Measurements of dynamics of nondegenerate optical nonlinearity in ZnS with pulses from optical parameter generation

We expand the degenerate PO pump-probe technique to nondegenerate field and use it to investigate optical nonlinear dynamics in ZnS single crystal. Excited by 532-nm laser pulses with 21-ps duration, the temporal response of nondegenerate nonlinear absorption and nondegenerate nonlinear refraction are probed by laser pulses from optical parameter generation (OPG) at 600 and 680 nm with pulse width of 10 ps. Based on the theory of free-carrier optical nonlinearity, we study the pure free-carrier refraction in ZnS. By numerically fitting based on the nondegenerate pump-probe theory, the nondegenerate two-photon absorption coefficient, the free-carrier lifetime, the free-carrier absorptive cross section and refractive coefficient at both probe wavelengths are determined respectively. The dispersion of the free-carrier refractive coefficients is discussed.     

Experimental study on terahertz radiation

In this letter, we describe a coherent subpicosecond terahertz (THz) spectroscopy system based on nonresonant optical rectification for the generation of THz radiation. We studied the two-photon absorption (TPA) of ZnTe induced by femtosecond laser pulses via THz generation, and its influence on the generation of THz radiation. Experimental results demonstrated that the intensity of pump beam against TPA must be traded off to get an optimum generation of THz radiation. As an example, we measured absorption spectrum of water vapor by time-domain spectroscopy (TDS) in the frequency range from 0.5 to 2.5 THzwith a high overall accuracy.     

硒化镉载流子的超快动力学研究

硒化镉是一种可用于X射线全光分幅相机和全光条纹相机的重要探测材料。用基于相位物体的泵浦探测方式,研究了硒化镉在1030nm波长,飞秒脉冲下的载流子超快动力学和非线性光学特性。得到了双光子吸收系数、载流子吸收截面、载流子复合时间等参数。实验表明,硒化镉载流子的动力学和非线性特性是由束缚电子和载流子共同决定的。束缚电子的克尔效应和双光子激发都是瞬态的,而载流子复合持续了较长时间。这些参数和载流子图像的的获得,为X射线超快探测器件的设计和改进提供了参考。     

Interband impact ionization and nonlinear absorption of terahertz radiation in semiconductor heterostructures

We have theoretically investigated nonlinear free-carrier absorption of terahertz (THz) radiation in InAs/AlSb heterojunctions. By considering multiple photon process and conduction-valence interband impact ionization (II), we have determined the field and frequency dependent absorption rate. It is shown that (i). electron-disorder scatterings are important at low to intermediate field, and (ii). most importantly, the high field absorption is dominated by II processes. Our theory can satisfactorily explain a long-standing experimental result on the nonlinear absorption in the THz regime.     

GaSe晶体的双光子吸收对太赫兹输出的影响

根据光整流效应,利用超快激光脉冲泵浦GaSe晶体实现了0.2~2.5 THz的宽带太赫兹辐射输出。禁带中的电子在两个800 nm光子的作用下激发到导带中形成自由载流子,进而吸收所产生的太赫兹辐射,最终导致太赫兹的输出随泵浦功率的增加而趋于饱和。为了研究双光子吸收对太赫兹输出的影响,测量了800 nm处的GaSe晶体的双光子吸收系数,结果为 0.165 cm/GW。通过对太赫兹输出实验数据的拟合,得到GaSe晶体中自由载流子对太赫兹输出的吸收截面为1×10^-15 cm²。本文的研究结果可用于优化GaSe晶体在强激光泵浦下的太赫兹转换效率。     

Free-carrier absorption in quantum well structures for acoustic phonon scattering

Free-carrier absorption has been studied for quantum well structures fabricated from III-V semiconducting materials where the acoustic phonon scattering is important. The energy band of carriers is assumed to be nonparabolic. We discuss the effect of acoustic phonon scattering on the free-carrier absorption for both deformation-potential coupling and piezoelectric coupling. It is found that the free-carrier absorption coefficient depends upon the polarization of the electromagnetic radiation relative to the layer plane or quantum well, the photon frequency, and the temperature. When the deformation-potential coupling is dominant, the free-carrier absorption coefficient increases with increasing temperature for photons polarized in the layer plane or perpendicular to the layer plane. However, when the piezoelectric coupling is dominant, the free-carrier absorption coefficient increases with increasing temperature for photons polarized in the layer plane, but for photons polarized perpendicularly to the layer plane, the free-carrier absorption coefficient decreases with increasing temperature. Moreover, at high temperatures such as T = 300 K, the free-carrier absorption coefficient oscillates with the film thickness in a small quantum well region and then decreases monotonically with increasing the film thickness. This is different from the result for three-dimensional semiconducting solids.     

