Showing papers on "Femtosecond published in 2017"

Metallic MXene Saturable Absorber for Femtosecond Mode-Locked Lasers.

Abstract: 2D transition metal carbides, nitrides, and carbonitides called MXenes have attracted much attention due to their outstanding properties. However, MXene's potential in laser technology is not explored. It is demonstrated here that Ti3 CN, one of MXene compounds, can serve as an excellent mode-locker that can produce femtosecond laser pulses from fiber cavities. Stable laser pulses with a duration as short as 660 fs are readily obtained at a repetition rate of 15.4 MHz and a wavelength of 1557 nm. Density functional theory calculations show that Ti3 CN is metallic, in contrast to other 2D saturable absorber materials reported so far to be operative for mode-locking. 2D structural and electronic characteristics are well conserved in their stacked form, possibly due to the unique interlayer coupling formed by MXene surface termination groups. Noticeably, the calculations suggest a promise of MXenes in broadband saturable absorber applications due to metallic characteristics, which agrees well with the experiments of passively Q-switched lasers using Ti3 CN at wavelengths of 1558 and 1875 nm. This study provides a valuable strategy and intuition for the development of nanomaterial-based saturable absorbers opening new avenues toward advanced photonic devices based on MXenes.

Light-field-driven currents in graphene

Abstract: The ability to steer electrons using the strong electromagnetic field of light has opened up the possibility of controlling electron dynamics on the sub-femtosecond (less than 10-15 seconds) timescale. In dielectrics and semiconductors, various light-field-driven effects have been explored, including high-harmonic generation, sub-optical-cycle interband population transfer and the non-perturbative change of the transient polarizability. In contrast, much less is known about light-field-driven electron dynamics in narrow-bandgap systems or in conductors, in which screening due to free carriers or light absorption hinders the application of strong optical fields. Graphene is a promising platform with which to achieve light-field-driven control of electrons in a conducting material, because of its broadband and ultrafast optical response, weak screening and high damage threshold. Here we show that a current induced in monolayer graphene by two-cycle laser pulses is sensitive to the electric-field waveform, that is, to the exact shape of the optical carrier field of the pulse, which is controlled by the carrier-envelope phase, with a precision on the attosecond (10-18 seconds) timescale. Such a current, dependent on the carrier-envelope phase, shows a striking reversal of the direction of the current as a function of the driving field amplitude at about two volts per nanometre. This reversal indicates a transition of light-matter interaction from the weak-field (photon-driven) regime to the strong-field (light-field-driven) regime, where the intraband dynamics influence interband transitions. We show that in this strong-field regime the electron dynamics are governed by sub-optical-cycle Landau-Zener-Stuckelberg interference, composed of coherent repeated Landau-Zener transitions on the femtosecond timescale. Furthermore, the influence of this sub-optical-cycle interference can be controlled with the laser polarization state. These coherent electron dynamics in graphene take place on a hitherto unexplored timescale, faster than electron-electron scattering (tens of femtoseconds) and electron-phonon scattering (hundreds of femtoseconds). We expect these results to have direct ramifications for band-structure tomography and light-field-driven petahertz electronics.

Time-resolved x-ray absorption spectroscopy with a water window high-harmonic source

Abstract: Time-resolved x-ray absorption spectroscopy (TR-XAS) has so far practically been limited to large-scale facilities, to subpicosecond temporal resolution, and to the condensed phase. We report the realization of TR-XAS with a temporal resolution in the low femtosecond range by developing a tabletop high-harmonic source reaching up to 350 electron volts, thus partially covering the spectral region of 280 to 530 electron volts, where water is transmissive. We used this source to follow previously unexamined light-induced chemical reactions in the lowest electronic states of isolated CF 4 + and SF 6 + molecules in the gas phase. By probing element-specific core-to-valence transitions at the carbon K-edge or the sulfur L-edges, we characterized their reaction paths and observed the effect of symmetry breaking through the splitting of absorption bands and Rydberg-valence mixing induced by the geometry changes.

