Attosecond streaking enables the measurement of quantum phase

Attosecond streaking, as a measurement technique, was originally conceived as a means to characterize attosecond light pulses, which is a good approximation if the relevant transition matrix elements are approximately constant within the bandwidth of the light pulse. Our analysis of attosecond streaking measurements on systems with complex response to the photoionizing pulse establishes a relation between the momentum-space wave function of the outgoing electron and the result of conventional retrieval algorithms. This finding enables the measurement of the quantum phase associated with bound-continuum transition matrix elements.Comment: similar to the version accepted for publication in PR

Sub-cycle optical control of current in a semiconductor: from the multiphoton to the tunneling regime

Nonlinear interactions between ultrashort optical waveforms and solids can be used to induce and steer electric current on a femtosecond (fs) timescale, holding promise for electronic signal processing at PHz frequencies [Nature 493, 70 (2013)]. So far, this approach has been limited to insulators, requiring extremely strong peak electric fields and intensities. Here, we show all-optical generation and control of directly measurable electric current in a semiconductor relevant for high-speed and high-power (opto)electronics, gallium nitride (GaN), within an optical cycle and on a timescale shorter than 2 fs, at intensities at least an order of magnitude lower than those required for dielectrics. Our approach opens the door to PHz electronics and metrology, applicable to low-power (non-amplified) laser pulses, and may lead to future applications in semiconductor and photonic integrated circuit technologies

Gold-Induced Desulfurization in a Bis(ferrocenyl) Alkane Dithiol

Thiol-modified ferrocenes on gold have been archetypical model systems for many fundamental charge transfer and other studies, since both thiol-gold and ferrocene redox chemistry are considered to be well-understood. Thus unexpectedly, we found that for a representative of a new class of flexibly linked bis-ferrocenyl compounds, namely, 1-10-bis­(1-ferrocenyl)­decane dithiol, surface immobilization on gold failed. Instead, in the presence of gold, molecular decomposition took place, resulting in sulfur-based adlayers and well-defined molecular elimination products, for which we provide spectroscopic evidence. Careful control experiments and comparison with related ferrocene compounds provide insight into the mechanism of the observed elimination reactions, as a combined effect of the molecular structure and the nature of the gold/sulfur bond. These findings, thus, have a broader impact on the design of molecular adlayers, for example, in the context of surface functionalization in sensing or the synthesis of gold nanoparticles

Attosecond optoelectronic field measurement in solids

The sub-cycle interaction of light and matter is one of the key frontiers of inquiry made accessible by attosecond science. Here, we show that when light excites a pair of charge carriers inside of a solid, the transition probability is strongly localized to instants slightly after the extrema of the electric field. The extreme temporal localization is utilized in a simple electronic circuit to record the waveforms of infrared to ultraviolet light fields. This form of petahertz-bandwidth field metrology gives access to both the modulated transition probability and its temporal offset from the laser field, providing sub-fs temporal precision in reconstructing the sub-cycle electronic response of a solid state structure. Characterization of light pulses is important in order to understand their interaction with matter. Here the authors demonstrate a nonlinear photoconductive sampling method to measure electric field wave-forms in the infrared, visible and ultraviolet spectral ranges

Cumulative plasma effects in cavity-enhanced high-order harmonic generation in gases

Modern ultrafast laser architectures enable high-order harmonic generation (HHG) in gases at (multi-) MHz repetition rates, where each atom interacts with multiple pulses before leaving the HHG volume. This raises the question of cumulative plasma effects on the nonlinear conversion. Utilizing a femtosecond enhancement cavity with HHG in argon and on-axis geometric extreme-ultraviolet (XUV) output coupling, we experimentally compare the single-pulse case with a double-pulse HHG regime in which each gas atom is hit by two pulses while traversing the interaction volume. By varying the pulse repetition rate (18.4 and 36.8 MHz) in an 18.4-MHz roundtrip-frequency cavity with a finesse of 187, and leaving all other pulse parameters identical (35-fs, 0.6-mu J input pulses), we observe a dramatic decrease in the overall conversion efficiency (output-coupled power divided by the input power) in the double-pulse regime. The plateau harmonics (25-50 eV) exhibit very similar flux despite the twofold difference in repetition rate and average power. We attribute this to a spatially inhomogeneous plasma distribution that reduces the HHG volume, decreasing the generated XUV flux and/or affecting the spatial XUV beam profile, which reduces the efficiency of output coupling through the pierced mirror. These findings demonstrate the importance of cumulative plasma effects for power scaling of high-repetition-rate HHG in general and for applications in XUV frequency comb spectroscopy and in attosecond metrology in particular

Electro-optic characterization of synthesized infrared-visible light fields.

The measurement and control of light field oscillations enable the study of ultrafast phenomena on sub-cycle time scales. Electro-optic sampling (EOS) is a powerful field characterization approach, in terms of both sensitivity and dynamic range, but it has not reached beyond infrared frequencies. Here, we show the synthesis of a sub-cycle infrared-visible pulse and subsequent complete electric field characterization using EOS. The sampled bandwidth spans from 700 nm to 2700 nm (428 to 110 THz). Tailored electric-field waveforms are generated with a two-channel field synthesizer in the infrared-visible range, with a full-width at half-maximum duration as short as 3.8 fs at a central wavelength of 1.7 µm (176 THz). EOS detection of the complete bandwidth of these waveforms extends it into the visible spectral range. To demonstrate the power of our approach, we use the sub-cycle transients to inject carriers in a thin quartz sample for nonlinear photoconductive field sampling with sub-femtosecond resolution

Supplementary document for Ultra-phase-stable infrared light source at Watt level - 6836675.pdf

Revised supplemental documen