Controlling the second harmonic in a phase-matched negative-index metamaterial.

Nonlinear metamaterials have been predicted to support new and exciting domains in the manipulation of light, including novel phase-matching schemes for wave mixing. Most notable is the so-called nonlinear-optical mirror, in which a nonlinear negative-index medium emits the generated frequency towards the source of the pump. In this Letter, we experimentally demonstrate the nonlinear-optical mirror effect in a bulk negative-index nonlinear metamaterial, along with two other novel phase-matching configurations, utilizing periodic poling to switch between the three phase-matching domains.

Coherent Control of High Harmonic Generation via Dual-Gas Multijet Arrays

High harmonic generation (HHG) is a central driver of the rapidly growing field of ultrafast science. We present a novel quasiphase-matching (QPM) concept with a dual-gas multijet target leading, for the first time, to remarkable phase control between multiple HHG sources (> 2) within the Rayleigh range. The alternating jet structure with driving and matching zones shows perfect coherent buildup for up to six QPM periods. Although not in the focus of the proof-of-principle studies presented here, we achieved competitive conversion efficiencies already in this early stage of development.

Two-dimensional infrared spectroscopy of peptides by phase-controlled femtosecond vibrational photon echoes

Two-dimensional infrared spectra of peptides are introduced that are the direct analogues of two- and three-pulse multiple quantum NMR. Phase matching and heterodyning are used to isolate the phase and amplitudes of the electric fields of vibrational photon echoes as a function of multiple pulse delays. Structural information is made available on the time scale of a few picoseconds. Line narrowed spectra of acyl-proline-NH2 and cross peaks implying the coupling between its amide-I modes are obtained, as are the phases of the various contributions to the signals. Solvent-sensitive structural differences are seen for the dipeptide. The methods show great promise to measure structure changes in biology on a wide range of time scales.

Excitation of surface plasmon-polariton waves at a semiconductor-metal interface

The excitation of surface plasmon-polariton waves propagating across an external magnetic field (Voigt geometry) in a semiconductor-metal structure by means of the attenuated total reflection method is investigated. The phase matching conditions for the surface waves excitation in the Kretchmann configuration are derived and analyzed. The effect of different nonlinearities on the excitation of the surface waves is studied as well.

Ultrafast Raman loss spectroscopy

This paper deals with a new form of nonlinear Raman spectroscopy called `ultrafast Raman loss spectroscopy (URLS)'. URLS is analogous to stimulated Raman spectroscopy (SRS) but is much more sensitive than SRS. The signals are background (noise) free unlike in coherent anti-Stokes Raman spectroscopy (CARS) and it provides natural fluorescence rejection, which is a major problem in Raman spectroscopy. In addition, being a self-phase matching process, the URLS experiment is much easier than CARS, which requires specific phase matching of the laser pulses. URLS is expected to be alternative if not competitive to CARS microscopy, which has become a popular technique in applications to materials, biology and medicine.

Normal-mode sound propagation in an ocean with sinusoidal surface waves

The normal-mode solution to the problem of acoustic wave propagation in an isovelocity ocean with a wavy surface is considered. The surface wave amplitude is assumed to be small compared to the acoustic wavelength, and the method of multiple scales is employed to study the interaction between normal-mode acoustic waves and the surface waves. A nonresonant interaction causes small fluctuations of the amplitude and phase of the acoustic wave at a rate dependent on the frequency of the surface wave. Backscatter occurs if the wavenumber of the surface wave is larger than that of the acoustic wave. The interaction becomes resonant if appropriate phase-matching conditions are satisfied. In this case, two acoustic normal modes get coupled, resulting in a large-scale periodic exchange of energy from one mode to another.

Lithium D-Isoascorbate Monohydrate, a New Nonlinear Optical Material

Single crystals of lithium D-isoascorbate monohydrate (LDAM), (C6H7O6Li center dot H2O), are grown by a solution growth method. The crystal structure of LDAM is solved using single crystal X-ray diffraction. The space group is orthorhombic P2(1)2(1)2(1) with four formula units per unit cell and lattice parameters a = 7.7836(3) angstrom, b = 8.7456(3) angstrom, and c = 11.0368(4) angstrom. Solubility of the material in water is determined thermogravimetrically and found to have a positive temperature coefficient of solubility. Large optical quality single crystals are subsequently grown from aqueous solution by a slow cooling method. The crystal has a bulky prismatic habit and among the prominent faces the c face appears as the only principal morphological face. The crystal exhibits a (010) cleavage. Dielectric spectroscopy reveals a nearly Debye type Cole-Cole behavior with anisotropy in relaxation. Optical transmission range is found to be from 300 to 1400 nm. The principal refractive indices of this biaxial crystal, measured using Brewster's angle method, at wavelengths 405, 543, and 632.8 nm, show high dispersion. The crystal is negative biaxial with 2V(z) = 107.8 degrees (405 nm) and belongs to the Hobden class 3. Theoretically generated type 1 and type 2 second order phase matching curves match very well with the experimental results. The second-order nonlinear coefficient d(14) was determined to be 7 x 10(-13) m/V. For the optimum phase matching direction (type 2), the second-order effective nonlinear coefficient and the walk off angle are determined to be 0.84 times d(14) and 3.5 degrees respectively. The crystal possesses high multiple surface damage thresholds of 18 GW/cm(2) and 8 GW/cm(2) at laser wavelengths 1064 and 532 nm, respectively.

