Electron trajectory control of odd and even order harmonics in high harmonic generation using an orthogonally polarised second harmonic field

We investigate quantum trajectory control in high-order harmonic generation using an additional orthogonally polarised second harmonic field. By controlling the relative phase between this field and the fundamental, we are able to suppress and enhance particular electron trajectories which results in a modulation of the harmonic emission. We observe a phase shift of the modulation between the short and long trajectories that is different for adjacent odd and even harmonics. These results show qualitative agreement with a full propagation calculation where the single atom response was obtained from the strong field approximation and the main results are explained by consideration of a single atom quantum orbit picture.     

色散介质中积累二次谐波的发生

对色散介质中平面波的积累二次谐波发生问题进行了研究。给出了形式简捷的积累二次谐波振幅和相位的解析表达式，还给出积累二次谐波发生的临界距离，据本文的分析方法，能很好地理解色散介质中积累二次谐波发生的物理过程。     

All-optical poling of a chalcohalogenide glass

Second harmonic generation has been achieved in a GeGaS chalcohalogenide glass (ChHg) after all-optical poling of the sample by coherent superposition of the fundamental and the second harmonic pulses of a Q-switched and mode-locked Nd:YAG laser. The set of parameters which optimize the effective quadratic non-linear coefficient has been identified.     

二次谐波在二维材料结构表征中的应用

二次谐波作为非线性光学的重要分支,逐渐成为表征晶体结构的重要手段之一。在众多表征方法中,二次谐波因其无损检测、高稳定性、可调谐性、超快响应、偏振敏感性、通用性、操作简单等特点被广泛应用于二维材料结构表征,为二维材料的物性研究和功能应用提供了重要信息,大大推动了二维材料基础研究的快速发展。本文综述了近几年二次谐波在二维材料结构表征中的研究,简述了二次谐波产生原理,介绍了飞秒激光器接入共聚焦拉曼光谱仪产生二次谐波测试装置,分别讨论了二次谐波在二维材料的层间堆垛层数、层间堆垛角度、单层二维材料晶界及晶体取向表征方面的应用。同时,本文还介绍了采用二次谐波强度直接、灵敏地检测晶体中应变幅度以及通过二次谐波信号变化跟踪材料中的缺陷变化,接着讨论了二次谐波与拉曼光谱、光致发光的多维度关联分析在材料全面深度表征方面的重要性。最后展望了二次谐波未来在材料结构表征中的潜在研究方向。     

Preparation of crystalline beta barium borate thin films on Sr-doped alpha barium borate substrates by liquid phase epitaxy

Thin films of beta barium borate have been prepared by liquid phase epitaxy on Sr²⁺-doped -BaB₂O₄ (-BBO, the high temperature phase of barium borate) (001) and (110) substrates. The results of X-ray diffraction indicate that the films show highly (00l) preferred orientation on (001)-oriented substrates while the films grown on (110) substrates are textured with (140) orientation. The crystallinity of these films was found to depend on growth temperature, rotation rate, dip time and orientation of substrate. Growth conditions were optimized to grow films with (00l) orientation on (001) substrates reproducibly. The films show second harmonic generation of 400 nm light upon irradiation with 800 nm Ti: Sapphire femtosecond laser light.     

Large enhancement of second harmonic generation in highly cerium doped lead-phosphate glass

The influence of lead and cerium concentration on photoinduced second harmonic generation (SHG) in lead-phosphate glasses has been studied. It has been shown that SHG can be considerably enhanced by increasing of lead and cerium concentration. We also have found that cerium greatly extends the induced nonlinearity lifetime. Physical mechanism of the phenomenon is discussed.     

An efficient method for analyzing second harmonic generation with the consideration of pump depletion

We propose a simple method to analyze second harmonic generation (SHG) in general quasi-phase-matching media with the consideration of pump depletion. It allows us to conveniently predict precise result from undepleted pump approximation solution. Based on this method, multi-wavelength generation with arbitrary target efficiency and wavelength spacing is engineered. The effect of pump depletion on the performance of constructed multi-wavelength generator is analyzed. We demonstrate that it is efficient to design nonlinear device for multi-wavelength SHG by proposed method.     

Optical Instruments and Techniques

We experimentally demonstrate that significant enhancement of third harmonic generation during filamentation in air can be achieved by terminating a filament with either a pair of uncoated glass plates or a thin plasma string created by a second laser pulse. By comparing the results obtained under these two conditions, it appears likely that the inserted plasma string plays a role as a phase plate, by which the phase mismatch induced by the Gouy phase can be partially corrected.     