Surface-emitted THz generation using a compact ultrashort pulse fiber amplifier at 1060 nm

Generation of InAs-surface-emitted terahertz radiation by application of an ultrashort pulse 1060 nm parabolic fiber amplifier source is reported for the first time. The fiber amplifier delivers 100 fs pulses at a repetition rate of 75 MHz and an average power of maximum 12 W. This new excitation laser for surface-emitters generates high brightness broadband THz radiation ranging from 100 GHz to over 2.5 THz. THz detection is demonstrated based on two-photon absorption at low-temperature-grown GaAs dipole receivers.     

Optical nonlinearities and photo-excited carrier lifetime in CdS at 532 nm

Bound-electronic and free-carrier optical nonlinearities, and relaxation of photo-excited free carriers in CdS have been investigated by the use of a single-beam Z-scan technique at 532 nm. Under pulsed radiation of 35-ps duration with the input irradiances up to 4.8 GW/cm², the two-photon absorption coefficient, the bound-electron nonlinear refractive index, the free-carrier absorption cross-section, and the change in the refractive index per unit carrier density are determined to be 5.4±0.8 cm/GW, −(5.3±0.8)×10⁻¹³ cm²/W, (3.0±0.5)×10⁻¹⁷ cm² and −(0.8±0.1)×10⁻²¹ cm³, respectively. By using these values in the open-aperture Z-scans conducted with 7-ns laser pulses, the carrier recombination time is extracted to be 3.6±0.7 ns. The measured parameters are compared to theoretical calculations.     

Multiphoton generation of electron-hole pairs involving free carriers in an indirect-gap crystal

The paper reports on a study of nonlinear absorption of high-intensity laser radiation in the case where the photon energy is less than one half of the indirect-gap width in a crystal. The deficiency in the energy needed for two-photon excitation of the electron-hole pair is made up by the kinetic energy of free electrons, which was acquired in intraband nonlinear absorption of light. The probabilities of Auger-type indirect two-photon interband transitions involving free electrons have been calculated by perturbation theory. It is shown that, for a free-carrier concentration in the conduction band n _c ? 10¹⁵ cm^?3, and the radiation intensity range of interest for the experiment, j ～ 3–10 GW/cm², the calculated probabilities of such transitions exceed by several orders of magnitude those of “conventional” direct and indirect (involving phonons) multiphoton transitions which can take place in the system considered.     

Effects of gain saturation on terahertz radiation via optical difference frequency generation

Numerical studies on stability of terahertz (THz) radiation generation based on difference frequency generation in nonlinear crystals are reported. When the gain saturation is achieved at a wavelength that corresponds to an optimal crystal length, the maximal output of THz radiation could be obtained. As a result of crystal absorption, the gain saturation region of THz radiation is unstable region for output. The stability of THz radiation is determined by the stability of pump in the stable region where behind of the gain saturation.     

Fe2O3纳米微粒溶胶非线性光学特性的Z-扫描研究

利用Z扫描技术在透明区域研究了Fe₂O₃纳米微粒水溶胶和表面包覆有机溶胶的非线性光学特性，给出了非线性折射率γ、双光子吸收系数β、自由载流子折射系数σ_r和自由载流子吸收截面σ_ab等重要物理参数，讨论了自由载流子效应对Fe₂O₃纳米微粒非线性特性的影响 关键词：     

The effect of two-photon absorption and optical excitation area on the generation of THz radiation

It was found experimentally that the THz radiation throughput based on optical rectification is strongly related to the optical excitation size in a ZeTe emitter. The factors affecting the THz radiation throughput are investigated in detail both experimentally and theoretically. By taking into account optical rectification, diffraction and two-photon absorption effects, a theoretical model is established to describe the emitting field intensity of THz radiation. There is excellent agreement between the theoretical results and the experimental data under high excitation power. Both theoretical and experimental results demonstrate that there is a trade-off between these three effects for THz radiation, and that in order to increase the THz radiation throughput based on optical rectification, one should choose suitable excitation size under a given pump power.     

GaAs在光通讯波段的超快非线性光学研究

采用Z-扫描和泵浦-探测技术,在光通讯波段对砷化镓(GaAs)单晶进行了非线性动力学以及非线性光学的实验研究.飞秒泵浦-探测实验结果表明,三阶非线性光学效应源于砷化镓单晶对飞秒激光的瞬态双光子吸收,而五阶非线性光学效应源于砷化镓单晶双光子吸收诱导的自由载流子吸收效应.通过Z扫描实验,得到了关于GaAs单晶所有的非线性光学参数,包括双光子吸收系数、三阶非线性折射系数、双光子吸收诱导的自由载流子吸收截面以及双光子吸收诱导的自由载流子折射截面.结果表明,砷化镓单晶在制造光限幅器件和光电探测器方面具有良好的发展前景.     

