Enhanced second-harmonic generation for multiple wavelengths by defect modes in one-dimensional photonic crystals

We present an effective design of aperiodically stacked layers of nonlinear material and air, sandwiched by two truncated photonic crystals, in terms of the simulation annealing method. The constructed structure can achieve multiple-wavelength second-harmonic generation (SHG) at the preassigned wavelengths. We derive a general solution of SHG in 1D inhomogeneous systems and apply it to evaluate the SHG conversion efficiency. Numerical simulations show that the conversion efficiency of SHG can be significantly enhanced when the fundamental wave frequencies are assigned to the designed defect states.     

Many-photon effects in inelastic light scattering

The usual approach to second harmonic generation (SHG) is based on low-order pertubation theory and neglects the changes in the electronic states that are induced by the exciting beam. To see whathappens in this approximation fails we propose a new formalism, based on the method of excitation amplitudes, to set up a theory of the SHG response and other inelastic light scattering phenomena. We develop the quantum theory in the dipole approximation and show that the inclusion of electron-photon coupling to all others leads to new features. Strong exciting fields produce a nonnegligible SHG response in highly polarisable centro-symmetric systems, and the emitted spectrum shows a dynamical Stark effect.     

Coherent control of the optical nonlinear and luminescence anisotropies in molecular thin films by multiphoton excitations

Photoinduced orientational distributions are implemented with one- and two-photon absorption interference in polymer films containing chromophores that exhibit luminescent and nonlinear properties. The odd- and even-order parameters of the final distribution are probed by simultaneous measurement of second-harmonic generation (SHG) and two-photon fluorescence (TPF). We show the possibility of engineering local SHG and TPF anisotropies by controlling the polarization states and intensities of the writing optical fields. Complex multipolar orders are modeled with an irreducible spherical tensor-based formalism jointly applied to the molecular polarizabilities and field tensors.     

Nonlinear optical spectroscopy of suboxides at oxidized Si(111) interfaces

Native oxidation of the Si(111)(1 x 1)H surface causes the appearance and disappearance of second-harmonic generation (SHG) resonances related to specific bonding configurations of Si atoms at the interface. Resonances at 3.52 eV two-photon energy observed in p-polarized SHG spectra are indicative of a Si suboxide configuration present in a partially oxidized Si surface bilayer. Similar resonances are observed in spectra of thermally oxidized Si(111) and point to Si2+ suboxide states at the buried interface.     

Computing for second harmonic generation in one-dimensional nonlinear photonic crystals

A numerical study of second harmonic generation (SHG) in one-dimensional nonlinear photonic crystals based on full nonlinear system of equations, implemented by a combination of the method of finite elements and fixed-point iterations, is reported. This model is derived from a nonlinear system of Maxwell’s equations, which partly overcomes the known shortcoming of some existing models relied on the undepleted-pump approximation. We derive a general solution of SHG in one-dimensional nonlinear photonic crystals structures. The convergence of our method is fast. Numerical simulations also show the conversion efficiency of SHG can be significantly enhanced when the frequencies of the fundamental wave are located at the photonic band edges or are assigned to the designed defect states.     

Second-harmonic spectroscopy of electronic structure of Si/SiO2 multiple quantum wells

Size effects in the resonant nonlinear optical response of amorphous Si/SiO₂ multiple quantum wells (MQW) are studied by second-harmonic generation (SHG) spectroscopy in a spectral interval of second-harmonic photon energies from 2.5 to 3.4 eV. The sensitivity of SHG spectroscopy to thickness-dependent electronic structure (sub-band energy position and density of states line shape) of MQW is demonstrated. A monotonic red shift of central energies of SHG resonances by 120 m eV upon increase of the well thickness from 2.5 to 10 ? is observed. This is interpreted as a size dependence of the position of singularities in the combined density of states for a 2D gas of electrons moving in an effective potential well. It is shown that, for agreement with experiment, the simplest (rectangular) shape of the well should be modified in order to take into account the lattice-potential distortion at the interfaces. Received: 16 October 2001 / Revised version: 16 April 2002 / Published online: 6 June 2002     

Spin and orbital quantization of electronic states as origins of second harmonic generation in semiconductors

Basically different mechanisms of optical second harmonic generation (SHG) in semiconductors, induced by an external magnetic field H, have been identified experimentally by studying the diluted magnetic semiconductor (Cd,Mn)Te. For paramagnetic (Cd,Mn)Te the SHG response is governed by spin quantization of electronic states, in contrast with diamagnetic CdTe with its dominating orbital quantization. The mechanisms can be identified by the distinct magnetic field dependence of the SHG intensity which scales with the spin splitting in the paramagnetic case as compared to the H2 dependence observed for the diamagnetic case.     

