8 fs laser pulses from a compact gas-filled multi-pass cell.

Compression of 42 fs, 0.29 mJ pulses from a Ti:Sapphire amplifier down to 8 fs (approximately 3 optical cycles) is demonstrated by means of spectral broadening in a compact multi-pass cell filled with argon. The efficiency of the nonlinear pulse compression is limited to 45 % mostly by losses in the mirrors of the cell. The experimental results are supported by 3-dimensional numerical simulations of the nonlinear pulse propagation in the cell that allow us to study spatio-spectral properties of the pulses after spectral broadening.

Photoemission from non-polar aromatic molecules in the gas and liquid phase.

The photoelectron spectra of both liquid and gas phase aromatic molecules are reported. The spectra were obtained using a 34.1 eV source produced by high harmonic generation and analysed with the help of high-level ab initio simulations using the reflection principle combined with path integral molecular dynamics simulations accounting for nuclear quantum effects for the gas phase. We demonstrate the suitability of three trimethylbenzenes (1,3,5-trimethylbenzene, 1,2,3-trimethylbenzene and 1,2,4-trimethylbenzene) as a solvent for liquid photoelectron spectroscopy of solute species. We also discuss the electrokinetic charging of a non-polar liquid jet.

State-Resolved Probing of Attosecond Timescale Molecular Dipoles.

We report an experimental study of iodomethane attosecond transient absorption spectroscopy (ATAS) in the region of iodine 4d core-to-valence/Rydberg excitation. Similar to previous atomic experiments, extreme ultraviolet near-infrared (XUV-NIR) delay-dependent absorbance changes reflect a light-induced phase due to an NIR-field driven AC Stark shift of the excited states, as well as pathway interferences arising from couplings between neighboring states. As a novel aspect of molecular ATAS, we observe pronounced differences between the ATAS signatures of valence and Rydberg states. While the core-to-valence transitions carry the majority of the XUV oscillator strength, the core-to-Rydberg transitions are dominantly affected by a moderately strong, nonionizing NIR field. Our experimental findings are corroborated by ab initio calculations and ATAS simulations.

Extreme-ultraviolet refractive optics.

Refraction is a well-known optical phenomenon that alters the direction of light waves propagating through matter. Microscopes, lenses and prisms based on refraction are indispensable tools for controlling light beams at visible, infrared, ultraviolet and X-ray wavelengths1. In the past few decades, a range of extreme-ultraviolet and soft-X-ray sources has been developed in laboratory environments2-4 and at large-scale facilities5,6. But the strong absorption of extreme-ultraviolet radiation in matter hinders the development of refractive lenses and prisms in this spectral region, for which reflective mirrors and diffractive Fresnel zone plates7 are instead used for focusing. Here we demonstrate control over the refraction of extreme-ultraviolet radiation by using a gas jet with a density gradient across the profile of the extreme-ultraviolet beam. We produce a gas-phase prism that leads to a frequency-dependent deflection of the beam. The strong deflection near to atomic resonances is further used to develop a deformable refractive lens for extreme-ultraviolet radiation, with low absorption and a focal length that can be tuned by varying the gas pressure. Our results open up a route towards the transfer of refraction-based techniques, which are well established in other spectral regions, to the extreme-ultraviolet domain.

Chirp-control of resonant high-order harmonic generation in indium ablation plumes driven by intense few-cycle laser pulses.

We have studied high-order harmonic generation (HHG) in an indium ablation plume driven by intense few-cycle laser pulses centered at 775 nm as a function of the frequency chirp of the laser pulse. We found experimentally that resonant emission lines between 19.7 eV and 22.3 eV (close to the 13th and 15th harmonic of the laser) exhibit a strong, asymmetric chirp dependence, with pronounced intensity modulations. The chirp dependence is reproduced by our numerical time-dependent Schrödinger equation simulations of a resonant HHG by the model indium ion. As demonstrated with our separate simulations of HHG within the strong field approximation, the resonance can be understood in terms of the chirp-dependent HHG photon energy coinciding with the energy of an autoionizing state to ground state transition with high oscillator strength. This supports the validity of the general theory of resonant four-step HHG in the few-cycle limit.

