Noninvasive characterization methods for ultra-short laser pulse induced volume modifications.

We present two noninvasive characterization methods to investigate laser induced modifications in bulk fused silica glasses. The methods discussed are immersion microscopy and scanning acoustic microscopy (SAM). SAM shows merits in measuring the distance from sample surface to the first detectable density change of the modification, while immersion microscopy offers a look into the modification. Both noninvasive methods are preferred over conventional polishing or etching techniques due to the facts, that multiple investigations can be done with only one sample and lower time expenditure. The type II modifications were introduced by focusing laser pulses with high repetition rates into the fused silica.

High-repetition rate attosecond beamline for multi-particle coincidence experiments.

In this paper, a 3-dimensional photoelectron/ion momentum spectrometer (reaction microscope) combined with a table-top attosecond beamline based on a high-repetition rate (49 kHz) laser source is presented. The beamline is designed to achieve a temporal stability below 50 attoseconds. Results from measurements on systems like molecular hydrogen and argon dimers demonstrate the capabilities of this setup in observing the attosecond dynamics in 3D while covering the full solid angle for ionization processes having low cross-sections.

Controlling photoionization using attosecond time-slit interferences.

When small quantum systems, atoms or molecules, absorb a high-energy photon, electrons are emitted with a well-defined energy and a highly symmetric angular distribution, ruled by energy quantization and parity conservation. These rules are based on approximations and symmetries which may break down when atoms are exposed to ultrashort and intense optical pulses. This raises the question of their universality for the simplest case of the photoelectric effect. Here we investigate photoionization of helium by a sequence of attosecond pulses in the presence of a weak infrared laser field. We continuously control the energy of the photoelectrons and introduce an asymmetry in their emission direction, at variance with the idealized rules mentioned above. This control, made possible by the extreme temporal confinement of the light-matter interaction, opens a road in attosecond science, namely, the manipulation of ultrafast processes with a tailored sequence of attosecond pulses.

Noise effects and the impact of detector responses on the characterization of extreme ultraviolet attosecond pulses.

We employ numerical simulations to study the effects of noise on the reconstruction of the duration and satellite intensity ratio for transform-limited single and double pulses of 200 as duration. The forms of noise we implement are delay jitters between the attosecond pulse and the near-IR laser field, energy resolution of the photoelectron detector, and Poisson noise in streaking spectrograms with different count levels. We use the streaking method to characterize the pulse and the extended ptychographic iterative engine retrieval algorithm to reconstruct the pulse from the simulated streaking spectrogram. We found that, for practical purposes, when implementing a combination of all three mentioned noise contributions, the attosecond pulse duration will be overestimated when the photoelectron count level is low. Furthermore, the satellite pulse amplitude of the attosecond double pulse can be retrieved within 10% accuracy.

Spatial Control of Multiphoton Electron Excitations in InAs Nanowires by Varying Crystal Phase and Light Polarization.

We demonstrate the control of multiphoton electron excitations in InAs nanowires (NWs) by altering the crystal structure and the light polarization. Using few-cycle, near-infrared laser pulses from an optical parametric chirped-pulse amplification system, we induce multiphoton electron excitations in InAs nanowires with controlled wurtzite (WZ) and zincblende (ZB) segments. With a photoemission electron microscope, we show that we can selectively induce multiphoton electron emission from WZ or ZB segments of the same wire by varying the light polarization. Developing ab initio GW calculations of first to third order multiphoton excitations and using finite-difference time-domain simulations, we explain the experimental findings: While the electric-field enhancement due to the semiconductor/vacuum interface has a similar effect for all NW segments, the second and third order multiphoton transitions in the band structure of WZ InAs are highly anisotropic in contrast to ZB InAs. As the crystal phase of NWs can be precisely and reliably tailored, our findings open up for new semiconductor optoelectronics with controllable nanoscale emission of electrons through vacuum or dielectric barriers.

Size and shape dependent few-cycle near-field dynamics of bowtie nanoantennas.

Metal nanostructures can transfer electromagnetic energy from femtosecond laser pulses to the near-field down to spatial scales well below the optical diffraction limit. By combining few-femtosecond laser pulses with photoemission electron microscopy, we study the dynamics of the induced few-cycle near-field in individual bowtie nanoantennas. We investigate how the dynamics depend on antenna size and exact bowtie shape resulting from fabrication. Different dynamics are, as expected, measured for antennas of different sizes. However, we also detect comparable dynamics differences between individual antennas of similar size. With Finite-difference time-domain simulations we show that these dynamics differences between similarly sized antennas can be due to small lateral shape variations generally induced during the fabrication.

Nanoscale Imaging of Local Few-Femtosecond Near-Field Dynamics within a Single Plasmonic Nanoantenna.

