Femtosecond Duration Research Articles

Efficiently parallelized modeling of tightly focused, large bandwidth laser pulses

The Stratton–Chu integral representation of electromagnetic fields is used to study the spatio-temporal properties of large bandwidth laser pulses focused by high numerical aperture mirrors. We review the formal aspects of the derivation of diffraction integrals from the Stratton–Chu representation and discuss the use of the Hadamard finite part in the derivation of the physical optics approximation. By analyzing the formulation we show that, for the specific case of a parabolic mirror, the integrands involved in the description of the reflected field near the focal spot do not possess the strong oscillations characteristic of diffraction integrals. Consequently, the integrals can be evaluated with simple and efficient quadrature methods rather than with specialized, more costly approaches. We report on the development of an efficiently parallelized algorithm that evaluates the Stratton–Chu diffraction integrals for incident fields of arbitrary temporal and spatial dependence. This method has the advantage that its input is the unfocused field coming from the laser chain, which is experimentally known with high accuracy. We use our method to show that the reflection of a linearly polarized Gaussian beam of femtosecond duration off a high numerical aperture parabolic mirror induces ellipticity in the dominant field components and generates strong longitudinal components. We also estimate that future high-power laser facilities may reach intensities of .

Structure Determination Using X-Ray Free-Electron Laser Pulses.

The intense X-ray pulses from free-electron lasers, of only femtoseconds duration, outrun most of the processes that lead to structural degradation in X-ray exposures of macromolecules. Using these sources it is therefore possible to increase the dose to macromolecular crystals by several orders of magnitude higher than usually tolerable in conventional measurements, allowing crystal size to be decreased dramatically in diffraction measurements and without the need to cool the sample. Such pulses lead to the eventual vaporization of the sample, which has required a measurement approach, called serial crystallography, of consolidating snapshot diffraction patterns of many individual crystals. This in turn has further separated the connection between dose and obtainable diffraction information, with the only requirement from a single pattern being that to give enough information to place it, in three-dimensional reciprocal space, in relation to other patterns. Millions of extremely weak patterns can be collected and combined in this way, requiring methods to rapidly replenish the sample into the beam while generating the lowest possible background . The method is suited to time-resolved measurements over timescales below 1 ps to several seconds, and opens new opportunities for phasing. Some straightforward considerations of achievable signal levels are discussed and compared with a wide variety of recent experiments carried out at XFEL, synchrotron, and even laboratory sources, to discuss the capabilities of these new approaches and give some perspectives on their further development.

A perspective for investigating photo-induced molecular dynamics from within with femtosecond free electron lasers.

Photo-induced molecular dynamics can now be investigated using free electron lasers (FELs) whose attributes are unprecedented brightness, few femtosecond pulses duration and in the near future few hundreds of attosecond pulse duration. These relatively new tools are utilized to investigate photon-induced physical and chemical processes by ionizing inner-shell electrons and thus unlocking molecular dynamics from within.

Advances and opportunities of ultrafast laser synthesis and processing

Abstract

Femtosecond plasmon and photon wave packets excited by a high-energy electron on a metal or dielectric surface

Swift electrons generate coherent transition radiation (TR) when crossing a material surface, as well as surface plasmon polaritons (SPPs) when the material is metallic. We present analytical and numerical calculations that describe the time- and space-dependent electric fields of TR and SPPs induced by 30--300 keV electrons on a Drude metal surface. The generated SPPs form wave packets a few-hundred femtoseconds in duration, depending on the material permittivity. High-frequency components close to the plasmon resonance are strongly damped, causing the wave packets to shift to lower frequencies as they propagate further. TR is emitted to the far field as ultrashort wave packets consisting of just a few optical cycles, with an intensity and angle dependence that is determined by the material permittivity. The excitation reaches its peak amplitude within a few femtoseconds and then drops off strongly for longer times. From a correlation between material permittivity and the calculated emission behavior, we determine qualitative predictions of the TR evolution for any given material. The results presented here provide key insights into the mechanisms enabling swift electrons to serve as nanoscale optical excitation sources.

