The speed limit of optoelectronics.

Light-field driven charge motion links semiconductor technology to electric fields with attosecond temporal control. Motivated by ultimate-speed electron-based signal processing, strong-field excitation has been identified viable for the ultrafast manipulation of a solid's electronic properties but found to evoke perplexing post-excitation dynamics. Here, we report on single-photon-populating the conduction band of a wide-gap dielectric within approximately one femtosecond. We control the subsequent Bloch wavepacket motion with the electric field of visible light. The resulting current allows sampling optical fields and tracking charge motion driven by optical signals. Our approach utilizes a large fraction of the conduction-band bandwidth to maximize operating speed. We identify population transfer to adjacent bands and the associated group velocity inversion as the mechanism ultimately limiting how fast electric currents can be controlled in solids. Our results imply a fundamental limit for classical signal processing and suggest the feasibility of solid-state optoelectronics up to 1 PHz frequency.

Water-Window X-Ray Pulses from a Laser-Plasma Driven Undulator.

Femtosecond (fs) x-ray pulses are a key tool to study the structure and dynamics of matter on its natural length and time scale. To complement radio-frequency accelerator-based large-scale facilities, novel laser-based mechanisms hold promise for compact laboratory-scale x-ray sources. Laser-plasma driven undulator radiation in particular offers high peak-brightness, optically synchronized few-fs pulses reaching into the few-nanometer (nm) regime. To date, however, few experiments have successfully demonstrated plasma-driven undulator radiation. Those that have, typically operated at single and comparably long wavelengths. Here we demonstrate plasma-driven undulator radiation with octave-spanning tuneability at discrete wavelengths reaching from 13 nm to 4 nm. Studying spontaneous undulator radiation is an important step towards a plasma-driven free-electron laser. Our specific setup creates a photon pulse, which closely resembles the plasma electron bunch length and charge profile and thus might enable novel methods to characterize the longitudinal electron phase space.

Watt-scale 50-MHz source of single-cycle waveform-stable pulses in the molecular fingerprint region.

We report a coherent mid-infrared (MIR) source with a combination of broad spectral coverage (6-18 µm), high repetition rate (50 MHz), and high average power (0.5 W). The waveform-stable pulses emerge via intrapulse difference-frequency generation (IPDFG) in a GaSe crystal, driven by a 30-W-average-power train of 32-fs pulses spectrally centered at 2 µm, delivered by a fiber-laser system. Electro-optic sampling (EOS) of the waveform-stable MIR waveforms reveals their single-cycle nature, confirming the excellent phase matching both of IPDFG and of EOS with 2-µm pulses in GaSe.

Broadband interferometric subtraction of optical fields.

We present a Mach-Zehnder-like interferometer capable of simultaneous super-octave (950 - 2100 nm) destructive interference with an intensity extinction of 4 × 10-4. Achromatic nulling is achieved by unbalancing the number of Fresnel reflections off optically denser media in the two interferometer arms. With a methane gas sample in one interferometer arm, we isolate the coherent molecular vibrational emission from the broadband, impulsive excitation and quantitatively examine the potential improvement in detectable concentration, compared to direct transmission geometry. The novel concept will benefit sensing applications requiring high detection sensitivity and dynamic range, including time-domain and frequency-domain spectroscopy.

Next Generation Driver for Attosecond and Laser-plasma Physics.

The observation and manipulation of electron dynamics in matter call for attosecond light pulses, routinely available from high-order harmonic generation driven by few-femtosecond lasers. However, the energy limitation of these lasers supports only weak sources and correspondingly linear attosecond studies. Here we report on an optical parametric synthesizer designed for nonlinear attosecond optics and relativistic laser-plasma physics. This synthesizer uniquely combines ultra-relativistic focused intensities of about 1020 W/cm2 with a pulse duration of sub-two carrier-wave cycles. The coherent combination of two sequentially amplified and complementary spectral ranges yields sub-5-fs pulses with multi-TW peak power. The application of this source allows the generation of a broad spectral continuum at 100-eV photon energy in gases as well as high-order harmonics in relativistic plasmas. Unprecedented spatio-temporal confinement of light now permits the investigation of electric-field-driven electron phenomena in the relativistic regime and ultimately the rise of next-generation intense isolated attosecond sources.