Studies on lithium L-ascorbate dihydrate: An interesting chiral nonlinear optical crystal

Lithium L-Ascorbate dihydrate (LLA) is a new metal organic nonlinear optical crystal belonging to the saccharide family. Single crystals of LLA were grown from aqueous solution. Solubility of the crystal has a positive temperature coefficient facilitating growth by slow cooling. Rietveld refinement was used to confirm the phase formation. The crystal has prismatic habit with (010), (001) and (10-1) prominent faces. Thermal analysis shows that the crystal is stable up to 102 degrees C. Transmission spectrum of the crystal extends from 302 nm to 1600 nm. Dielectric spectroscopic analysis revealed Cole Cole behaviour and prominent piezoelectric resonance peaks were observed in the range of 100-200 kHz. Second harmonic generation (SHG) conversion efficiency of up to 2.56 times that of a phase matched KDP crystal was achieved when the (010) plate of LLA single crystal was rotated about the +ve c axis, by 9.4 degrees in the clockwise direction. We also observed SHG conical sections which were attributed to noncollinear phase matching. The observation of the third conical section suggests very high birefringence and large nonlinear coefficients. A detailed study of surface laser damage showed that the crystal has high multiple damage thresholds of 9.7 GW cm(-2) and 42 GW cm(-2) at 1064 nm and 532 nm radiation respectively. (C) 2012 Elsevier B.V. All rights reserved.

Crystal growth and nonlinear optical properties of sodium D-isoascorbate monohydrate

Optical quality single crystals of sodium D-isoascorbate monohydrate were grown by a slow cooling technique. The crystal possesses a bulky prismatic morphology. Thermal analyses indicate that the crystals are stable up to 125 degrees C. The optical transmission window ranges from 307 nm to 1450 nm. The principal refractive indices have been measured employing Brewster's angle method. The crystallographic and the principal dielectric axes coincide with each other such that a lies along Z, b along X and c along Y. The optic axis is oriented 58 degrees (at 532 nm) to the crystallographic a axis in the XZ plane and the crystal is negative biaxial. Type 1 and type 2 phase matching curves are generated and experimentally verified. No polarization dependence of the light absorption was observed confirming the validity of Kleinman's symmetry conjecture, leading to a single nonvanishing nonlinear tensor component. According to Hobden's classification the crystal belongs to class 3. The crystal also exhibits second order noncollinear conic sections. The single shot and multiple shot surface laser damage thresholds are determined to be 32.7 GW cm(-2) and 6.5 GW cm(-2) respectively for 1064 nm radiation.

Fine interference fringes formed in high-order harmonic spectra generated by infrared driving laser pulses

We experimentally investigate the high-order harmonic generation in argon gas using a driving laser pulse at a center wavelength of 1240 nm. High-contrast fine interference fringes could be observed in the harmonic spectra near the propagation axis, which is attributed to the interference between long and short quantum paths. We also systematically examine the variation of the interference fringe pattern with increasing energy of the driving pulse and with different phase-matching conditions.

Spectral evolution of angularly resolved third-order harmonic generation by infrared femtosecond laser-pulse filamentation in air

We experimentally investigate the evolution of an angularly resolved spectrum of third harmonic generated by infrared femtosecond laser pulse filamentation in air. We show that at low pump intensity, phase matching between the fundamental and third-harmonic waves dominates the nonlinear optical effect and induces a ring structure of the third-harmonic beam, whereas at high pump intensity, the dispersion properties of air begin to affect the angular spectrum, leading to the formation of a nonlinear X wave at third harmonic.

Optimization of optical parametric chirped pulse amplification with different pump wavelengths

Optical parametric chirped pulse amplification with different pump wavelengths was investigated using LBO crystal, at signal central wavelength of 800 nm. According to our theoretical simulation, when pump wavelength is 492.5 nm, there is a maximal gain bandwidth of 190 nm. centered at 805 nm in optimal noncollinear angle using LBO. Presently, pump wavelength of 492.5 nm can be obtained from second harmonic generation of a Yb:Sr-5(PO4)(3)F laser. The broad gain bandwidth can completely support similar to 6 fs with a spectral centre of seed pulse at 800 nm. The deviation from optimal noncollinear angle can be compensated by accurately tuning crystal angle for phase matching. The gain spectrum with pump wavelength of 492.5 nm is much better than those with pump wavelengths of 400, 526.5 and 532 nm, at signal centre of 800 nm. (c) 2005 Elsevier B.V. All rights reserved.

消色差相位匹配在光参量啁啾脉冲放大中的应用

Optical parametric chirped-pulse amplification (OPCPA) supplies broadband gain for ultrashort pulses. A new theoretic explanation of OPCPA has been obtained by introducing the concept of tilted pulse front in this paper, and the distribution of broadband amplification has been twice expanded by introducing the technology of achromatic phase matching (APM). The prospect of APM in OPCPA has been discussed in detail. Finally, a design for the amplification of chirped pulses at 1600 nm has been firstly proposed and numerically simulated. (C) 2004 Elsevier B.V. All rights reserved.

Interaction of oblique incident electromagnetic wave with relativistic ionization front

Interactions of oblique incident probe wave with oncoming ionization fronts have been investigated using moving boundary conditions. Field conversion coefficients of reflection, transmission and magnetic modes produced in the interactions are derived. Phase matching conditions at the front and frequency up-shifting formulas for the three modes are also presented.

参变过程中的群速延迟对晶体匹配长度的影响

基于能量守恒和三波耦合波方程, 建立了超短脉冲在参变过程中二次谐波产生时的I类和II类相位匹配条件、基波与谐波之间的群速延迟时间、以及群速失配对晶体长度限制的理论基础。以负单轴非线性光学晶体CsLiB6O10为例, 分析和数值计算了超短脉冲宽度为100 fs时, 谐波的群速匹配长度随基波波长变化的规律。研究结果表明在I类相位匹配条件下, 基波波长为642 nm时, 群速延迟最小, 相应的群速匹配晶体长度最长为19.1 mm;在II类相位匹配条件下, 基波波长为767 nm, 群速延迟最小, 群速匹配长度最