Self-compression of ultrashort pulses through ionization-induced spatiotemporal reshaping

We present the first demonstration of a new mechanism for temporal compression of ultrashort light pulses that operates at high (i.e., ionizing) intensities. By propagating pulses inside a hollow waveguide filled with low-pressure argon gas, we demonstrate a self-compression from 30 to 13 fs, without the need for any external dispersion compensation. Theoretical models show that 3D spatiotemporal reshaping of the pulse due to a combination of ionization-induced spectral broadening, plasma-induced refraction, and guiding in the hollow waveguide are necessary to explain the compression mechanism.     

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.     

Generation of femtosecond vacuum-ultraviolet pulses

High power femtosecond pulses in the Vacuum Ultra Violet (VUV) have been generated through the nonlinear interaction of femtosecond KrF pulses with xenon and argon gas. Under near resonant two photon excitation of xenon by a femtosecond KrF laser, parametric four wave mixing processes lead to VUV pulses at 147 and 108 nm with pulse energies in the 10 µJ range. Tuning is demonstrated by mixing the KrF pulse with a 500 fs dye laser pulse at 497 nm, resulting in 165 nm emission. In argon, a three photon resonance leads to third harmonic generation at 83 nm and micro joule level pulses near 127 nm generated by a six wave mixing process. Since the spectra of the VUV pulses show an ionization-induced blue shift with increasing KrF laser intensity, the VUV pulses can be shown to have temporal duration less than the pulse width (450 fs) of the KrF laser. Blue shifting of the third harmonic of the KrF laser in argon is dominated by a reduction in the neutral gas density rather than by an increase in the electron density.     

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.     

Quasi-phase matching of high-order harmonic generation at high photon energies using counterpropagating pulses

We extend all-optical quasi-phase matching of high-order harmonic generation into spectral regions where conventional phase matching is not possible. The high laser intensities required to generate harmonics at energy >130 eV, coupled with the resulting high level of ionization, preclude conventional phase matching in all nonlinear media. Selective enhancement factors between 40 and 150 in the flux of harmonics at photon energies around 140 eV are demonstrated using a train of two counterpropagating pulses.     

Generation of coherent soft-X-ray radiation extending far beyond the titanium L edge

Coherent soft-x-ray radiation up to photon energies of 700 eV is obtained by focusing several-mJ, 10-fs near infrared laser pulses into a He gas jet. The observed nearly constant photon yield over several hundred eVs may be attributed to nonadiabatic self-phase matching, originating from a substantial ionization within a fraction of the optical cycle of the driving laser pulse.     

Photoemission electron microscopy as a tool for the investigation of optical near fields

Photoemission electron microscopy was used to image the electrons photoemitted from specially tailored Ag nanoparticles deposited on a Si substrate (with its native oxide SiO(x)). Photoemission was induced by illumination with a Hg UV lamp (photon energy cutoff homega(UV) = 5.0 eV, wavelength lambda(UV) = 250 nm) and with a Ti:sapphire femtosecond laser (homega(l) = 3.1 eV, lambda(l) = 400 nm, pulse width below 200 fs), respectively. While homogeneous photoelectron emission from the metal is observed upon illumination at energies above the silver plasmon frequency, at lower photon energies the emission is localized at tips of the structure. This is interpreted as a signature of the local electrical field therefore providing a tool to map the optical near field with the resolution of emission electron microscopy.     

Extended phase matching of high harmonics driven by mid-infrared light

We demonstrate that phase-matched frequency upconversion of ultrafast laser light can be extended to shorter wavelengths by using longer driving laser wavelengths. Experimentally, we show that the phase-matching cutoff for harmonic generation in argon increases from 45 to 100 eV when the driving laser wavelength is increased from 0.8 to 1.3 microm. Phase matching is also obtained at higher pressures using a longer-wavelength driving laser, mitigating the unfavorable scaling of the single-atom response. Theoretical calculations suggest that phase-matched high harmonic frequency upconversion driven by mid-infrared pulses could be extended to extremely high photon energies.     

Resonant photoemission at the 3s threshold of Ni

A resonant enhancement of valence band photoemission features in Ni near the 3s threshold is presented. The emission behavior with photon energy of the Ni-3d band is characteristic of a Fano-type resonance. In addition to the main 3d-band emission and 6eV binding energy satellite, a weak satellite is observed at 7.2eV below the Fermi level with photon energies in the vicinity of the 3s threshold.     

Grating-assisted phase matching in extreme nonlinear optics

We propose a new technique for phase matching high harmonic generation that can be used for generating bright, tabletop, tunable, and coherent x-ray sources at keV photon energies. A weak quasi-cw counterpropagating field induces a sinusoidal modulation in the phase of the emitted harmonics that can be used for correcting the large plasma-induced phase mismatch. We develop an analytical model that describes this grating-assisted x-ray phase matching and predicts that very modest intensities (<10(10) W/cm2) of quasi-cw counterpropagating fields are required for implementation.     

High-order harmonic generation up to 250 eV from highly ionized argon

We demonstrate the generation of very high-order harmonics, up to 250 eV, using argon gas. This extends by 100 eV the highest harmonics previously observed using Ar and exceeds the energies observed using any other medium besides helium. This advance is made possible by using a waveguide geometry to limit plasma-induced laser beam defocusing, making it possible to generate high harmonics from Ar ions. This work shows that high harmonic emission from ions can extend laser-based coherent up-conversion into the soft x-ray region of the spectrum.     