Corrugated structure insertion for extending the SASE bandwidth up to 3% at the European XFEL

The usage of x-ray free electron laser (XFEL) in femtosecond nanocrystallography involves sequential illumination of many small crystals of arbitrary orientation. Hence a wide radiation bandwidth will be useful in order to obtain and to index a larger number of Bragg peaks used for determination of the crystal orientation.Considering the baseline configuration of the European XFEL in Hamburg, and based on beam dynamics simulations, we demonstrate here that the usage of corrugated structures allows for a considerable increase in radiation bandwidth. Data collection with a 3% bandwidth, a few microjoule radiation pulse energy, a few femtosecond pulse duration, and a photon energy of 5.4keV is possible.For this study we have developed an analytical modal representation of the short-range wake function of the flat corrugated structures for arbitrary offsets of the source and the witness particles.

X-ray laser-induced electron dynamics observed by femtosecond diffraction from nanocrystals of Buckminsterfullerene.

X-ray free-electron lasers (XFELs) deliver x-ray pulses with a coherent flux that is approximately eight orders of magnitude greater than that available from a modern third-generation synchrotron source. The power density of an XFEL pulse may be so high that it can modify the electronic properties of a sample on a femtosecond time scale. Exploration of the interaction of intense coherent x-ray pulses and matter is both of intrinsic scientific interest and of critical importance to the interpretation of experiments that probe the structures of materials using high-brightness femtosecond XFEL pulses. We report observations of the diffraction of extremely intense 32-fs nanofocused x-ray pulses by a powder sample of crystalline C60. We find that the diffraction pattern at the highest available incident power significantly differs from the one obtained using either third-generation synchrotron sources or XFEL sources operating at low output power and does not correspond to the diffraction pattern expected from any known phase of crystalline C60. We interpret these data as evidence of a long-range, coherent dynamic electronic distortion that is driven by the interaction of the periodic array of C60 molecular targets with intense x-ray pulses of femtosecond duration.

The tight focusing of ultrashort pulse with dielectric cylinder

The tight focusing of light is observed during the propagation of a femtosecond laser pulses duration of 17 fs and 8 fs trough the dielectric cylinder with a refractive index n = 1.59 and the radius R = 0.7152λ0. It allows to reach the focal spot width at half intensity equal 0.235λ0.

A numerical solution algorithm and its application to studies of pulsed light fields propagation

A new method for studies of pulsed laser beams propagation in a turbulent atmosphere was proposed. The algorithm of numerical simulation is based on the solution of wave parabolic equation for complex spectral amplitude of wave field using method of splitting into physical factors. Examples of the use of the algorithm in the case the propagation pulsed Laguerre-Gaussian beams of femtosecond duration in the turbulence atmosphere has been shown.

Emission of terahertz waves in the interaction of a laser pulse with clusters

A theory of generation of terahertz radiation in the interaction of a femtosecond laser pulse with a spherical cluster is developed for the case in which the density of free electrons in the cluster plasma exceeds the critical value. The spectral, angular, and energy characteristics of the emitted terahertz radiation are investigated, as well as its spatiotemporal structure. It is shown that the directional pattern of radiation has a quadrupole structure and that the emission spectrum has a broad maximum at a frequency nearly equal to the reciprocal of the laser pulse duration. It is found that the total radiated energy depends strongly on the cluster size. Analysis of the spatiotemporal profile of the terahertz signal shows that it has a femtosecond duration and contains only two oscillation cycles.

Demonstration of acceleration of relativistic electrons at a dielectric microstructure using femtosecond laser pulses.

Acceleration of electrons using laser-driven dielectric microstructures is a promising technology for the miniaturization of particle accelerators. Achieving the desired GV m-1 accelerating gradients is possible only with laser pulse durations shorter than ∼1 ps. In this Letter, we present, to the best of our knowledge, the first demonstration of acceleration of relativistic electrons at a dielectric microstructure driven by femtosecond duration laser pulses. Using this technique, an electron accelerating gradient of 690±100 MV m-1 was measured-a record for dielectric laser accelerators.

