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Agostino Marinelli

Publications and source records attributed to Agostino Marinelli.

34 records · Page 2Linked to original sources

Efficient prediction of attosecond two-colour pulses from an X-ray free-electron laser with machine learning

X-ray free-electron lasers are sources of coherent, high-intensity X-rays with numerous applications in ultra-fast measurements and dynamic structural imaging. Due to the stochastic nature of the self-amplified spontaneous emission process and the difficulty in controlling injection of electrons, output pulses exhibit significant noise and limited temporal coherence. Standard measurement techniques used for characterizing two-coloured X-ray pulses are challenging, as they are either invasive or diagnostically expensive. In this work, we employ machine learning methods such as neural networks and decision trees to predict the central photon energies of pairs of attosecond fundamental and second harmonic pulses using parameters that are easily recorded at the high-repetition rate of a single shot. Using real experimental data, we apply a detailed feature analysis on the input parameters while optimizing the training time of the machine learning methods. Our predictive models are able to make predictions of central photon energy for one of the pulses without measuring the other pulse, thereby leveraging the use of the spectrometer without having to extend its detection window. We anticipate applications in X-ray spectroscopy using XFELs, such as in time-resolved X-ray absorption and photoemission spectroscopy, where improved measurement of input spectra will lead to better experimental outcomes.

physics.acc-ph↗

Attosecond Delays in X-ray Molecular Ionization

The photoelectric effect is not truly instantaneous, but exhibits attosecond delays that can reveal complex molecular dynamics. Sub-femtosecond duration light pulses provide the requisite tools to resolve the dynamics of photoionization. Accordingly, the past decade has produced a large volume of work on photoionization delays following single photon absorption of an extreme ultraviolet (XUV) photon. However, the measurement of time-resolved core-level photoionization remained out of reach. The required x-ray photon energies needed for core-level photoionization were not available with attosecond tabletop sources. We have now measured the x-ray photoemission delay of core-level electrons, and here report unexpectedly large delays, ranging up to 700 attoseconds in NO near the oxygen K-shell threshold. These measurements exploit attosecond soft x-ray pulses from a free-electron laser (XFEL) to scan across the entire region near the K-shell threshold. Furthermore, we find the delay spectrum is richly modulated, suggesting several contributions including transient trapping of the photoelectron due to shape resonances, collisions with the Auger-Meitner electron that is emitted in the rapid non-radiative relaxation of the molecule, and multi-electron scattering effects. The results demonstrate how x-ray attosecond experiments, supported by comprehensive theoretical modelling, can unravel the complex correlated dynamics of core-level photoionization.

physics.atom-ph↗

Experimental Demonstration of Attosecond Pump-Probe Spectroscopy with an X-ray Free-Electron Laser

Pump-probe experiments with sub-femtosecond resolution are the key to understanding electronic dynamics in quantum systems. Here we demonstrate the generation and control of sub-femtosecond pulse pairs from a two-colour X-ray free-electron laser (XFEL). By measuring the delay between the two pulses with an angular streaking diagnostic, we characterise the group velocity of the XFEL and demonstrate control of the pulse delay down to 270 as. We demonstrate the application of this technique to a pump-probe measurement in core-excited para-aminophenol. These results demonstrate the ability to perform pump-probe experiments with sub-femtosecond resolution and atomic site specificity.

physics.acc-ph↗

Wavelength scaling and multi-color operation of a plasma driven attosecond X-ray source via harmonic generation

The generation of high power coherent soft X-ray pulses of sub-100 as duration and 10 nm wavelength using beams from a GeV energy plasma wakefield accelerator has been recently investigated in Ref. [arXiv:2011.07163]. As a future upgrade to this concept, this contribution investigates scaling to shorter X-ray wavelengths by cascading undulators tuned to higher harmonics of the fundamental. We present two simulation studies for plasma-driven attosecond harmonic generation schemes with final photon wavelengths of 2 nm and 0.40 nm. We demonstrate in these schemes that using undulators with retuned fundamental frequencies can produce GW-scale pulses of sub-nm radiation with tens of attosecond-scale pulse lengths, an order of magnitude shorter than current state-of-the-art attosecond XFELs. This multi-pulse multi-color operation will be broadly applicable to attosecond pump-probe experiments.

physics.acc-ph↗

Nonlinearly Shaped Pulses in Photoinjectors and Free-Electron Lasers

Photoinjectors and Free Electron Lasers (FEL) are amongst the most advanced systems in accelerator physics and have consistently pushed the boundaries of emittance and x-ray peak power. In this paper, laser shaping at the cathode is proposed to further lower the emittance and reduce electron beam tails, which would result in brighter x-ray production. Using dispersion controlled nonlinear shaping (DCNS), laser pulses and beam dynamics were simulated in LCLS-II. The photoinjector emittance was optimized and the resulting e-beam profiles were then simulated and optimized in the linac. Finally, the expected FEL performance is estimated and compared to the current technology: Gaussian laser pulses on the cathode. The e-beams produced by DCNS pulses show a potential for 35% increase in x-ray power per pulse during SASE when compared to the standard Gaussian laser pulses.

