When is a laser a real laser?

Pulsed lasers are intense and coherent light sources, and the latest category is that of Free Electron Lasers, such as FERMI. First order coherence is a familiar phenomenon, and is manifested for example in diffraction phenomena. This represents the correlation between the amplitudesof a wave at different points in space (transverse coherence) or time (longitudinal coherence.) However, a high degree of first order coherence is not enough to define a laser, according to the Nobel laureate Roy Glauber, who stated that a laser can be defined as a source that is coherent in all orders. The higher order correlations are between intensityat different points in time and space. How are these correlations measured? For this one has to look at the statistics of the photons.
Glauber’s work was inspired by the famous Hanbury Brown and Twiss experiment, in which coincidences of photons (i.e. correlations) were measured of photons coming from distant stars. By varying the distance between two detectors, they were able to determine the degree of coherence of the star, and extract other information. This is the key to measuring the second order coherence of a light source: the intensity of light at different points is measured in coincidence, and statistical analysis is made. This experiment is considered by many as initiating the whole field of quantum optics. Now a team led by Ivan Vartaniants (DESY, Hamburg, and the National Research Nuclear University, Moscow) has performed a Hanbury Brown and Twiss experiment at FERMI. Instead of the two discrete photodetectors used originally, a CCD detector was used. Since all of the photons arrive in less than 100 fs, there is no need to use coincidence methods: the signal is naturally synchronised.

>Read more on the FERMI at Elettra Sincrotrone Trieste website

Figure 1.  Difference between chaotic and coherent light sources. (a) photon correlation map for FERMI operated in seeded mode. (b) corresponding spectrum. (c) correlation map for FERMI operated in Self Amplified Stimulated Emission mode (the mode of operation of most Free Electron Lasers). (d) corresponding spectrum.
Credit: Reprinted from O. Yu. Gorobtsov et al, Nature Communications 9 (2018) 4498. (Copyright Nature Publishing Group)

Steering the outcome of photoionization in a molecule

An important step towards the understanding and control of photoinduced fragmentation processes in molecules has been achieved in an experiment on the H2 molecule taking advantage of the unique properties of the FERMI free-electron laser source in the vacuum ultraviolet (VUV) photon energy range.
Molecular dissociation, i.e., the breaking of a chemical bond, is governed by the coupling of electronic and nuclear motion and, once understood and controlled in large systems, e.g., by utilizing ultrashort light pulses, has the potential to impact tremendously photochemical and biochemical applications. A team of both experimentalists and theoreticians from France (CNRS, Université Paris-Sud, Université de Bordeaux), Spain (Universidad Autónoma de Madrid), Germany (European XFEL), and Italy (Elettra-Sincrotrone Trieste) has demonstrated that the outcome of dissociative (DI) and nondissociative (NDI) photoionization in the simplest of all molecules, H2, can be controlled exploiting nonlinear two-photon ionization with intense femtosecond pulses in the VUV.
The FERMI seeded free-electron laser is currently the only light source worldwide that provides external users access to bright femtosecond pulses at wavelengths in the VUV up to 100 nm, the energy regime required for studying nonlinear two-photon single-ionization in H2. The high spectral resolution and precise tunability of the 100-fs pulses provided by FERMI made it possible to selectively excite single vibrational levels in the neutral intermediate B state of H2 (blue line in Fig. 1). Absorption of a second VUV photon then leads to NDI or DI into the ionic H2+ ground state (green in Fig. 1) or to DI into the first excited H2+2p continuum (orange in Fig. 1). In single-photon single-ionization of H2, the yield of DI is very low – less than 2%. By contrast, recent ab initiocalculations suggest that the ratio of DI/NDI can be increased significantly in resonance-enhanced two-photon ionization and that it can be controlled by varying the pulse duration between 2 and 10 fs.