Watt-Level Ultrafast Fiber Laser Based on Weak Evanescent Interaction With Reduced Graphene Oxide

We propose a Watt-level, all-fiber, ultrafast Er/Yb-codoped double-clad fiber laser mode-locked by reduced graphene oxide (rGO) interacting with photonic crystal fiber (PCF) ultraweakly. The rGO solution is filled into the cladding holes of PCF, and after evaporation, the rGO flakes, contributing saturable absorption and high nonlinearity, interact with a light intensity of only 1/ $10^{7}$ of that in the center of PCF. This ultraweakly interacting structure can enhance the thermal damage threshold and decrease the accumulated nonlinearity, which is proved to be an excellent choice for high-power mode-locked laser. By incorporating the saturable absorber into an Er/Yb-codoped fiber ring cavity, stable soliton laser with femtosecond duration is generated, and harmonic mode-locking is formed when increasing pump strength. The maximum average power of 1.14 W is obtained. To the best of our knowledge, this report is the highest power obtained directly from an all-fiber, graphene-mode-locked laser system operating with fundamental transverse mode. In addition, the experimental results demonstrate that our proposed structure is effective in generating high-power pulses when some other materials are used, including but not limited to graphene oxide, carbon nanotubes, topological insulator, or metal nanoparticles.

Attosecond nonlinear polarization and light-matter energy transfer in solids.

Electric-field-induced charge separation (polarization) is the most fundamental manifestation of the interaction of light with matter and a phenomenon of great technological relevance. Nonlinear optical polarization produces coherent radiation in spectral ranges inaccessible by lasers and constitutes the key to ultimate-speed signal manipulation. Terahertz techniques have provided experimental access to this important observable up to frequencies of several terahertz. Here we demonstrate that attosecond metrology extends the resolution to petahertz frequencies of visible light. Attosecond polarization spectroscopy allows measurement of the response of the electronic system of silica to strong (more than one volt per ångström) few-cycle optical (about 750 nanometres) fields. Our proof-of-concept study provides time-resolved insight into the attosecond nonlinear polarization and the light-matter energy transfer dynamics behind the optical Kerr effect and multi-photon absorption. Timing the nonlinear polarization relative to the driving laser electric field with sub-30-attosecond accuracy yields direct quantitative access to both the reversible and irreversible energy exchange between visible-infrared light and electrons. Quantitative determination of dissipation within a signal manipulation cycle of only a few femtoseconds duration (by measurement and ab initio calculation) reveals the feasibility of dielectric optical switching at clock rates above 100 terahertz. The observed sub-femtosecond rise of energy transfer from the field to the material (for a peak electric field strength exceeding 2.5 volts per ångström) in turn indicates the viability of petahertz-bandwidth metrology with a solid-state device.

Serial femtosecond crystallography: A revolution in structural biology

Macromolecular crystallography at synchrotron sources has proven to be the most influential method within structural biology, producing thousands of structures since its inception. While its utility has been instrumental in progressing our knowledge of structures of molecules, it suffers from limitations such as the need for large, well-diffracting crystals, and radiation damage that can hamper native structural determination. The recent advent of X-ray free electron lasers (XFELs) and their implementation in the emerging field of serial femtosecond crystallography (SFX) has given rise to a remarkable expansion upon existing crystallographic constraints, allowing structural biologists access to previously restricted scientific territory. SFX relies on exceptionally brilliant, micro-focused X-ray pulses, which are femtoseconds in duration, to probe nano/micrometer sized crystals in a serial fashion. This results in data sets comprised of individual snapshots, each capturing Bragg diffraction of single crystals in random orientations prior to their subsequent destruction. Thus structural elucidation while avoiding radiation damage, even at room temperature, can now be achieved. This emerging field has cultivated new methods for nanocrystallogenesis, sample delivery, and data processing. Opportunities and challenges within SFX are reviewed herein.

Characterization of a silica-PVA hybrid for high density and stable silver dissolution

A silica and polyvinyl alcohol (PVA) hybrid material mixed with a high density of silver ions is synthesised and characterized in this work. The hybrid material can be cast into thick films, which we determined to be homogeneous using Raman spectroscopy. We observed that the silver ions remain stable in the material over time and at temperatures of 100 °C, which represents a marked improvement over previous solid solutions of silver. Differential scanning calorimetry and thermogravimetric analysis indicate the rapid activation of silver at 173 °C, resulting in a dense formation of silver nanoparticles within the hybrid. The activation of silver was also demonstrated in 3-dimensional geometries using femtosecond duration laser pulses. These results illustrate the silica-PVA hybrid is an attractive material for developing silver-insulator composites.