Coherent diffractive imaging with table top high harmonic radiation at 13.5 nm

A highly coherent extreme ultraviolet source was obtained by phase-matched high-order harmonic generation in a semi-infinite gas cell filled with helium gas at ~550 Torr. The phase matching condition can be achieved for the generation of a few harmonic orders around 13.5 nm by variation of the gas pressure, focus position, and laser intensity. We demonstrate that the source is usable for coherent diffractive imaging and a spatial resolution of ~200 nm with short exposure times can be achieved.     

Electrical second harmonic generation and temperature autostabilized nonlinear dielectric element in ferroelectric solid solutions (Na x K1−x )VO3 and (Na x Li1−x )VO3

Second harmonic generation and temperature autostabilized nonlinear dielectric element (TANDEL) effect have been studied for ferroelectric solid solutions (Na _x K_1−x )VO₃ and (Na _x Li_1−x )VO₃ in the vicinity of the Curie temperature. The generated second harmonic is linear for low biasing d.c. fields with zero off-set. The deviations from linear behaviour and a sharp decrease in the amplitude of second harmonic is observed at higher d.c. bias voltages. The TANDEL elements, in the autostabilized state, adjust their impedance against the variation of applied a.c. voltage. The observed zero off-set might be due to the presence of defects which give internal bias and generate second harmonic.     

Remaining fatigue life prediction in the initiation regime using SAW NDE

Harmonic generation of surface acoustic waves (SAW) is shown to be a useful tool for the detection of the initiation of surface cracks during fatigue of high strength aluminum alloys. A model that relates the length and density of microcracks to the amplitude of a SAW harmonic signal is described, and an associated coefficient of generation efficiency for the second harmonic amplitude is derived. A correlation between experimentally measured harmonic amplitude and remaining fatigue life is then demonstrated, which allows the mean remaining fatigue lifetime to be estimated to within 5% over the last 50% of the fatigue life for an Al 7075 alloy if the cyclic stress amplitude, but not the duration of fatigue, is known.     

Bismuth Ferrite Second Harmonic Nanoparticles for Pulmonary Macrophage Tracking

Recently, second harmonic generation (SHG) nanomaterials have been generated that are efficiently employed in the classical (NIR) and extended (NIR‐II) near infrared windows using a multiphoton microscope. The aim was to test bismuth ferrite harmonic nanoparticles (BFO‐HNPs) for their ability to monitor pulmonary macrophages in mice. BFO‐loaded MH‐S macrophages are given intratracheally to healthy mice or BFO‐HNPs are intranasally instilled in mice with allergic airway inflammation and lung sections of up to 100 μM are prepared. Using a two‐photon‐laser scanning microscope, it is shown that bright BFO‐HNPs signals are detected from superficially localized cells as well as from deep within the lung tissue. BFO‐HNPs are identified with an excellent signal‐to‐noise ratio and virtually no background signal. The SHG from the nanocrystals can be distinguished from the endogenous collagen–derived SHG around the blood vessels and bronchial structures. BFO‐HNPs are primarily taken up by M2 alveolar macrophages in vivo. This SHG imaging approach provides novel information about the interaction of macrophages with cells and the extracellular matrix in lung disease as it is capable of visualizing and tracking NP‐loaded cells at high resolution in thick tissues with minimal background fluorescence.     

Harmonic generation in laser-produced plasmas containing atoms,ions and clusters: a review

A review of studies of the high-order harmonic generation of laser radiation in laser-produced plasma revealed recent developments in this field. These include new approaches in application of two-colour pumps, generation of extremely broadened harmonics, further developments in harmonic generation in clusters (fullerenes, carbon nanotubes), destructive interference of harmonics from different emitters, new approaches in resonance-induced enhancement of harmonics, applications of high pulse repetition rate lasers for the enhancement of average power of generating harmonics and observation of quantum path signatures, etc. We show that this method of frequency conversion of laser radiation towards the extreme ultraviolet range became mature during multiple sets of studies carried out in many laboratories worldwide and demonstrated new approaches in the generation of strong coherent short-wavelength radiation for various applications.     

