Femtosecond Extreme Ultraviolet Pulses Research Articles

Generation of entanglement using a short-wavelength seeded free-electron laser.

Quantum entanglement between the degrees of freedom encountered in the classical world is challenging to observe due to the surrounding environment. To elucidate this issue, we investigate the entanglement generated over ultrafast timescales in a bipartite quantum system comprising two massive particles: a free-moving photoelectron, which expands to a mesoscopic length scale, and a light-dressed atomic ion, which represents a hybrid state of light and matter. Although the photoelectron spectra are measured classically, the entanglement allows us to reveal information about the dressed-state dynamics of the ion and the femtosecond extreme ultraviolet pulses delivered by a seeded free-electron laser. The observed generation of entanglement is interpreted using the time-dependent von Neumann entropy. Our results unveil the potential for using short-wavelength coherent light pulses from free-electron lasers to generate entangled photoelectron and ion systems for studying spooky action at a distance.

Transient grating spectroscopy on a DyCo5 thin film with femtosecond extreme ultraviolet pulses.

Surface acoustic waves (SAWs) are excited by femtosecond extreme ultraviolet (EUV) transient gratings (TGs) in a room-temperature ferrimagnetic DyCo5 alloy. TGs are generated by crossing a pair of EUV pulses from a free electron laser with the wavelength of 20.8 nm matching the Co M-edge, resulting in a SAW wavelength of Λ = 44 nm. Using the pump-probe transient grating scheme in reflection geometry, the excited SAWs could be followed in the time range of -10 to 100 ps in the thin film. Coherent generation of TGs by ultrafast EUV pulses allows to excite SAW in any material and to investigate their couplings to other dynamics, such as spin waves and orbital dynamics. In contrast, we encountered challenges in detecting electronic and magnetic signals, potentially due to the dominance of the larger SAW signal and the weakened reflection signal from underlying layers. A potential solution for the latter challenge involves employing soft x-ray probes, albeit introducing additional complexities associated with the required grazing incidence geometry.

Observation of Rabi dynamics with a short-wavelength free-electron laser

Rabi oscillations are periodic modulations of populations in two-level systems interacting with a time-varying field1. They are ubiquitous in physics with applications in different areas such as photonics2, nano-electronics3, electron microscopy4 and quantum information5. While the theory developed by Rabi was intended for fermions in gyrating magnetic fields, Autler and Townes realized that it could also be used to describe coherent light–matter interactions within the rotating-wave approximation6. Although intense nanometre-wavelength light sources have been available for more than a decade7–9, Rabi dynamics at such short wavelengths has not been directly observed. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser10 can drive Rabi dynamics between the ground state and an excited state in helium atoms. The measured photoelectron signal reveals an Autler–Townes doublet and an avoided crossing, phenomena that are both fundamental to coherent atom–field interactions11. Using an analytical model derived from perturbation theory on top of the Rabi model, we find that the ultrafast build-up of the doublet structure carries the signature of a quantum interference effect between resonant and non-resonant photoionization pathways. Given the recent availability of intense attosecond12 and few-femtosecond13 extreme-ultraviolet pulses, our results unfold opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.

All-Optical Switching on the Nanometer Scale Excited and Probed with Femtosecond Extreme Ultraviolet Pulses

Ultrafast control of magnetization on the nanometer length scale, in particular all-optical switching, is key to putting ultrafast magnetism on the path toward future technological application in data storage technology. However, magnetization manipulation with light on this length scale is challenging due to the wavelength limitations of optical radiation. Here, we excite transient magnetic gratings in a GdFe alloy with a periodicity of 87 nm by the interference of two coherent femtosecond light pulses in the extreme ultraviolet spectral range. The subsequent ultrafast evolution of the magnetization pattern is probed by diffraction of a third, time-delayed pulse tuned to the Gd N-edge at a wavelength of 8.3 nm. By examining the simultaneously recorded first and second order diffractions and by performing reference real-space measurements with a wide-field magneto-optical microscope with femtosecond time resolution, we can conclusively demonstrate the ultrafast emergence of all-optical switching on the nanometer length scale.

