Field-free alignment of molecules observed with high-order harmonic generation

High-order harmonic generation is demonstrated to provide a sensitive way for an extensive study of dynamic processes in the field-free alignment of strong-field-induced molecular rotational wave packets. The time-dependent harmonic signal observed from field-free-aligned N2, O2, and CO2 has been found to include two sets of beat frequency for pairs of coherently populated rotational states. One of them is the well-known frequency component characterizing the field-free alignment of molecules, and the other is ascribed to the beat that arises from coherence embedded in the wave packet. We discuss the effect of each frequency component on the revival signal observed with the harmonic generation.     

Role of the longitudinal piston error in a tiled-grating compressor in second and high-order harmonic generation

In this work, we study the limitations for overcoming the longitudinal piston error in a femtosecond tiled-grating compressor using nonlinear measurements like second harmonic generation. In particular, we observe the influence of this error when developing high-power laser experiments such as high-order harmonic generation. The generation of nonlinear processes with femtosecond pulses compressed in tiled-grating systems is studied. Special attention is paid to the role of the longitudinal piston error which is the most difficult to overcome in the compressor alignment. A complex spatio-temporal structure is expected to appear due to that misalignment. Both second harmonic generation in nonlinear crystals and high-order harmonic generation in gases are studied and a strong dependence with piston error is found, thus leading to a sub-micron modulation in the generated signal. In particular, the high sensitivity of the high-order harmonics to the longitudinal position allows one to use this processes for the accurate alignment of the compressor to few tens of nanometers.     

Extracting continuum electron dynamics from high harmonic emission from molecules

We show that high harmonic generation is the most sensitive probe of rotational wave packet revivals, revealing very high-order rotational revivals for the first time using any probe. By fitting high-quality experimental data to an exact theory of high harmonic generation from aligned molecules, we can extract the underlying electronic dipole elements for high harmonic emission and uncover that the electron gains angular momentum from the photon field.     

Polarization state of high-order harmonic emission from aligned molecules

High harmonic emission in isotropic gases is polarized in the same direction as the incident laser polarization. Laser-induced molecular alignment allows us to break the symmetry of the gas medium. By using aligned molecules in high harmonic generation experiments, we show that the polarization of the extreme ultraviolet emission depends strongly on the molecular alignment and the orbital structure. Polarization measurements give insight into the molecular orbital symmetry. Furthermore, molecular alignment will allow us to produce attosecond pulses with time-dependent polarization.     

Spectral modulation of third-harmonic generation by molecular alignment and preformed plasma

We demonstrate spectral modulation of third-harmonic generation from molecular alignment effects. The third harmonic spectrum is broadened or narrowed under different influences of cross-phase modulations originating from various molecular alignment revivals. Furthermore, the spectrum and spatial distribution of the generated third harmonic pulse change dramatically in the presence of a preformed plasma. Under the influence of a preformed plasma, a narrower third harmonic spectrum is observed, and the conical third-harmonic pulse increases while the axial part decreases. The investigation provides an effective method to modulate the spectral characteristic and spatial distribution of third-harmonic generation from intense femtosecond filament.     

空气中等离子光栅诱导探测光丝三次谐波辐射放大的实验研究

对探测光丝的不同位置与等离子光栅相互作用和探测光丝作用到等离子光栅不同位置引起三次谐波的增强进行了实验研究.研究发现,探测光丝的三次谐波信号强度对于探测光丝不同位置与等离子光栅相互作用和等离子光栅内部钳制的激光强度具有极强的依赖关系.与等离子光栅相互作用,三次谐波信号与等离子光栅基波信号的相位匹配与否是解释探测光丝三次谐波信号强度变化的关键.控制探测光丝以小角度与等离子光栅相互作用是实现探测光丝三次谐波信号有效放大的最佳途径.     

Retrieving angular distributions of high-order harmonic generation from a single molecule

We present a novel method to retrieve angular distributions of high-order harmonic generation from a single molecule. This technique uses an iterative procedure based only on experimental results of time and angle-dependent harmonic signals, and no actual shape of molecular orbital is assumed. The molecular axis distribution in a target gas can simultaneously be deduced in this procedure. The angle-dependent signal retrieved for a single N2 and O2 molecule is demonstrated to reflect the highest occupied molecular orbital, excluding the ambiguity due to the imperfect alignment.     