Second harmonic generation from a ferroelectric film

We derive an expression for transmittivity (T_SHG) of second harmonic generation (SHG) signals from a ferroelectric (FE) film. Intensities of up and down fields in the medium are investigated in relation to T_SHG. The derivations are made based on undepletion of input fields and nonlinear wave equation derived from the Maxwell equations. We present two cases: film without mirrors and with partial mirrors. Expressions for the newly derived nonlinear susceptibility coefficients of SHG for real crystal symmetry [J. Opt. Soc. Am. B 19 (2002) 2007] are used to get more realistic results. Variations in T_SHG with respect to film thickness are illustrated.     

Flat broadband wavelength conversion based on cascaded second-harmonic generation and difference frequency generation in segmented quasi-phase matched gratings

Bandwidth enhancement and response flattening of wavelength conversion based on single-pass and double-pass cascaded second harmonic generation and difference frequency generation were investigated in segmented quasi-phase matched (QPM) gratings. It is shown that the signal and pump bandwidths are both efficiently widened by increasing the segment number of the QPM grating and optimising the poling period of each segment. The ripple on the matching response is also very small. The conversion bandwidth in a 3-cm-long three-segment waveguide reaches 150–160?nm, which is over the whole conventional band and long-wavelength band. Larger signal bandwidth can be obtained with a little response flatness penalty and conversion efficiency penalty, which can be compensated by increasing the input pump power. Compared with a sinusoidally chirped optical superlattice device, a wavelength converter based on the segmented gratings has higher conversion efficiency, broader bandwidth and better pump-wavelength tolerance, and is easier to fabricate in practice.     

Hole trapping in polydiacetylene field effect transistor studied by optical second harmonic generation

Hole trapping in polydiacetylene field effect transistor (PDA-FET) was studied by the electric field induced second harmonic generation (EFISHG). Response of SHG signal from PDA-FET with an application of external voltage was monitored. Applying positive voltage to source and drain electrodes with respect to gate electrode, SHG signal was not observed during bias application, whereas the signal was enhanced after turning off the bias. Since positive bias promotes hole injection from source and drain electrodes, electric field formed by trapped holes in PDA layer activated the SHG signal. Microscopic SHG measurement implies that the trapped holes are concentrated around source and drain electrodes.     

Laser-parameter effects on the generation of ultrabroad harmonic and ultrashort attosecond pulse in a long-plus-short scheme

By numerically solving the time-dependent Schrödinger equation for helium gas in a special two-color laser field, which is synthesized by a long (9?fs) driving pulse and a short (6?fs) controlling pulse, we discuss the influence of the carrier-envelope phase, frequency, and the intensity of the controlling pulse on the generation of harmonic spectra and isolated attosecond pluses. In the cutoff region, two or three plateaus can be controlled by optimizing these laser parameters, and an ultrabroad supercontinuum harmonic spectrum with a bandwidth of 800?eV can be produced, which can support an ultrashort isolated 4.5 as pulse generation by Fourier transformation. Furthermore, using classical ionizing and returning energy maps, time–frequency analyses are presented to explain the underlying physical mechanisms.     

Inorganic-organic hybrid nonlinear optical films containing thiophene-vinyl conjugated chromophore

A thiophene-vinyl conjugated FTC-type chromophore was synthesized and reacted with 3-isocyanatopropyltriethoxysilane to form alkoxysilane dye. The structure of alkoxysilane dye was confirmed via elemental analysis, FTIR and ¹H NMR. Stable and transparent hybrid films were fabricated following sol-gel process of alkoxysilane dye and tetraethoxysilane. The second harmonic generation coefficients (d₃₃) of the hybrid films were measured via in situ second harmonic generation measurement. The d₃₃ value of hybrid films was calculated to be 43 pm V⁻¹ when the chromophore loading density was 20 mol%. Furthermore, the thermal stability of optical nonlinearity was also investigated through a depoling experiment, showing a half decay temperature of 165 °C.     

Generation of an extreme ultraviolet supercontinuum in a two-color spatially inhomogeneous field

We theoretically investigate the high-order harmonic generation from the helium ion in a two-color spatially inhomogeneous laser field. The numerical calculations show that this spatiotemporally synthesized laser field can not only significantly extend the harmonic cut-off, but also generate an ultrabroad extreme ultraviolet supercontinuum with a 1737 eV bandwidth. In addition, the spatiotemporal combination can eliminate the long quantum path and select the short one, and then an ultrashort isolated 12.3 as pulse with a bandwidth of 310.2 eV is obtained directly. Further, the dependences of the harmonic spectrum on the parameters including spatial inhomogeneity, time delay, carrier-envelope phase, and intensity are further discussed.