physics.acc-ph↗

Phase retrieval from angular streaking of XUV atomic ionization

We demonstrate an accurate phase retrieval of XUV atomic ionization by streaking the photoelectron in a circularly polarized IR laser field. The streaking phase can then be converted to the atomic time delay containing the Wigner and continuum-continuum components. Our demonstration is based on a numerical solution of the time-dependent Schrödinger equation. We test this technique using the hydrogen atom ionized by an isolated attosecond XUV pulse across a wide range of photon energies. In parallel, we run a series of RABBITT simulations and demonstrate equivalence of the phase and timing information provided by the two methods. This validates the proposed technique and makes it a useful tool that can be applied to a broad range of atomic and molecular targets exposed to XUV radiation from novel free-electron laser sources.

physics.atom-ph↗

Enhanced ultrafast X-ray diffraction by transient resonances

Diffraction-before-destruction imaging with single ultrashort X-ray pulses has the potential to visualise non-equilibrium processes, such as chemical reactions, at the nanoscale with sub-femtosecond resolution in the native environment without the need of crystallization. Here, a nanospecimen partially diffracts a single X-ray flash before sample damage occurs. The structural information of the sample can be reconstructed from the coherent X-ray interference image. State-of-art spatial resolution of such snapshots from individual heavy element nanoparticles is limited to a few nanometers. Further improvement of spatial resolution requires higher image brightness which is ultimately limited by bleaching effects of the sample. We compared snapshots from individual 100 nm Xe nanoparticles as a function of the X-ray pulse duration and incoming X-ray intensity in the vicinity of the Xe M-shell resonance. Surprisingly, images recorded with few femtosecond and sub-femtosecond pulses are up to 10 times brighter than the static linear model predicts. Our Monte-Carlo simulation and statistical analysis of the entire data set confirms these findings and attributes the effect to transient resonances. Our simulation suggests that ultrafast form factor changes during the exposure can increase the brightness of X-ray images by several orders of magnitude. Our study guides the way towards imaging with unprecedented combination of spatial and temporal resolution at the nanoscale.

physics.optics↗

The Time-resolved Atomic, Molecular and Optical Science Instrument at the Linac Coherent Light Source

The newly constructed Time-resolved atomic, Molecular and Optical science instrument (TMO), is configured to take full advantage of both linear accelerators at SLAC National Accelerator Laboratory, the copper accelerator operating at a repetition rate of 120 Hz providing high per pulse energy, as well as the superconducting accelerator operating at a repetition rate of about 1 MHz providing high average intensity. Both accelerators build a soft X-ray free electron laser with the new variable gab undulator section. With this flexible light sources, TMO supports many experimental techniques not previously available at LCLS and will have two X-ray beam focus spots in line. Thereby, TMO supports Atomic, Molecular and Optical (AMO), strong-field and nonlinear science and will host a designated new dynamic reaction microscope with a sub-micron X-ray focus spot. The flexible instrument design is optimized for studying ultrafast electronic and molecular phenomena and can take full advantage of the sub-femtosecond soft X-ray pulse generation program.

physics.ins-det↗

Temporal shaping of narrow-band picosecond pulses via non-colinear sum-frequency mixing of dispersion-controlled pulses

A long sought-after goal for photocathode electron sources has been to improve performance by temporally shaping the incident exitation laser pulse. The narrow bandwidth, short wavelength, and picosecond pulse duration make it challenging to employ conventional spectral pulse shaping techniques. We present a novel and efficient intensity-envelope shaping technique achieved during nonlinear upconversion through opposite-chirp sum-frequency mixing. We also present a numerical case-study of the LCLS-II photoinjector where transverse electron emittance is improved by at least 25%.

physics.optics↗

Terawatt attosecond X-ray source driven by a plasma accelerator

Plasma accelerators can generate ultra high brightness electron beams which open the door to light sources with smaller physical footprint and properties un-achievable with conventional accelerator technology. In this paper we show that electron beams from Plasma WakeField Accelerators (PWFAs) can generate few-cycle coherent tunable soft X-ray pulses with TW peak power and a duration of tens of attoseconds, an order of magnitude more powerful, shorter and with better stability than state-of-the-art X-ray Free Electron Lasers (XFELs). Such a light source would significantly enhance the ability to experimentally investigate electron dynamics on ultrafast timescales, having broad-ranging impact across multiple scientific fields. Rather than starting from noise as in typical XFELs, the X-rays emission in this approach is driven by coherent radiation from a pre-bunched, near Mega Ampere (MA) current electron beam of attosecond duration. This relaxes the restrictive tolerances which have hindered progress towards utilizing plasma accelerators as coherent X-ray drivers thus far, presenting a new paradigm for advanced-accelerator light source applications.

