Field-resolved infrared spectroscopy of biological systems.

The proper functioning of living systems and physiological phenotypes depends on molecular composition. Yet simultaneous quantitative detection of a wide variety of molecules remains a challenge1-8. Here we show how broadband optical coherence opens up opportunities for fingerprinting complex molecular ensembles in their natural environment. Vibrationally excited molecules emit a coherent electric field following few-cycle infrared laser excitation9-12, and this field is specific to the sample's molecular composition. Employing electro-optic sampling10,12-15, we directly measure this global molecular fingerprint down to field strengths 107 times weaker than that of the excitation. This enables transillumination of intact living systems with thicknesses of the order of 0.1 millimetres, permitting broadband infrared spectroscopic probing of human cells and plant leaves. In a proof-of-concept analysis of human blood serum, temporal isolation of the infrared electric-field fingerprint from its excitation along with its sampling with attosecond timing precision results in detection sensitivity of submicrograms per millilitre of blood serum and a detectable dynamic range of molecular concentration exceeding 105. This technique promises improved molecular sensitivity and molecular coverage for probing complex, real-world biological and medical settings.

49 W carrier-envelope-phase-stable few-cycle 2.1†µm OPCPA at 10 kHz.

We demonstrate a mid-infrared optical parametric chirped pulse amplifier (OPCPA), delivering 2.1 µm center wavelength pulses with 20 fs duration and 4.9 mJ energy at 10 kHz repetition rate. This self-seeded system is based on a kW-class Yb:YAG thin-disk amplifier driving a CEP stable short-wavelength-infrared (SWIR) generation and three consecutive OPCPA stages. Our SWIR source achieves an average power of 49 W, while still maintaining excellent phase and average power stability with sub-100 mrad carrier-envelope-phase-noise and 0.8% average power fluctuations. These parameters enable the OPCPA setup to drive attosecond pump probe spectroscopy experiments with photon energies in the water window.

Complementary dispersive mirror pair produced in one coating run based on desired non-uniformity.

We report a novel one-coating-run method for producing an octave-spanning complementary dispersive mirror (DM) pair. The anti-phase group delay dispersion (GDD) oscillations are realized by two mirrors of the DM pair due to the certain thickness difference. Both mirrors are deposited within a single coating run enabled by the non-uniformity of the ion beam sputtering coating plant, which is obtained by tuning the distance between the source target and coating substrates. Since the DM pair is produced in a single deposition run, the GDD performance is more robust against deposition errors than that of the conventional complementary DM pair, in which two separated coating runs are necessary. Moreover, the new DM pair is compatible for both laser polarizations under the same angle of incidence, which could effectively reduce the difficulties of alignment for their implementation in laser systems than the double angle DM pair. The new DM pair is successfully applied to compress pulses from a Ti: Sapphire laser system down to 4.26 fs in pulse duration.

Second and third-order dispersion compensating mirror pairs for the spectral range from 1.2-3.2µm.

We demonstrate the design, production, characterization and application of two dispersive complementary mirror pairs compensating second- and third-order dispersion, respectively. Both mirror pairs operate in the spectral range from 1.2-3.2µm. This is an unprecedented bandwidth of over 1.4 octaves which can drive further improvements in Cr:ZnS, Cr:ZnSe and other laser systems with a central wavelength around 2µm. The first pair provides a constant group delay dispersion of -100fs2, while the second one enables the compensation of the third-order dispersion that is introduced by a TiO2 crystal.

Directly diode-pumped femtosecond Cr:ZnS amplifier with ultra-low intensity noise.

Diode-pumped Cr:ZnS oscillators have emerged as precursors for single-cycle infrared pulse generation with excellent noise performance. Here we demonstrate a Cr:ZnS amplifier with direct diode-pumping to boost the output of an ultrafast Cr:ZnS oscillator with minimum added intensity noise. Seeded with a 0.66-W pulse train at 50-MHz repetition rate and 2.4 µm center wavelength, the amplifier provides over 2.2 W of 35-fs pulses. Due to the low-noise performance of the laser pump diodes in the relevant frequency range, the amplifier output achieves a root mean square (RMS) intensity noise level of only 0.03% in the 10 Hz-1 MHz frequency range and a long-term power stability of 0.13% RMS over one hour. The diode-pumped amplifier reported here is a promising driving source for nonlinear compression to the single- or sub-cycle regime, as well as for the generation of bright, multi-octave-spanning mid-infrared pulses for ultra-sensitive vibrational spectroscopy.

Measurement and control of optical nonlinearities in dispersive dielectric multilayers.

Dispersive dielectric multilayer mirrors, high-dispersion chirped mirrors in particular, are widely used in modern ultrafast optics to manipulate spectral chirps of ultrashort laser pulses. Dispersive mirrors are routinely designed for dispersion compensation in ultrafast lasers and are assumed to be linear optical components. In this work, we report the experimental characterization of an unexpectedly strong nonlinear response in these chirped mirrors. At modest peak intensities <2 TW/cm2-well below the known laser-induced damage threshold of these dielectric structures-we observed a strong reflectivity decrease, local heating, transient spectral modifications, and time-dependent absorption of the incident pulse. Through computational analysis, we found that the incident laser field can be enhanced by an order of magnitude in the dielectric layers of the structure. The field enhancement leads to a wavelength-dependent nonlinear absorption, that shows no signs of cumulative damage before catastrophic failure. The nonlinear absorption is not a simply two-photon process but instead is likely mediated by defects that facilitate two-photon absorption. To mitigate this issue, we designed and fabricated a dispersive multilayer design that strategically suppresses the field enhancement in the high-index layers, shifting the high-field regions to the larger-bandgap, low-index layers. This strategy significantly increases the maximum peak intensity that the mirror can sustain. However, our finding of an onset of nonlinear absorption even at 'modest' fluence and peak intensity has significant implications for numerous past published experimental works employing dispersive mirrors. Additionally, our results will guide future ultrafast experimental work and ultrafast laser design.