Generation of elliptical isolated attosecond pulse from oriented H2+ in a linearly polarized laser field

We investigate the ellipticity of the high-order harmonic generation from the oriented H₂⁺ exposed to a linearly polarized laser field by numerically solving the two-dimensional time-dependent Schrödinger equation (2D TDSE). Numerical simulations show that the harmonic ellipticity is remarkably sensitive to the alignment angle. The harmonic spectrum is highly elliptically polarized at a specific alignment angle θ=30°, which is insensitive to the variation of the laser parameters. The position of the harmonic intensity minima indicates the high ellipticity, which can be attributed to the two-center interference effect. The high ellipticity can be explained by the phase difference of the harmonics. This result facilitates the synthesis of a highly elliptical isolated attosecond pulse with duration down to 65 as, which can be served as a powerful tool to explore the ultrafast dynamics of molecules and study chiral light-matter interaction.     

Ionization effects on field-free molecular alignment observed with high-order harmonic generation

In this paper, high-order harmonic generation (HHG) is demonstrated to provide a sensitive way for studying the dynamic process in the field-free molecular alignment. The dependence of the harmonic yield and the degree of alignment on the intensity of aligning pulse is observed in impulsively aligned CO₂ molecules. A good agreement is found between the experimental and calculated results. At low pump intensities, the harmonic yield increases monotonously until the ionization induced refractive index gradient and neutral molecule depletion are significant. The results show that the optimum intensity is around 8.95 × 10¹³ W/cm²; this value is related to the molecular ionization potential.     

Molecular recollision interferometry in high harmonic generation

We use extreme-ultraviolet interferometry to measure the phase of high-order harmonic generation from transiently aligned CO(2) molecules. We unambiguously observe a reversal in phase of the high-order harmonic emission for higher harmonic orders with a sufficient degree of alignment. This results from molecular-scale quantum interferences between the molecular electronic wave function and the recolliding electron as it recombines with the molecule, and is consistent with a two-center model. Furthermore, using the combined harmonic intensity and phase information, we extract accurate information on the dispersion relation of the returning electron wave packet as a function of harmonic order. This analysis shows evidence of the effect of the molecular potential on the recolliding electron wave.     

Minimum structure of high-harmonic spectrafrom aligned O2 and N2 molecules

We experimentally investigated the high-order harmonic generation (HHG) from aligned O₂ and N₂ molecules in a linearly polarized laser field, and presented the dependence of the harmonic spectrum on the driving laser intensity and molecular alignment angle. The minimum position of HHG of O₂ varies with changing the laser intensity, which is caused by multi-orbital interference. However, the location of the observed minimum structure in N₂ harmonic spectrum remained unchanged upon changing the laser intensity. The mechanism of the spectral minimum for N₂ case is regarded as a Cooper-like minimum in HHG associated with the molecular electronic structure. This work indicates that harmonic spectroscopy can effectively uncover information about molecular structure and electron dynamics.     

Three-phase contact line energetics from nanoscale liquid surface topographies

We observed light-induced alignment of the nematic liquid crystal, 4, 4(')-n-pentylcyanobiphenyl (5CB), on a fused quartz. Irradiation of the adsorbed layer with polarized ultraviolet light produced homogeneous alignment in a 5CB-filled liquid crystal cell with the easy orientation axis perpendicular to the polarization direction. The measured anchoring energy increases with illumination up to 10(-4) erg/cm (2). Phase retardation and pretilt measurements confirmed near homogeneous alignment of the LC in a cell, while the polarization dependence of second harmonic generation suggested a near normal alignment of the adsorbed layer. We believe that light-induced rearrangement or phototransformation of the adsorbed layer causes the observed phenomenon.     

Probe of high-order harmonic generation in a hollow waveguide geometry using counterpropagating light

We use counterpropagating light to directly observe the coherent buildup of high harmonic generation in a hollow waveguide geometry. We measure, for the first time, coherence lengths for high photon energies that cannot be phase matched using conventional approaches. We also probe the transition through phase matching, the ionization level at which different harmonic orders are generated, and the change in the coherence length as the driving laser is depleted. These results directly prescribe the optimal structures or pulse trains required for implementing quasiphase matching.     

