Nonlinear optical response from single spheres coated by a nonlinear monolayer

We detected the second-order nonlinear response from single isolated spheres comprised from a centrosymmetric material but covered by a layer of a material with strong second-order nonlinear properties and isolated from an ensemble by the optical trapping technique. We show that when large size parameter spheres are used, the measured second-harmonic efficiency deviates strongly from the prediction of the nonlinear Rayleigh scattering theory. Our results are in very good agreement with the predictions from the exact nonlinear Mie scattering theory.     

A cascaded second-order approach to computing third-order scattering of noncollinear acoustic beams

A theoretical development of the third-order nonlinear scattering of sound from two noncollinear ultrasonic beams produced by baffled piston sources is presented. The third-order intermodulation (IM3) frequency components are derived by exploiting cascaded second-order nonlinear effects where the quadratic nonlinear interaction of second-order frequency components with first-order (primary) frequency components is considered. It is shown that cascaded second-order interactions generate intermodulation frequency components that are equivalent to those generated by cubic nonlinear effects. Comparison of measured and modeled amplitude sweeps demonstrate the three-to-one gain in decibels of the amplitudes of the third-order intermodulation frequency components to that of the primary frequency components. Measurements are also presented for the farfield interaction of distantly spaced sources, which results in a highly focused ultrasonic parametric array. Also considered are the nearfield interaction of closely spaced sources, which results in scattering, with good agreement to the theory.     

Circular dichroism in core level photoemission from an adsorbed chiral molecule

The results of experimental measurements and theoretical simulations of circular dichroism in the angular dependence (CDAD) of photoemission from atomic core levels of each of the enantiomers of a chiral molecule, alanine, adsorbed on Cu(110) are presented. Measurements in, and out of, substrate mirror planes distinguish CDAD due to the chirality of the sample and the experimental geometry. The effect due to sample chirality is relatively weak, so such measurements may not provide a routine spectral fingerprint of adsorbate chirality.     

超常介质中超短电磁脉冲的传输特性研究

将超常介质的色散磁导率合并到非线性极化项中,借鉴常规介质中超短脉冲传输方程的推导方法,得到了非线性超常介质中超短脉冲的传输方程。在德鲁德(Drude)色散模型下,根据脉冲中心频率的不同在传输方程中出现了可正、可负、可为零的自陡峭系数,以及高阶非线性色散项。此外,利用矩方法对传输方程进行分析,得到了超常介质中超短脉冲传输方程的能量守恒定律表达式,揭示了色散磁导率导致的超短脉冲传输的新特性,发现二阶非线性色散使超短脉冲的能量、脉冲频移、脉冲宽度、中心位置和啁啾都随传输距离呈现振荡式变化。     

Parametric frequency conversion in layered nonlinear media

Frequency-angular distributions of signal wave intensity are calculated for spontaneous parametric down-conversion and parametric frequency conversion in spatially nonuniform nonlinear media. Wave reflection from interfaces is taken into account, and both regular and irregular nonuniform distributions of second-order nonlinear susceptibility are considered. A unified approach using a scattering matrix and a generalized Kirchhoff law is applied in calculations of spontaneous and stimulated processes in dissipative nonlinear media. Interference of electromagnetic zero-point fluctuations of the vacuum, nonlinear interference, and nonlinear diffraction are examined for media with various absorptive properties. Theoretical foundations are developed for diagnostics of nonuniform distributions of the second-order susceptibility, based on measurement of the line profiles of nonlinear signals.     

Chiral and antichiral order in bent-core liquid crystals

Recent experiments have found a bent-core liquid crystal in which the layer chirality alternates from layer to layer, giving a racemic or "antichiral" material, even though the molecules are uniformly chiral. To explain this effect, we map the liquid crystal onto an Ising model, analogous to a model for chiral order in polymers. We calculate the phase diagram for this model and show that it has a second-order phase transition between antichiral order and homogeneous chiral order. We discuss how this transition can be studied by further chemical synthesis or by doping experiments.     

Pulse Propagation with Self-Phase Modulation in Nonlinear Chiral Fiber and Its Applications

From Maxwell's equations and Post's formalism,a generalized chiral nonlinear Schrodinger equation(CNLSE) is obtained for the nonlinear chiral fiber.This equation governs light transmission through a dispersive nonlinear chiral fiber with joint action of chirality in linear and nonlinear ways.The generalized CNLSE shows a modulation of chirality to the effect of attenuation and nonlinearity compared with the case for a conventional fiber.Simulations based on the split-step beam propagation method reveal the role of nonlinearity with cooperation to chirality playing in the pulse evolution.By adjusting its strength the role of chirality in forming solitons is demonstrated for a given circularly polarized component.The application of nonlinear optical rotation is also discussed in an all-optical switch.     

