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Register a new userDistinguishing resonance symmetries with energy-resolved photoion angular distributions from ion-pair formation in O$_2$ following two-photon absorption of a 9.3 eV femtosecond pulse
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We present a combined experimental and theoretical study on the photodissociation dynamics of ion-pair formation in O$_2$ following resonant two-photon absorption of a 9.3 eV femtosecond pulse, where the resulting O$^+$ ions are detected using 3-D momentum imaging. Ion-pair formation states of $^3Sigma^-_g$ and $^3Pi_g$ symmetry are accessed through predissociation of optically dark continuum Rydberg states converging to the B $^2Sigma^-_g$ ionic state, which are resonantly populated via a mixture of both parallel-parallel and parallel-perpendicular two-photon transitions. This mixture is evident in the angular distribution of the dissociation relative to the light polarization, and varies with the kinetic energy release (KER) of the fragmenting ion-pair. The KER-dependent photoion angular distribution reveals the underlying two-photon absorption dynamics involved in the ion-pair production mechanism and indicates the existence of two nearly degenerate continuum resonances possessing different symmetries, which can both decay by coupling to ion-pair states of the same total symmetry through internal conversion.
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We present an experimental study on the photoionization dynamics of non-resonant one-color two-photon single valence ionization of neutral argon atoms. Using 9.3 eV photons produced via high harmonic generation and a 3-D momentum imaging spectrometer, we detect the photoelectrons and ions produced from non-resonant two-photon ionization in coincidence. Photoionization from the $3p$ orbital produces a photoelectron scattering wave function with $p$ and $f$ partial wave components, which interfere and result in a photoelectron angular distribution with peak amplitude perpendicular to the VUV polarization. The comparison between the present results and two previous sets of theoretical calculations [Pan, C. & Starace, A. F. (1991). $textit{Physical Review A}$, 44(1), 324., and Moccia, R., Rahman, N. K., & Rizzo, A. (1983). $textit{Journal of Physics B: Atomic and Molecular Physics}$, 16(15), 2737.] indicates that electron-electron correlation contributes appreciably to the two-photon ionization dynamics.
We experimentally investigated the rotationally resolved polarization characteristics of N$_2^+$ lasing at 391 and 428 nm using a pump-seed scheme. By varying the relative angle between the linear polarizations of the pump and seed, it is found that the polarizations of the P and R branches of 391-nm lasing are counter-rotated. By contrast, both branches of 428-nm lasing remain polarized along the pump. The origin of the puzzled abnormal polarization characteristics is found based on a complete physical model that simultaneously includes the transient photoionization and the subsequent coupling among the electronic, vibrational and rotational quantum states of ions.It suggests that the cascaded resonant Raman processes following ionization create negative coherence between the rotational states of $J$ and $J$+2 in the ionic ground state X$^2Sigma_g^+( u=0)$, which leads to mirror-symmetrical polarization for the P and R branches of 391-nm lasing. Both the experiment and theory indicate that the demonstrated rotational coherence plays an extremely pivotal role in clarifying the gain mechanism of N$_2^+$ lasing and opens up the route toward quantum optics under ultrafast strong fields.
Using a quantum wave packet simulation including the nuclear and electronic degrees of freedom, we investigate the femtosecond and picosecond energy- and angle-resolved photoelectron spectra of the E($^1Sigma_g^+$) electronic state of Li$_2$. We find that the angular distributions of the emitted photoelectrons depend strongly on the pulse duration in the regime of ultrashort laser pulses. This effect is illustrated by the extraction of a time-dependent asymmetry parameter whose variation with pulse duration can be explained by an incoherent average over different ion rotational quantum numbers. We then derive for the variation of the asymmetry parameter a simple analytical formula, which can be used to extract the asymptotic CW asymmetry parameters of individual transitions from measurements performed with ultra-short pulses.
It is well known that energy-time entanglement can enhance two photon absorption (TPA) by simultaneously optimizing the two photon resonance and the coincidence rate of photons at the absorber. However, the precise relation between entanglement and the TPA rate depends on the coherences of intermediate states involved in the transition, making it a rather challenging task to identify universal features of TPA processes. In the present paper, we show that the theory can be simplified greatly by separating the two photon resonance from the temporal dynamics of the intermediate levels. The result is a description of the role of entanglement in the TPA process by a one-dimensional coherence in the Hilbert space defined by the arrival time difference of the two photons. Transformation into the frequency difference basis results in Kramers-Kronig relations for the TPA process, separating off-resonant contributions of virtual levels from resonant contributions. In particular, it can be shown that off-resonant contributions are insensitive to the frequencies of the associated virtual states, indicating that virtual-state spectroscopy of levels above the final two photon excited state is not possible.
The propagation of a superintense laser pulse in an underdense, inhomogeneous plasma has been studied numerically by two-dimensional particle-in-cell simulations on a time scale extending up to several picoseconds. The effects of the ion dynamics following the charge-displacement self-channeling of the laser pulse have been addressed. Radial ion acceleration leads to the ``breaking of the plasma channel walls, causing an inversion of the radial space-charge field and the filamentation of the laser pulse. At later times a number of long-lived, quasi-periodic field structures are observed and their dynamics is characterized with high resolution. Inside the plasma channel, a pattern of electric and magnetic fields resembling both soliton- and vortex-like structures is observed.
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