Method for direct observation of Bloch oscillations in semiconductors.

We propose a scheme for real-time observations of Bloch oscillations in semiconductors using time-resolved band gap emission spectroscopy. By solving the time-dependent Schrödinger equation, we find one remarkable band gap emission besides the normal high harmonics generated in the interaction of a mid-infrared laser pulse and a semiconductor. It is shown that the band gap emission yield is directly connected to the population in the conduction band (CB). By adopting a pump-probe scheme, the time-dependent population in the CB, that is the dynamical Bloch oscillation, can be probed by measuring the band gap emission signal versus pump-probe delay. We also present a model based on accelerated Bloch states to explain the time-resolved measurement of dynamical Bloch oscillation.

Near- and Extended-Edge X-Ray-Absorption Fine-Structure Spectroscopy Using Ultrafast Coherent High-Order Harmonic Supercontinua.

Recent advances in high-order harmonic generation have made it possible to use a tabletop-scale setup to produce spatially and temporally coherent beams of light with bandwidth spanning 12 octaves, from the ultraviolet up to x-ray photon energies >1.6 keV. Here we demonstrate the use of this light for x-ray-absorption spectroscopy at the K- and L-absorption edges of solids at photon energies near 1 keV. We also report x-ray-absorption spectroscopy in the water window spectral region (284-543 eV) using a high flux high-order harmonic generation x-ray supercontinuum with 10^{9} photons/s in 1% bandwidth, 3 orders of magnitude larger than has previously been possible using tabletop sources. Since this x-ray radiation emerges as a single attosecond-to-femtosecond pulse with peak brightness exceeding 10^{26} photons/s/mrad^{2}/mm^{2}/1% bandwidth, these novel coherent x-ray sources are ideal for probing the fastest molecular and materials processes on femtosecond-to-attosecond time scales and picometer length scales.

High-dynamic-range arrival time control for flexible, accurate and precise parametric sub-cycle waveform synthesis.

We introduce a simple all-inline variation of a balanced optical cross-correlator (BOC) that allows to measure the arrival time difference (ATD), over the full Nyquist bandwidth, with increased common-mode rejection and long-term stability. An FPGA-based signal processing unit allows for real-time signal normalization and enables locking to any setpoint with an unprecedented accuracy of 0.07 % within an increased ATD range of more than 400 fs, resulting in attosecond resolution locking. The setup precision is verified with an out-of-loop measurement to be less than 80 as residual jitter paving the way for highly demanding applications such as parametric waveform synthesizers.

Impact of the Electronic Band Structure in High-Harmonic Generation Spectra of Solids.

An accurate analytic model describing the microscopic mechanism of high-harmonic generation (HHG) in solids is derived. Extensive first-principles simulations within a time-dependent density-functional framework corroborate the conclusions of the model. Our results reveal that (i) the emitted HHG spectra are highly anisotropic and laser-polarization dependent even for cubic crystals; (ii) the harmonic emission is enhanced by the inhomogeneity of the electron-nuclei potential; the yield is increased for heavier atoms; and (iii) the cutoff photon energy is driver-wavelength independent. Moreover, we show that it is possible to predict the laser polarization for optimal HHG in bulk crystals solely from the knowledge of their electronic band structure. Our results pave the way to better control and optimize HHG in solids by engineering their band structure.

Jitter analysis of timing-distribution and remote-laser synchronization systems.

We present a powerful jitter analysis method for timing-distribution and remote-laser synchronization systems based on feedback flow between setup elements. We synchronize two different mode-locked lasers in a master-slave configuration locally and remotely over a timing-stabilized fiber link network. Local synchronization reveals the inherent jitter of the slave laser as 2.1 fs RMS (>20 kHz), whereas remote synchronization exhibits an out-of-loop jitter of 8.55 fs RMS integrated for 1 Hz - 1 MHz. Our comprehensive feedback model yields excellent agreement with the experimental results and identifies seven uncorrelated noise sources, out of which the slave laser's jitter dominates with 8.19 fs RMS.

40-µJ passively CEP-stable seed source for ytterbium-based high-energy optical waveform synthesizers.

