the realization of novel optical devices.
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