Coherent field sensing of nitrogen dioxide.

We introduce a portable dual-comb spectrometer operating in the visible spectral region for atmospheric monitoring of NO2, a pollution gas of major importance. Dual-comb spectroscopy, combining key advantages of fast, broadband and accurate measurements, has been established in the infrared as a method for the investigation of atmospheric gases with kilometer-scale absorption path lengths. With the presented dual-comb spectrometer centered at 517 nm, we make use of the strong absorption cross section of NO2 in this spectral region. In combination with a multi-pass approach through the atmosphere, we achieve an interaction path length of almost a kilometer while achieving both advanced spatial resolution (90 m) and a detection sensitivity of 5 ppb. The demonstrated temporal resolution of one minute outperforms the standard chemiluminescence-based NO2 detector that is commercially available and used in this experiment, by a factor of three.

Ultraviolet dual comb spectroscopy: a roadmap.

Dual Comb Spectroscopy proved its versatile capabilities in molecular fingerprinting in different spectral regions, but not yet in the ultraviolet (UV). Unlocking this spectral window would expand fingerprinting to the electronic energy structure of matter. This will access the prime triggers of photochemical reactions with unprecedented spectral resolution. In this research article, we discuss the milestones marking the way to the first UV dual comb spectrometer. We present experimental and simulated studies towards UV dual comb spectroscopy, directly applied to planned absorption measurements of formaldehyde (centered at 343 nm, 3.6 eV) and argon (80 nm, 16 eV). This will enable an unparalleled relative resolution of up to 10-9 - with a table-top UV source surpassing any synchrotron-linked spectrometer by at least two and any grating-based UV spectrometer by up to six orders of magnitude.

Agile spectral tuning of high order harmonics by interference of two driving pulses.

In this work, the experimental realization of a tunable high photon flux extreme ultraviolet light source is presented. This is enabled by high harmonic generation of two temporally delayed driving pulses with a wavelength of 1030 nm, resulting in a tuning range of 0.8 eV at the 19th harmonic at 22.8 eV. The implemented approach allows for fast tuning of the spectrum, is highly flexible and is scalable towards full spectral coverage at higher photon energies.

Coherent Raman spectro-imaging with laser frequency combs.

Advances in optical spectroscopy and microscopy have had a profound impact throughout the physical, chemical and biological sciences. One example is coherent Raman spectroscopy, a versatile technique interrogating vibrational transitions in molecules. It offers high spatial resolution and three-dimensional sectioning capabilities that make it a label-free tool for the non-destructive and chemically selective probing of complex systems. Indeed, single-colour Raman bands have been imaged in biological tissue at video rates by using ultra-short-pulse lasers. However, identifying multiple, and possibly unknown, molecules requires broad spectral bandwidth and high resolution. Moderate spectral spans combined with high-speed acquisition are now within reach using multichannel detection or frequency-swept laser beams. Laser frequency combs are finding increasing use for broadband molecular linear absorption spectroscopy. Here we show, by exploring their potential for nonlinear spectroscopy, that they can be harnessed for coherent anti-Stokes Raman spectroscopy and spectro-imaging. The method uses two combs and can simultaneously measure, on the microsecond timescale, all spectral elements over a wide bandwidth and with high resolution on a single photodetector. Although the overall measurement time in our proof-of-principle experiments is limited by the waiting times between successive spectral acquisitions, this limitation can be overcome with further system development. We therefore expect that our approach of using laser frequency combs will not only enable new applications for nonlinear microscopy but also benefit other nonlinear spectroscopic techniques.

Thin-disk pumped optical parametric chirped pulse amplifier delivering CEP-stable multi-mJ few-cycle pulses at 6 kHz.

We present an optical parametric chirped pulse amplifier (OPCPA) delivering CEP-stable ultrashort pulses with 7 fs, high energies of more than 1.8 mJ and high average output power exceeding 10 W at a repetition rate of 6 kHz. The system is pumped by a picosecond regenerative thin-disk amplifier and exhibits an excellent long-term stability. In a proof-of-principle experiment, high harmonic generation is demonstrated in neon up to the 61st order.