Guing of intense femtosecond pulses in preformed plasma channels

We report guiding of sub-100-fs pulses at intensities up to 5x10(15) W/cm (2) over a distance of 1 cm in a preformed plasma channel. The width of the guided pulse was shortened, which we attribute to ionization-induced refraction at the channel entrance. A pulse energy throughput of 30% in the lowest-order was measured.     

Detection of Fe 3d electronic states in valence band and magnetic properties of Fe-doped ZnO film

Fe-doped ZnO film has been grown by laser molecular beam epitaxy (L-MBE) and structurally characterized by X-ray diffraction (XRD) and scanning electron microscopy (SEM), all of which reveal the high quality of the film. No secondary phase was detected. Resonant photoemission spectroscopy (RPES) with photon energies around the Fe 2p-3d absorption edge is performed to detect the electronic structure in the valence band. A strong resonant effect at a photon energy of 710 eV is observed. Fe³⁺ is the only valence state of Fe ions in the film and the Fe 3d electronic states are concentrated at binding energies of about 3.8 eV and 7 eV～ 8 eV. There are no electronic states related to Fe near the Fermi level. Magnetic measurements reveal a typical superparamagnetic property at room temperature. The absence of electronic states related to Fe near the Fermi level and the high quality of the film, with few defects, provide little support to ferromagnetism.     

Stimulated emission from a single excited atom in a waveguide

We study stimulated emission from an excited two-level atom coupled to a waveguide containing an incident single-photon pulse. We show that the strong photon correlation, as induced by the atom, plays a very important role in stimulated emission. Additionally, the temporal duration of the incident photon pulse is shown to have a marked effect on stimulated emission and atomic lifetime.     

Unified microscopic-macroscopic formulation of high-order difference-frequency mixing in plasmas

We investigate high-order difference-frequency mixing in plasmas, taking into account the microscopic rescattering physics and propagation effects for the first time. We show that phase matching can occur over a broad frequency range, up to very high photon energies, and that it is confined to specific temporal and spatial windows. This gated phase matching mechanism is driven by the continuous phase slip between two driving fields and can be employed for manipulating the temporal, spatial, and spectral properties of high harmonic emission.     

Quenching of photoluminescence in ZnS:Cu single crystals

Experiments on the quenching of photoluminescence in ZnS:Cu single crystals by secondary radiation are reported. Quenching of emission at photon energies of 1.4, 1.7, 2.4 and 2.75 eV by photons at 0.93, 1.6, 2.0, 2.4 eV is found, with a possible fifth peak at 2.7 eV. The effect of each secondary band on each emission band is found to be equivalent. This is explained in terms of a model in which all quenching transitions effectively fill a common ground state for the green/blue emission.     

Generation of high-energy few-cycle laser pulses by using the ionization-induced self-compression effect

A mechanism behind the ionization-induced self-compression effect for ultrashort laser pulses propagating in gas-filled capillaries is proposed. It is shown that as a result of excitation of the nonlinear-plasma waveguide laser pulses producing gas ionization can be self-compressed to few-cycle duration. This effect is used for high-energy laser pulses and its scalability to J-level energies is demonstrated.     

衰减匹配的超声Barker码激励方法

为增加超声穿透高声衰减介质的能力,提出了一种衰减匹配的超声Barker码激励方法。基于换能器高斯响应与材料非频散线性衰减的假设,得到了Barker码激励的信号模型,求解旁瓣抑制滤波后脉冲压缩的信噪比表达式可知,该方法仅需要根据材料衰减特性与轴向分辨率的要求,分别调整Barker码的中心频率与时长,便可以获得更高的信噪比。取衰减系数为1.4 Np/(MHz·cm)、厚度为5 cm的橡胶为试样进行验证。当与方波激励方法的轴向分辨率相近时,衰减匹配的Barker码激励方法比传统Barker码激励方法的信噪比增益提高接近5 dB;当牺牲一定轴向分辨率时,信噪比增益提高接近11 dB。结果表明,衰减匹配的Barker码激励方法可以降低依频率衰减对脉冲压缩的影响,有效提高衰减回波的信噪比。      

Optical pulse compression of ultrashort laser pulses in an argon-filled planar waveguide

We investigate the possibility of optical pulse compression of high energy ultrashort laser pulses in an argon-filled planar waveguide, based on two level coupled mode theory and the full 3D nonlinear Schr?dinger equation. We derive general expressions for controlling the spatial beam profile and the extent of the spectral broadening. The analysis and simulations suggest that the proposed method should be appropriate for optical pulse compression of ultrashort laser pulses with energies as high as 600 mJ.     

Photon emission with the scanning tunneling microscope

By placing a photon detector near the tip-sample region of a scanning tunneling microscope, we have measured isochromat photon-emission spectra of polycrystalline tantalum and Si(111)7×7 at photon energies of 9.5 eV. Such spectra contain electronic-structure information comparable to inverse photoemission spectroscopy, but with high lateral/spatial resolution. The implications of this new observation are discussed.