Temporal solitons in microresonators driven by optical pulses

Abstract: Continuous-wave laser-driven, high-Q Kerr–nonlinear optical microresonators have enabled the generation of optical frequency combs, ultralow-noise microwaves and ultrashort optical pulses at tens of gigahertz repetition rate. Here, we break with the paradigm of the continuous-wave driving and instead use periodic, picosecond optical pulses. In a fibre-based Fabry–Perot microresonator we observe the deterministic generation of stable femtosecond dissipative cavity solitons ‘on top’ of the resonantly enhanced driving pulses. The solitons lock to the driving pulse, which enables direct all-optical control of the soliton's repetition rate and tuning of its carrier-envelope offset frequency. When compared with continuous-wave-driven microresonators or non-resonant pulsed supercontinuum generation, this new approach is more efficient and can yield broadband frequency combs at an average driving power significantly below the continuous-wave parametric threshold. Bridging the fields of continuous-wave-driven resonant and pulse-driven non-resonant nonlinear optics, these results enable efficient microresonator frequency combs, resonant supercontinuum generation and microphotonic pulse compression. By driving a high-Q fibre-based Fabry–Perot microresonator with periodic, picosecond optical pulses, deterministic generation of stable femtosecond dissipative cavity solitons has been experimentally realized.

Ultrafast nonthermal photo-magnetic recording in a transparent medium

Abstract: Discovering ways to control the magnetic state of media with the lowest possible production of heat and at the fastest possible speeds is important in the study of fundamental magnetism, with clear practical potential. In metals, it is possible to switch the magnetization between two stable states (and thus to record magnetic bits) using femtosecond circularly polarized laser pulses. However, the switching mechanisms in these materials are directly related to laser-induced heating close to the Curie temperature. Although several possible routes for achieving all-optical switching in magnetic dielectrics have been discussed, no recording has hitherto been demonstrated. Here we describe ultrafast all-optical photo-magnetic recording in transparent films of the dielectric cobalt-substituted garnet. A single linearly polarized femtosecond laser pulse resonantly pumps specific d-d transitions in the cobalt ions, breaking the degeneracy between metastable magnetic states. By changing the polarization of the laser pulse, we deterministically steer the net magnetization in the garnet, thus writing '0' and '1' magnetic bits at will. This mechanism outperforms existing alternatives in terms of the speed of the write-read magnetic recording event (less than 20 picoseconds) and the unprecedentedly low heat load (less than 6 joules per cubic centimetre).

Femtosecond x-ray spectroscopy of an electrocyclic ring-opening reaction

Abstract: The ultrafast light-activated electrocyclic ring-opening reaction of 1,3-cyclohexadiene is a fundamental prototype of photochemical pericyclic reactions. Generally, these reactions are thought to proceed through an intermediate excited-state minimum (the so-called pericyclic minimum), which leads to isomerization via nonadiabatic relaxation to the ground state of the photoproduct. Here, we used femtosecond (fs) soft x-ray spectroscopy near the carbon K-edge (~284 electron volts) on a tabletop apparatus to directly reveal the valence electronic structure of this transient intermediate state. The core-to-valence spectroscopic signature of the pericyclic minimum observed in the experiment was characterized, in combination with time-dependent density functional theory calculations, to reveal overlap and mixing of the frontier valence orbital energy levels. We show that this transient valence electronic structure arises within 60 ± 20 fs after ultraviolet photoexcitation and decays with a time constant of 110 ± 60 fs.

Femtosecond optical polarization switching using a cadmium oxide-based perfect absorber

Abstract: Ultrafast control of the polarization state of light may enable a plethora of applications in optics, chemistry and biology. However, conventional polarizing elements, such as polarizers and waveplates, are either static or possess only gigahertz switching speeds. Here, with the aid of high-mobility indium-doped cadmium oxide (CdO) as the gateway plasmonic material, we realize a high-quality factor Berreman-type perfect absorber at a wavelength of 2.08 μm. On sub-bandgap optical pumping, the perfect absorption resonance strongly redshifts because of the transient increase of the ensemble-averaged effective electron mass of CdO, which leads to an absolute change in the p-polarized reflectance from 1.0 to 86.3%. By combining the exceedingly high modulation depth with the polarization selectivity of the perfect absorber, we experimentally demonstrate a reflective polarizer with a polarization extinction ratio of 91 that can be switched on and off within 800 fs. Indium-doped cadmium oxide performs polarization switching on a subpicosecond timescale.