Angle-resolved coherent wave mixing using a 4 fs ultra-broad bandwidth laser.

We demonstrate angle-resolved coherent (ARC) wave mixing using 4 fs light pulses derived from a laser source that spans 550-1000 nm. We believe this to be the shortest pulse duration used to date in coherent multi-dimensional spectroscopy. The marriage of this ultra-broad band, few-cycle coherent source with the ARC technique will permit new investigations of the interplay between energy transfers and quantum superposition states spanning 8200 cm-1. We applied this configuration to measurements on the photosynthetic low light (LL) complex from Rhodopseudomonas palustris in solution at ambient temperature. We observe bi-exponential population dynamics for energy transfer across 5500 cm-1 (0.65 eV), which we attribute to energy transfer from the Qx transition of bacteriochlorophylls to the B850 pigment of the complex. We believe for the first time, to the best of our knowledge, we demonstrate that ARC maps can be recorded using a single laser pulse.

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.

Time-domain ptychography of over-octave-spanning laser pulses in the single-cycle regime.

We report, to the best of our knowledge, the first application of time-domain ptychography for the characterization of few-cycle laser pulses. Our method enables zero-additional phase measurements of over-octave-spanning laser pulses in the single cycle regime. The spectral phase is recovered using a robust ptychography algorithm that requires no input apart from the measured data trace. In addition to numerical tests, we validate our new device experimentally by reconstructing the complex electric field of a 1.5 cycle laser pulse with a bandwidth spanning 490 to 1060 nm. We further check the accuracy of our device by comparing the measured phases of octave-spanning chirped pulses to the known dispersion of fused silica glass.

X-SEA-F-SPIDER characterization of over octave spanning pulses in the infrared range.

We show a practical implementation of a pulse characterization method for sub-cycle pulse measurements in the infrared spectral range based on spectral shearing interferometry. We employ spatially-encoded arrangement filter-based spectral phase interferometry for direct electric field reconstruction with external ancila pulses (X-SEA-F-SPIDER). We show merits and limitations of the setup and an in-depth comparison to another widely used temporal characterization technique - Second-Harmonic Generation Frequency Resolved Optical Gating (SHG-FROG). The X-SEA-F-SPIDER implementation presented in this paper allows measurement of sub-cycle pulses with over one octave wide spectrum spanning the 900-2400 nm range without adding any extra dispersion due to the pulse characterization apparatus.

Self-referenced characterization of space-time couplings in near-single-cycle laser pulses.

We report on the characterization of space-time couplings in high-energy sub-2-cycle 770 nm laser pulses using a self-referencing single-frame method. Using spatially encoded arrangement filter-based spectral phase interferometry for direct electric field reconstruction, we characterize few-cycle pulses with a wavefront rotation of 2.8×1011 rev/s (1.38 mrad per half-cycle) and pulses with pulse front tilts ranging from -0.33 fs/µm to -3.03 fs/µm in the focus.

Single-shot implementation of dispersion-scan for the characterization of ultrashort laser pulses.

We demonstrate a single-shot ultrafast diagnostic, based on the dispersion-scan (d-scan) technique. In this implementation, rather than translating wedges to vary the dispersion as in scanning d-scan, the pulse to be measured experiences a spatially varying amount of dispersion in a prism. The resulting beam is then imaged into a second-harmonic generation crystal and an imaging spectrometer is used to measure the two-dimensional trace, which is analyzed using the d-scan retrieval algorithm. We compare the single-shot implementation with the scanning d-scan for the measurement of sub-3.5-fs pulses from a hollow core fiber pulse compressor. We show that the retrieval algorithm used to extract amplitude and phase of the pulse provides comparable results, proving the validity of the new single-shot implementation in the near single-cycle regime.

A strong-field driver in the single-cycle regime based on self-compression in a kagome fibre.