We demonstrate experimentally for the first time a ~40-µJ two-octave-wide passively carrier-envelope phase (CEP)-stable parametric front-end for seeding an ytterbium (Yb)-pump-based, few-optical-cycle, high-energy optical parametric waveform synthesizer. The system includes a CEP-stable white-light continuum and two-channel optical parametric chirped pulse amplifiers (OPCPAs) in the near- and mid-infrared spectral regions spanning altogether a two-octave-wide spectrum driven by a regenerative amplifier. The output pulses are compressed and fully characterized to demonstrate the well-behaved spectral phase of this seed source.

Cascaded parametric amplification for highly efficient terahertz generation.

A highly efficient, practical approach to high-energy multi-cycle terahertz (THz) generation based on spectrally cascaded optical parametric amplification (THz-COPA) is introduced. Feasible designs are presented that enable the THz wave, initially generated by difference frequency generation between a narrowband optical pump and optical seed (0.1-10% of pump energy), to self-start a cascaded (or repeated) energy downconversion of pump photons in a single pass through a single crystal. In cryogenically cooled, periodically poled lithium niobate, unprecedented energy conversion efficiencies >8% achievable with existing pump laser technology are predicted using realistic simulations. The calculations account for cascading effects, absorption, dispersion, and laser-induced damage. Due to the simultaneous, coupled nonlinear evolution of multiple phase-matched three-wave mixing processes, THz-COPA exhibits physics distinctly different from conventional three-wave mixing parametric amplifiers. This, in turn, governs optimal phase-matching conditions, evolution of optical spectra, and limitations of the nonlinear process. Circumventing these limitations is shown to yield conversion efficiencies ≫10%.

Broadband continuum generation in mode-locked lasers with phase-matched output couplers.

The concept of intracavity phase matching is proposed and demonstrated both theoretically and experimentally with a broadband phase-matched dielectric output coupler for linear-cavity few-cycle Ti:sapphire oscillators. The spectrum in the matched wavelength range is enhanced by >10 dB while maintaining good beam quality via resonantly enhanced continuum generation. The enhanced spectral components can be continuously tuned by varying the intracavity dispersion. Because dielectric coatings offer flexible design capabilities, this approach is applicable to various lasers with different gain media to obtain custom-tailored spectra, which have the potential to benefit several applications, such as shorter pulse generation, seeding of ytterbium lasers for pumping optical parametric amplifiers, and direct f-2f detection of the carrier-envelope phase.

Terahertz generation in lithium niobate driven by Ti:sapphire laser pulses and its limitations.

We experimentally investigate the limits of 800-nm-to-terahertz (THz) energy conversion in lithium niobate at room temperature driven by amplified Ti:sapphire laser pulses with tilted pulse front. The influence of the pump central wavelength, pulse duration, and fluence on THz generation is studied. We achieved a high peak efficiency of 0.12% using transform limited 150 fs pulses and observed saturation of the optical-to-THz conversion efficiency at a fluence of 15 mJ/cm(2) for this pulse duration. We experimentally identify two main limitations for the scaling of optical-to-THz conversion efficiencies: (i) the large spectral broadening of the optical pump spectrum in combination with large angular dispersion of the tilted pulse front and (ii) free-carrier absorption of THz radiation due to multi-photon absorption of the 800 nm radiation.

Dual-chirped optical parametric amplification for generating few hundred mJ infrared pulses.

An ultrafast high-power infrared pulse source employing a dual-chirped optical parametric amplification (DC-OPA) scheme based on a Ti:sapphire pump laser system is theoretically investigated. By chirping both pump and seed pulses in an optimized way, high-energy pump pulses can be utilized for a DC-OPA process without exceeding the damage threshold of BBO crystals, and broadband signal and idler pulses at 1.4 µm and 1.87 µm can be generated with a total conversion efficiency approaching 40%. Furthermore, few-cycle idler pulses with a passively stabilized carrier-envelope phase (CEP) can be generated by the difference frequency generation process in a collinear configuration. DC-OPA, a BBO-OPA scheme pumped by a Ti:sapphire laser, is efficient and scalable in output energy of the infrared pulses, which provides us with the design parameters of an ultrafast infrared laser system with an energy up to a few hundred mJ.