Nonlinear optical properties of metal nanoparticles: a review

Abstract: Metal nanoparticles (MNPs) hold great technological promise because of the possibility of engineering their electronic and optical properties through material design. One of the effective methods to fabricate MNPs is ion implantation. In this review, recent results on the nonlinear optical properties of nanoparticles (including copper, silver, gold, and bismuth nanoparticles) doped in various bases have been discussed. Some specific optical nonlinear properties, such as nonlinear refraction, two-photon absorption, and optical limiting, for femtosecond, picosecond, and nanosecond laser pulses have also been covered. In addition to ion implantation, we have summarized several other methods for the preparation of composite materials, and Z-scan has been used to study the nonlinear optical properties of these materials.

Femtosecond laser reshaping yields gold nanorods with ultranarrow surface plasmon resonances.

Abstract: The irradiation of gold nanorod colloids with a femtosecond laser can be tuned to induce controlled nanorod reshaping, yielding colloids with exceptionally narrow localized surface plasmon resonance bands. The process relies on a regime characterized by a gentle multishot reduction of the aspect ratio, whereas the rod shape and volume are barely affected. Successful reshaping can only occur within a narrow window of the heat dissipation rate: Low cooling rates lead to drastic morphological changes, and fast cooling has nearly no effect. Hence, a delicate balance must be achieved between irradiation fluence and surface density of the surfactant on the nanorods. This perfection process is appealing because it provides a simple, fast, reproducible, and scalable route toward gold nanorods with an optical response of exceptional quality, near the theoretical limit.

All Polarization-Maintaining Fiber Laser Architecture for Robust Femtosecond Pulse Generation

Abstract: We report on a novel architecture for robust mode-locked femtosecond fiber lasers using a nonlinear optical loop mirror with all polarization-maintaining fibers. Due to a nonreciprocal phase shift, the loop mirror can be operated in a compact and efficient reflection mode, offering the possibility to reach high repetition rates and easy implementation of tuning elements. In particular, longitudinal mode spacing and carrier-envelope offset frequency may be controlled in order to operate the laser as an optical frequency comb. We demonstrate femtosecond pulse generation at three different wavelengths (1030, 1565, and 2050 nm) using Ytterbium, Erbium, and co-doped Thulium–Holmium as gain media, respectively. Robust operation is achieved for a wide range of parameters, including repetition rates from 10 to 250 MHz.

Femtosecond electron-phonon lock-in by photoemission and x-ray free-electron laser.

Abstract: The interactions that lead to the emergence of superconductivity in iron-based materials remain a subject of debate. It has been suggested that electron-electron correlations enhance electron-phonon coupling in iron selenide (FeSe) and related pnictides, but direct experimental verification has been lacking. Here we show that the electron-phonon coupling strength in FeSe can be quantified by combining two time-domain experiments into a “coherent lock-in” measurement in the terahertz regime. X-ray diffraction tracks the light-induced femtosecond coherent lattice motion at a single phonon frequency, and photoemission monitors the subsequent coherent changes in the electronic band structure. Comparison with theory reveals a strong enhancement of the coupling strength in FeSe owing to correlation effects. Given that the electron-phonon coupling affects superconductivity exponentially, this enhancement highlights the importance of the cooperative interplay between electron-electron and electron-phonon interactions.

Plasmonic nano-printing: large-area nanoscale energy deposition for efficient surface texturing.