Attosecond physics at the nanoscale.

Recently two emerging areas of research, attosecond and nanoscale physics, have started to come together. Attosecond physics deals with phenomena occurring when ultrashort laser pulses, with duration on the femto- and sub-femtosecond time scales, interact with atoms, molecules or solids. The laser-induced electron dynamics occurs natively on a timescale down to a few hundred or even tens of attoseconds (1 attosecond = 1 as = 10-18 s), which is comparable with the optical field. For comparison, the revolution of an electron on a 1s orbital of a hydrogen atom is ∼152 as. On the other hand, the second branch involves the manipulation and engineering of mesoscopic systems, such as solids, metals and dielectrics, with nanometric precision. Although nano-engineering is a vast and well-established research field on its own, the merger with intense laser physics is relatively recent. In this report on progress we present a comprehensive experimental and theoretical overview of physics that takes place when short and intense laser pulses interact with nanosystems, such as metallic and dielectric nanostructures. In particular we elucidate how the spatially inhomogeneous laser induced fields at a nanometer scale modify the laser-driven electron dynamics. Consequently, this has important impact on pivotal processes such as above-threshold ionization and high-order harmonic generation. The deep understanding of the coupled dynamics between these spatially inhomogeneous fields and matter configures a promising way to new avenues of research and applications. Thanks to the maturity that attosecond physics has reached, together with the tremendous advance in material engineering and manipulation techniques, the age of atto-nanophysics has begun, but it is in the initial stage. We present thus some of the open questions, challenges and prospects for experimental confirmation of theoretical predictions, as well as experiments aimed at characterizing the induced fields and the unique electron dynamics initiated by them with high temporal and spatial resolution.

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.

Attosecond nanoscale near-field sampling.

The promise of ultrafast light-field-driven electronic nanocircuits has stimulated the development of the new research field of attosecond nanophysics. An essential prerequisite for advancing this new area is the ability to characterize optical near fields from light interaction with nanostructures, with sub-cycle resolution. Here we experimentally demonstrate attosecond near-field retrieval for a tapered gold nanowire. By comparison of the results to those obtained from noble gas experiments and trajectory simulations, the spectral response of the nanotaper near field arising from laser excitation can be extracted.

All-optical control and metrology of electron pulses.

Short electron pulses are central to time-resolved atomic-scale diffraction and electron microscopy, streak cameras, and free-electron lasers. We demonstrate phase-space control and characterization of 5-picometer electron pulses using few-cycle terahertz radiation, extending concepts of microwave electron pulse compression and streaking to terahertz frequencies. Optical-field control of electron pulses provides synchronism to laser pulses and offers a temporal resolution that is ultimately limited by the rise-time of the optical fields applied. We used few-cycle waveforms carried at 0.3 terahertz to compress electron pulses by a factor of 12 with a timing stability of <4 femtoseconds (root mean square) and measure them by means of field-induced beam deflection (streaking). Scaling the concept toward multiterahertz control fields holds promise for approaching the electronic time scale in time-resolved electron diffraction and microscopy.

Optical attosecond pulses and tracking the nonlinear response of bound electrons.