LB膜的各向异性与二次谐波超平方增长

用偏振紫外－可见吸收及旋转样品二次谐波方法研究了半花菁／花生酸Ｙ型交替ＬＢ多层膜中由垂直浸渍过程诱导和层间相互作用增强的分子在基板平面内的定向排列，提出并证实了随层数增长的平面内附加偶极矩导致光学二次谐波强度随ＬＢ膜厚度的超平方增长关系。     

Numerical characterization of high harmonic attosecond pulses

A numerical simulation of attosecond harmonic pulse generation in a three-dimensional field-ionizing gas is presented. Calculated harmonic efficiencies quantitatively reproduce experimental findings. This allows a quantitative characterization of attosecond pulse generation revealing information currently not accessible by experiment. The rapid phase variation and spatiotemporal distortions of harmonics are smaller than anticipated, allowing focusing of 30-nm, 750-as pulses to intensities in excess of 10(13) W/cm(2). Feasibility of such pulses brings novel applications such as extreme ultraviolet nonlinear optics and attosecond pump probe spectroscopy within reach.     

Nonlinear optical probe of tunable surface electrons on a topological insulator

We use ultrafast laser pulses to experimentally demonstrate that the second-order optical response of bulk single crystals of the topological insulator Bi(2)Se(3) is sensitive to its surface electrons. By performing surface doping dependence measurements as a function of photon polarization and sample orientation we show that second harmonic generation can simultaneously probe both the surface crystalline structure and the surface charge of Bi(2)Se(3). Furthermore, we find that second harmonic generation using circularly polarized photons reveals the time-reversal symmetry properties of the system and is surprisingly robust against surface charging, which makes it a promising tool for spectroscopic studies of topological surfaces and buried interfaces.     

High-order harmonic generation from ions in a capillary discharge

We demonstrate a significant extension of the high-order harmonic cutoff by using a fully-ionized capillary discharge plasma as the generation medium. The preionized plasma dramatically reduces ionization-induced defocusing and energy loss of the driving laser due to ionization. This allows for significantly higher photon energies, up to 150 eV, to be generated from xenon ions, compared with the 70 eV observed previously. We also demonstrate enhancement of the harmonic flux of nearly 2 orders of magnitude at photon energies around 90 eV when the capillary discharge is used to ionize xenon, compared with harmonic generation in a hollow waveguide. The use of a plasma as a medium for high-order harmonic generation shows great promise for extending efficient harmonic generation to much shorter wavelengths using ions.     

飞秒时间分辨实验中相关函数和时间零点的确定

结合飞秒激光在研究分子激发态弛豫动力学中的应用,介绍了几种飞秒时间分辨实验中确定泵浦激光脉冲与探测激光脉冲的相关函数和时间零点的方法.对于波长在可见波段的泵浦和探测激光脉冲,我们可以利用非线性光学的技术手段,探测泵浦光与探测光的和频光的强度随二者间的时间延迟的变化来确定相关函数和时间零点;对于波长在紫外甚至更短的波段的泵浦和探测激光脉冲,由于单脉冲能量比较低,目前还很难利用技术手段来测定泵浦激光与探测激光的相关函数及时间零点,可以利用某些原子气体(如Xe)或某些具有短寿命态的分子作平行实验进行间接测量.     

Strong P-band emission and third harmonic generation from ZnO nanorods

We report the room-temperature photoluminescence (PL) and broadband nonlinear optical (NLO) responses from high-quality ZnO nanorods grown by hydrothermal deposition. Based on the PL measurements, we find that the optical quality of ZnO nanorods critically depends on the packing and alignment of the rod structures. Our ZnO nanorods exhibit very strong third harmonic generation with suppressed second harmonic generation when the fundamental wavelength is varied in the range of 1060–2120 nm. Our results imply that ZnO nanostructures can potentially be utilized for various optoelectronic applications involving third-order NLO processes.     

High-order harmonic generation in nitrogen molecules with subpicosecond visible dye-laser pulses

An experimental study of high-order harmonic generation in nitrogen molecules (N₂) has been made using intense visible (616 nm) dye-laser pulses, where the harmonic radiation up to the 21st order is observed. The harmonic distribution represents a plateau that is preceded by an intensity minimum at the 7th order. The harmonic generation characteristics were atomic-like. It has been found that there are some similarities in the high-order harmonic generation characteristics for N₂ and Ar, including the highest-order harmonics, harmonic distributions, and the influence of the multiphoton ionization on the high-order harmonic generation. These similarities are reasonably attributed to the energetic correspondence of excited levels and ionization potentials. It is pointed out that the ac Stark shift of excited levels and ionization potentials plays an important role also in the high-order harmonic generation in N₂.