arXiv subjects

Nina Rohringer

Publications and source records attributed to Nina Rohringer.

30 records · Page 2Linked to original sources

arXiv2018

Introduction to the theory of x-ray matter interaction

This contribution summarises the theoretical basics for the theory of x-ray matter interaction and is based on a quantised description of the electromagnetic field. In view of a formally transparent presentation, we adopt the approach of second quantisation for the electronic degrees of freedom. We start out from the minimal coupling Hamiltonian that in principle contains all levels of electron correlation and treat the x-ray matter interaction in lowest order perturbation theory. We give the explicit derivation of the photoionisation (x-ray absorption) cross section and the doubly differential cross sections for elastic and inelastic Thomson scattering, as well as resonant inelastic x-ray scattering. A connection to relevant experimental techniques is attempted. At some instances, the electronic Hamiltonian is approximated by a mean-field Hamiltonian, in order to facilitate the interpretation of the results and connect experimental observables with the underlying fundamental quantities of the quantum system under study.

quant-ph↗

arXiv2018

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.

physics.atom-ph↗

arXiv2018

Quantum theory of superfluorescence based on two-point correlation functions

Irradiation of a medium by short intense pulses from x-ray / XUV free electron lasers can result in saturated photoionization of inner electronic shells. As a result an inversion of populations between core levels appears. The resulting fluorescent radiation can be amplified during its propagation through the inverted medium and results in intense, quasi transform-limited radiation bursts. While the optical counterpart of this phenomena, known as superfluorescence, was intensively investigated, a generalized treatment is needed in the x-ray / XUV domain, where the dynamics of pumping and evolution due to fast decay processes play a crucial role. To provide a general theoretical approach, we start from the fundamental, quantized minimal coupling Hamiltonian of light-matter interaction and after a series of approximations arrive at a closed system of equations for the two-point correlation function of atomic coherences and the two-time correlation function of the emitted field. The obtained formalism enables us to investigate collective spontaneous emission in various regimes. It is extended consistently to include incoherent processes that are relevant in the x-ray / XUV domain. These processes are introduced into the formalism by corresponding Lindblad superoperators. The connection to other approaches is discussed and numerical examples related to recent experiments are presented.

quant-ph↗

arXiv2017

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.

physics.atom-ph↗

arXiv2016

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.

physics.atom-ph↗

arXiv2015

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-π* 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.

physics.chem-ph↗

arXiv2015

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.

physics.atom-ph↗

arXiv2015

All-optical control of superradiance and matter waves using a dispersive cavity

Cavity quantum electrodynamics (CQED) plays an elegant role of studying strong coupling between light and matter. However, a non-mechanical, direct and dynamical control of the used mirrors is still unavailable. Here we theoretically investigate a novel type of dynamically controllable cavity composed of two atomic mirrors. Based on the electromagnetically induced transparency (EIT), the reflectance of atomic mirror is highly controllable through its dispersive properties by varying the intensity of applied coupling fields or the optical depth of atomic media. To demonstrate the uniqueness of the present cavity, we further show the possibility of manipulating vacuum-induced diffraction of a binary Bose-Einstein condensate (BEC) when loading it into a dispersive cavity and experiencing superradiant scatterings. Our results may provide a novel all-optical element for atom optics and shine new light on controlling light-matter interaction.

cond-mat.quant-gas↗

arXiv2015

Theoretical Study of Molecular Electronic and Rotational Coherences by High-Harmonic Generation

The detection of electron motion and electronic wavepacket dynamics is one of the core goals of attosecond science. Recently, choosing the nitric oxide (NO) molecule as an example, we have introduced and demonstrated a new experimental approach to measure coupled valence electronic and rotational wavepackets using high-harmonic generation (HHG) spectroscopy [Kraus et al., Phys. Rev. Lett. 111, 243005 (2013)]. A short outline of the theory to describe the combination of the pump and HHG probe process was published together with an extensive discussion of experimental results [Baykusheva et al., Faraday Discuss 171, 113 (2014)]. The comparison of theory and experiment showed good agreement on a quantitative level. Here, we present the generalized theory in detail, which is based on a generalized density matrix approach that describes the pump process and the subsequent probing of the wavepackets by a semiclassical quantitative rescattering approach. An in-depth analysis of the different Raman scattering contributions to the creation of the coupled rotational and electronic spin-orbit wavepackets is made. We present results for parallel and perpendicular linear polarizations of the pump and probe laser pulses. Furthermore, an analysis of the combined rotational-electronic density matrix in terms of irreducible components is presented, that facilitates interpretation of the results.

physics.atm-clus↗

arXiv2013

Photoemission spectroscopy with high-intensity short-wavelength lasers

We theoretically study the process of photoelectron emission of the Helium atom by a high-intensity short-wavelength laser at a resonance condition of the residual singly charged ion. Photoionization followed by strong resonance coupling in the ion leads to a change in the photoelectron spectrum due to Rabi oscillations in the residual ion. Similarly to resonance fluorescence at high laser intensity, the photoelectron spectrum at high intensities evolves into a multi-peaked structure. The number of peaks in the photoelectron spectrum is related to the number of Rabi cycles following the photoionization process. Moreover, the strong laser-induced coupling to nonresonant states of the residual ion have an imprint on the photoelectron spectrum, leading to additional, isolated peaks at the lower or higher energy sides. The effect should be observable at current seeded XUV free-electron lasers and persists after volume integration in a realistic experimental geometry.

physics.atom-ph↗

arXiv2008

Using strong electromagnetic fields to control x-ray processes

Exploration of a new ultrafast-ultrasmall frontier in atomic and molecular physics has begun. Not only is is possible to control outer-shell electron dynamics with intense ultrafast optical lasers, but now control of inner-shell processes has become possible by combining intense infrared/optical lasers with tunable sources of x-ray radiation. This marriage of strong-field laser and x-ray physics has led to the discovery of methods to control reversibly resonant x-ray absorption in atoms and molecules on ultrafast timescales. Using a strong optical dressing field, resonant x-ray absorption in atoms can be markedly suppressed, yielding an example of electromagnetically induced transparency for x rays. Resonant x-ray absorption can also be controlled in molecules using strong non-resonant, polarized laser fields to align the framework of a molecule, and therefore its unoccupied molecular orbitals to which resonant absorption occurs. At higher laser intensities, ultrafast field ionization produces an irreversible change in x-ray absorption. Finally, the advent of x-ray free electron lasers enables first exploration of non-linear x-ray processes.

physics.atom-ph↗

arXiv2005

Calculating state-to-state transition probabilities within TDDFT

The determination of the elements of the S-matrix within the framework of time-dependent density-functional theory (TDDFT) has remained a widely open question. We explore two different methods to calculate state-to-state transition probabilities. The first method closely follows the extraction of the S-matrix from the time-dependent Hartree-Fock approximation. This method suffers from cross-channel correlations resulting in oscillating transition probabilities in the asymptotic channels. An alternative method is proposed which corresponds to an implicit functional in the time-dependent density. It gives rise to stable and accurate transition probabilities. An exactly solvable two-electron system serves as benchmark for a quantitative test.

quant-ph↗