Extreme Ultraviolet Light Pulses Research Articles

Continuous-variable quantum state tomography of photoelectrons

We propose a continuous variable quantum state tomography protocol of electrons which result from the ionization of atoms or molecules by the absorption of extreme ultraviolet light pulses. Our protocol is benchmarked against a direct calculation of the quantum state of photoelectrons ejected from helium and argon in the vicinity of a Fano resonance. In the latter case, we furthermore distill ion-photoelectron entanglement due to spin-orbit splitting. This opens routes toward the investigation of quantum coherence and entanglement properties on the ultrafast timescale.

Interference of two-photon transitions induced by XUV light

The relative phase of first ( ω 1 ) and third harmonics ( ω 3 ) extreme ultraviolet light pulses was varied to control the population of the 2 s 2 state in helium through the interference of ω 1 + ω 1 and ω 3 − ω 1 two-photon excitation paths. The population was monitored by observing the total electron yield due to the 2 s 2 autoionization decay. Maximum yield occurs when the relative phase of the two harmonics matches the phase difference of complex atomic amplitudes governing the two excitation paths. The calculated trend of atomic phase differences agrees well with the measured data in the spectral region of the resonance, provided that time-reversed − ω 1 + ω 3 path is also taken into account. These results open the way to accessing phase differences of two-photon ionization paths involving energetically distant intermediate states and to perform interferometry in the extreme ultraviolet range by monitoring final state populations.

Diffraction-limited coherent wake emission

The plasma mirror is a relativistic optical element that under certain irradiation conditions generates intense attosecond extreme-ultraviolet light pulses, in a process known as coherent wake emission (CWE). CWE has been previously characterized by its high spatial divergence, originating from an intrinsic intensity-dependent phase accumulation. In this Letter, we show that the transverse variations of the plasma expansion can completely cancel the CWE intrinsic phase. Accordingly, we experimentally demonstrate nearly diffraction-limited CWE with unprecedented divergence, under 6 mrad. We validate our analytical model with particle in cell simulations. This understanding facilitates the development of plasma mirrors as applicable ultraviolet light sources.Received 9 March 2021Accepted 5 August 2021DOI:https://doi.org/10.1103/PhysRevResearch.3.L032059Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasHigh intensity laser-plasma interactionsHigh-order harmonic generationPhysical SystemsRelativistic plasmasAtomic, Molecular & OpticalPlasma Physics

Complete phase retrieval of photoelectron wavepackets

Coherent, broadband pulses of extreme ultraviolet light provide a new and exciting tool for exploring attosecond electron dynamics. Using photoelectron streaking, interferometric spectrograms can be generated that contain a wealth of information about the phase properties of the photoionization process. If properly retrieved, this phase information reveals attosecond dynamics during photoelectron emission such as multielectron dynamics and resonance processes. However, until now, the full retrieval of the continuous electron wavepacket phase from isolated attosecond pulses has remained challenging. Here, after elucidating key approximations and limitations that hinder one from extracting the coherent electron wavepacket dynamics using available retrieval algorithms, we present a new method called absolute complex dipole transition matrix element reconstruction (ACDC). We apply the ACDC method to experimental spectrograms to resolve the phase and group delay difference between photoelectrons emitted from Ne and Ar. Our results reveal subtle dynamics in this group delay difference of photoelectrons emitted form Ar. These group delay dynamics were not resolvable with prior methods that were only able to extract phase information at discrete energy levels, emphasizing the importance of a complete and continuous phase retrieval technique such as ACDC. Here we also make this new ACDC retrieval algorithm available with appropriate citation in return.

Nanoscale transient gratings excited and probed by extreme ultraviolet femtosecond pulses.

Advances in developing ultrafast coherent sources operating at extreme ultraviolet (EUV) and x-ray wavelengths allow the extension of nonlinear optical techniques to shorter wavelengths. Here, we describe EUV transient grating spectroscopy, in which two crossed femtosecond EUV pulses produce spatially periodic nanoscale excitations in the sample and their dynamics is probed via diffraction of a third time-delayed EUV pulse. The use of radiation with wavelengths down to 13.3 nm allowed us to produce transient gratings with periods as short as 28 nm and observe thermal and coherent phonon dynamics in crystalline silicon and amorphous silicon nitride. This approach allows measurements of thermal transport on the ~10-nm scale, where the two samples show different heat transport regimes, and can be applied to study other phenomena showing nontrivial behaviors at the nanoscale, such as structural relaxations in complex liquids and ultrafast magnetic dynamics.

Three-Dimensional Shapes of Spinning Helium Nanodroplets.