Intense laser-induced electronic and optical properties in double finite oscillator potential

In the present paper, a theoretically study of the non-resonant laser field effect on the optical response, such as nonlinear optical rectification (NOR), second (SHG) and third harmonic generation (THG) coefficients in double finite oscillator potential (DFO) quantum wells is performed in the framework of the effective mass approximation. The obtained results reveal that, energy states and optical response is significantly affected by the non-resonant intense laser field (ILF) intensity and symmetry of the structure. Also it was found that the laser field is more effective on the optical response in the DFO potential when the asymmetric character of the confinement potential is strong. Thus, the NOR, SHG and THG coefficients with designated values can be obtained by using a properly adjusted ILF intensity and symmetry parameter of confinement potential.     

Changes of phase and intensity of optical SHG with Ag deposition on Si(111)-7×7 surfaces

The phase and intensity of optical second harmonic generation (SHG) were studied in Ag deposition on the Si(1 1 1) surfaces. The 7×7 reconstruction of the surface changed to the 1×1 structure in room temperature deposition. The SHG intensity reduced and the phase shifted to +180° with this structural change. Meanwhile, the 7×7 reconstruction changed to the reconstruction in 400 °C deposition. With this structural change, the SHG intensity increased and the phase shifted to −250°. An analysis with anharmonic oscillator model showed that the changes in room temperature deposition were due to the quenching of the surface dangling bond states of the 7×7 reconstruction by the Ag deposition, whereas those in 400 °C deposition were due to the appearance of new surface states of the reconstruction.     

Thin noble metal films on Si (111) investigated by optical second-harmonic generation and photoemission

Thin noble metal films (Ag, Au and Cu) on Si (111) have been investigated by optical second-harmonic generation (SHG) in combination with synchrotron radiation photoemission spectroscopy. The valence band spectra of Ag films show a quantization of the sp-band in the 4-eV energy range from the Fermi level down to the onset of the d-bands. For Cu and Au the corresponding energy range is much narrower and quantization effects are less visible. Quantization effects in SHG are observed as oscillations in the signal as a function of film thickness. The oscillations are strongest for Ag and less pronounced for Cu, in agreement with valence band photoemission spectra. In the case of Au, a reacted layer floating on top of the Au film masks the observation of quantum well levels by photoemission. However, SHG shows a well-developed quantization of levels in the Au film below the reacted layer. For Ag films, the relation between film thickness and photon energy of the SHG resonances indicates different types of resonances, some of which involve both quantum well and substrate states. Received: 16 October 2001 / Revised version: 14 March 2002 / Published online: 29 May 2002     

Amplitude ambiguities in second-harmonic generation frequency-resolved optical gating

We construct field shapes with distinct amplitude profiles that have nearly identical second-harmonic generation frequency-resolved optical gating (SHG FROG) traces. Although such fields are not true mathematical ambiguities, they result in experimentally indistinguishable FROG traces. These fields are neither time-reversed copies nor pulselets with a mere relative phase difference, which are well known nontrivial ambiguities for SHG FROG. We also show that for certain example fields, second-order interferometric autocorrelation is more sensitive to the pulse shape than is SHG FROG.     

Maximum-exponent scaling behavior of optical second-harmonic generation in finite multilayer photonic crystals

Scaling laws of second-harmonic generation (SHG) in nonlinear Bragg stacks (or finite one-dimensional photonic crystals) as a function of the number N of periods are explored. While it is known that SHG scales like the sixth power of N when phase matching is achieved, we find maximal scaling like the eighth power of N under appropriate non-phase-matching conditions with the pump and harmonic waves being resonant with band-edge states. In this framework we introduce the concept of self-adaptive coherence length that scales with the system length. An analytical treatment based on coupled-mode equations clarifies the conditions for obtaining different scaling laws as a function of filling factor in the photonic gap map.     

半导体材料AAl2C4(A=Zn, Cd, Hg; C=S, Se)的电子结构和光学性质

采用基于密度泛函理论的第一性原理方法, 对具有缺陷型黄铜矿结构的半导体材料A^ⅡAl₂C₄^Ⅵ(A=Zn, Cd, Hg; C =S, Se)的构型和电子结构进行研究, 并系统考察了各晶体的光学性质. 对于线性光学性质, 五种晶体在红外区和部分可见光区具有良好的透光性能, 其中HgAl₂S₄和HgAl₂Se₄晶体具有适中的双折射率. 在非线性光学性质方面, 该类晶体倍频效应较强, 理论预测得到的二阶静态倍频系数均较大(>20 pm/V). 体系的倍频效应主要来源于价带顶附近以S/Se 价p轨道为主要成分的能带向含有较多Al/Hg 价p成分的空带之间的跃迁. 通过与已商业化的AgGaC₂晶体光学性质的对比, 结果表明HgAl₂S₄和HgAl₂Se₄是一类性能优良的红外非线性光学晶体材料.     

