M. Hemmer

Multi-octave supercontinuum generation from mid-infrared filamentation in a bulk crystal

In supercontinuum generation, various propagation effects combine to produce a dramatic spectral broadening of intense ultrashort optical pulses. With a host of applications, supercontinuum sources are often required to possess a range of properties such as spectral coverage from the ultraviolet across the visible and into the infrared, shot-to-shot repeatability, high spectral energy density and an absence of complicated pulse splitting. Here we present an all-in-one solution, the first supercontinuum in a bulk homogeneous material extending from 450 nm into the mid-infrared. The spectrum spans 3.3 octaves and carries high spectral energy density (2 pJ nm−1–10 nJ nm−1), and the generation process has high shot-to-shot reproducibility and preserves the carrier-to-envelope phase. Our method, based on filamentation of femtosecond mid-infrared pulses in the anomalous dispersion regime, allows for compact new supercontinuum sources.

Spatiotemporal isolation of attosecond soft X-ray pulses in the water window.

Attosecond pulses at photon energies that cover the principal absorption edges of the building blocks of materials are a prerequisite for time-resolved probing of the triggering events leading to electronic dynamics such as exciton formation and annihilation. We demonstrate experimentally the isolation of individual attosecond pulses at the carbon K-shell edge (284 eV) in the soft X-ray water window with pulse duration below 400 as and with a bandwidth supporting a 30-as pulse duration. Our approach is based on spatiotemporal isolation of long-wavelength-driven harmonics and validates a straightforward and scalable approach for robust and reproducible attosecond pulse isolation.

Imaging an aligned polyatomic molecule with laser-induced electron diffraction

Laser-induced electron diffraction is an evolving tabletop method that aims to image ultrafast structural changes in gas-phase polyatomic molecules with sub-Ångström spatial and femtosecond temporal resolutions. Here we demonstrate the retrieval of multiple bond lengths from a polyatomic molecule by simultaneously measuring the C–C and C–H bond lengths in aligned acetylene. Our approach takes the method beyond the hitherto achieved imaging of simple diatomic molecules and is based on the combination of a 160 kHz mid-infrared few-cycle laser source with full three-dimensional electron–ion coincidence detection. Our technique provides an accessible and robust route towards imaging ultrafast processes in complex gas-phase molecules with atto- to femto-second temporal resolution.

Sub-250-mrad, passively carrier–envelope-phase-stable mid-infrared OPCPA source at high repetition rate

An all-optical and passively carrier-to-envelope-phase-stabilized (CEP-stabilized) optical parametric chirped pulse amplification (OPCPA) system is demonstrated with sub-250-mrad CEP stability over 11 min and better than 100 mrad over 11 s. This is achieved without any electronic CEP stabilization loop for 160 kHz pulse repetition rate in the few cycle regime.

High-flux table-top soft x-ray source driven by sub-2-cycle, CEP stable, 1.85-μm 1-kHz pulses for carbon K-edge spectroscopy

We report on the first table-top high-flux source of coherent soft x-ray radiation up to 400 eV, operating at 1 kHz. This source covers the carbon K-edge with a beam brilliance of (4.3±1.2)×10(15) photons/s/mm(2)/strad/10% bandwidth and a photon flux of (1.85±0.12)×10(7) photons/s/1% bandwidth. We use this source to demonstrate table-top x-ray near-edge fine-structure spectroscopy at the carbon K-edge of a polyimide foil and retrieve the specific absorption features corresponding to the binding orbitals of the carbon atoms in the foil.

Self-compression to sub-3-cycle duration of mid-infrared optical pulses in dielectrics

We present the first demonstration of sub-3 cycle optical pulses at 3.1 μm central wavelength generated through self-compression in the anomalous dispersion regime in a dielectric. The pulses emerging from this compact and efficient self-compression setup could be focused to intensities exceeding 10(14) W/cm(2), a suitable range for high field physics experiments. Numerical simulations performed with a 3D nonlinear propagation code, provide theoretical insight on the processes involved and support our experimental findings.