Carrier envelope phase stabilization of a Yb:KGW laser amplifier.

In this paper we report on the active stabilization of the carrier envelope phase (CEP) of a Yb:KGW chirped pulse amplifier laser system seeded by a Yb-doped solid-state Kerr-lens mode-locked oscillator. The regenerative amplifier delivers 180 fs CEP stable pulses of 30 µJ-1 mJ energy at a repetition rate tunable from 1 to 200 kHz. The bandwidth of the feedback loop was extended by a factor of 5 using a specially designed high-pass filter, which resulted in a dramatic decrease of CEP jitter below 0.45 rad after the amplifier.

Narrow-linewidth chirped frequency comb from a frequency-shifted feedback Ti:sapphire laser seeded by a phase-modulated single-frequency fiber laser.

Frequency-shifted feedback (FSF) lasers have emerged as powerful tools for precision distance metrology. At the output of a Michelson interferometer, the detected rf spectra of the FSF laser light contain a length-dependent heterodyne beat signal whose linewidth ultimately limits the achievable accuracy of length measurements. Here, we demonstrate a narrow-linewidth chirped frequency comb from an FSF Ti:sapphire ring laser seeded by a phase-modulated, ultra-low-phase-noise, single-frequency fiber laser. We experimentally investigate the influence of the seed laser linewidth on the resulting width and shape of the length-dependent rf beat signal. An ultranarrow heterodyne beat linewidth of <20 Hz is observed.

Infrared two-color multicycle laser field synthesis for generating an intense attosecond pulse.

We propose and demonstrate the generation of a continuum high-order harmonic spectrum by mixing multicycle two-color (TC) laser fields with the aim of obtaining an intense isolated attosecond pulse. By optimizing the wavelength of a supplementary infrared pulse in a TC field, a continuum harmonic spectrum was created around the cutoff region without carrier-envelope phase stabilization. The obtained harmonic spectra clearly show the possibility of generating isolated attosecond pulses from a multicycle TC laser field, which is generated by an 800 nm, 30 fs pulse mixed with a 1300 nm, 40 fs pulse. Our proposed method enables us not only to relax the requirements for the pump pulse duration but also to reduce ionization of the harmonic medium. This concept opens the door to create an intense isolated attosecond pulse using a conventional femtosecond laser system.

Fully stabilized multi-TW optical waveform synthesizer: Toward gigawatt isolated attosecond pulses.

A stable 50-mJ three-channel optical waveform synthesizer is demonstrated and used to reproducibly generate a high-order harmonic supercontinuum in the soft x-ray region. This synthesizer is composed of pump pulses from a 10-Hz repetition-rate Ti:sapphire pump laser and signal and idler pulses from an infrared two-stage optical parametric amplifier driven by this pump laser. With full active stabilization of all relative time delays, relative phases, and the carrier-envelope phase, a shot-to-shot stable intense continuum harmonic spectrum is obtained around 60 eV with pulse energy above 0.24 µJ. The peak power of the soft x-ray continuum is evaluated to be beyond 1 GW with a 170-as transform limit duration. We found a characteristic delay dependence of the multicycle waveform synthesizer and established its control scheme. Compared with the one-color case, we experimentally observe an enhancement of the cutoff spectrum intensity by one to two orders of magnitude using three-color waveform synthesis.

Self-compression of millijoule 1.5 microm pulses.

We demonstrate a four-stage optical parametric chirped-pulse amplification system that delivers carrier-envelope phase-stable approximately 1.5 microm pulses with energies up to 12.5 mJ before recompression. The system is based on a fusion of femtosecond diode-pumped solid-state Yb technology and a picosecond 100 mJ Nd:YAG pump laser. Pulses with 62 nm bandwidth are recompressed to a 74.4 fs duration close to the transform limit. To show the way toward a terawatt-peak-power single-cycle IR source, we demonstrate self-compression of 2.2 mJ pulses down to 19.8 fs duration in a single filament in argon with a 1.5 mJ output energy and 66% energy throughput.

Molecular polarizability anisotropy of liquid water revealed by terahertz-induced transient orientation.

