Stefano M. Cavaletto

X-ray quantum optics

Quantum optics with X-rays has long been a somewhat exotic activity, but it is now rapidly becoming relevant as precision x-ray optics and novel X-ray light sources, and high-intensity lasers are becoming available. This article gives an overview of the current state of the field and an outlook to future prospects.

Broadband high-resolution X-ray frequency combs

An optical-frequency-comb laser manipulating a dipole response can imprint the comb on an excited transition with a high photon energy. The concept can be implemented using existing X-ray technology.

Resonance fluorescence in ultrafast and intense x-ray free-electron-laser pulses

The spectrum of resonance fluorescence is calculated for a two-level system excited by an intense, ultrashort x-ray pulse made available for instance by free-electron lasers such as the Linac Coherent Light Source. We allow for inner-shell hole decay widths and destruction of the system by further photoionization. This two-level description is employed to model neon cations strongly driven by x rays tuned to the 1s 2p-1 --> 1s-1 2p transition at 848 eV; the x rays induce Rabi oscillations which are so fast that they compete with Ne 1s-hole decay. We predict resonance fluorescence spectra for two different scenarios: first, chaotic pulses based on the self-amplified spontaneous emission principle, like those presently generated at x-ray free-electron-laser facilities and, second, Gaussian pulses which will become available in the foreseeable future with self-seeding techniques. As an example of the exciting opportunities derived from the use of seeding methods, we predict, in spite of above obstacles, the possibility to distinguish at x-ray frequencies a clear signature of Rabi flopping in the spectrum of resonance fluorescence.

Astrophysical line diagnosis requires non-linear dynamical atomic modeling

Line intensities and oscillator strengths for the controversial 3C and 3D astrophysically relevant lines in neonlike Fe(16+) ions are calculated. A large-scale configuration-interaction calculation of oscillator strengths is performed with the inclusion of higher-order electron-correlation effects, suggesting that these contributions cannot explain existing discrepancies between theory and experiment. Then, we investigate nonlinear dynamical effects, showing that, for strong x-ray sources, the modeling of the spectral lines by a peak with an area proportional to the oscillator strength is not sufficient. The dynamical effects give a possible resolution of discrepancies of theory and experiment found by recent measurements, which motivates the use of light-matter interaction models also valid for strong light fields in the analysis and interpretation of astrophysical and laboratory spectra.

Generation of high-frequency combs locked to atomic resonances by quantum phase modulation

A general mechanism for the generation of frequency combs referenced to atomic resonances is put forward. The mechanism is based on the periodic phase control of a quantum systemʼs dipole response. We develop an analytic description of the combʼs spectral structure, depending on both its atomic and phase-control properties. We further suggest an experimental implementation of our scheme, i.e. generating a frequency comb in the soft x-ray spectral region, which can be realized with currently available techniques and radiation sources. The universality of this mechanism allows the generalization of frequency comb technology to arbitrary frequencies, including the hard x-ray regime, by using reference transitions in highly charged ions.

X-ray frequency combs from optically controlled resonance fluorescence

An x-ray pulse-shaping scheme is put forward for imprinting an optical frequency comb onto the radiation emitted on a driven x-ray transition, thus producing an x-ray frequency comb. A four-level system is used to describe the level structure of N ions driven by narrow-bandwidth x rays, an optical auxiliary laser, and an optical frequency comb. By including many-particle enhancement of the emitted resonance fluorescence, a spectrum is predicted consisting of equally spaced narrow lines which are centered on an x-ray transition energy and separated by the same tooth spacing as the driving optical frequency comb. Given a known x-ray reference frequency, our comb could be employed to determine an unknown x-ray frequency. While relying on the quality of the light fields used to drive the ensemble of ions, the model has validity at energies from the 100 eV to the keV range.

Observation and quantification of the quantum dynamics of a strong-field excited multi-level system

The quantum dynamics of a V-type three-level system, whose two resonances are first excited by a weak probe pulse and subsequently modified by another strong one, is studied. The quantum dynamics of the multi-level system is closely related to the absorption spectrum of the transmitted probe pulse and its modification manifests itself as a modulation of the absorption line shape. Applying the dipole-control model, the modulation induced by the second strong pulse to the system’s dynamics is quantified by eight intensity-dependent parameters, describing the self and inter-state contributions. The present study opens the route to control the quantum dynamics of multi-level systems and to quantify the quantum-control process.

Deterministic strong-field quantum control

Strong-field quantum-state control is investigated, taking advantage of the full---amplitude and phase---characterization of the interaction between matter and intense ultrashort pulses via transient-absorption spectroscopy. A sequence of intense delayed pulses is used, whose parameters are tailored to steer the system into a desired quantum state. We show how to experimentally enable this optimization by retrieving all quantum features of the light-matter interaction from observable spectra. This provides a full characterization of the action of strong fields on the atomic system, including the dependence upon possibly unknown pulse properties and atomic structures. Precision and robustness of the scheme are tested, in the presence of surrounding atomic levels influencing the systems dynamics.

X-ray fluorescence spectrum of highly charged Fe ions driven by strong free-electron-laser fields

The influence of nonlinear dynamical effects is analyzed on the observed spectra of controversial 3C and 3D astrophysically relevant x-ray lines in neonlike Fe

Transient-absorption phases with strong probe and pump pulses

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