Model of third harmonic generation and electric field induced optical second harmonic using simplified bond-hyperpolarizability model

Abstract

We report for the first time a comprehensive study of the fourth rank tensor describing third harmonic generation (THG) and electric field induced second harmonic (EFISH) in centrosymmetric material from two different viewpoints: Group Theory (GT) and the Simplified Bond Hyperpolarizability Model (SBHM).We show that the fourth rank tensor related to THG and direct current (DC) EFISH can be reduced to two independent elements whereas SBHM always gives only one, reproducing perfectly well EFISH experimental results in Metal Oxyde Semiconductor (MOS). We argue that it is possible to reduce the fourth rank tensor describing EFISH to a third rank tensor and further deliver a classical explanation of EFISH regarding symmetry breaking where the term containing r 3 in the potential immediately leads to second harmonic generation (SHG). 1 arXiv:1505.06696v1 [cond-mat.mtrl-sci]

Impact of Plasmon-Induced Optically Rectified Electric Fields on Second Harmonic Generation

“…A linear response is observed in the double-layer region (see Figure S1, Supporting Information), where no electron transfer reactions alter the oxidation state of the Au surface. The experimentally derived Stark tuning coefficient is consistent with our previous reports from MBN on Au nanowire array electrodes, and the trend seen with the SHG signal is consistent with the electric field-induced SHG literature. ,,, …”

“…The experimentally derived Stark tuning coefficient is consistent with our previous reports from MBN on Au nanowire array electrodes, and the trend seen with the SHG signal is consistent with the electric field-induced SHG literature. 16,17,42,43 Optical rectification on the Au nanoisland surface was demonstrated by measuring the change in the SHG signal and Stark tuning of the CN stretch with increased laser power in air without an applied bias. Figure 3 shows the observed change in CN stretching frequency from increased laser power using two excitation wavelengths, 633 and 785 nm.…”

Bond Model of Second‐ and Third‐Harmonic Generation in Body‐ and Face‐Centered Crystal Structures

“…Another important step towards the understanding of SHG in diamond and zincblende lattices was the investigation of the third-rank susceptibility tensor that was obtained from the simplified bond-hyperpolarizability model (SBHM) and group theory (GT) [14,15], where it was shown that one can derive from GT the SBHM tensor. e work was later extended to show that the model can fit electric-field-induced second-harmonic (EFISH) experimental results in metal-Oxide semiconductor (MOS) with good accuracy [16]. Further test upon the validity of SBHM to model experimental RASHG data from zincblende samples which are noncentrosymmetric confirmed the existence of bulk dipole radiation as the dominant source of SHG [17].…”

Ab initio nonlinear optics in solids: linear electro-optic effect and electric-field induced second-harmonic generation

“…Concerning EFISH, most of the calculations have been performed using phenomenological models [24,25] in some cases integrated with group theory formalism in order to investigate the relation of EFISH with the symmetry of the crystal [26]. A frequency-dependent formulation of the third-order susceptibility was presented [27].…”