The time it takes a bound electron to respond to the electromagnetic force of light sets a fundamental speed limit on the dynamic control of matter and electromagnetic signal processing. Time-integrated measurements of the nonlinear refractive index of matter indicate that the nonlinear response of bound electrons to optical fields is not instantaneous; however, a complete spectral characterization of the nonlinear susceptibility tensors--which is essential to deduce the temporal response of a medium to arbitrary driving forces using spectral measurements--has not yet been achieved. With the establishment of attosecond chronoscopy, the impulsive response of positive-energy electrons to electromagnetic fields has been explored through ionization of atoms and solids by an extreme-ultraviolet attosecond pulse or by strong near-infrared fields. However, none of the attosecond studies carried out so far have provided direct access to the nonlinear response of bound electrons. Here we demonstrate that intense optical attosecond pulses synthesized in the visible and nearby spectral ranges allow sub-femtosecond control and metrology of bound-electron dynamics. Vacuum ultraviolet spectra emanating from krypton atoms, exposed to intense waveform-controlled optical attosecond pulses, reveal a finite nonlinear response time of bound electrons of up to 115 attoseconds, which is sensitive to and controllable by the super-octave optical field. Our study could enable new spectroscopies of bound electrons in atomic, molecular or lattice potentials of solids, as well as light-based electronics operating on sub-femtosecond timescales and at petahertz rates.

Sub-phonon-period compression of electron pulses for atomic diffraction.

Visualizing the rearrangement of atoms in a wide range of molecular and condensed-matter systems requires resolving picometre displacements on a 10-fs timescale, which is achievable using pump-probe diffraction, given short enough pulses. Here we demonstrate the compression of single-electron pulses with a de Broglie wavelength of 0.08 ångström to a full-width at half-maximum duration of 28 fs or equivalently 12-fs root-mean square, substantially shorter than most phonon periods and molecular normal modes. Atomic resolution diffraction from a complex organic molecule is obtained with good signal-to-noise ratio within a data acquisition period of minutes. The electron-laser timing is found to be stable within 5 fs (s.d.) over several hours, allowing pump-probe diffraction at repetitive excitation. These measurements show the feasibility of laser-pump/electron-probe scans that can resolve the fastest atomic motions relevant in reversible condensed-matter transformations and organic chemistry.

Enhancement cavities for zero-offset-frequency pulse trains.

The optimal enhancement of broadband optical pulses in a passive resonator requires a seeding pulse train with a specific carrier-envelope-offset frequency. Here, we control the phase of the cavity mirrors to tune the offset frequency for which a given comb is optimally enhanced. This enables the enhancement of a zero-offset-frequency train of sub-30-fs pulses to multi-kW average powers. The combination of pulse duration, power, and zero phase slip constitutes a crucial step toward the generation of attosecond pulses at multi-10-MHz repetition rates. In addition, this control affords the enhancement of pulses generated by difference-frequency mixing, e.g., for mid-infrared spectroscopy.

Femtosecond Enhancement Cavities in the Nonlinear Regime.

We combine high-finesse optical resonators and spatial-spectral interferometry to a highly phase-sensitive investigation technique for nonlinear light-matter interactions. We experimentally validate an ab initio model for the nonlinear response of a resonator housing a gas target, permitting the global optimization of intracavity conversion processes like high-order harmonic generation. We predict the feasibility of driving intracavity high-order harmonic generation far beyond intensity limitations observed in state-of-the-art systems by exploiting the intracavity nonlinearity to compress the pulses in time.

High-power multi-megahertz source of waveform-stabilized few-cycle light.

Waveform-stabilized laser pulses have revolutionized the exploration of the electronic structure and dynamics of matter by serving as the technological basis for frequency-comb and attosecond spectroscopy. Their primary sources, mode-locked titanium-doped sapphire lasers and erbium/ytterbium-doped fibre lasers, deliver pulses with several nanojoules energy, which is insufficient for many important applications. Here we present the waveform-stabilized light source that is scalable to microjoule energy levels at the full (megahertz) repetition rate of the laser oscillator. A diode-pumped Kerr-lens-mode-locked Yb:YAG thin-disk laser combined with extracavity pulse compression yields waveform-stabilized few-cycle pulses (7.7 fs, 2.2 cycles) with a pulse energy of 0.15 µJ and an average power of 6 W. The demonstrated concept is scalable to pulse energies of several microjoules and near-gigawatt peak powers. The generation of attosecond pulses at the full repetition rate of the oscillator comes into reach. The presented system could serve as a primary source for frequency combs in the mid infrared and vacuum UV with unprecedented high power levels.