A sensitive detection method for magnetization-induced second-harmonic generation under an externally applied field

We describe the instrumentation related to the first observation of magnetization-induced enhancement of surface second-harmonic generation (SHG) from the paramagnetic Si(111)-7×7 surfaces. A judicious choice of polarization and sample orientation enabled us to isolate the magnetic-field-dependent tensor element of the nonlinear susceptibility. A conductive liquid-nitrogen system, coupled to an ultrahigh-vacuum system that is immune to the high magnetic field of 10 T, cooled the sample to about 120 K. A high extinction that is necessary to detect the magnetization-induced SHG (MSHG) was accomplished by minimizing stray optical effects such as Faraday rotation, photoluminescence and thermal birefringence in all optical components, with extra care taken for the UHV window. Consistent and stable operation of this sensitive measurement system permitted experiments involving MSHG at multiple wavelengths and temperatures. Probing the magnetization-induced optical nonlinearity was validated by quenching the surface states by oxidation of the surface layers. From MSHG measurements at two wavelengths resonant with different surface-state transitions, we were able to suggest that the observed MSHG is proportional to the number of dangling bond states of Si(111)-7×7. Received: 15 January 2002 / Published online: 2 May 2002     

Quadripartite entangled state from cascaded second-harmonic generation

A generation system of continuous-variable （CV） quadripartite entangled state based on two cascaded second- harmonic generation （SHG） cavities below the threshold is investigated. Two reflected fundamental bearias of the first cavity, the reflected second-harmonic beam and the output fourth-harmonic beam of the second cavity are proved to be entangled, and the dependence of the entanglement degree on the normalized frequency, pump parameter, fourth-harmonic loss parameter, and second-harmonic loss parameter is also analyzed. Due to the fact that the cavity parameters and the nonlinear crystals of the two SHG cavities can be freely chosen, the practicality of the proposed protocol is relatively perfect and the system can also be extended to the preparation of multicolor entangled states for a quantum network.     

高效外腔倍频产生426 nm激光的实验研究

利用与铯原子吸收线对应的852 nm半导体激光作为基频光,泵浦基于周期极化磷酸钛氧钾(PPKTP)晶体的环形腔,进行高效外腔谐振倍频并产生426 nm激光.在理论分析小角度环形腔内的热透镜效应基础上,发现晶体中等效热透镜中心位置并非在晶体的几何中心.在理论分析的基础上,实验上通过精密平移台精细调节PPKTP晶体在腔内位置,使得等效热透镜中心位置与谐振腔的腰斑位置重合,进而减小晶体热透镜效应导致的模式失配对倍频效率的影响.在泵浦功率为515 mW时产生了428 mW的426 nm激光输出,对应的倍频转换效率为83.1%.此高效倍频过程为制备与铯原子吸收线相匹配的非经典光场提供有效泵浦光,为推动量子非经典光场的应用以及量子信息科学的发展奠定基础.     

用非共线二次谐波法实现对锁模激光器超短脉冲宽度的测定

用非共线自相关SHG方法测量了Nd:YAG被动锁模激光器的脉冲宽度。非线性晶体ADP的取向是使仅在两束光都存在时才有位相匹配的SHG。两束寻常光之间的夹角在晶体中是20°50′。SHG出现在它们的角分线方向上;倍频输出是非寻常光。所测得的自相关函数的宽度对应着Nd:YAG被动锁模激光器的脉冲宽度为24ps。 关键词：     

Unidirectional second harmonic generation based on electromagnetic induced transparency-like phenomenon derived from standing waves

The nonlinearity and one-way response associated with an electromagnetically induced transparency-like (EIT-like) phenomenon based on a standing wave are theoretically analyzed and experimentally measured. The dark-meta-atom's strong energy localization results in strong second harmonic generation (SHG), while input for the opposite direction elicits no EIT-like response and a 20 dB decrease in SHG strength. The second-order standing wave can be tuned to affect the efficiency of SHG. The results presented here may represent a novel approach to designing nonreciprocal devices such as high signal-to-noise ratio electromagnetic diodes.     

Sensing and compensation of femtosecond waveform distortion induced by all-order polarization mode dispersion at selected polarization states

We demonstrate full characterization of femtosecond pulse distortion induced by all-order polarization mode dispersion (PMD) at selected polarization states via second-harmonic generation (SHG) frequency-resolved optical gating (FROG) measurements at an average power of under 28 nW. By applying the inverse of the measured spectral phase via a programmable pulse shaper, we compress the distorted pulses from more than 3 ps to nearly bandwidth-limited durations of less than 500 fs. Our results show that SHG FROG measurements performed by using fiber-pigtailed aperiodically poled lithium niobate waveguides can serve as a robust and sensitive tool for characterization of PMD-induced spectral phase.