Nanoscale Transient Magnetization Gratings Created and Probed by Femtosecond Extreme Ultraviolet Pulses.

We utilize coherent femtosecond extreme ultraviolet (EUV) pulses from a free electron laser (FEL) to generate transient periodic magnetization patterns with periods as short as 44 nm. Combining spatially periodic excitation with resonant probing at the M-edge of cobalt allows us to create and probe transient gratings of electronic and magnetic excitations in a CoGd alloy. In a demagnetized sample, we observe an electronic excitation with a rise time close to the FEL pulse duration and ∼0.5 ps decay time indicative of electron-phonon relaxation. When the sample is magnetized to saturation in an external field, we observe a magnetization grating, which appears on a subpicosecond time scale as the sample is demagnetized at the maxima of the EUV intensity and then decays on the time scale of tens of picoseconds via thermal diffusion. The described approach opens multiple avenues for studying dynamics of ultrafast magnetic phenomena on nanometer length scales.

Ablation threshold and crater morphology of amorphous and crystalline SiO2 glass for extreme ultraviolet femtosecond pulses

The ablation threshold fluence and crater morphology of amorphous and crystalline SiO2 glass were analyzed in the regime of an extreme ultraviolet femtosecond pulse. Despite the difference between the densities (or optical penetration depths) of amorphous and crystalline SiO2 glass, the ablation threshold fluences and crater morphologies were found to be comparable. In addition, we compared our experimental results at a 10.3 nm wavelength with those in a previous work at a 13.5 nm wavelength. We conclude that the impact of the difference in density or optical penetration depth of several tens of percent on the ablation process is limited.

Multiple Sequential Ionization of Valence n = 4 Shell of Krypton by Intense Femtosecond XUV Pulses

Sequential photoionization of krypton by intense extreme ultraviolet femtosecond pulses is studied theoretically for the photon energies below the 3d excitation threshold. This regime with energetically forbidden Auger decay is characterized by special features, such as time scaling of the level population. The model is based on the solution of rate equations with photoionization cross sections of krypton in different charge and multiplet states determined using R-matrix calculations. Predictions of the ion yields and photoelectron spectra for various photon fluence are presented and discussed.

Dissociation dynamics of the diamondoid adamantane upon photoionization by XUV femtosecond pulses

This work presents a photodissociation study of the diamondoid adamantane using extreme ultraviolet femtosecond pulses. The fragmentation dynamics of the dication is unraveled by the use of advanced ion and electron spectroscopy giving access to the dissociation channels as well as their energetics. To get insight into the fragmentation dynamics, we use a theoretical approach combining potential energy surface determination, statistical fragmentation methods and molecular dynamics simulations. We demonstrate that the dissociation dynamics of adamantane dications takes place in a two-step process: barrierless cage opening followed by Coulomb repulsion-driven fragmentation.

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.

Real-Time Dynamics of the Formation of Hydrated Electrons upon Irradiation of Water Clusters with Extreme Ultraviolet Light.

Free electrons in a polar liquid can form a bound state via interaction with the molecular environment. This so-called hydrated electron state in water is of fundamental importance, e.g., in cellular biology or radiation chemistry. Hydrated electrons are highly reactive radicals that can either directly interact with DNA or enzymes, or form highly excited hydrogen (H^{*}) after being captured by protons. Here, we investigate the formation of the hydrated electron in real-time employing extreme ultraviolet femtosecond pulses from a free electron laser, in this way observing the initial steps of the hydration process. Using time-resolved photoelectron spectroscopy we find formation timescales in the low picosecond range and resolve the prominent dynamics of forming excited hydrogen states.

Deep-hole drilling of amorphous silica glass by extreme ultraviolet femtosecond pulses

A free-electron laser (FEL) is a robust tool for studying the interaction of intense X-rays with matter. In this study, we investigate the damage threshold and morphology of fused silica irradiated by extreme ultraviolet femtosecond pulses of a FEL. The experimental results indicate the superiority of the FEL processing. The FEL-damage threshold of fused silica at a wavelength of 13.5 nm is 0.17 J/cm2, which is 20 times lower than that of a near infrared (NIR) femtosecond laser. The relationship between the crater depth and laser fluence reveals that the effective absorption length is αeff−1 = 58 nm. The damage threshold and the absorption length are the key values for smooth crater formation. In addition, the formation of rim structures and microcracks, which are usually the critical issues in NIR laser processing, cannot be found in the interaction region. The hole diameter is maintained below the beam size at the exit.

