Third-order nonlinear optical response in transparent solids using ultrashort laser pulses

The third-order optical nonlinearity, χ ⁽³⁾, is measured in transparent glasses (BK7 and fused silica) and crystals (BaF₂ and quartz) using 36-fs, 800-nm laser pulses and the optical Kerr gate (OKE) technique; values are found to lie in the range 1.3–1.7×10^-14 esu, in accordance with theoretical estimates. We probe the purely electronic response to the incident ultrashort laser pulse in fused silica and BK7 glass. In BaF₂ and quartz, apart from the electronic response we also observe contribution from the nuclear response to the incident ultrashort pulses. We observe oscillatory modulations that persist for ～400 fs. The response of the media (glasses and crystals) to ultrashort pulses is also measured using two-beam self-diffraction; the diffraction efficiency in the first-order grating is measured to be in the range of 0.06–0.13 %. Third harmonic generation due to self-phase matching in the transient grating geometry is measured as a function of temporal delay between the two incident ultrashort pulses, yielding the autocorrelation signal.     

Comment on “propagation of ultrashort light pulses in a resonant medium”

Previous conclusions on the propagation of ultrashort light pulses in a resonant medium are found to be in error. There is no physical basis for rejecting the nd u and dn u solutions.     

Phonon autoecho in bismuth and antimony single crystals

Phonon autoecho is observed upon pumping Bi and Sb semimetals with ultrashort high-energy laser pulses. The autoecho is manifested as a revival of reflection oscillations generated by an A_1g coherent phonon after their complete disappearance. The phenomenon of phonon autoecho offers decisive evidence of the nonclassical character of the state of the crystal lattice that is accomplished in pumping-probing experiments by femtosecond laser pulses.     

A Temporal Method for Dispersion Measurements with Ultrashort Pulses in the Visible and Near-Infrared Region

We investigate a temporal method using ultrashort pulses for measuring the whole set of dispersion characteristics of birefringent crystals. The principle consists in measuring the time of flight of ultrashort pulses through the crystal. It allows the determination of the principle axes, the indices, the group velocities and the group velocity dispersion. These measurements are realized on an AgGaS₂ crystal in the visible and near-infrared spectrum.     

The Bloch Equations for an AB System and the Design of Spin-State-Selective RF Pulses for Coupled Spin Systems

Optimized AM/FM pulses are described which excite an arbitrary coherence of a coupled spin system with optimal intensity. These pulses may become important for creating maximum signal intensity in MQC-filtered and polarization-transfer experiments in HRNMR and in vivo spectroscopy. For an AB system, for example, a pure DQC or ZQC state is obtained (100%) compared to maximal 50% with a conventional π/2-π/2 MQC pulse sequence. The design and numerical optimization of these pulses, with pulse times of about 1/2J (J is the coupling constant), are described. Examples of three of these spin-state-selective pulses (SSSP) for an AB system are given; simulations and experiments confirm their expected performance. To get some insight in the relations between the expectation values of the several coherences under the influence of Zeeman, J-coupling, and RF terms, Bloch-like equations for a proton AB system are derived, with neglection of relaxation. A system of 15 first-order coupled differential equations is found. A solution to these equations is given for the evolution of the zero-quantum coherence and longitudinal magnetization.     

Nonlinear lattice dynamics of bismuth as a means of clarifying the nature of coherent phonons

The nonlinear regime of generation of coherent phonons in bismuth single crystals irradiated by ultrashort high-energy laser pulses has been investigated. In this regime, autoecho phenomenon is implemented at a low (helium) crystal temperature, manifesting itself as a collapse and revival of reflection oscillations generated by coherent A _1g phonons. Different mechanisms of the observed phenomena are considered.     