>Read more on the Elettra website

Image: (a) Schematic of resonant two-photon ionization viathe B intermediate state (12.51 eV). The grey shaded area shows the Franck-Condon region for one-photon absorption from the H2electronic ground state. The dashed purple arrows visualize the range for the absorption of the second FEL photon. The green (red) horizontal line shows the ionization threshold at 15.43 eV (dissociation limit at 18.08 eV). (b) The experimental photoelectron spectrum shows a clear separation of electrons correlated to NDI and DI. For DI, it is close to the prediction of the Condon-reflection approximation, i.e., the projection of the vibrational wavefunction onto the dissociative 2p continuum state. The infinite-time limit calculation (grey line for the convolution of the contributions from the two first ionization continua) reproduces the main features of the spectrum. The differences between experiment and calculation indicates that at FERMI a timescale between ultrafast dynamics and steady-state excitation is probed.

Ultralow-fluence for phase-change process

Ultrafast active materials with tunable properties are currently investigated for producing successful memory and data-processing devices. Among others, Phase-Change Materials (PCMs) are eligible for this purpose. They can reversibly switch between a high-conductive crystalline state (SET) and a low-conductive amorphous state (RESET), defining a binary code. The transformation is triggered by an electrical or optical pulse of different intensity and time duration. 3D Ge-Sb-Te based alloys, of different stoichiometry, are already employed in DVDs or Blu-Ray Disks, but they are expected to function also in non-volatile memories and RAM. The challenge is to demonstrate that the scalability to 2D, 1D up to 0D of the GST alloys improves the phase-change process in terms of lower power threshold and faster switching time. Nowadays, GST thin films and nanoparticles have been synthetized and have beenshown to function with competitive results.
A team of researchers from the University of Trieste and the MagneDyn beamline at Fermi demonstrated the optical switch from crystalline to amorphous state of Ge2Sb2Te5nanoparticles (GST NPs) with size <10 nm, produced via magnetron sputtering by collaborators from the University of Groeningen. Details were reported in the journal Nanoscale.
This work aims at showing the very low power limit of an optical pulse needed to amorphize crystalline Ge2Sb2Te5 nanoparticles. Particles of 7.8 nm and 10.4 nm diameter size were deposited on Mica and capped with ~200nm of PMMA. Researchers made use of a table-top Ti:Sapphire regenerative amplified system-available at the IDontKerr (IDK) laboratory (MagneDyn beamline support laboratory) to produce pump laser pulses at 400 nm, of ~100 fs and with a repetition rate from 1kHz to single shot.

>Read more on the Elettra Sincrotrone Trieste website

Image (extract): Trasmission Electron Microscopy image of the nanoparticles sample. Ultafast single-shot optical process with fs-pulse at 400 nm. Microscope images of amorphized and amorphized/ablated areas obtained on the nanoparticles sample. Comparison of amorphization threshold fluences between thin films and nanoparticles cases.
Please see here the entire image.

LEAPS and FELs of Europe meetings at Elettra

On March 12-13 Elettra-Sincrotrone Trieste hosted the 2nd meeting of General Assembly (GA) of the League of European Accelerator-based Photon Sources (LEAPS), a strategic consortium that includes 16 Synchrotron Radiation and Free Electron Laser (FEL) user facilities in Europe based in 10 different European countries .
This followed the LEAPS Launch Event in Brussels on November 13, 2017. The main topics of the GA meeting were the LEAPS Governance Structure and the LEAPS Strategy Paper to be forwarded to the EU Commission during the Bulgarian Presidency Conference on Research Infrastructures in Sofia, 22-23 March.

>Read more on the Elettra and FERMI website

Image: LEAPS General Assembly and Coordination Board group picture.
Credit: Fotorolli

High coherence and intensity at FERMI enables new X-ray interfacial probe

Interfaces are involved in a wide range of systems and have significant implications in many fields of scientific and technological advancement, often determining device performance or chemical reactivity. Vital examples include solar cells, protein folding, and computer chips. A class of commonly used surface science techniques are comprised of even-ordered nonlinear spectroscopies (i.e., second harmonic and sum frequency generation) which exhibit no response in centrosymmetric media due to symmetry constraints.As a result, they have been widely used at optical wavelengths to explore physical and chemical properties of interfaces, where centrosymmetry is broken. Extending this to x-ray wavelengths would effectively combine the element specificity and spectral sensitivity of x-ray spectroscopy with the rigorous interfacial/surface specificity of optical even-ordered nonlinear spectroscopies. Unfortunately, at hard x-ray energies (x-ray wavelength order of the spacing between atoms) these even-ordered nonlinear spectroscopies are effectively bulk probes, as each individual atom breaks inversion symmetry. As soft x-ray wavelengths fall in between the UV and hard x-ray regimes, there has been uncertainty regarding the interface specificity of soft x-ray second harmonic generation.

