Quasi-phasematching of harmonic generation via multimode beating in waveguides

A new scheme for quasi-phasematching high harmonic generation (HHG) in gases is proposed. In this, the rapid variation of the axial intensity resulting from excitation of more than one mode of a waveguide is used to achieve quasi phasematching. Numerical modeling demonstrates enhancement of the harmonic signal over that achieved for a single coherence length by factors > 10(4). (C) 2007 Optical Society of America

Role of the plasma scale length in the harmonic generation from solid targets

We have investigated the generation of high harmonics from the interaction of 150 fsec, 790 nm, and 395 nm laser pulses with solid targets. Experiments are presented that demonstrate a strong dependence of the conversion efficiency on the temporal pulse shape and the resulting density scale length (L/lambda) of the preformed plasma. The highest conversion efficiencies are achieved for short density scale lengths (L/lambda less than or equal to 0.4), which result from high contrast ratio pulse interactions. [S1063-651X(98)50211-5].

Feasibility study of high harmonic generation from short wavelength lasers interacting with solid targets

The generation of the third and fourth harmonics from the interaction of a 1 ps, ultraviolet (UV), krypton fluoride (KrF) laser with a solid surface is investigated. The conversion efficiency is seen to increase linearly with I lambda(2), with a transition from specular harmonic emission to emission into 2 pi steradians occurring between 10(15) and 10(16) W cm(-2) mu m(2). The diffuse emission is strongly dependent on the incidence angle of the laser, with the peak in emission at around 30 degrees being consistent with measurements for resonance absorption. Finally, the conversion efficiencies are found to be in agreement with particle-in-cell (PIC) simulations including appropriate density scalelengths. (C) 1998 Elsevier Science B.V.

SPECTRALLY MODULATED 2ND-HARMONIC EMISSION FROM LASER-PLASMA FILAMENTS

Spectra of forward emitted second harmonic light from laser interaction with filamentary plasmas have been experimentally studied. Rather regular modulations in the frequency domain have been observed into overall red-shifted spectra. The observed spectral features are consistent with self-phase-modulation of the intense laser light in growing filaments. A model accounts for this effect.

Relativistic High Harmonic Generation In Gas Jet Targets

We experimentally demonstrate a new regime of high-order harmonic generation by relativistic-irradiance lasers in gas jet targets. Bright harmonics with both odd and even orders, generated by linearly as well as circularly polarized pulses, are emitted in the forward direction, while the base harmonic frequency is downshifted. A 9 TW laser generates harmonics up to 360 eV, within the 'water window' spectral region. With a 120 TW laser producing 40 uJ/sr per harmonic at 120 eV, we demonstrate the photon number scalability. The observed harmonics cannot be explained by previously suggested scenarios. A novel high-order harmonics generation mechanism [T. Zh. Esirkepov et al., AIP Proceedings, this volume], which explains our experimental findings, is based on the phenomena inherent in the relativistic laser - underdense plasma interactions (self-focusing, cavity evacuation, and bow wave generation), mathematical catastrophe theory which explains formation of electron density singularities (cusps), and collective radiation due to nonlinear oscillations of a compact charge.

Atomic harmonic generation in time-dependent R-matrix theory

We have developed the capability to determine accurate harmonic spectra for multielectron atoms within time-dependent R-matrix (TDRM) theory. Harmonic spectra can be calculated using the expectation value of the dipole length, velocity, or acceleration operator. We assess the calculation of the harmonic spectrum from He irradiated by 390-nm laser light with intensities up to 4 x 10(14) W cm(-2) using each form, including the influence of the multielectron basis used in the TDRM code. The spectra are consistent between the different forms, although the dipole acceleration calculation breaks down at lower harmonics. The results obtained from TDRM theory are compared with results from the HELIUM code, finding good quantitative agreement between the methods. We find that bases which include pseudostates give the best comparison with the HELIUM code, but models comprising only physical orbitals also produce accurate results.

