We investigate the capability of attosecond transient absorption spectroscopy to characterize the dynamics of inner-shell-excited systems. In the transient absorption spectroscopy setup considered, wave packets are prepared by an attosecond XUV pulse and probed by a femtosecond NIR pulse. By using this, we study coherent electron dynamics in core-excited xenon atoms. In particular, we clarify which aspects of the dynamics can be revealed when the wave packets are probed using an NIR pulse and analyze why the inner-shell hole dynamics is more difficult to probe than the dynamics of the excited electron. We perform a theoretical analysis of the transient absorption signal as a function of the time delay between the XUV pump and NIR probe pulses, treating the excitation pulse perturbatively and the probe pulse nonperturbatively. We also demonstrate that an additional NIR dressing field can dramatically influence the transient absorption spectrum. Our theoretical predictions are compared with experimental results, suggesting that a precise characterization of the NIR pulse is necessary for a qualitative and quantitative comparison.
High-order harmonic generation (HHG) is investigated theoretically in the over-the-barrier ionization regime revealing the strong signature of interference between two separately ionized and separately propagating free wave packets of a single electron. The interference leads to the emission of coherent light at a photon energy corresponding to the kinetic-energy difference of the two recolliding electron quantum paths, thus complementary to the well-known classical three-step picture of HHG. As will be shown by time-frequency analysis of the emitted radiation, the process entirely dominates the coherent HHG emission after the atomic ground state has been depleted by a strong field. Moreover, it can be isolated from the continuum--bound harmonics via phase matching.
We propose and study the manipulation of the macroscopic transient absorption of an ensemble of open two-level systems via temporal engineering. The key idea is to impose an ultrashort temporal gate on the polarization decay of the system by transient absorption spectroscopy, thus confining its free evolution and the natural reshaping of the excitation pulse. The numerical and analytical results demonstrate that even at moderate optical depths, the resonant absorption of light can be reduced or significantly enhanced by more than 5 orders of magnitude relative to that without laser manipulation. The achievement of the quasicomplete extinction of light at the resonant frequency, here referred to as resonant perfect absorption, arises from the full destructive interference between the excitation pulse and its subpulses developed and tailored during propagation, and is revealed to be connected with the formation of zero-area pulses in the time domain.
By using a two-color strong/weak-field combination of carrier-envelope-phase(CEP) stable laser fields interacting with an atom, we control the process of high-harmonic generation to create isolated and double attosecond pulses. Using this multi-parameter control approach, we can manipulate several properties of the attosecond double pulses independently, such as their intensity ratio and relative phase, being important prerequisites for interferometry and attosecond quantum control experiments. Both experiments and simulations will be presented.
Abstract We study the interaction of intense extreme ultraviolet (XUV) light with the 2s2p doubly excited state in helium. In addition to previously understood energy-level and phase shifts, high XUV intensities may lead to other absorption-line-shape distortions. Here, we report on experimental transient-absorption spectroscopy results on the 2s2p line-width modification in helium in intense stochastic XUV fields. A few-level-model simulation is realized to investigate the origins of this effect. We find that the line-shape broadening is connected to the strong coupling of the ground state to the 2s2p doubly excited state which is embedded in the ionization continuum. As the broadening takes place for intensities lower than for other strong-coupling processes, e.g. observed asymmetry changes of the absorption profile, this signature can be identified already in an intermediate intensity regime. These findings are in general relevant for resonant inner-shell transitions in nonlinear experiments with XUV and x-ray photon energies at high intensity.
A setup for an all-XUV transient absorption spectroscopy at free-electron lasers, was developed and employed to explore XUV-excited dynamics and XUV-driven nonlinear phenomena.
Abstract The Fano absorption line shape of an autoionizing state encodes information on its internal atomic structure and dynamics. When driven near-resonantly with intense extreme ultraviolet (XUV) electric fields, the absorption profile can be deliberately modified, including observable changes of both the line-shape asymmetry and strength of the resonance, revealing information on the underlying dynamics of the system in response to such external driving. We report on the influence of the XUV pulse parameters at high intensity that can be achieved with a free-electron laser (FEL) with statistically broadened spectra based on self-amplified spontaneous emission (SASE). More specifically, the impact of the FEL pulse duration is studied for the example of the doubly excited 2s2p resonance in helium, where line-shape modifications have been measured with XUV transient absorption spectroscopy in Fraunhofer-type transmission geometry. A computational few-level-model provides insight into the impact of different average pulse durations of the stochastic FEL pulses. These findings are supported by measurements performed at the Free-Electron Laser in Hamburg (FLASH) and provide further insight into XUV strong-coupling dynamics of resonant transitions driven by intense high-frequency FEL sources.
Objective: Hypertension management is directed by cuff blood pressure (BP), but this may be inaccurate, potentially influencing cardiovascular disease (CVD) events and health costs. This study aimed to determine the impact on CVD events and related costs of the differences between cuff and invasive SBP. Methods: Microsimulations based on Markov modelling over one year were used to determine the differences in the number of CVD events (myocardial infarction or coronary death, stroke, atrial fibrillation or heart failure) predicted by Framingham risk and total CVD health costs based on cuff SBP compared with invasive (aortic) SBP. Modelling was based on international consortium data from 1678 participants undergoing cardiac catheterization and 30 separate studies. Cuff underestimation and overestimation were defined as cuff SBP less than invasive SBP and cuff SBP greater than invasive SBP, respectively. Results: The proportion of people with cuff SBP underestimation versus overestimation progressively increased as SBP increased. This reached a maximum ratio of 16 : 1 in people with hypertension grades II and III. Both the number of CVD events missed (predominantly stroke, coronary death and myocardial infarction) and associated health costs increased stepwise across levels of SBP control, as cuff SBP underestimation increased. The maximum number of CVD events potentially missed (11.8/1000 patients) and highest costs ($241 300 USD/1000 patients) were seen in people with hypertension grades II and III and with at least 15 mmHg of cuff SBP underestimation. Conclusion: Cuff SBP underestimation can result in potentially preventable CVD events being missed and major increases in health costs. These issues could be remedied with improved cuff SBP accuracy.
Interference effects arising during the highly nonlinear interaction of intense laser pulses with matter are presented for applications in attosecond spectroscopy and interferometry. In the first part we theoretically describe an approach to excite and measure bound electron wavepackets where temporal interference in the photoelectron momentum spectrum reveals the complete energy-level structure of an atom. In the second part we analyse and discuss experimentally observed interference patterns of few adjacent attosecond pulses generated in neon gas that can be controlled by varying experimental parameters such as carrier-envelope phase (CEP) or pressure.
