Effect of dressing on high-order harmonic generation in vibrating H2 molecules

Wir entwickeln die Starkfeldnäherung für die Erzeugung hoher Harmonischer in Wasserstoffmolekülen, wobei die Vibrationsbewegung berücksichtigt wird, sowie die laserinduzierte Kopplung zwischen den beiden untersten Born-Oppenheimer-Zuständen im Molekülion, das durch die anfängliche Ionisation des Moleküls erzeugt wird. Wir zeigen, dass die Kopplung bei längeren Laserwellenlängen (≈ 2 μm) wichtig wird und zu einer Reduzierung der Erzeugung von Harmonischen führt, sowie zu einer Änderung des Verhältnisses von Harmonischen in verschiedenen Isotopen. ----------------------------------------------------------------------- We develop the strong-field approximation for high-order harmonic generation in hydrogen molecules, including the vibrational motion and the laser-induced coupling of the lowest two Born-Oppenheimer states in the molecular ion that is created by the initial ionization of the molecule. We show that the field dressing becomes important at long laser wavelengths (≈ 2 μm), leading to an overall reduction of harmonic generation and modifying the ratio of harmonic signals from different isotopes.

Extreme-Ultraviolet-Initated High-Order Harmonic Generation: Driving Inner-Valence Electrons Using Below-Threshold-Energy Extreme-Ultraviolet Light

We propose a novel scheme for resolving the contribution of inner- and outer-valence electrons in XUV-initiated high-harmonic generation in neon. By probing the atom with a low energy (below the 2s ionisation threshold) ultrashort XUV pulse, the 2p electron is steered away from the core, while the 2s electron is enabled to describe recollision trajectories. By selectively suppressing the 2p recollision trajectories we can resolve the contribution of the 2s electron to the high-harmonic spectrum. We apply the classical trajectory model to account for the contribution of the 2s electron, which allows for an intuitive understanding of the process.

Comparison of natural and forced amplification regimes in plasma-based soft-x-ray lasers seeded by high-order harmonic

The amplification of high-order harmonics (HOH) in a plasma-based amplifier is a multiscale, temporal phenomenon that couples plasma hydrodynamics, atomic processes, and HOH electromagnetic fields. We use a one-dimensional, time-dependent Maxwell-Bloch code to compare the natural amplification regime and another regime where plasma polarization is constantly forced by the HOH. In this regime, a 10-MW (i.e., 100 times higher than current seeded soft x-ray laser power), 1.5-μJ, 140-fs pulse free from the parasitic temporal structures appearing on the natural amplification regime can be obtained.

Electron-Nuclear Correlation in Laser-Driven Diatomic Molecules

The interaction of short intense laser pulses with atoms/molecules produces a multitude of highly nonlinear processes requiring a non-perturbative treatment. Detailed study of these highly nonlinear processes by numerically solving the time-dependent Schrodinger equation becomes a daunting task when the number of degrees of freedom is large. Also the coupling between the electronic and nuclear degrees of freedom further aggravates the computational problems. In the present work we show that the time-dependent Hartree (TDH) approximation, which neglects the correlation effects, gives unreliable description of the system dynamics both in the absence and presence of an external field. A theoretical framework is required that treats the electrons and nuclei on equal footing and fully quantum mechanically. To address this issue we discuss two approaches, namely the multicomponent density functional theory (MCDFT) and the multiconfiguration time-dependent Hartree (MCTDH) method, that go beyond the TDH approximation and describe the correlated electron-nuclear dynamics accurately. In the MCDFT framework, where the time-dependent electronic and nuclear densities are the basic variables, we discuss an algorithm to calculate the exact Kohn-Sham (KS) potentials for small model systems. By simulating the photodissociation process in a model hydrogen molecular ion, we show that the exact KS potentials contain all the many-body effects and give an insight into the system dynamics. In the MCTDH approach, the wave function is expanded as a sum of products of single-particle functions (SPFs). The MCTDH method is able to describe the electron-nuclear correlation effects as the SPFs and the expansion coefficients evolve in time and give an accurate description of the system dynamics. We show that the MCTDH method is suitable to study a variety of processes such as the fragmentation of molecules, high-order harmonic generation, the two-center interference effect, and the lochfrass effect. We discuss these phenomena in a model hydrogen molecular ion and a model hydrogen molecule. Inclusion of absorbing boundaries in the mean-field approximation and its consequences are discussed using the model hydrogen molecular ion. To this end, two types of calculations are considered: (i) a variational approach with a complex absorbing potential included in the full many-particle Hamiltonian and (ii) an approach in the spirit of time-dependent density functional theory (TDDFT), including complex absorbing potentials in the single-particle equations. It is elucidated that for small grids the TDDFT approach is superior to the variational approach.