Abstract: The lossy nature of plasmonic wave due to absorption is shown to become an advantage for scaling-up a large area surface nanotexturing of transparent dielectrics and semiconductors by a self-organized sub-wavelength energy deposition leading to an ablation pattern—ripples—using this plasmonic nano-printing. Irreversible nanoscale modifications are delivered by surface plasmon polariton (SPP) using: (i) fast scan and (ii) cylindrical focusing of femtosecond laser pulses for a high patterning throughput. The mechanism of ripple formation on ZnS dielectric is experimentally proven to occur via surface wave at the substrate–plasma interface. The line focusing increase the ordering quality of ripples and facilitates fabrication over wafer-sized areas within a practical time span. Nanoprinting using SPP is expected to open new applications in photo-catalysis, tribology, and solar light harvesting via localized energy deposition rather scattering used in photonic and sensing applications based on re-scattering of SPP modes into far-field modes. Femtosecond laser pulses focused onto a dielectric induce ripples on its surface that are useful for photovoltaic and sensing applications. Light-driven excitation of surface charge waves—plasmons—achieves light localization on surfaces down to the deep-subwavelength nanoscale. Now, Hong-Bo Sun of Jilin University in China and co-workers from China and Australia have used surface plasmon polaritons to create permanent surface modifications whose period is smaller than the laser wavelength. They achieved this by using a cylindrical lens to create a line focus for near-infrared ultrashort laser pulses on silicon and zinc sulfide surfaces. This nanoprinting technique is well suited for texturing large areas on a wafer scale, since the patterning speed is determined simply by the repetition rate of the laser used. Potential applications include enhanced light harvesting for solar cells and improved photocatalysis.

Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites

Abstract: Femtosecond resolution electron scattering techniques are applied to resolve the first atomic-scale steps following absorption of a photon in the prototypical hybrid perovskite methylammonium lead iodide. Following above-gap photoexcitation, we directly resolve the transfer of energy from hot carriers to the lattice by recording changes in the mean square atomic displacements on 10-ps time scales. Measurements of the time-dependent pair distribution function show an unexpected broadening of the iodine-iodine correlation function while preserving the Pb-I distance. This indicates the formation of a rotationally disordered halide octahedral structure developing on picosecond time scales. This work shows the important role of light-induced structural deformations within the inorganic sublattice in elucidating the unique optoelectronic functionality exhibited by hybrid perovskites and provides new understanding of hot carrier-lattice interactions, which fundamentally determine solar cell efficiencies.

Relativistic electron beams driven by kHz single-cycle light pulses

Abstract: Laser-plasma acceleration(1,2) is an emerging technique for accelerating electrons to high energies over very short distances. The accelerated electron bunches have femtosecond duration(3,4), making them particularly relevant for applications such as ultrafast imaging(5) or femtosecond X-ray generation(6,7). Current laser-plasma accelerators deliver 100 MeV (refs 8-10) to GeV (refs 11, 12) electrons using Joule-class laser systems that are relatively large in scale and have low repetition rates, with a few shots per second at best. Nevertheless, extending laser-plasma acceleration to higher repetition rates would be extremely useful for applications requiring lower electron energy. Here, we use single-cycle laser pulses to drive high-quality MeV relativistic electron beams, thereby enabling kHz operation and dramatic downsizing of the laser system. Numerical simulations indicate that the electron bunches are only similar to 1 fs long. We anticipate that the advent of these kHz femtosecond relativistic electron sources will pave the way to applications with wide impact, such as ultrafast electron diffraction in materials(13,14) with an unprecedented sub-10 fs resolution(15).

The Role of Electronic and Phononic Excitation in the Optical Response of Monolayer WS2 after Ultrafast Excitation

Abstract: Transient changes of the optical response of WS2 monolayers are studied by femtosecond broadband pump–probe spectroscopy. Time-dependent absorption spectra are analyzed by tracking the line width broadening, bleaching, and energy shift of the main exciton resonance as a function of time delay after the excitation. Two main sources for the pump-induced changes of the optical response are identified. Specifically, we find an interplay between modifications induced by many-body interactions from photoexcited carriers and by the subsequent transfer of the excitation to the phonon system followed by cooling of the material through the heat transfer to the substrate.