Theoretical model for electromagnetic wave propagation in negative index material induced by cubic-quintic nonlinearities and third-order dispersion effects

We analyze the problem of characterization of electromagnetic (EM) wave that propagates in a negative index material (NIM) and compare to the behavior that observes in a positive index material (PIM), from the conventional technique of characterization of the pulse intensity profile. Firstly, we establish the nonlinear Schrödinger equation (NLSE) and use the Drude model to obtained the NLSE terms. Secondly, we apply the collective variables technique at each frequency range and show that the stability and the light pulse intensity are significantly depending on specific normalized frequencies. We determine the specific frequency range allowing a fear characterization of the intensity profile of light pulse when the frequency increases. We illustrate the effectiveness of this EM wave stabilization by applying the indicated frequency range. This conventional technique in NIM and PIM systems where the second-order dispersion, third-order dispersion, self phase modulation (SPM) and quintic effects originated from SPM called quintic phase modulation act to provoke strong perturbations.     

Organic second-order non-linear optical materials and devices

Organic second-order nonlinear materials are currently receiving considerable attention for fabrication of frequency mixing and electro-optic devices. In this paper the key concepts in the development of organic nonlinear materials and waveguide device design are introduced. The recent advances in nonlinear waveguides for frequency doubling and electro-optic devices are reviewed.An invited paper     

Enhancement of the second harmonic generation from monolayer WS2 coupled with a silica microsphere

Monolayer transition metal dichalcogenides (TMDs) are widely used for integrated optical and photoelectric devices. Owing to their broken inversion symmetry, monolayer TMDs have a large second-order optical nonlinearity. However, the optical second-order nonlinear conversion efficiency of monolayer TMDs is still limited by the interaction length. In this work, we theoretically study the second harmonic generation (SHG) from monolayer tungsten sulfide (WS₂) enhanced by a silica microsphere cavity. By tuning the position, size, and crystal orientation of the material, second-order nonlinear coupling can occur between the fundamental pump mode and different second harmonic cavity modes, and we obtain an optimal SHG conversion efficiency with orders of magnitude enhancement. Our work demonstrates that the microsphere cavity can significantly enhance SHG from monolayer 2D materials under flexible conditions.     

Exploring fundamental limits to terahertz generation in electrooptic materials: From bulk to nanolayers

We review the progress made by us on the exploration of the fundamental limits to terahertz (THz) generation from several semiconductor electrooptic materials. Through the measurements of the THz output versus the pump beam in terms of incident angle, polarization, azithumal angle, and pump intensity, we have demonstrated that we can precisely determine the contributions made by the optical rectification and photocurrent surge. When a material is pumped below its bandgap, optical rectification is always the mechanism for the THz generation. Above the bandgap, however, these two mechanisms often compete with each other, depending on the material characteristics and pump intensity. At a sufficiently high pump intensity, optical rectification usually becomes the dominant mechanism for a second-order nonlinear material. Our analysis indicates that second-order nonlinear coefficients are resonantly enhanced when a material is pumped above its bandgap. In such a case, the THz output power and normalized conversion efficiency can be dramatically increased. We have also illustrated that, for some materials, two-photon absorption can be one of the fundamental limits to the THz generation.     

Second harmonic generations in aperiodic optical superlattices with finite width and in one-dimensional defective photonic crystals made of nonlinear optical materials

The characteristics of the second harmonic generations (SHGs) in homogeneous and inhomogeneous systems are investigated. We consider two kinds of structures: one is aperiodic optical superlattices (AOSs) with homogeneous linear susceptibility and the modulated second-order nonlinear susceptibility; the second is linear and nonlinear susceptibilities both the system with inhomogeneous. We derive a general solution of SHG for the AOS with finite lateral width and of SHG in considering the depletion of the pump light power. We carry out the design of AOSs by using simulation annealing (SA) algorithm and show that the constructed AOSs can implement multiple wavelength SHGs with identical effective nonlinear coefficient at the preassigned wavelengths of incident light. We observe great enhancement of SHGs in the one-dimensional photonic crystals (PCs) with defects consisting of multiple photonic quantum wells made of nonlinear material when the frequency of fundamental wave aims at one of the defect states. We also propose an effective design approach of aperiodically stacked layers of nonlinear material and air in terms of the SA method. The constructed structure can achieve multiple-wavelength SHGs at the preas-signed wavelengths.      