Scalable high-order UWB pulse generation employing an FBG-based photonic superstructure

In this letter, we propose and experimentally demonstrate a compact, flexible, and scalable ultrawideband (UWB) generator based on the merge of phase-to-intensity conversion and pulse shaping employing an fiber Bragg Grating-based superstructure. Our approach offers the capacity for generating high-order UWB pulses by means of the combination of various low-order derivatives. Moreover, the scheme permits the implementation of binary and multilevel modulation formats. Experimental measurements of the generated UWB pulses, in both time and frequency domain, are presented revealing efficiency and a proper fit in terms of Federal Communications Commission settled standards.

Fractional order of poling period for broadly tunable second harmonic generation

We demonstrate the possibility to use a fractional order of poling period of nonlinear crystal waveguides for tunable second harmonic generation. This approach allows one to extend wavelength coverage in the visible spectral range by frequency doubling in a single crystal waveguide.

Femtosecond third-harmonic generation in a glass ceramic containing sodium niobate nanocrystals

The third-harmonic optical susceptibility, chi((3))(3 omega; omega, omega, omega) of a silicate glass ceramic containing sodium niobate nanocrystals was measured for incident broadband light with central frequency omega corresponding to 1900nm. Absolute values of |chi((3))| and the dispersion of the refractive index from 600 to 1900nm were measured using the spectrally resolved femtosecond Maker fringes technique. The experiments show that |chi((3))| is 1 order of magnitude larger than silica, and it grows by similar to 50% when the volume fraction occupied by the nanocrystals increases up to 40%. (C) 2011 Optical Society of America

Hyperglycemia-induced abnormalities in rat and human corneas: the potential of second harmonic generation microscopy.

BACKGROUND: Second Harmonic Generation (SHG) microscopy recently appeared as an efficient optical imaging technique to probe unstained collagen-rich tissues like cornea. Moreover, corneal remodeling occurs in many diseases and precise characterization requires overcoming the limitations of conventional techniques. In this work, we focus on diabetes, which affects hundreds of million people worldwide and most often leads to diabetic retinopathy, with no early diagnostic tool. This study then aims to establish the potential of SHG microscopy for in situ detection and characterization of hyperglycemia-induced abnormalities in the Descemet's membrane, in the posterior cornea. METHODOLOGY/PRINCIPAL FINDINGS: We studied corneas from age-matched control and Goto-Kakizaki rats, a spontaneous model of type 2 diabetes, and corneas from human donors with type 2 diabetes and without any diabetes. SHG imaging was compared to confocal microscopy, to histology characterization using conventional staining and transmitted light microscopy and to transmission electron microscopy. SHG imaging revealed collagen deposits in the Descemet's membrane of unstained corneas in a unique way compared to these gold standard techniques in ophthalmology. It provided background-free images of the three-dimensional interwoven distribution of the collagen deposits, with improved contrast compared to confocal microscopy. It also provided structural capability in intact corneas because of its high specificity to fibrillar collagen, with substantially larger field of view than transmission electron microscopy. Moreover, in vivo SHG imaging was demonstrated in Goto-Kakizaki rats. CONCLUSIONS/SIGNIFICANCE: Our study shows unambiguously the high potential of SHG microscopy for three-dimensional characterization of structural abnormalities in unstained corneas. Furthermore, our demonstration of in vivo SHG imaging opens the way to long-term dynamical studies. This method should be easily generalized to other structural remodeling of the cornea and SHG microscopy should prove to be invaluable for in vivo corneal pathological studies.

Generation of attosecond pulses in molecular nitrogen

We have generated attosecond pulse trains in an ensemble of randomly aligned nitrogen molecules. Measurements of the high-order harmonic relative phases and amplitudes allow us to reconstruct the temporal profile of the attosecond pulses. We show that in the considered spectral range, the latter is very similar to the pulse train generated in argon under the same conditions. We discuss the possible influence of the molecular structure in the generation process, and how it can induce subtle differences on the relative phases.