The local enhancement of few-cycle laser pulses by plasmonic nanostructures opens up for spatiotemporal control of optical interactions on a nanometer and few-femtosecond scale. However, spatially resolved characterization of few-cycle plasmon dynamics poses a major challenge due to the extreme length and time scales involved. In this Letter, we experimentally demonstrate local variations in the dynamics during the few strongest cycles of plasmon-enhanced fields within individual rice-shaped silver nanoparticles. This was done using 5.5 fs laser pulses in an interferometric time-resolved photoemission electron microscopy setup. The experiments are supported by finite-difference time-domain simulations of similar silver structures. The observed differences in the field dynamics across a single particle do not reflect differences in plasmon resonance frequency or dephasing time. They instead arise from a combination of retardation effects and the coherent superposition between multiple plasmon modes of the particle, inherent to a few-cycle pulse excitation. The ability to detect and predict local variations in the few-femtosecond time evolution of multimode coherent plasmon excitations in rationally synthesized nanoparticles can be used in the tailoring of nanostructures for ultrafast and nonlinear plasmonics.

Spatiotemporal characterization of ultrashort laser pulses using spatially resolved Fourier transform spectrometry.

We present a method for characterizing ultrashort laser pulses in space and time, based on spatially resolved Fourier transform spectrometry. An unknown pulse is interfered with a delayed, spatially uniform reference on a CCD camera. The reference pulse is created by spatially filtering a portion of the unknown pulse. By scanning the delay between the two pulses, an interferogram is obtained at each pixel, allowing us to determine the spatially resolved phase difference between the unknown pulse and the reference pulse. High-resolution spatiotemporal characterization of an ultrashort pulse is demonstrated, and the sensitivity of the method to spatiotemporal coupling is shown for the case of a pulse with pulse front tilt.

Temporal and spatial effects inside a compact and CEP stabilized, few-cycle OPCPA system at high repetition rates.

We present a compact and ultra-stable few-cycle OPCPA system. In two non-collinear parametric amplification stages pulse energies up to 17 µJ at 200 kHz repetition rate are obtained. Recompression of the broadband pulses down to 6.3 fs is performed with chirped mirrors leading to peak powers above 800 MW. The parametric amplification processes were studied in detail employing (2 + 1) dimensional numerical simulations and compared to experimental observations in terms of spectral shapes, pulse energy, spatial effects as well as delay dependent nonlinear mixing products. This gives new insights into the parametric process and design guidelines for high repetition rate OPCPA systems.

Two-color pumped OPCPA system emitting spectra spanning 1.5 octaves from VIS to NIR.

We present a two-color pumped OPCPA system which delivers an ultra-broadband spectrum spanning from 430 nm to 1.3 µm with a Fourier limited pulse duration of sub-3 fs and 1 µJ of pulse energy at a repetition rate of 200 kHz. All frequency components propagate on a common path, thus the spectral phase along the whole spectrum is well-defined. The inner part of the spectrum has been compressed to sub-5 fs pulses.

Few-cycle oscillator pulse train with constant carrier-envelope- phase and 65 as jitter.

We report on an octave-spanning Ti:sapphire laser oscillator stabilized to carrier-envelope-offset frequency zero, generating a pulse train with constant field profile for every pulse. Stabilization is realized using an extended self-referenced locking scheme enabling to lock the carrier envelope-offset phase with less than 65 attosecond rms timing jitter. The stabilized system features a pulse repetition rate of 100 MHz with pulses as short as 4.5 fs and 220 mW average output power. With this laser system it was possible for the first time to demonstrate a spectral interference pattern of 1011 oscillator pulses in an out-of-loop f-to-2f-interferometer.

Few-cycle femtosecond field synthesizer.

We report on an optical field synthesizer consisting of a CEO-phase stabilized octave-spanning Ti:sapphire laser oscillator, a double-LCD prism-based pulse shaper, and a SPIDER pulse characterization apparatus. This field synthesizer allows for generating pulses with durations as short as 3.6 fs and enables to control the electric field on a sub-cycle scale. Within the limits of the ultrabroad spectrum arbitrary spectral and temporal pulse shapes and pulse sequences can be realized. Together with the ability to stabilize the pulses with respect to their CEO-phase, this system forms a versatile tool for coherent control experiments of field sensitive processes and precision spectroscopy.

Controlled waveforms on the single-cycle scale from a femtosecond oscillator.

We present an octave-spanning Ti:sapphire oscillator supporting Fourier-limited pulses as short as 3.7 fs. This laser system can be directly CEO-phase stabilized delivering an average output power of about 90 mW with a pulse duration of 4.4 fs. The phase-stabilization is realized without additional spectral broadening using an f-2f interferometer approach allowing for full control of the electric pulse field on a sub-femtosecond time-scale.