>Read more on the FERMI webpage

Figure: (extract)  Experimental Design. X-ray pulses are passed through a 2 mm iris and focused onto the graphite sample at normal incidence. The transmitted beam is then passed through a 600 nm aluminum filter and onto a spectrometer grating, spatially resolving the second harmonic signal from the fundamental. Inset: A schematic energy level diagram of the second harmonic generation process. (entire figure here)

 

Extreme-ultraviolet vortices from a free-electron laser

Extreme-ultraviolet vortices may be exploited to steer the magnetic properties of nanoparticles, increase the resolution in microscopy, and gain insight into local symmetry and chirality of a material; they might even be used to increase the bandwidth in long-distance space communications. However, in contrast to the generation of vortex beams in the infrared and visible spectral regions, production of intense, extreme-ultraviolet (XUV) and x-ray optical vortices still remains a challenge. Here, we present an in-situ and an ex-situ technique for generating intense, femtosecond, coherent optical vortices with tunable topological charge at a free-electron laser (FEL) in the XUV.

The first method takes advantage of nonlinear harmonic generation in a helical undulator and exploits the fact that such harmonics carry a topological charge of l = n-1, where n is the harmonic number. The experiment was performed at the FERMI FEL. An ultraviolet (250-nm) seed laser was used to energy modulate the electron beam (e-beam) in the first undulator (modulator), as shown in the top panel of Figure 1. The e-beam was then sent through a dispersive section (a four-dipole-magnet chicane), where the energy modulation was transformed into a current-density modulation (bunching) with Fourier components spanning many harmonics of the seed laser frequency. Such a bunched e-beam entered the helical radiator tuned to a fundamental wavelength of 31.2 nm (i.e., the 8th harmonic of the seed), producing coherent light in the XUV. The FEL was operated in the high-gain regime, close to the saturation point. Under these conditions, the interaction between the radiation at the fundamental FEL wavelength and the e-beam induced bunching at the second harmonic (15.6 nm), resulting in emission of coherent XUV vortices carrying unit topological charge (l = 1) at intensities on the order of 10−3 of the fundamental FEL emission; see bottom panel in Figure 1.

>Read more on the FERMI website

Image:
Top: The scheme to generate optical vortices at harmonics (in the present case at the 2nd harmonic) of the fundamental FEL wavelength. The optical vortex is separated from the fundamental FEL emission using a Zr filter.
Bottom: Intensity profile of the generated optical vortex with a topological charge of l =1 (left), and interference with a Gaussian beam revealing the twisted nature of the vortex (right).

 

Molecular dynamics on the femtosecond timescale

A photochemical reaction in its becoming has been observed with unprecedented detail at the Free Electron Laser FERMI in Trieste.

The result of the experiment published in Nature Communications paves the way for investigations that can shed new light on photochemical processes.

“Shooting the movie” of a photochemical reaction, interpreting its hidden details with the help of a computer: this is what has been done, thanks to the extraordinary capabilities of the FERMI free electron laser source in Trieste, by a research team composed of the Universities of Uppsala and Gothenburg in Sweden, the Institut Ruđer Bošković of Zagreb, the Elettra-FERMI Laboratory, the University of Trieste and the Laboratory of Physical Chemistry, Matter and Radiation in Paris. The study was published in Nature Communications.

The researchers wanted to capture the details of a chemical reaction promoted by the absorption of light (photochemical process), to understand how the excitation generated by a light beam induces changes on a target molecule. The first steps in a photochemical process involve changes in the electronic and geometric structure of a molecule over extremely short times measured in femtoseconds (1 fs = 10-15 s), which had so far hindered the accurate reconstruction of the entire sequence of the reaction.