Non-covalently bonded diastereomeric adducts of amino acids and (S)-1-phenylethanol in low-energy dissociative collisions

We have studied the collision induced dissociation reactions of proton-bound diastereomeric adducts of S-1-phenylethanol and enantiomers of three different amino acids (tryptophan, phenylalanine, methionine). In all cases, the loss of S-1-phenylethanol from the adduct ion is the only observed process, and the relative abundance is found to be independent of the chirality of the amino acid. This is in contrast to earlier experiments on the dissociation of protonated tryptophan–2-butanol adducts, where chirality affected the results. Results obtained from quantum chemical computations support and provide a rationale for the experimental observations and highlight temperature as a possible factor of importance for the chiral effect in these types of systems.     

Chiral separation in microflows

Molecules that only differ by their chirality, so-called enantiomers, often possess different properties with respect to their biological function. Therefore, the separation of enantiomers presents a prominent challenge in molecular biology and has long been a main pursuit of organic chemistry. We suggest a new separation technique for chiral molecules that is based on the transport properties in a microfluidic flow with spatially variable vorticity. Because of their size the thermal fluctuating motion of the molecules must be taken into account. These fluctuations play a decisive role in the proposed separation mechanism.     

Recent advances in ultrafast time‐resolved chirality measurements: perspective and outlook

Observing chirality changes as they occur is an important topic of research. It provides information that deepens the understanding of biomolecular configuration and conformation under environmental changes. Also, knowing the specific steps in chiral synthesis would simplify the production of specific chiral enantiomers that have a specific function. To gain better insight to the initial steps of conformational and configurational changes, the time‐resolution of chiral spectroscopy is continually pushed toward a shorter time‐scale. Recent advances have produced measurements of chirality changes with a femtosecond time‐resolution. These measurements are hindered by the inherently weak chirality signal, which can be overshadowed by different optical artefacts. This minireview will look at the so far successful techniques which measure chirality changes with femtosecond time‐resolution and discuss the advantages and disadvantages of these techniques. A short outlook will also look at new techniques that could improve the ability to measure chirality changes on an ultrafast time‐scale.     

共振增强的光学参变下转换

多光子纠缠态是量子通讯网络中的重要资源,光与二阶非线性介质相互作用的自发参变下转换过程是目前制备多光子态较成熟的方案之一.尽管脉冲光可以提高非线性转换效率并简化通信协议,但是进一步增强光与介质间的相互作用对提高多光子的产生效率依然必要.设计了飞秒脉冲激光谐振腔系统,在不改变脉冲重复频率和频率梳结构的情况下,提高了下转换...     

Three-dimensional second-harmonic generation imaging with femtosecond laser pulses

A three-dimensional reflectance scanning optical microscope based on the nonlinear optical phenomenon of second-harmonic generation is presented. A mode-locked Ti:sapphire laser producing <90-fs pulses at ~790nm was used, and the images were constructed by scanning of an object, which possessed local second-order nonlinearity, relative to a focused spot from the laser. The second-harmonic light at ~395nm generated by the specimen was separated from the fundamental beam by use of dichroic and interference filters and was detected by a photodiode. The technique was then used to characterize the distribution of second-order nonlinearity and microstructure of the nonlinear material lithium triborate.     

Broadband third-harmonic generation in two-dimensional short-range ordered nonlinear photonic structure

We study parametric frequency conversion in two-dimensional nonlinear photonic crystal with short-range ordered ferroelectric domains. We demonstrate that the short-range order enables broadband third-harmonic generation via cascading of two second-order quasi-phase matched nonlinear processes. We obtain conversion efficiencies that are much higher than those achieved from a randomized medium, owing to the unique distribution of reciprocal lattice vectors in the short-range ordered structure.     

Second harmonic generation in planar chiral nanostructures

The effect of the chirality of planar spiral nanostructures on optical second harmonic generation (SHG) is studied in the paper. It is shown that the intensity of left and right circularly polarized SHG differs for structures of different handedness and the direction of the SHG polarization rotation plane is opposite for enantiomers.     

Analytic upper and lower bounds for the period of nonlinear oscillators

We show that analytic expressions for the frequency of second-order nonlinear oscillations can be obtained from dual variational principles. At each amplitude two analytic expressions can be constructed which constitute upper and lower bounds to the exact value of the frequency. The results are accurate at small and large amplitude and compare well with the perturbative approach.