Bioinspired Design of Underwater Superaerophobic and Superaerophilic Surfaces by Femtosecond Laser Ablation for Anti- or Capturing Bubbles.

Abstract: A micro-/nanoscale hierarchical rough structure inspired by the underwater superaerophobicity of fish scales was fabricated by ablation of a silicon surface by a femtosecond laser. The resultant silicon surface showed superhydrophilicity in air and became superaerophobic after immersion in water. Additionally, inspired by the underwater superaerophilicity of lotus leaves, we showed that the polydimethylsiloxane surface after femtosecond laser ablation exhibits superhydrophobicity in air and becomes superaerophilic in water. The underwater superaerophobic surface showed excellent antibubble ability, whereas the underwater superaerophilic surface could absorb and capture air bubbles in a water medium. The experimental results revealed that the in-air superhydrophilic surface generally shows superaerophobicity in water and that the in-air superhydrophobic surface generally shows underwater superaerophilicity. An underwater superaerophobic porous aluminum sheet with through microholes was prepared, and this s...

Femtosecond response of polyatomic molecules to ultra-intense hard X-rays

Abstract: Upon exposure to ultra-intense, hard X-ray pulses, polyatomic molecules containing one heavy atom reach a much higher degree of ionization than do individual heavy atoms, contrary to previous assumptions X-ray free-electron lasers offer many new applications such as the ability to structurally probe fast biological processes This requires the use of hard and intense X-ray pulses, but the behaviour of matter under such conditions has not been fully explored Artem Rudenko et al show that when exposing small polyatomic molecules that contain one heavy atom to hard X-ray pulses with ultra-high intensities, the response is qualitatively different from what is seen in experiments carried out under less extreme conditions The observed ionization of the molecule is considerably enhanced compared to that of an individual heavy atom under the same conditions, owing to ultrafast charge transfer within the molecule that replenishes the electrons removed from the heavy atom, enabling further ionization Being able to account for this effect will aid further use of X-ray free-electron lasers for studying biological systems X-ray free-electron lasers enable the investigation of the structure and dynamics of diverse systems, including atoms, molecules, nanocrystals and single bioparticles, under extreme conditions1,2,3,4,5,6,7 Many imaging applications that target biological systems and complex materials use hard X-ray pulses with extremely high peak intensities (exceeding 1020 watts per square centimetre)3,5 However, fundamental investigations have focused mainly on the individual response of atoms and small molecules using soft X-rays with much lower intensities8,9,10,11,12,13,14,15,16,17 Studies with intense X-ray pulses have shown that irradiated atoms reach a very high degree of ionization, owing to multiphoton absorption8,12,13,18, which in a heteronuclear molecular system occurs predominantly locally on a heavy atom (provided that the absorption cross-section of the heavy atom is considerably larger than those of its neighbours) and is followed by efficient redistribution of the induced charge14,15,16,17,19,20 In serial femtosecond crystallography of biological objects—an application of X-ray free-electron lasers that greatly enhances our ability to determine protein structure2,3—the ionization of heavy atoms increases the local radiation damage that is seen in the diffraction patterns of these objects21,22 and has been suggested as a way of phasing the diffraction data23,24 On the basis of experiments using either soft or less-intense hard X-rays14,15,16,17,18,19,25, it is thought that the induced charge and associated radiation damage of atoms in polyatomic molecules can be inferred from the charge that is induced in an isolated atom under otherwise comparable irradiation conditions Here we show that the femtosecond response of small polyatomic molecules that contain one heavy atom to ultra-intense (with intensities approaching 1020 watts per square centimetre), hard (with photon energies of 83 kiloelectronvolts) X-ray pulses is qualitatively different: our experimental and modelling results establish that, under these conditions, the ionization of a molecule is considerably enhanced compared to that of an individual heavy atom with the same absorption cross-section This enhancement is driven by ultrafast charge transfer within the molecule, which refills the core holes that are created in the heavy atom, providing further targets for inner-shell ionization and resulting in the emission of more than 50 electrons during the X-ray pulse Our results demonstrate that efficient modelling of X-ray-driven processes in complex systems at ultrahigh intensities is feasible

