Standardized Electric-Field-Resolved Molecular Fingerprinting.

Field-resolved infrared spectroscopy (FRS) of impulsively excited molecular vibrations can surpass the sensitivity of conventional time-integrating spectroscopies, owing to a temporal separation of the molecular signal from the noisy excitation. However, the resonant response carrying the molecular signal of interest depends on both the amplitude and phase of the excitation, which can vary over time and across different instruments. To date, this has compromised the accuracy with which FRS measurements could be compared, which is a crucial factor for practical applications. Here, we utilize a data processing procedure that overcomes this shortcoming while preserving the sensitivity of FRS. We validate the approach for aqueous solutions of molecules. The employed approach is compatible with established processing and evaluation methods for the analysis of infrared spectra and can be applied to existing spectra from databases, facilitating the spread of FRS to new molecular analytical applications.

Deep search methods for multilayer coating design.

Many existing well-known multilayer design methods are based on so-called greedy algorithms. New deep search algorithms developed for needle optimization, gradual evolution, and design cleaner methods are presented. The algorithms possess machine learning features. The advantages of the deep search methods are demonstrated on a set of examples including the OIC Design Contest 2019.

Broadband phase-shifting mirrors for ultrafast lasers.

Metal-dielectric phase-shifting multilayer optical elements have been developed, providing broadband, virtually dispersion-free polarization manipulation down to the few-cycle level. These optical elements are Ag/Al2O3 mirrors that operate in the spectral range from 500 to 100 nm, exhibiting reflectance higher than 95%, and a differential phase shift between the s- and p-polarization of about 90° distributed over four bounces. The mirrors have been designed, produced, and reliably characterized based on spectral photometric and ellipsometric data using a non-parametric approach as well as a multi-oscillator model. The optical elements were implemented into a few-cycle laser system, where they transformed linearly polarized few-cycle light pulses to circular polarization.

10 W CEP-stable few-cycle source at 2 µm with 100 kHz repetition rate.

We developed a high repetition rate optical parametric chirped-pulse amplification (OPCPA) laser system based on fiber-laser-seeded Innoslab to generate few-cycle pulses around 2 µm with passively stable carrier-envelope phase (CEP) by difference frequency generation (DFG). Incorporating a piezo mirror before the DFG stage permits rapid CEP control. The OPCPA system is seeded by a stable supercontinuum generated in bulk material with the picosecond Innoslab pulses. Few-cycle pulses with durations of 17 fs and energies of over 100 µJ were produced in a single OPCPA stage. Three different nonlinear crystals: BBO, BiBO, and LNB were tested in the final parametric amplifier, and their average power related limitations are addressed.

Compact and flexible harmonic generator and three-color synthesizer for femtosecond coherent control and time-resolved studies.

Intense, multi-color laser fields permit the control of the ionization of atoms and the steering of electron dynamics. Here, we present the efficient collinear creation of the second and third harmonic of a 790 nm femtosecond laser followed by a versatile field synthesizer for the three color fields' composition. Using the device, we investigate the strong-field ionization of neon by fields composed of the fundamental, and the second or third harmonic. The three-color device offers sufficient flexibility for the coherent control of strong-field processes and for time-resolved pump-probe studies.

Production of Brewster angle thin film polarizers using a ZrO2/SiO2 pair of materials.

The production of polarizers for high-intensity applications based on a ZrO2/SiO2 pair of thin film materials is discussed. A special approach to accurate determination of a ZrO2 refractive index and the application of direct broadband optical monitoring enable obtaining good manufacturing results.

Enhancement cavities for few-cycle pulses.

We address the challenge of increasing the bandwidth of high-finesse femtosecond enhancement cavities and demonstrate a broad spectrum spanning 1800 cm-1 (195 nm) at -10 dB around a central wavelength of 1050 nm in an EC with an average finesse exceeding 300. This will benefit a host of spectroscopic applications, including transient absorption spectroscopy, direct frequency comb spectroscopy, and Raman spectroscopy. The pulse circulating in the EC is composed of only 5.4 optical cycles, at a kilowatt-level average power. Together with a suitable gating technique, this paves the way to the efficient generation of multi-megahertz-repetition-rate isolated extreme ultraviolet attosecond pulses via intracavity high-order harmonic generation.