Vacuum ultraviolet frequency combs generated by a femtosecond enhancement cavity in the visible.

We present the first (to our best knowledge) femtosecond enhancement cavity in the visible wavelength range for ultraviolet frequency comb generation. The cavity is seeded at 518 nm by a frequency-doubled Yb fiber laser and operates at a peak intensity of 1.2×10(13) W/cm(2). High harmonics of up to the ninth order (~57 nm) are generated in an intracavity xenon gas jet. Intracavity high harmonic powers of several milliwatts for the third harmonic order and microwatts for the fifth harmonic order prove the potential of the "green cavity" as an efficient ultraviolet frequency comb source for future spectroscopic experiments. A limiting degradation effect of the cavity mirrors is avoided by operating at a constant oxygen background pressure.

Improved measurement of the hydrogen 1S-2S transition frequency.

We have measured the 1S-2S transition frequency in atomic hydrogen via two-photon spectroscopy on a 5.8 K atomic beam. We obtain f(1S-2S) = 2,466,061,413,187,035 (10)  Hz for the hyperfine centroid, in agreement with, but 3.3 times better than the previous result [M. Fischer et al., Phys. Rev. Lett. 92, 230802 (2004)]. The improvement to a fractional frequency uncertainty of 4.2 × 10(-15) arises mainly from an improved stability of the spectroscopy laser, and a better determination of the main systematic uncertainties, namely, the second order Doppler and ac and dc Stark shifts. The probe laser frequency was phase coherently linked to the mobile cesium fountain clock FOM via a frequency comb.

Power scaling of a high-repetition-rate enhancement cavity.

A passive optical resonator is used to enhance the power of a pulsed 78 MHz repetition rate Yb laser providing 200 fs pulses. We find limitations relating to the achievable time-averaged and peak power, which we distinguish by varying the duration of the input pulses. An intracavity average power of 18 kW is generated with close to Fourier-limited pulses of 10 W average power. Beyond this power level, intensity-related effects lead to resonator instabilities, which can be removed by chirping the seed laser pulses. By extending the pulse duration in this way to 2 ps, we could obtain 72 kW of intracavity circulating power with 50 W of input power.

Implementation and characterization of a stable optical frequency distribution system.

An optical frequency distribution system has been developed that continuously delivers a stable optical frequency of 268 THz (corresponding to a wavelength of 1118 nm) to different experiments in our institute. For that purpose, a continuous wave (cw) fiber laser has been stabilized onto a frequency comb and distributed across the building by the use of a fiber network. While the light propagates through the fiber, acoustic and thermal effects counteract against the stability and accuracy of the system. However, by employing proper stabilization methods a stability of 2 x 10(-13) tau(-1/2) is achieved, limited by the available radio frequency (RF) reference. Furthermore, the issue of counter-dependant results of the Allan deviation was examined during the data evaluation.

Ultrafast quantum control of ionization dynamics in krypton.

Ultrafast spectroscopy with attosecond resolution has enabled the real time observation of ultrafast electron dynamics in atoms, molecules and solids. These experiments employ attosecond pulses or pulse trains and explore dynamical processes in a pump-probe scheme that is selectively sensitive to electronic state of matter via photoelectron or XUV absorption spectroscopy or that includes changes of the ionic state detected via photo-ion mass spectrometry. Here, we demonstrate how the implementation of combined photo-ion and absorption spectroscopy with attosecond resolution enables tracking the complex multidimensional excitation and decay cascade of an Auger auto-ionization process of a few femtoseconds in highly excited krypton. In tandem with theory, our study reveals the role of intermediate electronic states in the formation of multiply charged ions. Amplitude tuning of a dressing laser field addresses different groups of decay channels and allows exerting temporal and quantitative control over the ionization dynamics in rare gas atoms.