Ultrafast magnetization reversal by picosecond electrical pulses

Abstract: The field of spintronics involves the study of both spin and charge transport in solid-state devices. Ultrafast magnetism involves the use of femtosecond laser pulses to manipulate magnetic order on subpicosecond time scales. We unite these phenomena by using picosecond charge current pulses to rapidly excite conduction electrons in magnetic metals. We observe deterministic, repeatable ultrafast reversal of the magnetization of a GdFeCo thin film with a single sub–10-ps electrical pulse. The magnetization reverses in ~10 ps, which is more than one order of magnitude faster than any other electrically controlled magnetic switching, and demonstrates a fundamentally new electrical switching mechanism that does not require spin-polarized currents or spin-transfer/orbit torques. The energy density required for switching is low, projecting to only 4 fJ needed to switch a (20 nm) 3 cell. This discovery introduces a new field of research into ultrafast charge current–driven spintronic phenomena and devices.

Ultrabroadband single-cycle terahertz pulses with peak fields of 300 kV cm−1 from a metallic spintronic emitter

Abstract: We explore the capabilities of metallic spintronic thin-film stacks as a source of intense and broadband terahertz electromagnetic fields. For this purpose, we excite a W/CoFeB/Pt trilayer (thickness of 5.6 nm) on a large-area glass substrate (diameter of 7.5 cm) by a femtosecond laser pulse (energy 5.5 mJ, duration 40 fs, and wavelength 800 nm). After focusing, the emitted terahertz pulse is measured to have a duration of 230 fs, a peak field of 300 kV cm−1, and an energy of 5 nJ. In particular, the waveform exhibits a gapless spectrum extending from 1 to 10 THz at 10% of its amplitude maximum, thereby facilitating nonlinear control over matter in this difficult-to-reach frequency range on the sub-picosecond time scale.

Refractive index measurements of photo-resists for three-dimensional direct laser writing

Abstract: Femtosecond 3D printing is an important technology for manufacturing of nano- and microscopic devices and elements. Crucial for the design of such structures is the detailed knowledge of the refractive index in the visible and near-infrared spectral range and its dispersion. Here, we characterize 5 photoresists that are used with femtosecond 3D direct laser writers, namely IP-S, IP-Dip, IP-L, IP-G, and OrmoComp with a modified and automized Pulfrich refractometer setup, utilizing critical angles of total internal reflection. We achieve an accuracy of 5⋅10−4 and reference our values to a BK-7 glass plate. We also give Abbe numbers and Schott Catalog numbers of the different resists. Their refractive indices are in the 1.49-1.57 range, while their Abbe numbers are in the range between 35 and 51.

Optically Clear and Resilient Free-Form µ-Optics 3D-Printed via Ultrafast Laser Lithography

Abstract: We introduce optically clear and resilient free-form micro-optical components of pure (non-photosensitized) organic-inorganic SZ2080 material made by femtosecond 3D laser lithography (3DLL). This is advantageous for rapid printing of 3D micro-/nano-optics, including their integration directly onto optical fibers. A systematic study of the fabrication peculiarities and quality of resultant structures is performed. Comparison of microlens resiliency to continuous wave (CW) and femtosecond pulsed exposure is determined. Experimental results prove that pure SZ2080 is ∼20 fold more resistant to high irradiance as compared with standard lithographic material (SU8) and can sustain up to 1.91 GW/cm2 intensity. 3DLL is a promising manufacturing approach for high-intensity micro-optics for emerging fields in astro-photonics and atto-second pulse generation. Additionally, pyrolysis is employed to homogeneously shrink structures up to 40% by removing organic SZ2080 constituents. This opens a promising route towards downscaling photonic lattices and the creation of mechanically robust glass-ceramic microstructures.