Ultrafast electron diffraction imaging of bond breaking in di-ionized acetylene

Acetylenes scission visualized by selfie Can molecules take pictures of themselves? That is more or less the principle underlying laser-induced electron diffraction (LIED): A laser field strips an electron from a molecule and then sends it back to report on the structure of the remaining ion. Wolter et al. applied this technique to acetylene to track the cleavage of its C–H bond after double ionization (see the Perspective by Ruan). They imaged the full structure of the molecule and also distinguished more rapid dissociative dynamics when it was oriented parallel rather than perpendicular to the LIED field. Science, this issue p. 308; see also p. 283 An electron transiently stripped from a molecule is used to image that molecules dissociation. Visualizing chemical reactions as they occur requires atomic spatial and femtosecond temporal resolution. Here, we report imaging of the molecular structure of acetylene (C2H2) 9 femtoseconds after ionization. Using mid-infrared laser–induced electron diffraction (LIED), we obtained snapshots as a proton departs the [C2H2]2+ ion. By introducing an additional laser field, we also demonstrate control over the ultrafast dissociation process and resolve different bond dynamics for molecules oriented parallel versus perpendicular to the LIED field. These measurements are in excellent agreement with a quantum chemical description of field-dressed molecular dynamics.

0.5-keV Soft X-ray attosecond continua.

Attosecond light pulses in the extreme ultraviolet have drawn a great deal of attention due to their ability to interrogate electronic dynamics in real time. Nevertheless, to follow charge dynamics and excitations in materials, element selectivity is a prerequisite, which demands such pulses in the soft X-ray region, above 200 eV, to simultaneously cover several fundamental absorption edges of the constituents of the materials. Here, we experimentally demonstrate the exploitation of a transient phase matching regime to generate carrier envelope controlled soft X-ray supercontinua with pulse energies up to 2.9±0.1 pJ and a flux of (7.3±0.1) × 107 photons per second across the entire water window and attosecond pulses with 13 as transform limit. Our results herald attosecond science at the fundamental absorption edges of matter by bridging the gap between ultrafast temporal resolution and element specific probing.

2-μm wavelength, high-energy Ho:YLF chirped-pulse amplifier for mid-infrared OPCPA

A 2-μm wavelength laser delivering up to 39-mJ energy, ∼10  ps duration pulses at 100-Hz repetition rate is reported. The system relies on chirped pulse amplification (CPA): a modelocked Er:Tm:Ho fiber-seeder is followed by a Ho:YLF-based regenerative amplifier and a cryogenically cooled Ho:YLF single pass amplifier. Stretching and compressing are performed with large aperture chirped volume Bragg gratings (CVBG). At a peak power of 3.3 GW, the stability was <1%  rms over 1 h, confirming high suitability for OPCPA and extreme nonlinear optics applications.

Performance of MgO:PPLN, KTA, and KNbO 3 for mid-wave infrared broadband parametric amplification at high average power

The performance of potassium niobate (KNbO₃), MgO-doped periodically poled lithium niobate (MgO:PPLN), and potassium titanyl arsenate (KTA) were experimentally compared for broadband mid-wave infrared parametric amplification at a high repetition rate. The seed pulses, with an energy of 6.5 μJ, were amplified using 410 μJ pump energy at 1064 nm to a maximum pulse energy of 28.9 μJ at 3 μm wavelength and at a 160 kHz repetition rate in MgO:PPLN while supporting a transform limited duration of 73 fs. The high average powers of the interacting beams used in this study revealed average power-induced processes that limit the scaling of optical parametric amplification in MgO:PPLN; the pump peak intensity was limited to 3.8  GW/cm² due to nonpermanent beam reshaping, whereas in KNbO₃ an absorption-induced temperature gradient in the crystal led to permanent internal distortions in the crystal structure when operated above a pump peak intensity of 14.4  GW/cm².