Carrier-wave Rabi-flopping signatures in high-order harmonic generation for alkali atoms.

We present a theoretical investigation of carrier-wave Rabi flopping in real atoms by employing numerical simulations of high-order harmonic generation (HHG) in alkali species. Given the short HHG cutoff, related to the low saturation intensity, we concentrate on the features of the third harmonic of sodium (Na) and potassium (K) atoms. For pulse areas of 2π and Na atoms, a characteristic unique peak appears, which, after analyzing the ground state population, we correlate with the conventional Rabi flopping. On the other hand, for larger pulse areas, carrier-wave Rabi flopping occurs, and is associated with a more complex structure in the third harmonic. These characteristics observed in K atoms indicate the breakdown of the area theorem, as was already demonstrated under similar circumstances in narrow band gap semiconductors.

Compressing µJ-level pulses from 250 fs to sub-10 fs at 38-MHz repetition rate using two gas-filled hollow-core photonic crystal fiber stages.

Compression of 250-fs, 1-µJ pulses from a KLM Yb:YAG thin-disk oscillator down to 9.1 fs is demonstrated. A kagomé-PCF with a 36-µm core-diameter is used with a pressure gradient from 0 to 40 bar of krypton. Compression to 22 fs is achieved by 1200 fs2 group-delay-dispersion provided by chirped mirrors. By coupling the output into a second kagomé-PCF with a pressure gradient from 0 to 25 bar of argon, octave spanning spectral broadening via the soliton-effect is observed at 18-W average output power. Self-compression to 9.1 fs is measured, with compressibility to 5 fs predicted. Also observed is strong emission in the visible via dispersive wave generation, amounting to 4% of the total output power.

Balancing of thermal lenses in enhancement cavities with transmissive elements.

Thermal lensing poses a serious challenge for the power scaling of enhancement cavities, in particular when these contain transmissive elements. We demonstrate the compensation of the lensing induced by thermal deformations of the cavity mirrors with the thermal lensing in a thin Brewster plate. Using forced convection to fine-tune the lensing in the plate, we achieve average powers of up to 160 kW for 250-MHz-repetition-rate picosecond pulses with a power-independent mode size. Furthermore, we show that the susceptibility of the cavity mode size to thermal lensing allows highly sensitive absorption measurements.

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.

Dual frequency comb spectroscopy with a single laser.

We demonstrate a simple scheme for dual frequency comb spectroscopy in which the second frequency comb is generated by propagating the primary pulse train through a dazzler. The two frequency combs are combined behind a Mach-Zehnder interferometer, and the optical spectrum is read out by an rf-spectrum analyzer. The method is applied to record the overtone absorption spectrum of C2H2 (acetylene) in the wavelength region around 1.03 µm. A spectrum with a resolution of 4 cm(-1) is obtained, which compares well with that from the HITRAN database. A simple method for improving the spectral resolution is demonstrated.

Efficient generation of THz pulses with 0.4 mJ energy.

Efficient generation of THz pulses with high energy was demonstrated by optical rectification of 785-fs laser pulses in lithium niobate using tilted-pulse-front pumping. The enhancement of conversion efficiency by a factor of 2.4 to 2.7 was demonstrated up to 186 µJ THz energy by cryogenic cooling of the generating crystal and using up to 18.5 mJ/cm2 pump fluence. Generation of THz pulses with more than 0.4 mJ energy and 0.77% efficiency was demonstrated even at room temperature by increasing the pump fluence to 186 mJ/cm2. The spectral peak is at about 0.2 THz, suitable for charged-particle manipulation.