Enhancement cavities for zero-offset-frequency pulse trains.

The optimal enhancement of broadband optical pulses in a passive resonator requires a seeding pulse train with a specific carrier-envelope-offset frequency. Here, we control the phase of the cavity mirrors to tune the offset frequency for which a given comb is optimally enhanced. This enables the enhancement of a zero-offset-frequency train of sub-30-fs pulses to multi-kW average powers. The combination of pulse duration, power, and zero phase slip constitutes a crucial step toward the generation of attosecond pulses at multi-10-MHz repetition rates. In addition, this control affords the enhancement of pulses generated by difference-frequency mixing, e.g., for mid-infrared spectroscopy.

Femtosecond Enhancement Cavities in the Nonlinear Regime.

We combine high-finesse optical resonators and spatial-spectral interferometry to a highly phase-sensitive investigation technique for nonlinear light-matter interactions. We experimentally validate an ab initio model for the nonlinear response of a resonator housing a gas target, permitting the global optimization of intracavity conversion processes like high-order harmonic generation. We predict the feasibility of driving intracavity high-order harmonic generation far beyond intensity limitations observed in state-of-the-art systems by exploiting the intracavity nonlinearity to compress the pulses in time.

High-power multi-megahertz source of waveform-stabilized few-cycle light.

Waveform-stabilized laser pulses have revolutionized the exploration of the electronic structure and dynamics of matter by serving as the technological basis for frequency-comb and attosecond spectroscopy. Their primary sources, mode-locked titanium-doped sapphire lasers and erbium/ytterbium-doped fibre lasers, deliver pulses with several nanojoules energy, which is insufficient for many important applications. Here we present the waveform-stabilized light source that is scalable to microjoule energy levels at the full (megahertz) repetition rate of the laser oscillator. A diode-pumped Kerr-lens-mode-locked Yb:YAG thin-disk laser combined with extracavity pulse compression yields waveform-stabilized few-cycle pulses (7.7 fs, 2.2 cycles) with a pulse energy of 0.15 µJ and an average power of 6 W. The demonstrated concept is scalable to pulse energies of several microjoules and near-gigawatt peak powers. The generation of attosecond pulses at the full repetition rate of the oscillator comes into reach. The presented system could serve as a primary source for frequency combs in the mid infrared and vacuum UV with unprecedented high power levels.

Automated construction of monochromatic monitoring strategies.

We focus our efforts on development of an advanced monochromatic monitoring strategy to assist the optical coating engineer in finding a single wavelength or a sequence of monitoring wavelengths that meet simultaneously several practical demands, namely, specified input and output swing values, specified amplitude of a monitoring signal variation, and the distance between trigger point and the last signal extremum. Additionally, the most important demand is that the number of different monitoring wavelengths must be as small as possible. Manual construction of such a monitoring strategy is almost impossible because of a large number of conditions to be satisfied. We propose an algorithm that automatically generates a monitoring spreadsheet so that all demands can be satisfied as closely as possible. We consider six typical design problems and obtain a series of solutions for each of them. Then, we provide computational simulations of deposition processes assuming that they are controlled by monochromatic monitoring with the monitoring strategy generated by our algorithm, and we demonstrate how an optical coating engineer can select design solutions that exhibit the highest production yields.

Sensitivity-directed refinement for designing broadband blocking filters.

We developed a new method aimed at designing short-pass filters, long-pass filters and filters blocking sidebands of Fabry-Perot bandpasses. The method is an automated version of a non-straightforward empirical approach invented as a result of many years' experience in design and production of optical coatings. The method allows obtaining near-quarter-wave solutions in a few seconds. In many cases these solutions are more advantageous for deposition systems.

Reverse engineering of multilayer coatings for ultrafast laser applications.

We propose a reliable reverse engineering approach for a postproduction characterization of complicated optical coatings for ultrafast laser applications. We perform the postproduction characterization on the basis of in situ broadband monitoring data and validate the results using ex situ transmittance data and group delay measurements.

Study of HfO2/SiO2 dichroic laser mirrors with refractive index inhomogeneity.