A significant fraction of superfluid helium nanodroplets produced in a free-jet expansion has been observed to gain high angular momentum resulting in large centrifugal deformation. We measured single-shot diffraction patterns of individual rotating helium nanodroplets up to large scattering angles using intense extreme ultraviolet light pulses from the FERMI free-electron laser. Distinct asymmetric features in the wide-angle diffraction patterns enable the unique and systematic identification of the three-dimensional droplet shapes. The analysis of a large data set allows us to follow the evolution from axisymmetric oblate to triaxial prolate and two-lobed droplets. We find that the shapes of spinning superfluid helium droplets exhibit the same stages as classical rotating droplets while the previously reported metastable, oblate shapes of quantum droplets are not observed. Our three-dimensional analysis represents a valuable landmark for clarifying the interrelation between morphology and superfluidity on the nanometer scale.

Near infrared and extreme ultraviolet light pulses induced modifications of ultrathin Co films

We report on comparative study of magnetic properties of Pt/Co/Pt trilayers after irradiation with different light sources. Ultrathin Pt/Co/Pt films were deposited by molecular beam epitaxy technique on sapphire (0001) substrates. Pt buffers were grown at room temperature (RT) and at 750°C (high temperature, HT). The samples were irradiated with a broad range of light energy densities (up to film ablation) using two different single pulse irradiation sources: (i) 40 fs laser with 800 nm wavelength and (ii) 3 ns laser-plasma source of extreme ultraviolet (EUV) with the most intense emission centered at 11 nm. The light pulse-driven irreversible structural and as a consequence, magnetic modifications were investigated using polar magneto-optical Kerr effect-based microscopy and atomic and magnetic force microscopies. The light pulse-induced transitions from the out-of-plane to in-plane magnetization state, and from in-plane to out-of-plane, were observed for both types of samples and irradiation methods. Diagrams of the magnetic states as a function of the Co layer thickness and energy density of the absorbed femtosecond pulses were constructed for the samples with both the RT and HT buffers. The energy density range responsible for the creation of the out-of-plane magnetization was wider for the HT than for RT buffer. This is correlated with the higher (for HT) crystalline quality and much smoother Pt/Co surface deduced from the X-ray diffraction studies. Submicrometer magnetic domains were observed in the irradiated region while approaching the out-of-plane magnetization state. Changes of Pt/Co/Pt structures are discussed for both types of light pulses.

Spin-resolved photoelectron spectroscopy using femtosecond extreme ultraviolet light pulses from high-order harmonic generation.

The fundamental mechanism responsible for optically induced magnetization dynamics in ferromagnetic thin films has been under intense debate since almost two decades. Currently, numerous competing theoretical models are in strong need for a decisive experimental confirmation such as monitoring the triggered changes in the spin-dependent band structure on ultrashort time scales. Our approach explores the possibility of observing femtosecond band structure dynamics by giving access to extended parts of the Brillouin zone in a simultaneously time-, energy- and spin-resolved photoemission experiment. For this purpose, our setup uses a state-of-the-art, highly efficient spin detector and ultrashort, extreme ultraviolet light pulses created by laser-based high-order harmonic generation. In this paper, we present the setup and first spin-resolved spectra obtained with our experiment within an acquisition time short enough to allow pump-probe studies. Further, we characterize the influence of the excitation with femtosecond extreme ultraviolet pulses by comparing the results with data acquired using a continuous wave light source with similar photon energy. In addition, changes in the spectra induced by vacuum space-charge effects due to both the extreme ultraviolet probe- and near-infrared pump-pulses are studied by analyzing the resulting spectral distortions. The combination of energy resolution and electron count rate achieved in our setup confirms its suitability for spin-resolved studies of the band structure on ultrashort time scales.

Structural investigation of ultrathin Pt/Co/Pt trilayer films under EUV irradiation

Trilayer systems containing ultrathin (3nm) cobalt layer grown on 5nm thick Pt buffer layer and covered with 3nm thick Pt cap layer grown at room temperature by molecular beam epitaxy on the Al2O3(00.1) substrate have been irradiated by nanosecond extreme ultraviolet light pulses. It was previously evidenced that light irradiation induced irreversible change of direction of magnetization in such nanostructures. In order to understand the reasons of such behavior the structural studies with the use of X-ray diffraction and transmission electron microscopy of the as-grown and irradiated samples have been done. It was found that irradiation leads to intermixing of cobalt with platinum giving rise to creation of Pt1−xCox disordered alloy. The methodology of determination of the strain state of the layers, relaxed lattice parameter of the unit cell and the composition of Pt1−xCox alloys has been developed and described in details. The results of structural studies of the as grown Pt/Co/Pt nanostructures as well as those modified by irradiation are presented in this paper.