Ultrabroadband single-cycle terahertz pulses with peak fields of 300 kV cm$^{-1}$ from a metallic spintronic emitter

Abstract: To explore the capabilities of metallic spintronic thin-film stacks as a source of intense and broadband terahertz electromagnetic fields, we excite a W/CoFeB/Pt trilayer on a large-area glass substrate (diameter of 7.5 cm) by a femtosecond laser pulse (energy 5.5 mJ, duration 40 fs, wavelength 800 nm). After focusing, the emitted terahertz pulse is measured to have a duration of 230 fs, a peak field of 300 kV cm$^{-1}$ and an energy of 5 nJ. In particular, the waveform exhibits a gapless spectrum extending from 1 to 10 THz at 10% of amplitude maximum, thereby facilitating nonlinear control over matter in this difficult-to-reach frequency range and on the sub-picosecond time scale.

Biomimetic surface structuring using cylindrical vector femtosecond laser beams.

Abstract: We report on a new, single-step and scalable method to fabricate highly ordered, multi-directional and complex surface structures that mimic the unique morphological features of certain species found in nature. Biomimetic surface structuring was realized by exploiting the unique and versatile angular profile and the electric field symmetry of cylindrical vector (CV) femtosecond (fs) laser beams. It is shown that, highly controllable, periodic structures exhibiting sizes at nano-, micro- and dual- micro/nano scales can be directly written on Ni upon line and large area scanning with radial and azimuthal polarization beams. Depending on the irradiation conditions, new complex multi-directional nanostructures, inspired by the Shark’s skin morphology, as well as superhydrophobic dual-scale structures mimicking the Lotus’ leaf water repellent properties can be attained. It is concluded that the versatility and features variations of structures formed is by far superior to those obtained via laser processing with linearly polarized beams. More important, by exploiting the capabilities offered by fs CV fields, the present technique can be further extended to fabricate even more complex and unconventional structures. We believe that our approach provides a new concept in laser materials processing, which can be further exploited for expanding the breadth and novelty of applications.

Ultrafast radiative heat transfer

Abstract: Light absorption in conducting materials produces heating of their conduction electrons, followed by relaxation into phonons within picoseconds, and subsequent diffusion into the surrounding media over longer timescales. This conventional picture of optical heating is supplemented by radiative cooling, which typically takes place at an even lower pace, only becoming relevant for structures held in vacuum or under extreme thermal isolation. Here, we reveal an ultrafast radiative cooling regime between neighboring plasmon-supporting graphene nanostructures in which noncontact heat transfer becomes a dominant channel. We predict that more than 50% of the electronic heat energy deposited on a graphene disk can be transferred to a neighboring nanoisland within a femtosecond timescale. This phenomenon is facilitated by the combination of low electronic heat capacity and large plasmonic field concentration in doped graphene. Similar effects should occur in other van der Waals materials, thus opening an unexplored avenue toward efficient heat management.Electron relaxation, which is the dominant release channel of electronic heat in nanostructures, occurs with characteristic times of several picoseconds. Here, the authors predict that an ultrafast (femtosecond) radiative cooling regime takes place in plasmonically active neighboring graphene nanodisks prior to electron relaxation.

Magnetisation switching of FePt nanoparticle recording medium by femtosecond laser pulses

Abstract: Manipulation of magnetisation with ultrashort laser pulses is promising for information storage device applications. The dynamics of the magnetisation response depends on the energy transfer from the photons to the spins during the initial laser excitation. A material of special interest for magnetic storage are FePt nanoparticles, for which switching of the magnetisation with optical angular momentum was demonstrated recently. The mechanism remained unclear. Here we investigate experimentally and theoretically the all-optical switching of FePt nanoparticles. We show that the magnetisation switching is a stochastic process. We develop a complete multiscale model which allows us to optimize the number of laser shots needed to switch the magnetisation of high anisotropy FePt nanoparticles in our experiments. We conclude that only angular momentum induced optically by the inverse Faraday effect will provide switching with one single femtosecond laser pulse.