Orbital mechanism of the circular photogalvanic effect in quantum wells

It is shown that the free-carrier (Drude) absorption of circularly polarized radiation in quantum well structures leads to an electric current flow. The photocurrent reverses its direction upon switching the light helicity. A pure orbital mechanism of such a circular photogalvanic effect is proposed that is based on the interference of different pathways contributing to light absorption. Calculation shows that the magnitude of the helicity-dependent photocurrent in n-doped quantum well structures corresponds to recent experimental observations. The text was submitted by the author in English.     

Measurement of two-photon absorption using the photo-thermal lens effect

We report on new schemes for pump-probe photo-thermal lens methods aimed for measuring the two-photon absorption coefficient of a given material. We show that by focusing a probe beam in the presence of a nearly collimated pump beam, we create a thermal lens which yields measurement of the two-photon absorption coefficient of nitrobenzene of (3.9 ± 0.3) 10⁻¹⁰ cm/W at 532 nm. We also show that when the pump field is focused in the presence of a nearly collimated probe beam the width of the z-scan signature of a two-photon absorption process is nearly one order of magnitude smaller than that of a one-photon process. We show experimental evidence of the effect obtained for nitrobenzene.     

双光子激发ZnSe自由载流子超快动力学研究

采用Z扫描和抽运-探测实验技术, 在波长为532 nm、脉冲宽度为41 fs的条件下测得ZnSe晶体的双光子吸收系数, 并获得了不同激发光强下的自由载流子吸收截面、电子-空穴带间复合时间和电子-声子耦合时间. 研究发现, 随着激发光强的增大, 自由载流子吸收截面减小, 复合时间变短. 当激发光强增大导致载流子浓度大于10¹⁸ cm^-3时, 抽运-探测信号出现明显改变, 原因归结为强光场激发导致样品在短时间内带隙变窄和电子-空穴等离子体的形成.     

Two-photon absorption-induced self-phase modulation in GaAs-AlGaAs waveguides for surface-emitted second-harmonic generation

Performance-limiting asymmetric distortion is observed in the spectra of fundamental pulses transmitted through GaAs-Al(0.9)Ga(0.1)As multilayer waveguides designed for surface-emitted second-harmonic generation. This behavior is attributed to refractive-index changes resulting from the accumulation of free carriers created by two-photon absorption in the GaAs layers. Numerical simulations of the intensity-dependent spectra by use of the separately measured two-photon absorption coefficient are shown to be in good agreement with the observed spectra.     

Impact of two-photon absorption on self-phase modulation in silicon waveguides

We study the effects of two-photon absorption on the self-phase modulation (SPM) process in silicon waveguides while including both free-carrier absorption and free-carrier dispersion. An analytical solution is provided in the case in which the density of generated carriers is relatively low; it is useful for estimating spectral bandwidth of pulses at low repetition rates. The free-carrier effects are studied numerically with emphasis on their role on the nonlinear phase shift and spectral broadening. We also consider how the repetition rate of a pulse train affects the SPM process.     

Specific features of the two-photon absorption of cationic symmetric polymethine dyes

The two-photon absorption of a number of cationic symmetric polymethine dyes based on 3H-indolium and benzothiazolium is experimentally studied upon excitation by nanosecond radiation from a Nd:YAG laser (1064 nm, 12 ns). The two-photon absorption cross section of dye molecules is determined by the two-quantum standard method. The influence of the spectral-luminescent properties and structure of the polymethine dyes on the two-photon absorption cross section is discussed. It is shown that, upon excitation in the range of the long-wavelength band of the dyes studied (the S ₀ → S ₁ transition), the maximum of their two-photon absorption is blue shifted. The reasons for a considerable increase in the two-photon absorption of symmetric polymethine dyes upon their excitation in the range of the S ₂ state are discussed. Using the data of quantum-chemical calculations, it is shown that, along with changes in the selection rules for two-photon transitions, this increase is connected with an increase in the size of the delocalized π electron cloud of HOMOs involved in the S ₀ → S ₂ transition.     

UWB monocycle pulse generation using two-photon absorption in a silicon waveguide

We propose and experimentally demonstrate ultrawideband monocycle pulse generation using nondegenerate two-photon absorption in a silicon waveguide. The free-carrier absorption induced pulse tail at the rising edge of inverted probe pulse is largely compensated by the overlapped pump pulse and results in a symmetric negative monocycle pulse. A 143 ps Gaussian monocycle pulse is successfully obtained with a 131.7% fractional 10 dB bandwidth using a 68 ps pulsed pump. The 10 dB bandwidth and center frequency of the RF spectrum for the generated monocycle pulse can be largely tuned using an optical delay line. An operational bandwidth of 30 nm is demonstrated experimentally with stable performance, and larger optical bandwidth is expected.