physics.acc-ph↗

Attosecond Coherent Electron Motion in Auger-Meitner Decay

In quantum systems, coherent superpositions of electronic states evolve on ultrafast timescales (few femtosecond to attosecond, 1 as = 0.001 fs = 10^{-18} s), leading to a time dependent charge density. Here we exploit the first attosecond soft x-ray pulses produced by an x-ray free-electron laser to induce a coherent core-hole excitation in nitric oxide. Using an additional circularly polarized infrared laser pulse we create a clock to time-resolve the electron dynamics, and demonstrate control of the coherent electron motion by tuning the photon energy of the x-ray pulse. Core-excited states offer a fundamental test bed for studying coherent electron dynamics in highly excited and strongly correlated matter.

physics.chem-ph↗

Generation of terawatt, attosecond pulses from relativistic transition radiation

When a fs duration and hundreds of kA peak current electron beam traverses the vacuum and high-density plasma interface a new process, that we call relativistic transition radiation (R-TR) generates an intense $\sim100$ as pulse containing $\sim$ TW power of coherent VUV radiation accompanied by several smaller fs duration satellite pulses. This pulse inherits the radial polarization of the incident beam field and has a ring intensity distribution. This R-TR is emitted when the beam density is comparable to the plasma density and the spot size much larger than the plasma skin depth. Physically, it arises from the return current or backward relativistic motion of electrons starting just inside the plasma that Doppler up-shifts the emitted photons. The number of R-TR pulses is determined by the number of groups of plasma electrons that originate at different depths within the first plasma wake period and emit coherently before phase mixing.

physics.plasm-ph↗

Attosecond Transient Absorption Spooktroscopy: a ghost imaging approach to ultrafast absorption spectroscopy

The recent demonstration of isolated attosecond pulses from an X-ray free-electron laser (XFEL) opens the possibility for probing ultrafast electron dynamics at X-ray wavelengths. An established experimental method for probing ultrafast dynamics is X-ray transient absorption spectroscopy, where the X-ray absorption spectrum is measured by scanning the central photon energy and recording the resultant photoproducts. The spectral bandwidth inherent to attosecond pulses is wide compared to the resonant features typically probed, which generally precludes the application of this technique in the attosecond regime. In this paper we propose and demonstrate a new technique to conduct transient absorption spectroscopy with broad bandwidth attosecond pulses with the aid of ghost imaging, recovering sub-bandwidth resolution in photoproduct-based absorption measurements.

physics.chem-ph↗

Phase-stable self-modulation of an electron-beam in a magnetic wiggler

Electron-beams with a sinusoidal energy modulation have the potential to emit sub-femtosecond x-ray pulses in a free-electron laser. The energy modulation can be generated by overlapping a powerful infrared laser with an electron-beam in a magnetic wiggler. Here we report on a new infrared source for this modulation, coherent radiation from the electron-beam itself. In this self-modulation process, the current spike on the tail of the electron-beam radiates coherently at the resonant wavelength of the wiggler, producing a six-period carrier-envelope-phase (CEP) stable infrared field with gigawatt power. This field creates a few MeV, phase-stable modulation in the electron-beam core. The modulated electron-beam is immediately useful for generating sub-femtosecond x-ray pulses at any machine repetition rate, and the CEP-stable infrared field may find application as an experimental pump or timing diagnostic.

physics.acc-ph↗

Tunable Isolated Attosecond X-ray Pulses with Gigawatt Peak Power from a Free-Electron Laser

The quantum mechanical motion of electrons in molecules and solids occurs on the sub-femtosecond timescale. Consequently, the study of ultrafast electronic phenomena requires the generation of laser pulses shorter than 1 fs and of sufficient intensity to interact with their target with high probability. Probing these dynamics with atomic-site specificity requires the extension of sub-femtosecond pulses to the soft X-ray spectral region. Here we report the generation of isolated GW-scale soft X-ray attosecond pulses with an X-ray free-electron laser. Our source has a pulse energy that is six orders of magnitude larger than any other source of isolated attosecond pulses in the soft X-ray spectral region, with a peak power in the tens of gigawatts. This unique combination of high intensity, high photon energy and short pulse duration enables the investigation of electron dynamics with X-ray non-linear spectroscopy and single-particle imaging.

physics.optics↗

Coherent Space-Charge to X-ray Up-Conversion in Gas

We theoretically investigate the use of the intense transverse field created by a relativistic electron bunch to drive strong-field processes. Such bunches can be easily implemented from beam shaping in existing electron accelerators. We focus on the process of strong-field driven high harmonic generation and calculate the single-atom dipole response to the space-charge field of relativistic tilted electron beam. We compare the emitted radiation spectrum of the space-charge field to that of a few-cycle laser pulse and show that the space-charge field creates a spectrum which extends much further into the X-ray domain. We apply simple classical trajectory analysis to understand this result.

physics.acc-ph↗