Influence of multiple ionization thresholds on harmonic generation from Ar+

We apply time-dependent R-matrix theory to investigate harmonic generation from ground-state Ar+ with M = 0 at a wavelength of 390 nm. Contributions associated with the different 3s(2)3p(4) ionization thresholds are assessed, including the interference between these. The dominant contribution originates from the second ionization threshold, 3s(2)3p(4 1)D. Changes to the harmonic yields arising from the higher 3s3p(5) thresholds are also assessed. We further confirm that Ar+ has a higher harmonic yield than He for the same laser pulse, despite having a higher ionization threshold. 

Probing Ferroelectrics Using Optical Second Harmonic Generation

Nonlinear optics is an essential component of modern laser systems and optoelectronic devices. It has also emerged as an important tool in probing the electronic, vibrational, magnetic, and crystallographic structure of materials ranging from oxides and metals, to polymers and biological samples. This review focuses on the specific technique of optical second harmonic generation (SHG), and its application in probing ferroelectric complex oxide crystals and thin films. As the dominant SHG interaction mechanism exists only in materials that lack inversion symmetry, SHG is a sensitive probe of broken inversion symmetry, and thus also of bulk polar phenomena in materials. By performing in-situ SHG polarimetry experiments in different experimental conditions such as sample orientation, applied electric field, and temperature, one can probe ferroelectric hysteresis loops and phase transitions. Careful modeling of the polarimetry data allows for the determination of the point group symmetry of the crystal. In epitaxial thin films with a two-dimensional arrangement of well-defined domain orientations, one can extract information about intrinsic material properties such as nonlinear coefficients, as well as microstructural information such as the local statistics of the different domain variants being probed. This review presents several detailed examples of ferroelectric systems where such measurements and modeling are performed. The use of SHG microscopic imaging is discussed, and its ability to reveal domain structures and phases not normally visible with linear optics is illustrated.

Enhanced harmonic generation from Ar+ aligned with M =1

We investigate harmonic generation (HG) from ground-state Ar+ aligned with M=1 at a laser wavelength of 390 nm and intensity of 4×1014Wcm−2. Using time-dependent R-matrix theory, we find that an initial state with magnetic quantum number M=1 provides a fourfold increase in harmonic yield over M=0. HG arises primarily from channels associated with the 3Pe threshold of Ar2+, in contrast with M=0 for which channels associated with the excited, 1De threshold dominate HG. Multichannel and multielectron interferences lead to a more marked suppression of HG for M=1 than M=0.

Nonlinear optics from an ab initio approach by means of the dynamical Berry phase: Application to second- and third-harmonic generation in semiconductors

We present an ab initio real-time-based computational approach to study nonlinear optical properties in condensed matter systems that is especially suitable for crystalline solids and periodic nanostructures. The equations of motion and the coupling of the electrons with the external electric field are derived from the Berry-phase formulation of the dynamical polarization [Souza et al., Phys. Rev. B 69, 085106 (2004)]. Many-body effects are introduced by adding single-particle operators to the independent-particle Hamiltonian. We add a Hartree operator to account for crystal local effects and a scissor operator to correct the independent particle band structure for quasiparticle effects. We also discuss the possibility of accurately treating excitonic effects by adding a screened Hartree-Fock self-energy operator. The approach is validated by calculating the second-harmonic generation of SiC and AlAs bulk semiconductors: an excellent agreement is obtained with existing ab initio calculations from response theory in frequency domain [Luppi et al., Phys. Rev. B 82, 235201 (2010)]. We finally show applications to the second-harmonic generation of CdTe and the third-harmonic generation of Si. 

Second harmonic generation in h-BN and MoS2 monolayers: Role of electron-hole interaction

We study second-harmonic generation in h-BN and MoS$_2$ monolayers using a novel \emph{ab initio} approach based on Many-body theory. We show that electron-hole interaction doubles the signal intensity at the excitonic resonances with respect to the contribution from independent electronic transitions. This implies that electron-hole interaction is essential to describe second-harmonic generation in those materials. We argue that this finding is general for nonlinear optical properties in nanostructures and that the present methodology is the key to disclose these effects.