Deterministic all-optical switching of synthetic ferrimagnets using single femtosecond laser pulses

Abstract: We experimentally demonstrate single-pulse all-optical switching in Pt/Co/Gd stacks using linearly polarized laser pulses. This shows that thermal single-pulse switching is not limited to ferrimagnetic alloys, but is also possible in ferrimagnetic multilayers that are highly suitable for future applications due to easy fabrication and (interface) engineering. Moreover, it is shown that the threshold fluence needed for the optical switch strongly depends on the thickness of the Co layer, with a remarkable low threshold fluence of $\ensuremath{\approx}1.2$ mJ/${\mathrm{cm}}^{2}$ for a Co thickness of 0.8 nm. Lastly, helicity-dependent measurements showed no significant effect of the magnetic circular dichroism in these thin magnetic layers.

Optically excited structural transition in atomic wires on surfaces at the quantum limit

Abstract: Transient control over the atomic potential-energy landscapes of solids could lead to new states of matter and to quantum control of nuclear motion on the timescale of lattice vibrations. Recently developed ultrafast time-resolved diffraction techniques combine ultrafast temporal manipulation with atomic-scale spatial resolution and femtosecond temporal resolution. These advances have enabled investigations of photo-induced structural changes in bulk solids that often occur on timescales as short as a few hundred femtoseconds. In contrast, experiments at surfaces and on single atomic layers such as graphene report timescales of structural changes that are orders of magnitude longer. This raises the question of whether the structural response of low-dimensional materials to femtosecond laser excitation is, in general, limited. Here we show that a photo-induced transition from the low- to high-symmetry state of a charge density wave in atomic indium (In) wires supported by a silicon (Si) surface takes place within 350 femtoseconds. The optical excitation breaks and creates In-In bonds, leading to the non-thermal excitation of soft phonon modes, and drives the structural transition in the limit of critically damped nuclear motion through coupling of these soft phonon modes to a manifold of surface and interface phonons that arise from the symmetry breaking at the silicon surface. This finding demonstrates that carefully tuned electronic excitations can create non-equilibrium potential energy surfaces that drive structural dynamics at interfaces in the quantum limit (that is, in a regime in which the nuclear motion is directed and deterministic). This technique could potentially be used to tune the dynamic response of a solid to optical excitation, and has widespread potential application, for example in ultrafast detectors.

Electron Vortices in Femtosecond Multiphoton Ionization

Abstract: Multiphoton ionization of potassium atoms with a sequence of two counter-rotating circularly polarized femtosecond laser pulses produces vortex-shaped photoelectron momentum distributions in the polarization plane describing Archimedean spirals. The pulse sequences are produced by polarization shaping and the three-dimensional photoelectron distributions are tomographically reconstructed from velocity map imaging measurements. We show that perturbative ionization leads to electron vortices with c_{6} rotational symmetry. A change from c_{6} to c_{4} rotational symmetry of the vortices is demonstrated for nonperturbative interaction.

FRAME: femtosecond videography for atomic and molecular dynamics

Abstract: Many important scientific questions in physics, chemistry and biology require effective methodologies to spectroscopically probe ultrafast intra- and inter-atomic/molecular dynamics However, current methods that extend into the femtosecond regime are capable of only point measurements or single-snapshot visualizations and thus lack the capability to perform ultrafast spectroscopic videography of dynamic single events Here we present a laser-probe-based method that enables two-dimensional videography at ultrafast timescales (femtosecond and shorter) of single, non-repetitive events The method is based on superimposing a structural code onto the illumination to encrypt a single event, which is then deciphered in a post-processing step This coding strategy enables laser probing with arbitrary wavelengths/bandwidths to collect signals with indiscriminate spectral information, thus allowing for ultrafast videography with full spectroscopic capability To demonstrate the high temporal resolution of our method, we present videography of light propagation with record high 200 femtosecond temporal resolution The method is widely applicable for studying a multitude of dynamical processes in physics, chemistry and biology over a wide range of time scales Because the minimum frame separation (temporal resolution) is dictated by only the laser pulse duration, attosecond-laser technology may further increase video rates by several orders of magnitude