Temporal broadening of attosecond photoelectron wavepackets from solid surfaces

The response of solids to electromagnetic fields is of crucial importance in many areas of science and technology. Many fundamental questions remain to be answered about the dynamics of the photoexcited electrons that underpin this response, which can evolve on timescales of tens to hundreds of attoseconds. How, for example, is the photoexcited electron affected by the periodic potential as it travels in the solid, and how do the other electrons respond in these strongly correlated systems? Furthermore, control of electronic motion in solids with attosecond precision would pave the way for the development of ultrafast optoelectronics. Attosecond electron dynamics can be traced using streaking, a technique in which a strong near-infrared laser field accelerates an attosecond electron wavepacket photoemitted by an extreme ultraviolet light pulse, imprinting timing information onto it. We present attosecond streaking measurements on the wide-bandgap semiconductor tungsten trioxide, and on gold, a metal used in many nanoplasmonic devices. Information about electronic motion in the solid is encoded on the temporal properties of the photoemitted electron wavepackets, which are consistent with a spread of electron transport times to the surface following photoexcitation.

Direct observation of electron propagation and dielectric screening on the atomic length scale.

The propagation and transport of electrons in crystals is a fundamental process pertaining to the functioning of most electronic devices. Microscopic theories describe this phenomenon as being based on the motion of Bloch wave packets. These wave packets are superpositions of individual Bloch states with the group velocity determined by the dispersion of the electronic band structure near the central wavevector in momentum space. This concept has been verified experimentally in artificial superlattices by the observation of Bloch oscillations--periodic oscillations of electrons in real and momentum space. Here we present a direct observation of electron wave packet motion in a real-space and real-time experiment, on length and time scales shorter than the Bloch oscillation amplitude and period. We show that attosecond metrology (1 as = 10(-18) seconds) now enables quantitative insight into weakly disturbed electron wave packet propagation on the atomic length scale without being hampered by scattering effects, which inevitably occur over macroscopic propagation length scales. We use sub-femtosecond (less than 10(-15) seconds) extreme-ultraviolet light pulses to launch photoelectron wave packets inside a tungsten crystal that is covered by magnesium films of varied, well-defined thicknesses of a few ångströms. Probing the moment of arrival of the wave packets at the surface with attosecond precision reveals free-electron-like, ballistic propagation behaviour inside the magnesium adlayer--constituting the semi-classical limit of Bloch wave packet motion. Real-time access to electron transport through atomic layers and interfaces promises unprecedented insight into phenomena that may enable the scaling of electronic and photonic circuits to atomic dimensions. In addition, this experiment allows us to determine the penetration depth of electrical fields at optical frequencies at solid interfaces on the atomic scale.

Femtosecond time-resolved XUV + UV photoelectron imaging of pure helium nanodroplets.

Liquid helium nanodroplets, consisting of on average 2 × 10(6) atoms, are examined using femtosecond time-resolved photoelectron imaging. The droplets are excited by an extreme ultraviolet light pulse centered at 23.7 eV photon energy, leading to states within a band that is associated with the 1s3p and 1s4p Rydberg levels of free helium atoms. The initially excited states and subsequent relaxation dynamics are probed by photoionizing transient species with a 3.2 eV pulse and using velocity map imaging to measure time-dependent photoelectron kinetic energy distributions. Significant differences are seen compared to previous studies with a lower energy (1.6 eV) probe pulse. Three distinct time-dependent signals are analyzed by global fitting. A broad intense signal, centered at an electron kinetic energy (eKE) of 2.3 eV, grows in faster than the experimental time resolution and decays in ~100 fs. This feature is attributed to the initially excited droplet state. A second broad transient feature, with eKE ranging from 0.5 to 4 eV, appears at a rate similar to the decay of the initially excited state and is attributed to rapid atomic reconfiguration resulting in Franck-Condon overlap with a broader range of cation geometries, possibly involving formation of a Rydberg-excited (He(n))* core within the droplet. An additional relaxation pathway leads to another short-lived feature with vertical binding energies ≳2.4 eV, which is identified as a transient population within the lower-lying 1s2p Rydberg band. Ionization at 3.2 eV shows an enhanced contribution from electronically excited droplet states compared to ejected Rydberg atoms, which dominate at 1.6 eV. This is possibly the result of increased photoelectron generation from the bulk of the droplet by the more energetic probe photons.

Optimization of Quantum Trajectories Driven by Strong-Field Waveforms

Lasers can be used to steer an electron, yielding extreme-ultraviolet light pulses when the accelerated electron recollides with its parent atom. Researchers have enhanced the flux of the extreme-ultraviolet pulses by a factor of 100, enabling the study of extremely fast (subfemtosecond) electron dynamics.

