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Register a new userNonlinear coherence effects in transient-absorption ion spectroscopy with stochastic extreme-ultraviolet free-electron laser pulses
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We demonstrate time-resolved nonlinear extreme-ultraviolet absorption spectroscopy on multiply charged ions, here applied to the doubly charged neon ion, driven by a phase-locked sequence of two intense free-electron laser pulses. Absorption signatures of resonance lines due to 2$p$--3$d$ bound--bound transitions between the spin-orbit multiplets $^3$P$_{0,1,2}$ and $^3$D$_{1,2,3}$ of the transiently produced doubly charged Ne$^{2+}$ ion are revealed, with time-dependent spectral changes over a time-delay range of $(2.4pm0.3),text{fs}$. Furthermore, we observe 10-meV-scale spectral shifts of these resonances owing to the AC Stark effect. We use a time-dependent quantum model to explain the observations by an enhanced coupling of the ionic quantum states with the partially coherent free-electron-laser radiation when the phase-locked pump and probe pulses precisely overlap in time.
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Phase-shift differences and amplitude ratios of the outgoing $s$ and $d$ continuum wave packets generated by two-photon ionization of helium atoms are determined from the photoelectron angular distributions obtained using velocity map imaging. Helium atoms are ionized with ultrashort extreme-ultraviolet free-electron laser pulses with a photon energy of 20.3, 21.3, 23.0, and 24.3 eV, produced by the SPring-8 Compact SASE Source test accelerator. The measured values of the phase-shift differences are distinct from scattering phase-shift differences when the photon energy is tuned to an excited level or Rydberg manifold. The difference stems from the competition between resonant and non-resonant paths in two-photon ionization by ultrashort pulses. Since the competition can be controlled in principle by the pulse shape, the present results illustrate a new way to tailor the continuum wave packet.
In conditions where the interaction betweeen an atom and a short high-frequency extreme ultraviolet laser pulse is a perturbation, we show that a simple theoretical approach, based on Coulomb-Volkov-type states, can make reliable predictions for ionization. To avoid any additional approximation, we consider here a standard case : the ionization of hydrogen atoms initially in their ground state. For any field parameter, we show that the method provides accurate energy spectra of ejected electrons, including many above threshold ionization peaks, as long as the two following conditions are simultaneously fulfilled : (i) the photon energy is greater than or equal to the ionization potential ; (ii) the ionization process is not saturated. Thus, ionization of atoms or molecules by the high order harmonic laser pulses which are generated at present may be addressed through this Coulomb-Volkov treatment.
The $3p^{4}$ $^{3}$P$_{J}$ - $3p^{3}4p$ $^{3}$P$_{J}$ transition in the sulphur atom is investigated in a precision two-photon excitation scheme under Doppler-free and collision-free circumstances yielding an absolute accuracy of 0.0009 cm$^{-1}$, using a narrowband pulsed laser. This verifies and improves the level separations between amply studied odd parity levels with even parity levels in S I. An improved value for the $^{3}$P$_{2}$ - $^{3}$P$_{1}$ ground state fine structure splitting is determined at $396.0564$ (7) cm$^{-1}$. A $^{34}$S - $^{32}$S atomic isotope shift was measured from combining time-of-flight mass spectrometry with laser spectroscopy.
Probing an atomic resonance without disturbing it is an ubiquitous issue in physics. This problem is critical in high-accuracy spectroscopy or for the next generation of atomic optical clocks. Ultra-high resolution frequency metrology requires sophisticated interrogation schemes and robust protocols handling pulse length errors and residual frequency detuning offsets . This review reports recent progress and perspective in such schemes, using sequences of composite laser-pulses tailored in pulse duration, frequency and phase, inspired by NMR techniques and quantum information processing. After a short presentation of Rabi technique and NMR-like composite pulses allowing efficient compensation of electromagnetic field perturbations to achieve robust population transfers, composite laser-pulses are investigated within Ramseys method of separated oscillating fields in order to generate non-linear compensation of probe-induced frequency shifts. Laser-pulses protocols such as Hyper-Ramsey (HR), Modified Hyper-Ramsey (MHR), Generalized Hyper-Ramsey (GHR) and hybrid schemes are reviewed. These techniques provide excellent protection against both probe induced light-shift perturbations and laser intensity variations. More sophisticated schemes generating synthetic frequency-shifts are presented. They allow to reduce or completely eliminate imperfect correction of probe-induced frequency-shifts even in presence of decoherence due to the laser line-width. Finally, two universal protocols are presented which provide complete elimination of probe-induced frequency shifts in the general case where both decoherence and relaxation dissipation effects are present by using exact analytic expressions for phase-shifts and the clock frequency detuning. These techniques might be applied to atomic, molecular and nuclear frequency metrology, mass spectrometry as well as precision spectroscopy.
Transient absorption is a very powerful observable in attosecond experiments on atoms, molecules and solids and is frequently used in experiments employing phase-locked few-cycle infrared and XUV laser pulses derived from high harmonic generation. We show numerically and analytically that in non-centrosymmetric systems, such as many polyatomic molecules, which-way interference enabled by the lack of parity conservation leads to new spectral absorption features, which directly reveal the laser electric field. The extension of Attosecond Transient Absorption Spectroscopy (ATAS) to such targets hence becomes sensitive to global and local inversion symmetry. We anticipate that ATAS will find new applications in non-centrosymmetric systems, in which the carrier-to-envelope phase of the infrared pulse becomes a relevant parameter and in which the orientation of the sample and the electronic symmetry of the molecule can be addressed.
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