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Register a new userExtreme UV generation from molecules in intense Ti:Sapphire light
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We simulate the dynamics of H2+ and HD+ by direct solution of the time-dependent Schroedinger equation for the electronic and nuclear motion for the interaction of intense femtosecond pulses. On these timescales the rotational motion, even for such light molecules, is frozen. Therefore it is a reasonable assumption that the nuclear alignment is fixed during the pulse interaction and that rotation can be neglected. In terms of vibrational relaxation, and since the nuclei are light, vibration will be important over femtosecond timescales. Although homonuclear diatomics are IR-inactive, in an intense field one can create vibrational excitation through continuum coupling. To show the effect of vibration, consider a first approximation in which the nuclei are infinitely massive so they maintain their positions at a fixed bond length of R=2 a.u., throughout the process.
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In our model the electron dynamics are described by a two-state approximation. This might appear a rough approximation since it neglects coupling through excited electronic states and ionization channels. However at high intensity (laser fields equivalent to the Coulomb force) and long wavelength (photon energy much lower than the ionization potential) the dissociation process occurs by adiabatic polarization involving the lowest electronic states. For the experiment in question, with intensities above 10x14 W cm-2 and photon energies of 1.5eV, such an approach is well justified. More contentious is the neglect of rotational heating (that is molecular realignment) during the pulse. However, this process is essentially an internal relaxation and for a 50fs pulse it has a small effect. To calculate the dissociation spectrum, we have applied discretization methods developed for photoionization of molecules4) to solve the quantum equations in a dual configuration and momentum space. Technical details are discussed in the paper by Peng et al.
We show that high-order harmonics generated from molecules by intense laser pulses can be expressed as the product of a returning electron wave packet and the photo-recombination cross section (PRCS) where the electron wave packet can be obtained from simple strong-field approximation (SFA) or from a companion atomic target. Using these wave packets but replacing the PRCS obtained from SFA or from the atomic target by the accurate PRCS from molecules, the resulting HHG spectra are shown to agree well with the benchmark results from direct numerical solution of the time-dependent Schrodinger equation, for the case of H$_2^+$ in laser fields. The result illustrates that these powerful theoretical tools can be used for obtaining high-order harmonic spectra from molecules. More importantly, the results imply that the PRCS extracted from laser-induced HHG spectra can be used for time-resolved dynamic chemical imaging of transient molecules with temporal resolutions down to a few femtoseconds.
We identify that both the dynamic core polarization and dynamic orbital deformation are important in the orientation-dependent high-harmonic generation of CO molecules subjected to intense few cycle laser fields. These polarization dynamics allow for the observation of strong orientation effects and dynamic minimum in the harmonic spectra. The generated attosecond pulses can be greatly affected by these multielectron effects. This work sheds light on future development of dynamic orbital imaging on attosecond time scale.
Diatomic molecules (e.g., O$_2$) in intense laser field exhibit a peculiar suppressed ionization behavior compared to their companion atoms. Several physical models have been proposed to account for this suppression while no consensus has been achieved. In this letter, we aim to clarify the underlying mechanisms behind this molecular ionization suppression. Experimental data recorded at midinfrared laser wavelength and its comparison with that at near-infrared wavelength revealed a peculiar wavelength and intensity dependence of the suppressed ionization of O$_2$ with respect to its companion atom of Xe, while N$_2$ behaves like a structureless atom. It is found that the S-matrix theory calculation can reproduce well the experimental observations and unambiguously identifies the significant role of two-center interference effect in the ionization suppression of O$_2$.
Intense fluctuations of energy dissipation rate in turbulent flows result from the self-amplification of strain rate via a quadratic nonlinearity, with contributions from vorticity (via the vortex stretching mechanism) and the pressure Hessian tensor, which we analyze here using direct numerical simulations of isotropic turbulence in periodic domains of up to $12288^3$ grid points, and Taylor-scale Reynolds numbers in the range $140-1300$. We extract the statistics of various terms involved in amplification of strain and additionally condition them on the magnitude of strain. We find that strain is overall self-amplified by the quadratic nonlinearity, and depleted via vortex stretching; whereas pressure Hessian acts to redistribute strain fluctuations towards the mean-field and thus depleting intense strain. Analyzing the intense fluctuations of strain in terms of its eigenvalues reveals that the net amplification is solely produced by the third eigenvalue, resulting in strong compressive action. In contrast, the self-amplification terms acts to deplete the other two eigenvalues, whereas vortex stretching acts to amplify them, both effects canceling each other almost perfectly. The effect of the pressure Hessian for each eigenvalue is qualitatively similar to that of vortex stretching, but significantly weaker in magnitude. Our results conform with the familiar notion that intense strain is organized in sheet-like structures, which are in the vicinity of, but never overlap with regions of intense vorticity due to fundamental differences in their amplifying mechanisms.
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