Laser-driven nonadiabatic electron dynamics in molecules

In this review, we briefly summarize more than a decade of experimental and theoretical investigations regarding the nonadiabatic electron response to intense femtosecond duration laser fields in a variety of molecular systems. Historically, experimental signatures of nonadiabaticity have emerged readily in large, conjugated, or multi-electron systems, disrupting fragmentation behavior and modulating observed rates of ionization. As model theoretical studies performed in H2+ and other diatomic species show, departure from traditional quasi-static or cycle-averaged descriptions of laser-induced ionization is often necessary to accommodate the rich and frequently counterintuitive electron dynamics that characterize the nonadiabatic response. Nonadiabatic effects such as transient electron localization or the observation of multiple ionization bursts per driving field cycle possess the capacity to modulate the signal of many strong-field physical effects, such as high-order harmonic generation, photoelectron momentum distributions, and molecular fragmentation products. As the advancement of experimental technologies expands the pursuit of laser-driven physics further into the mid-infrared wavelength regime, we suggest that these nonadiabatic effects will become increasingly pronounced and relevant to the imaging and control of a wide array of molecular species.

Laser-driven powerful kHz hard x-ray source

A powerful hard x-ray source based on laser plasma interaction is developed. By introducing the kHz, 800nm pulses onto a rotating molybdenum (Mo) disk target, intense Mo Kα x-rays are emitted with suppressed bremsstrahlung background. Results obtained with different laser intensities suggest that the dominant absorption mechanism responsible for the high conversion efficiency is vacuum heating (VH). The high degree of spatial coherence is verified. With the high average flux and a source size comparable to the laser focus spot, absorption contrast imaging and phase contrast imaging are carried out to test the imaging capability of the source. Not only useful for imaging application, this compact x-ray source is also holding great potential for ultrafast x-ray diffraction (XRD) due to the intrinsic merits such as femtosecond pulse duration and natural synchronization with the driving laser pulses.

Observation of femtosecond X-ray interactions with matter using an X-ray–X-ray pump–probe scheme

Resolution in the X-ray structure determination of noncrystalline samples has been limited to several tens of nanometers, because deep X-ray irradiation required for enhanced resolution causes radiation damage to samples. However, theoretical studies predict that the femtosecond (fs) durations of X-ray free-electron laser (XFEL) pulses make it possible to record scattering signals before the initiation of X-ray damage processes; thus, an ultraintense X-ray beam can be used beyond the conventional limit of radiation dose. Here, we verify this scenario by directly observing femtosecond X-ray damage processes in diamond irradiated with extraordinarily intense (∼10(19) W/cm(2)) XFEL pulses. An X-ray pump-probe diffraction scheme was developed in this study; tightly focused double-5-fs XFEL pulses with time separations ranging from sub-fs to 80 fs were used to excite (i.e., pump) the diamond and characterize (i.e., probe) the temporal changes of the crystalline structures through Bragg reflection. It was found that the pump and probe diffraction intensities remain almost constant for shorter time separations of the double pulse, whereas the probe diffraction intensities decreased after 20 fs following pump pulse irradiation due to the X-ray-induced atomic displacement. This result indicates that sub-10-fs XFEL pulses enable conductions of damageless structural determinations and supports the validity of the theoretical predictions of ultraintense X-ray-matter interactions. The X-ray pump-probe scheme demonstrated here would be effective for understanding ultraintense X-ray-matter interactions, which will greatly stimulate advanced XFEL applications, such as atomic structure determination of a single molecule and generation of exotic matters with high energy densities.

Nonuniform Atmospheric Scatter of Short-Pulse Optical Radiation

The results of calculation of the mean intensity of spatially partially coherent pulsed optical beam scattered by an atmospheric layer are presented. It is shown that in contrast to cw radiation, which scatters uniformly, the scatter of pulsed beam becomes nonuniform for shorter pulses. For the femtosecond pulse duration the backscattered radiation is localized near the strictly backward direction in the area with transverse dimensions comparable with the initial size of the sensing beam.

The Laser-assisted photoelectric effect of He, Ne, Ar and Xe in intense extreme ultraviolet and infrared laser fields

In this paper, we report results on two-colour above-threshold ionisation, where extreme ultraviolet pulses of femtosecond duration were synchronised to intense infrared laser pulses of picosecond duration, in order to study the laser-assisted photoelectric effect of atomic helium, neon, krypton and xenon which leads to the appearance of characteristic sidebands in the photoelectron spectra. The observed trends are found to be well described by a simple model based on the soft-photon approximation, at least for the relatively low optical intensities of up to employed in these early experiments.