Mapping the Complete Reaction Path of a Complex Photochemical Reaction.

We probe the dynamics of dissociating CS_{2} molecules across the entire reaction pathway upon excitation. Photoelectron spectroscopy measurements using laboratory-generated femtosecond extreme ultraviolet pulses monitor the competing dissociation, internal conversion, and intersystem crossing dynamics. Dissociation occurs either in the initially excited singlet manifold or, via intersystem crossing, in the triplet manifold. Both product channels are monitored and show that, despite being more rapid, the singlet dissociation is the minor product and that triplet state products dominate the final yield. We explain this by a consideration of accurate potential energy curves for both the singlet and triplet states. We propose that rapid internal conversion stabilizes the singlet population dynamically, allowing for singlet-triplet relaxation via intersystem crossing and the efficient formation of spin-forbidden dissociation products on longer timescales. The study demonstrates the importance of measuring the full reaction pathway for defining accurate reaction mechanisms.

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.

Interference effects in angular streaking with a rotating terahertz field

A method of angular streaking with a rotating terahertz electric field for photoelectrons produced by femtosecond extreme ultraviolet pulses is suggested and theoretically analyzed. The method can be used for free electron laser (FEL) pulse characterization on a shot-to-shot basis. It is shown that in related measurements an interesting phenomenon appears: formation of very bright and sharp features in the angular resolved electron spectra measured in the plane perpendicular to the collinear beam direction. These features are similar to the conventional caustics in the wave propagation. The caustics are accompanied by a well-developed interference structure. The intensity distribution along the caustic is determined by the envelope of the FEL pulse.

Bright high-repetition-rate source of narrowband extreme-ultraviolet harmonics beyond 22 eV.

Novel table-top sources of extreme-ultraviolet light based on high-harmonic generation yield unique insight into the fundamental properties of molecules, nanomaterials or correlated solids, and enable advanced applications in imaging or metrology. Extending high-harmonic generation to high repetition rates portends great experimental benefits, yet efficient extreme-ultraviolet conversion of correspondingly weak driving pulses is challenging. Here, we demonstrate a highly-efficient source of femtosecond extreme-ultraviolet pulses at 50-kHz repetition rate, utilizing the ultraviolet second-harmonic focused tightly into Kr gas. In this cascaded scheme, a photon flux beyond ≈3 × 1013 s−1 is generated at 22.3 eV, with 5 × 10−5 conversion efficiency that surpasses similar harmonics directly driven by the fundamental by two orders-of-magnitude. The enhancement arises from both wavelength scaling of the atomic dipole and improved spatio-temporal phase matching, confirmed by simulations. Spectral isolation of a single 72-meV-wide harmonic renders this bright, 50-kHz extreme-ultraviolet source a powerful tool for ultrafast photoemission, nanoscale imaging and other applications.

Mapping spin-orbit activated interchannel coupling

Recent advances in the generation of femtosecond extreme ultraviolet pulses have opened up the possibility to study final-state wave functions in photoemission experiments. Here, we investigate, for the first time using femtosecond time-resolved core-level spectroscopy, the feasibility of observing the buildup of a state correlation in a direct time domain. Giant changes in the ratio of photoemission cross-sections of spin-orbit split core states, the branching ratio, are identified. Multi-configuration Dirac-Fock calculations show that the origin of the branching ratio deviation is due to strong core-valence interactions. The possibility to tune this interaction by charge transfer offers intriguing opportunities to study correlation effects in solid and molecular systems in the future.