Reaction pathways of biochemical processes are influenced by the dissipative electrostatic interaction of the reagents with solvent water molecules. The simulation of these interactions requires a parametrization of the permanent and induced dipole moments. However, the underlying molecular polarizability of water and its dependence on ions are partially unknown. Here, we apply intense terahertz pulses to liquid water, whose oscillations match the timescale of orientational relaxation. Using a combination of terahertz pump / optical probe experiments, molecular dynamics simulations, and a Langevin dynamics model, we demonstrate a transient orientation of their dipole moments, not possible by optical excitation. The resulting birefringence reveals that the polarizability of water is lower along its dipole moment than the average value perpendicular to it. This anisotropy, also observed in heavy water and alcohols, increases with the concentration of sodium iodide dissolved in water. Our results enable a more accurate parametrization and a benchmarking of existing and future water models.

Publisher Correction: Ellipticity dependence of high-harmonic generation in solids originating from coupled intraband and interband dynamics.

The published version of this Article contained an error in the second sentence of the fourth paragraph of the subheaded section "Ellipticity and helicity of the emitted harmonics". The final exponent in this sentence should read: inπ/2. This has now been corrected in the PDF and HTML versions of the Article.

Ellipticity dependence of high-harmonic generation in solids originating from coupled intraband and interband dynamics.

The strong ellipticity dependence of high-harmonic generation (HHG) in gases enables numerous experimental techniques that are nowadays routinely used, for instance, to create isolated attosecond pulses. Extending such techniques to solids requires a fundamental understanding of the microscopic mechanism of HHG. Here we use first-principles simulations within a time-dependent density-functional framework and show how intraband and interband mechanisms are strongly and differently affected by the ellipticity of the driving laser field. The complex interplay between intraband and interband effects can be used to tune and improve harmonic emission in solids. In particular, we show that the high-harmonic plateau can be extended by as much as 30% using a finite ellipticity of the driving field. We furthermore demonstrate the possibility to generate, from single circularly polarized drivers, circularly polarized harmonics. Our work shows that ellipticity provides an additional knob to experimentally optimize HHG in solids.The mechanisms of high-order harmonic generation in bulk system and dilute gas are different. Here the authors use first-principle methods to explore the ellipticity dependence and control of the HHG in periodic solids by involving the interband and intraband dynamics in Si and MgO.

Attosecond precision multi-kilometer laser-microwave network.

Synchronous laser-microwave networks delivering attosecond timing precision are highly desirable in many advanced applications, such as geodesy, very-long-baseline interferometry, high-precision navigation and multi-telescope arrays. In particular, rapidly expanding photon-science facilities like X-ray free-electron lasers and intense laser beamlines require system-wide attosecond-level synchronization of dozens of optical and microwave signals up to kilometer distances. Once equipped with such precision, these facilities will initiate radically new science by shedding light on molecular and atomic processes happening on the attosecond timescale, such as intramolecular charge transfer, Auger processes and their impacts on X-ray imaging. Here we present for the first time a complete synchronous laser-microwave network with attosecond precision, which is achieved through new metrological devices and careful balancing of fiber nonlinearities and fundamental noise contributions. We demonstrate timing stabilization of a 4.7-km fiber network and remote optical-optical synchronization across a 3.5-km fiber link with an overall timing jitter of 580 and 680 attoseconds root-mean-square, respectively, for over 40 h. Ultimately, we realize a complete laser-microwave network with 950-attosecond timing jitter for 18 h. This work can enable next-generation attosecond photon-science facilities to revolutionize many research fields from structural biology to material science and chemistry to fundamental physics.

Carrier-envelope phase dynamics and noise analysis in octave-spanning Ti:sapphire lasers.

We investigate the carrier-envelope phase dynamics of octave-spanning Ti:sapphire lasers and perform a complete noise analysis of the carrier-envelope phase stabilization. We model the effect of the laser dynamics on the residual carrier-envelope phase noise by deriving a transfer function representation of the octave-spanning frequency comb. The modelled phase noise and the experimental results show excellent agreement. This greatly enhances our capability of predicting the dependence of the residual carrier-envelope phase noise on the feedback loop filter, the carrier-envelope frequency control mechanism and the pump laser used.