The combination of intensity, energy resolution and very short pulse duration of the FERMI seeded free-electron laser source can now for the first time provide exceptionally detailed information on photoexcitation-deexcitation and fragmentation processes of isolated molecules in pump-probe experiments on the 50-femtosecond time scale.

Photoelectron spectroscopy with high resolution in energy and time, combined with accurate electronic structure and molecular dynamics calculations, has allowed to visualize in its entirety the temporal evolution of the prototype system chosen for the experiment: acetylacetone—a stable molecule used in environmental and medical applications.

“Besides revealing the dynamics of the reaction—explains Maria Novella Piancastelli of the University of Uppsala, principal investigator—a strong point of the experiment lies in the general applicability of the method, which leads us to consider it as the best way to investigate fundamental photochemical processes such as photosynthesis, photovoltaic energy production and vision.  The stairway that goes from simple to complex molecules, and from the understanding of phenomena to practical applications is of course a long one, and we are specifically interested in its ‘first step’.

>Read more on the FERMI website

Figure: A pictorial representation of the potential energy surfaces involved in the relaxation mechanism of acetylacetone: the ground state S0 (darker blue), two singlet S2 (ππ*) (light blue) and S1 (nπ*) (orange), and two triplet T2 (nπ*) (light green) and T1 (ππ*) (green) states. This approach based on high-resolution valence spectra backed by high-level calculations is the ultimate way to shed light on fundamental, basic photo processes such as photosynthesis, photovoltaic energy production, and vision.

 

 

Observation and Control of Laser-Enabled Auger Decay

When isolated atoms are electronically excited, they have two possible ways of releasing electronic energy: by radiation or by Auger decay. The Auger process, in which the decaying electron transfers its energy to another electron causing it to detach (ionization), has played an important part in modern physics, particularly surface science, because it is by far the strongest decay channel for core holes of light elements such as carbon, nitrogen, and oxygen. In some cases, the Auger process is energetically forbidden, because the energy being exchanged is not sufficient for ionization. In this case, new electronic mechanisms for deexcitation may be discovered that “borrow” energy from the surroundings. One of these is interatomic Coulombic decay (ICD) where the energy is “borrowed” from surrounding atoms. Another mechanism is laser enabled Auger Decay (LEAD), where the energy is “borrowed” from an ancillary laser field; up to now LEAD has been observed with low-energy photons, meaning that more than one photon must be absorbed to make the process possible.

>Read more

Time-resolved measurement of interatomic Coulombic decay

… induced by two-photon double excitation of Ne2

On the 24th of March 2017, Tsukasa Takanashi gained his doctorate from the University of Tohoku (Japan), together with the President’s Award prize (総長賞). The prize is awarded each year to the best PhD students in recognition of their outstanding academic curriculum, and particularly for the excellent results obtained during their studies. Tsukasa carried out his studies under the supervision of Professor Kiyoshi Ueda, a leading figure on the international scene of atomic and molecular physics, and until recently, a member of the FERMI Review Panel. In his thesis, Tsukasa used the light from Free Electron Lasers (FELs) to study the dynamics of highly excited molecular systems; in his home country, he utilized the Japanese FEL SACLA, and he studied the Coulomb explosion of the molecule CH2I2 (diiodomethane). This process is the fragmentation by multiple ionization of a sample, and the successive repulsion of the ions by the positive charge which is generated.

An important part of his work was carried out at FERMI, currently the only FEL source in the world able to provide Tsukasa the wavelength (75.6 nm) and temporal resolution (10-13 s) necessary to study the dynamics of his system: the Ne2 molecule, which consists of two neon atoms bound by their weak van der Waals interaction. The apparent simplicity of this system allows the detailed study of complex phenomena, such as the exchange of energy after electronic excitation, which is basic to all photochemical processes.

>Read more on the FERMI website

Image: Schematic representation of the resonant absorption of two FEL photons by a neon dimer (upper panel) and the ICD relaxation process by ionization (lower panel).