Measurement of higher-order harmonic azimuthal anisotropy in PbPb collisions at root s(NN)=2.76 TeV

Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)

Temporal and spatio-temporal regimes of generation of Raman fibre lasers

Temporal dynamics of Raman fibre lasers tend to have very complex nature, owing to great cavity lengths and high nonlinearity, being stochastic on short time scales and quasi-continuous on longer time scales. Generally fibre laser intensity dynamics is represented by one-dimensional time-series, which in case of quasi-continuous wave generation in Raman fibre lasers gives little insight into the processes underlying the operation of a laser. New methods of analysis and data representation could help to uncover the underlying physical processes, understand the dynamics or improve the performance of the system. Using intrinsic periodicity of laser radiation, one dimensional intensity time series of a Raman fibre laser was analysed over fast and slow variation time. This allowed to experimentally observe various spatio-temporal regimes of generation, such as laminar, turbulent, partial mode-lock, as well as transitions between them and identify the mechanisms responsible for the transitions. Great cavity length and high nonlinearity also make it difficult to achieve stable high repetition rate mode-locking in Raman fibre lasers. Using Faraday parametric instability in extremely simple linear cavity experimental configuration, a very high order harmonic mode-locking was achieved in ò.ò kmlong Raman fibre laser. The maximum achieved pulse repetition rate was 12 GHz, with 7.3 ps long Gaussian shaped pulses. There is a new type of random lasers – random distributed feedback Raman fibre laser, which temporal properties cannot be controlled by conventionalmode-locking or Q-switch techniques and mechanisms. By adjusting the pump configuration, a very stable pulsed operation of random distributed feedback Raman fibre laser was achieved. Pulse duration varied in the range from 50 to 200 μs depending on the pump power and the cavity length. Pulse repetition rate scaling on the parameters of the system was experimentally identified.

Extreme Harmonic Generation In Electrically Driven Spin Resonance.

We report the observation of multiple harmonic generation in electric dipole spin resonance in an InAs nanowire double quantum dot. The harmonics display a remarkable detuning dependence: near the interdot charge transition as many as eight harmonics are observed, while at large detunings we only observe the fundamental spin resonance condition. The detuning dependence indicates that the observed harmonics may be due to Landau-Zener transition dynamics at anticrossings in the energy level spectrum.

Optical second harmonic generation in the centrosymmetric magnetic semiconductors EuTe and EuSe

The magnetic europium chalcogenide semiconductors EuTe and EuSe are investigated by the spectroscopy of second harmonic generation (SHG) in the vicinity of the optical band gap formed by transitions involving the 4f and 5d electronic orbitals of the magnetic Eu(2+) ions. In these materials with centrosymmetric crystal lattice the electric-dipole SHG process is symmetry forbidden so that no signal is observed in zero magnetic field. Signal appears, however, in applied magnetic field with the SHG intensity being proportional to the square of magnetization. The magnetic field and temperature dependencies of the induced SHG allow us to introduce a type of nonlinear optical susceptibility determined by the magnetic-dipole contribution in combination with a spontaneous or induced magnetization. The experimental results can be described qualitatively by a phenomenological model based on a symmetry analysis and are in good quantitative agreement with microscopic model calculations accounting for details of the electronic energy and spin structure.

Theory of near-gap second harmonic generation in centrosymmetric magnetic semiconductors: Europium chalcogenides

Second harmonic generation is strictly forbidden in centrosymmetric materials, within the electric dipole approximation. Recently, it was found that the centrosymmetric magnetic semiconductors EuTe and EuSe can generate near-gap second harmonics, if the system is submitted to an external magnetic field. Here, a theoretical model is presented, which well describes the observed phenomena. The model shows that second harmonic generation becomes efficient when the magnetic dipole oscillations between the band-edge excited states of the system, induced by the excitation light, enter the in-phase regime, which can be achieved by applying a magnetic field to the material.

Spin-Induced Optical Second Harmonic Generation in the Centrosymmetric Magnetic Semiconductors EuTe and EuSe

Spectroscopy of the centrosymmetric magnetic semiconductors EuTe and EuSe reveals spin-induced optical second harmonic generation (SHG) in the band gap vicinity at 2.1-2.4 eV. The magnetic field and temperature dependence demonstrates that the SHG arises from the bulk of the materials due to a novel type of nonlinear optical susceptibility caused by the magnetic dipole contribution combined with spontaneous or induced magnetization. This spin-induced susceptibility opens access to a wide class of centrosymmetric systems by harmonics generation spectroscopy.