HfO2/SiO2 dichroic mirrors, having high reflectance at 1064 nm and high transmittance at 532 nm, play an important role in high-power laser systems. However, the half-wave hole effect, caused mainly by the refractive index inhomogeneity of hafnia, affects the spectra and application of these mirrors. Two approaches to eliminate the half-wave hole effect have been proposed. Both approaches attempt to shift the location of the half-wave hole in comparison with the original wavelength. One approach broadens the reflectance band of the first harmonic wavelength and simultaneously adjusts the central reflectance band to a longer wavelength, whereas the other approach combines the two stacks to adjust the location of the half-wave hole far away from the wavelength of interest. Two kinds of dichroic mirrors have been successfully fabricated; moreover, it was found that the method of a two-stack combination, 0.9(HL)8 and 1.1(HL)8, provides designs that can be fabricated more easily and with better quality spectral characteristics.

Reliable optical characterization of e-beam evaporated TiO2 films deposited at different substrate temperatures.

We studied e-beam evaporated TiO2 films deposited at two different substrate temperatures between 120°C and 300°C. We reliably characterized the film samples on the basis of in situ and ex situ measurements. We carried out annealing on the samples and studied the induced changes in the properties of the films. The results can be useful for further laser-induced damage threshold investigations.

Design and production of antireflection coating for the 8-10 µm spectral region.

A special design procedure allowing to trap layer thicknesses inside specified limits is applied for designing of antireflection coating (AR) for the infrared spectral band of 8-10 µm. The obtained AR design has no too thick layers that may cause delaminating of the deposited AR coating. A special monitoring procedure taking into account wavelength positions of monitoring signal extrema is applied for coating deposition. The manufactured coating features excellent AR properties in the requested spectral region and possesses high mechanical stability.

Empirical study of the group delay dispersion achievable with multilayer mirrors.

With the help of the most advanced algorithms we obtained many dozens of multilayer dispersive mirror designs to empirically find limits for the maximum achievable negative value of the group delay dispersion (GDD). This value depends on the total thickness of coatings and layer material combination. Nb(2)O(5)/SiO(2) and Ta(2)O(50/SiO(2) combinations are studied in detail, for combinations HfO(2)/SiO(2) and TiO(2)/SiO(2) we obtained estimations for two bandwidths. We also show that reasonable values of third-order dispersion have no significant impact on the obtained results. Current state-of-the-art technology allows to produce designs with total physical thicknesses slightly higher than 10 µm and to achieve maximum negative GDD values corresponding to this total design thickness. Designs with total physical thickness of 15 µm and 20 µm are not realized yet due to high sensitivity to deposition errors.

Measurements of the group delay and the group delay dispersion with resonance scanning interferometer.

We developed a method for group delay and group delay dispersion measurements, based on location of interference resonance peaks. Such resonance peaks can be observed in transmittance or in reflectance when two mirrors are placed parallel to each other and separated by a thin air spacer. By using a novel approach, based on simultaneous processing of the data acquired for different spacer distances we obtained reliable results with high resolution. Measurements were performed both in transmittance and reflectance layouts depending on the reflectivity of the mirror to be measured. The developed method allows dispersion measurements of ultraviolet mirrors and ultra-broadband mirrors spanning more than one optical octave to be performed.

High-dispersive mirrors for high power applications.

We report on the development and manufacturing of two different types of high-dispersive mirrors (HDM). One of them provides a record value for the group delay dispersion (GDD) of -4000 fs2 and covers the wavelength range of 1027-1033 nm, whereas the other one provides -3000 fs2 over the wavelength range of 1020-1040 nm. Both of the fabricated mirrors exhibit a reflectance of >99.9% and are well suited for intracavity applications. Mirrors of the second type have been successfully employed in a Kerr-lens mode-locked Yb:YAG thin-disk oscillator for the generation of 200-fs pulses with multi-10-W average power.

Robust synthesis of dispersive mirrors.

A synthesis technique allowing to obtain a set of robust designs is reported. The robust synthesis is based on simultaneous optimization of spectral characteristics of multiple designs located in a small neighborhood of a so-called pivotal design. Efficiency of this technique is demonstrated by the synthesis and successful experimental realization of a high dispersive mirror. The fabricated dispersive mirror covers 690-890 nm wavelength range and provides the dispersion of -300 fs2 at 800 nm.