超短激光脉冲驱动的Thomson散射空间分布特性

研究了超短激光脉冲驱动的Thomson散射的辐射空间分布. 发现辐射的空间分布对称性显著地依赖于超短脉冲的载波相位η₀，在η₀＝0，π时，辐射的空间分布呈现出二重或一重对称性；而在其他载波相位时，这些空间分布对称性遭到破坏. 辐射光的准直性也依赖于驱动脉冲的载波相位，在η₀＝±π/2时辐射光的准直性最好. 这些结果表明可以通过改变驱动激光脉冲的载波相位来控制辐射光的空间分布，也可以利用辐射空间分布对相位的依赖特性来测量超短激光脉冲的载波相位. 关键词： Thomson散射 空间分布 载波相位     

Advanced time-resolved absorption spectroscopy with an ultrashort visible/near IR laser and a multi-channel lock-in detector

Ultrashort visible-near infrared (NIR) pulse generation and its applications to ultrafast spectroscopy are discussed. Femtosecond pulses of around 800 nm from a Ti:sapphire laser are used as a pump of an optical parametric amplifier (OPA) in a non-collinear configuration to generate ultrashort visible (500–780 nm) pulses and deep-ultraviolet (DUV, 259–282 nm) pulses. The visible-NIR pulses and DUV pulses were compressed to 3.9 fs and 10.4 fs, respectively, and used to elucidate various ultrafast dynamics in condensed matter with a sub-10 fs resolution by pump-probe measurements. We have also developed a 128-channel lock-in amplifier. The combined system of the world-shortest visible pulse from the OPA and the lock-in amplifier with the world-largest channel-number can clarify the sub-10 fs-dynamics in condensed matter. This system clarified structural changes in an excited state, reaction intermediate, and a transition state. This is possible even during molecular vibration and reactions via a real-time-resolved vibronic spectrum, which provides molecular structural change information. Also, ultrafast dynamics in exotic materials like carbon nanotubes, topological insulators, and novel solar battery systems have been clarified. Furthermore, the carrier-envelope phase in the ultrashort pulse has been controlled and measured.     

Spatiotemporal behaviors and singularity of ultrashort pulsed Elegant Hermite-Gaussian beams

Analytical propagation expressions of ultrashort pulsed Elegant Hermite-Gaussian beams are derived and spatiotemporal properties of the pulses with different transverse modes are studied. Singularity of the complex amplitude envelope solution of the pulses obtained under slowly varying envelope approximation is analyzed in detail. The rigorous analytical solution of the pulse is deduced and no singularity emerges in the solution. The obtained results indicate that the transverse mode affects not only the spatiotemporal properties but also the singularity of the pulses. Time delay of the off-axis maximum intensity is more obvious and the singularity is located nearer to the z-axis for the pulse with higher transverse modes.     

Calculus removal on a root cement surface by ultrashort laser pulses

Ultrashort-pulse-laser ablation of dental calculus (tartar) and cement is performed on root surfaces. The investigation shows that the threshold fluence for ablation of calculus is a factor of two to three times smaller than that of a healthy root cement surface. This indicates that ultrashort laser pulses may provide an appropriate tool for selective removal of calculus with minimal damage to the underlying root cement. Future application of an in situ profiling technique allows convenient on-line monitoring of the ablation process.     

Dispersion and nonlinear management for femtosecond optical solitons

We consider the concept of femtosecond propagation for optical solitons in a dispersion management fiber and study the optimal amplification of optical solitons through dispersion wells and barriers and also for the dispersion tailored profile case. For the former, we observed periodic soliton trapping for the in-phase injection case when their respective velocities were equal and opposite with their amplitudes being unequal and no soliton trapping for the off-phase injection case when the two pulses are having a phase difference of π. For the latter, we observed an enormous amplification of the soliton pulses which is one of our main results in this Letter.     

Coherent control of the lattice dynamics of bismuth near the lindemann stability limit

The relative contributions of the anharmonicity of the lattice potential and the nonequilibrium concentration of charge carriers to the time dependence of the coherent A _1g phonon frequency in bismuth excited by high-energy ultrashort laser pulses are studied by the coherent control method. The contributions are separated by the pump-probe method in which excitation is performed by two pulses with a controlled time delay. It is shown that, depending on the relative delay between the pump pulses, both correlation and anticorrelation between the amplitude and the initial frequency of oscillations are observed while the chirp and the initial frequency of the coherent phonon are anticorrelated. In addition, it has been found that the contributions of the lattice and the electronic subsystem are always anticorrelated. Therefore, a certain phase can be assigned to an electronic excitation and it may be suggested that the time dependence of the phonon frequency is determined not only by instantaneous values of the lattice and electronic response but also by the phase relations between them.     