An extreme ultraviolet interferometer using high order harmonic generation

We present a new interferometer technique based on the interference of high-order harmonic generation radiation from translatable successive gas jets. The phase shifts in the apparatus are shown to originate from the Gouy phase shift of the driving laser. The technique can be used to deliver time delays between light pulses and we demonstrate the unprecedented capability of delivering pulses of extreme ultraviolet light delayed in time by as small as 100 zeptoseconds.

Extreme Ultraviolet Interferometer Using High-Order Harmonic Generation from Successive Sources

We present a new interferometer technique whereby multiple extreme ultraviolet light pulses are generated at different positions within a single laser focus (i.e., from successive sources) with a highly controllable time delay. The interferometer technique is tested with two generating media to create two extreme ultraviolet light pulses with a time delay between them. The delay is found to be a consequence of the Gouy phase shift. Ultimately the apparatus is capable of accessing unprecedented time scales by allowing stable and repeatable delays as small as 100zs.

Ultrafast Demagnetization Measurements Using Extreme Ultraviolet Light: Comparison of Electronic and Magnetic Contributions

Ultrashort pulses of extreme ultraviolet light from high-harmonic generation are a new tool for probing coupled charge, spin, and phonon dynamics with element specificity, attosecond pump-probe synchronization, and time resolution of a few femtoseconds in a tabletop apparatus. In this paper, we address an important question in magneto-optics that has implications for understanding magnetism on the fastest time scales: Is the signal from the transverse magneto-optical Kerr effect at the M2,3 edges of a magnetic material purely magnetic or is it perturbed by nonmagnetic artifacts? Our measurements demonstrate conclusively that transverse magneto-optical Kerr measurements at the M2,3 edges sensitively probe the magnetic state, with almost negligible contributions from the transient variation of the refractive index by the nonequilibrium hot-electron distribution. In addition, we compare pump-probe demagnetization dynamics measured by both high harmonics and conventional visible-wavelength magneto-optics and find that the measured demagnetization times are in agreement.Received 26 October 2011DOI:https://doi.org/10.1103/PhysRevX.2.011005This article is available under the terms of the Creative Commons Attribution 3.0 License. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.Published by the American Physical Society

Monitoring and Controlling the Electron Dynamics in Helium with Isolated Attosecond Pulses

Helium atoms in the presence of extreme ultraviolet light pulses can lose electrons through direct photoionization or through two-electron excitation followed by autoionization. Here we demonstrate that, by combining attosecond extreme ultraviolet pulses with near infrared femtosecond lasers, electron dynamics in helium autoionization can be not only monitored but also controlled. Furthermore, the interference between the two ionization channels was modified by the intense near infrared laser pulse. To the best of our knowledge, this is the first time that double excitation and autoionization were studied experimentally by using isolated attosecond pulses.

Ion-ion coincidence studies on multiple ionizations of N2 and O2 molecules irradiated by extreme ultraviolet free-electron laser pulses

We have investigated multiple ionization of N(2) and O(2) molecules by 52 nm extreme-ultraviolet light pulses at the free-electron laser facility SCSS in Japan. Coulomb break-up of parent ions with charge states up to 5+ is found by the ion-ion coincidence technique. The charge-state dependence of kinetic energy release distributions suggests that the electrons are emitted sequentially in competition with the elongation of the bond length.

Cold-target recoil-ion momentum spectroscopy for diagnostics of high harmonics of the extreme-ultraviolet free-electron laser light source at SPring-8

We have developed a cold-target recoil-ion momentum spectroscopy apparatus dedicated to the experiments using the extreme-ultraviolet light pulses at the free-electron laser facility, SPring-8 Compact SASE Source test accelerator, in Japan and used it to measure spatial distributions of fundamental, second, and third harmonics at the end station.

Dead-time-free ion momentum spectroscopy of multiple ionization of Xe clusters irradiated by euv free-electron laser pulses

We have investigated multiple ionization of Xe clusters by 61-nm ${10}^{11}--{10}^{12}\text{ }\text{W}/{\text{cm}}^{2}$ extreme-ultraviolet light pulses at the free-electron laser facility, SPring-8 Compact SASE Source test accelerator, in Japan, using a dead-time-free three-dimensional momentum spectrometer. It was found that the average kinetic energy of atomic ${\text{Xe}}^{+}$ ions increases when increasing the laser power density and the cluster size. For these experimental conditions significant frustration of the cluster photoionization occurs but no indication for heating mechanisms other than sequential photoabsorption by individual atoms in the cluster was found.