Over the past decade intense laser fields with a single-cycle duration and even shorter, subcycle multicolour field transients have been generated and applied to drive attosecond phenomena in strong-field physics. Because of their extensive bandwidth, single-cycle fields cannot be emitted or amplified by laser sources directly and, as a rule, are produced by external pulse compression-a combination of nonlinear optical spectral broadening followed up by dispersion compensation. Here we demonstrate a simple robust driver for high-field applications based on this Kagome fibre approach that ensures pulse self-compression down to the ultimate single-cycle limit and provides phase-controlled pulses with up to a 100 µJ energy level, depending on the filling gas, pressure and the waveguide length.

A simple electron time-of-flight spectrometer for ultrafast vacuum ultraviolet photoelectron spectroscopy of liquid solutions.

We present a simple electron time of flight spectrometer for time resolved photoelectron spectroscopy of liquid samples using a vacuum ultraviolet (VUV) source produced by high-harmonic generation. The field free spectrometer coupled with the time-preserving monochromator for the VUV at the Artemis facility of the Rutherford Appleton Laboratory achieves an energy resolution of 0.65 eV at 40 eV with a sub 100 fs temporal resolution. A key feature of the design is a differentially pumped drift tube allowing a microliquid jet to be aligned and started at ambient atmosphere while preserving a pressure of 10(-1) mbar at the micro channel plate detector. The pumping requirements for photoelectron (PE) spectroscopy in vacuum are presented, while the instrument performance is demonstrated with PE spectra of salt solutions in water. The capability of the instrument for time resolved measurements is demonstrated by observing the ultrafast (50 fs) vibrational excitation of water leading to temporary proton transfer.

Spatio-temporal characterization of mid-infrared laser pulses with spatially encoded spectral shearing interferometry.

We report on the spatially resolved full amplitude and phase characterization of mid-infrared high intensity laser pulses generated in a three stage OPA. We use a spatially-encoded arrangement (SEA-)SPIDER with spectral filters for ancilla generation for spatially resolved characterization. Using five interchangeable filter sets we are able to characterize pulses from 1 to 2 µm with one single device with minimal adjustments.

Isolated sub-fs XUV pulse generation in Mn plasma ablation.

We report studies of high-order harmonic generation in laser-produced manganese plasmas using sub-4-fs drive laser pulses. The measured spectra exhibit resonant enhancement of a small spectral region of about 2.5 eV width around the 31st harmonic (~50eV). The intensity contrast relative to the directly adjacent harmonics exceeds one order of magnitude. This finding is in sharp contrast to the results reported previously for multi-cycle laser pulses [Physical Review A 76, 023831 (2007)]. Theoretical modelling suggests that the enhanced harmonic emission forms an isolated sub-femtosecond pulse.

Invited review article: technology for attosecond science.

We describe a complete technological system at Imperial College London for Attosecond Science studies. The system comprises a few-cycle, carrier envelope phase stabilized laser source which delivers sub 4 fs pulses to a vibration-isolated attosecond vacuum beamline. The beamline is used for the generation of isolated attosecond pulses in the extreme ultraviolet (XUV) at kilohertz repetition rates through laser-driven high harmonic generation in gas targets. The beamline incorporates: interferometers for producing pulse sequences for pump-probe studies; the facility to spectrally and spatially filter the harmonic radiation; an in-line spatially resolving XUV spectrometer; and a photoelectron spectroscopy chamber in which attosecond streaking is used to characterize the attosecond pulses. We discuss the technology and techniques behind the development of our complete system and summarize its performance. This versatile apparatus has enabled a number of new experimental investigations which we briefly describe.

Enhancement of high harmonics from plasmas using two-color pump and chirp variation of 1 kHz Ti:sapphire laser pulses.

We have investigated resonance effects in high-order harmonic generation (HHG) within laser-produced plasmas. We demonstrate a significantly improved harmonic yield by using two-color pump-induced enhancement and a 1 kHz pulse repetition rate. Together with an increased HHG output, the even harmonics in the cutoff region were enhanced with respect to odd harmonics. We report the observation of a resonance-induced growth in intensity of 20th harmonic in silver plasma (2×), 26th harmonic in vanadium plasma (4×), and 28th harmonic in chromium plasma (5×).