Core-Excited Molecules by Resonant Intense X-Ray Pulses Involving Electron-Rotation Coupling

It has been reported that electron-rotation coupling plays a significant role in diatomic nuclear dynamics induced by intense VUV pulses [Phys. Rev. A 102(2020) 033114;Phys. Rev. Res. 2(2020) 043348]. As a further step, we present here investigations of the electron-rotation coupling effect in the presence of Auger decay channel for core-excited molecules, based on theoretical modeling of the total electron yield(TEY), resonant Auger scattering(RAS) and x-ray absorption spectra(XAS) for two showcases of CO and CH^(+) molecules excited by resonant intense x-ray pulses. The Wigner D-functions and the universal transition dipole operators are introduced to include the electron-rotation coupling for the core-excitation process. It is shown that with the pulse intensity up to 10^(16) W/cm^(2), no sufficient influence of the electron-rotation coupling on the TEY and RAS spectra can be observed. This can be explained by a suppression of the induced electron-rotation dynamics due to the fast Auger decay channel, which does not allow for effective Rabi cycling even at extreme field intensities,contrary to transitions in optical or VUV range. For the case of XAS, however, relative errors of about 10% and 30% are observed for the case of CO and CH^(+), respectively, when the electron-rotation coupling is neglected.It is concluded that conventional treatment of the photoexcitation, neglecting the electron-rotation coupling,can be safely and efficiently employed to study dynamics at the x-ray transitions by means of electron emission spectroscopy, yet the approximation breaks down for nonlinear processes as stimulated emission, especially for systems with light atoms.

Charge Resonance Enhanced Multiple Ionization of H2O Molecules in Intense Laser Fields

We perform a kinetically complete measurement on the fragmentation of Coulomb explosion of 1-120 molecules in intense few-cycle linearly and circularly polarized laser fields. Both the fragmentations of 1t203＋ and H204＋ reveal the concerted pathway of dissociation. The length of the OH bond prior to the Coulomb explosion of both molecular ions is sensitive to the laser pulse duration and laser intensity. However, the bending angle of H-O-H is less sensitive to the pulse duration and laser intensity. We introduce the mechanism of charge resonance enhanced double ionization to elucidate the triple （or quadruple） dissociative ionization dynamics of H20, in which two electrons are non-adiabatically localized at the protons of the precursor ion H2O^＋ （or H2O^2＋） and are released simultaneously due to the over barrier ionization in the combined laser field and molecular ionic potential. Such charge resonance enhanced multiple ionization is not suppressed in few-cycle laser fields and elliptically polarized laser fields.

Collisional broadening of some 2~1Δ_g←B^1Π_u lines in Na_2 molecules by optical-optical double resonance spectroscopy

Using the optical-optical double resonance （OODR） technique, we have studied the collisional broadening of some 21△g←B1πu lines in Na2 molecules. A single line Ar＋ laser is used to pump the sodium dimers from thermally populated ground state X^1∑^＋g level to the intermediate B1πu state. Then, a single-mode diode laser is used to probe the doubly excited 21△g state. The broadening rate coefficient is determined from the slope of the total linewidth versus Ne density curve. We obtain the average value kbr = （1.1 ± 0.5）×10^-8 cm^3 8^-1. The collisional excitation transfer between rotational levels of the B1πu state （i.e.,B1πu（2,83/84） ←B1Ⅱu （2,82）） is also investigated. The rates can be determined from the relative intensities of the main peak and satellite lines, combined with a rate equation model. The rates of 1.25 × 106 and 1.07 × 106 s^-1 are obtained, respectively.