Nonlinear photoionization and laser-induced damage in silicate glasses by infrared ultrashort laser pulses

We show that photoionization of wide band gap silicate glasses by infrared ultrashort laser pulses can occur without laser-induced damage. Two glasses are studied, fused silica and a multi-component silicate photo-thermo-refractive (PTR) glass. Experiments are performed by low numerical aperture focusing of ultrashort laser pulses (100 fsec<τ<1.5 psec) at the wavelengths 780 nm, 1430 nm, and 1550 nm. Filaments form inside both glasses and are visibly observable due to intrinsic luminescence. Keldysh’s theory of nonlinear photoionization is used to model the formation of filaments and values of about 10¹³ W cm⁻² for the laser intensity and 10¹⁹ cm⁻³ for the free electron density are estimated for stable filaments to arise. Laser-induced damage is studied by the generation of a third harmonic from an interface created between a damage site and the surrounding glass matrix. It is found that third harmonic generation occurs only after several thousands of laser shots indicating that damage is not a single-shot phenomena. The ability to photoionize PTR glass without damage by ultrashort laser pulses offers a new approach for fabricating diffractive optical elements in photosensitive glass.     

A study of ultrafast electron diffusion kinetics in ultrashort-pulse laser ablation of metals

Temperature dependence of the electron diffusion in metallic targets, where the electron--electron collision is the dominant process, is investigated with the help of an extended two-temperature model. In sharp contrast to the low electron temperature case, where only the electron---phonon collisions are commonly considered, the electron diffusion process underlying the high electron temperatures evolves dramatically different in both temporal and spatial domains. Calculated results of the ablation yield at different pulse durations are presented for a copper plate impinged by ultrashort laser pulses with energy fluences ranging from 0.1 J/cm² to 10 J/cm². The excellent agreement between the simulation results and the experimental data indicates the significant role of electron--electron collisions in material ablations using intense ultrashort laser pulses.     

Experimental demonstration of concatenated composite pulses robustness to non-static errors

We examine the robustness of composite pulses to non-static classic noise in the NMR facility. Though these pulses are proposed to eliminate static, systematic errors, they are shown to be robust to time-varying noise with high-cut frequency up to near 10% of the Rabi frequency in a recent theoretical work. The CP pulses that are only robust to one kind of error have been implemented in various experiment platforms. In this paper we have compared the performance of reduced CinSK π pulse, which is designed to cancel both the pulse length error and the off resonance error, to that of the primitive π pulse in a hybrid error environment. In order to achieve this target we have simultaneously injected noise to the RF output wave. The filter function formalism is employed to predict the evolution fidelity decay, which shows great consistency with the experiment data. Our work not only validates the superiority of reduced CinSK pulse but also indicates its sensitivity to the initial states, providing practical guidance in the noise suppression domain.     

Second-harmonic generation taking into account dispersion of nonlinear susceptibility

Second-harmonic generation in the field of an ultrashort pulse and the propagation of extremely short pulses in a medium with quadratic nonlinearity are analyzed. Second-harmonic generation is analyzed taking into account the effect of second-and third-order group velocity dispersion and dispersion of nonlinear susceptibility up to the second order. Corrections, whose order of smallness is determined by the parameter (ω_L t _p)^?1, where t _p is the pulse duration and ω_L is the carrier frequency of the pump wave, are obtained. For a large phase mismatch, two new solutions are found that describe the stationary evolution of solitary pump and second-harmonic waves in the regions of both anomalous and normal group velocity dispersions.     

Talbot effect under illumination of double femtosecond laser pulses

The Talbot effect under illumination of double femtosecond laser pulses has been reported. Spectrums of double femtosecond laser pulses with phase differences are quite different from that of one single femtosecond laser pulse. Therefore, the Talbot images of the double femtosecond laser pulses with phase differences are different from that of one single femtosecond laser pulse. Specifically, for the phase difference corresponding to π, the Talbot image shows the largest difference from that of one single pulse. Experimental results are in good agreement with the theoretical analysis. The behaviors of Talbot images under double femtosecond laser pulses illumination cannot be obtained under one femtosecond laser pulse, monochromatic or polychromatic light illumination. Therefore, it is a new interesting optical phenomenon for the Talbot effect which should have potential applications.