Stochastic stimulated electronic x-ray Raman spectroscopy

Resonant inelastic x-ray scattering (RIXS) is a well-established tool for studying electronic, nuclear and collective dynamics of excited atoms, molecules and solids. An extension of this powerful method to a time-resolved probe technique at x-ray free electron lasers (XFELs) to ultimately unravel ultrafast chemical and structural changes on a femtosecond time scale is often challenging, due to the small signal rate in conventional implementations at XFELs that rely on the usage of a monochromator set up to select a small frequency band of the broadband, spectrally incoherent XFEL radiation. Here, we suggest an alternative approach, based on stochastic spectroscopy, that uses the full bandwidth of the incoming XFEL pulses. Our proposed method is relying on stimulated resonant inelastic x-ray scattering, where in addition to a pump pulse that resonantly excites the system a probe pulse on a specific electronic inelastic transition is provided, that serves as seed in the stimulated scattering process. The limited spectral coherence of the XFEL radiation defines the energy resolution in this process and stimulated RIXS spectra of high resolution can be obtained by covariance analysis of the transmitted spectra. We present a detailed feasibility study and predict signal strengths for realistic XFEL parameters for the CO molecule resonantly pumped at the O1s-{\pi}* transition. Our theoretical model describes the evolution of the spectral and temporal characteristics of the transmitted x-ray radiation, by solving the equation of motion for the electronic and vibrational degrees of freedom of the system self consistently with the propagation by Maxwell's equations

Stimulated resonant inelastic x-ray scattering with chirped, broadband pulses

We present an approach for initiating and tracing ultra-fast electron dynamics in core-excited atoms, molecules and solids. The approach is based on stimulated resonant inelastic x-ray scattering induced by a single, chirped, broadband XUV/x-ray pulse. A first interaction with this pulse prepares a core-excited state wave packet by resonant core-excitation. A second interaction with the pulse at a later time induces the transition to valence-excited states which is associated with stimulated emission. The preparation of the core-excited wave packet and the transition from the core-excited states to the valence-excited states occur at distinct chirp-dependent times. As a consequence, the stimulated emission carries information about the time evolution of the core-excited state wave packet

Quantum-beat Auger spectroscopy

The concept of nonlinear quantum-beat pump-probe Auger spectroscopy is introduced by discussing a relatively simple four-level model system. We consider a coherent wave packet involving two low-lying states that was prepared by an appropriate pump pulse. This wave packet is subsequently probed by a weak, time-delayed probe pulse with nearly resonant coupling to a core-excited state of the atomic or molecular system. The resonant Auger spectra are then studied as a function of the duration of the probe pulse and the time delay. With a bandwidth of the probe pulse approaching the energy spread of the wave packet, the Auger yields and spectra show quantum beats as a function of pump-probe delay. An analytic theory for the quantum-beat Auger spectroscopy will be presented, which allows for the reconstruction of the wave packet by analyzing the delaydependent Auger spectra. The possibility of extending this method to a more complex manifold of electronic and vibrational energy levels is also discussed.Comment: 13 papees,6 figure

Attosecond dynamics of light-induced resonant hole transfer in high-order-harmonic generation

We present a study of high-order-harmonic generation (HHG) assisted by extreme ultraviolet (XUV) attosecond pulses, which can lead to the excitation of inner-shell electrons and the generation of a second HHG plateau. With the treatment of a one-dimensional model of krypton, based on time-dependent configuration interaction singles (TDCIS) of an effective two-electron system, we show that the XUV-assisted HHG spectrum reveals the duration of the semiclassical electron trajectories. The results are interpreted by the strong-field approximation (SFA) and the importance of the hole transfer during the tunneling process is emphasized. Finally, coherent population transfer between the inner and outer holes with attosecond pulse trains is discussed.Comment: 13 pages, 8 figure

Attosecond photoionization dynamics with stimulated core-valence transitions

We investigate ionization of neon atoms by an isolated attosecond pump pulse in the presence of two coherent extreme ultraviolet or x-ray probe fields. The probe fields are tuned to a core-valence transition in the residual ion and induce spectral shearing of the photoelectron distributions. We show that the photoelectron-ion coincidence signal contains an interference pattern that depends on the temporal structure of the attosecond pump pulse and the stimulated core-valence transition. Many-body perturbation theory is used to compute "atomic response times" for the processes and we find strikingly different behavior for stimulation to the outer-core hole (2p - 2s) and stimulation to the inner-core hole (2p - 1s). The response time of the inner-core transition is found to be comparable to that of state-of-the-art laser-based characterization techniques for attosecond pulses.Comment: 12 pages, 5 figure