Novel Collective Autoionization Process Observed in Electron Spectra of He Clusters

The ionization dynamics of He nanodroplets irradiated with intense femtosecond extreme ultraviolet pulses of up to 1013 W/cm2 power density have been investigated by photoelectron spectroscopy. Helium droplets were resonantly excited to atomiclike 2p states with a photon energy of 21.4eV, below the ionization potential (Ip), and directly into the ionization continuum with 42.8eV photons. While electron emission following direct ionization above Ip is well explained within a model based on a sequence of direct electron emission events, the resonant excitation provides evidence of a new, collective ionization mechanism involving many excited atomiclike 2p states. With increasing power density the direct photoline due to an interatomic Coulombic decay disappears. It indicates that ionization occurs due to energy exchange between at least three excited atoms proceeding on a femtosecond time scale. In agreement with recent theoretical work the novel ionization process is very efficient and it is expected to be important for many other systems.

Snapshots of non-equilibrium Dirac carrier distributions in graphene

The optical properties of graphene are made unique by the linear band structure and the vanishing density of states at the Dirac point. It has been proposed that even in the absence of a bandgap, a relaxation bottleneck at the Dirac point may allow for population inversion and lasing at arbitrarily long wavelengths. Furthermore, efficient carrier multiplication by impact ionization has been discussed in the context of light harvesting applications. However, all of these effects are difficult to test quantitatively by measuring the transient optical properties alone, as these only indirectly reflect the energy- and momentum-dependent carrier distributions. Here, we use time- and angle-resolved photoemission spectroscopy with femtosecond extreme-ultraviolet pulses to directly probe the non-equilibrium response of Dirac electrons near the K-point of the Brillouin zone. In lightly hole-doped epitaxial graphene samples, we explore excitation in the mid- and near-infrared, both below and above the minimum photon energy for direct interband transitions. Whereas excitation in the mid-infrared results only in heating of the equilibrium carrier distribution, interband excitations give rise to population inversion, suggesting that terahertz lasing may be possible. However, in neither excitation regime do we find any indication of carrier multiplication, questioning the applicability of graphene for light harvesting.

Collapse of long-range charge order tracked by time-resolved photoemission at high momenta

Intense femtosecond (10(-15) s) light pulses can be used to transform electronic, magnetic and structural order in condensed-matter systems on timescales of electronic and atomic motion. This technique is particularly useful in the study and in the control of materials whose physical properties are governed by the interactions between multiple degrees of freedom. Time- and angle-resolved photoemission spectroscopy is in this context a direct and comprehensive, energy- and momentum-selective probe of the ultrafast processes that couple to the electronic degrees of freedom. Previously, the capability of such studies to access electron momentum space away from zero momentum was, however, restricted owing to limitations of the available probing photon energy. Here, using femtosecond extreme-ultraviolet pulses delivered by a high-harmonic-generation source, we use time- and angle-resolved photoemission spectroscopy to measure the photoinduced vaporization of a charge-ordered state in the potential excitonic insulator 1T-TiSe(2 )(refs 12, 13). By way of stroboscopic imaging of electronic band dispersions at large momentum, in the vicinity of the edge of the first Brillouin zone, we reveal that the collapse of atomic-scale periodic long-range order happens on a timescale as short as 20 femtoseconds. The surprisingly fast response of the system is assigned to screening by the transient generation of free charge carriers. Similar screening scenarios are likely to be relevant in other photoinduced solid-state transitions and may generally determine the response times. Moreover, as electron states with large momenta govern fundamental electronic properties in condensed matter systems, we anticipate that the experimental advance represented by the present study will be useful to study the ultrafast dynamics and microscopic mechanisms of electronic phenomena in a wide range of materials.

Grating monochromators for the spectral selection of femtosecond extreme-ultraviolet pulses

The design of grating monochromators for the spectral selection of extreme-ultraviolet femtosecond pulses without altering significantly the pulse time duration is discussed here. Time-preserving monochromators are realized in a single-grating configuration if the number of illuminated grooves is minimum for a given spectral resolution; therefore the grating time response is close to the Fourier limit for such a resolution. The classical-diffraction mount and the off-plane mount are compared for applications in the extreme-ultraviolet region—the classical mount should be preferred for monochromators with time responses in the 100–200 fs range, while the off-plane mount gives responses in the 10–50 fs range, and is therefore suitable to realize femtosecond time-preserving monochromators.