Spectral broadening of 112 mJ, 1.3 ps pulses at 5 kHz in a LG10 multipass cell with compressibility to 37 fs.

The first-order helical Laguerre-Gaussian mode (also called donut mode) is used to improve the energy throughput of nonlinear spectral broadening in gas-filled multipass cells. The method proposed in this Letter enables, for the first time to the best of our knowledge, the nonlinear spectral broadening of pulses with energies beyond 100 mJ and is suitable for an average power of more than 500 W while conserving an excellent spatio-spectral homogeneity of ∼98% and a Gaussian-like focus profile. Additionally compressibility from 1.3 ps to 37 fs is demonstrated.

Efficient nonlinear compression of a thin-disk oscillator to 8.5 fs at 55 W average power.

We demonstrate an efficient hybrid-scheme for nonlinear pulse compression of high-power thin-disk oscillator pulses to the sub-10 fs regime. The output of a home-built, 16 MHz, 84 W, 220 fs Yb:YAG thin-disk oscillator at 1030 nm is first compressed to 17 fs in two nonlinear multipass cells. In a third stage, based on multiple thin sapphire plates, further compression to 8.5 fs with 55 W output power and an overall optical efficiency of 65% is achieved. Ultrabroadband mid-infrared pulses covering the spectral range 2.4-8µm were generated from these compressed pulses by intra-pulse difference frequency generation.

3-6 µm dispersive mirrors compensating for dispersion introduced by the GaAs crystal.

A new broadband dispersive mirror (DM), which consists of Si and SiO2 layer materials operating in the spectral range of 3-6 µm, is developed for the first time, to our knowledge. The DM is able to compensate for the dispersion of a 0.5 mm thick GaAs crystal per bounce. Pulse analysis proves that the compensation effect of the DM is much better than a CaF2 plate, which is the commonly used dispersion compensation element in mid-infrared optical parametric oscillators (MIR OPOs), and the new MIR DM could improve the MIR OPO spectrum with better pulse quality and short pulse duration.

Design, fabrication and measurement of highly-dispersive mirrors with total internal reflection.

High group delay dispersion (GDD) is often required for ultrafast laser applications. To achieve GDD level higher than -10000 fs2 in a single mirror setting is difficult due to the high sensitivity to unavoidable production inaccuracies. To overcome the problem, total internal reflection (TIR) based dispersive mirrors have been proposed in theory. In this paper, we report our continuous effort to further design, fabricate and measure TIR based dispersive mirrors.

Characterization of e-beam evaporated Ge, YbF3, ZnS, and LaF3 thin films for laser-oriented coatings.

Thin films of Ge, ZnS, YbF3, and LaF3 produced using e-beam evaporation on ZnSe and Ge substrates were characterized in the range of 0.4-12 µm. It was found that the Sellmeier model provides the best fit for refractive indices of ZnSe substrate, ZnS, and LaF3 films; the Cauchy model provides the best fit for YbF3 film. Optical constants of Ge substrate and Ge film as well as extinction coefficients of ZnS, YbF3, LaF3, and ZnSe substrate are presented in the frame of a non-parametric model. For the extinction coefficient of ZnS, the exponential model is applicable. Stresses in Ge, ZnS, YbF3, and LaF3 were estimated equal to (-50)MPa, (-400)MPa, 140 MPa, and 380 MPa, respectively. The surface roughness does not exceed 5 nm for all films and substrates.

Optical interference coating design contest 2019: a non-polarizing beam splitter and a color-mixing challenge [Invited].

A non-polarizing beam splitter and a light color-mixing challenge were the topics of the design contest held in conjunction with the 2019 Optical Interference Coatings topical meeting of the Optical Society of America. A total of 10 designers from China, France, Germany, Japan, and the United States submitted over 70 designs for problems A and B. The design problems and the submitted solutions are described and evaluated.

Comparative study of NIR-MIR beamsplitters based on ZnS/YbF3 and Ge/YbF3.

Two beamsplitters operating across the near-infrared (770-1050 nm) and mid-infrared (4-8 µm) spectral ranges are developed. For the first time, the beamsplitters based on thin-film materials combinations of ZnS/YbF3 and Ge/YbF3 are investigated. The multilayers operate at the Brewster angle of ZnSe substrate. There are no special temperature conditions. The dichroic coatings are designed, produced, and carefully characterized. Potentials of the ZnS/YbF3 and Ge/YbF3 thin-film material combinations are discussed based on analytical estimations, as well as on optical and non-optical characterization results. The ZnS/YbF3 pair provides high reflectance in the near-infrared spectral range. The Ge/YbF3 solutions exhibit very broadband reflection zones. The Ge/YbF3 coatings are thinner and comprise fewer layers than ZnS/YbF3 multilayers. Ge/YbF3 pair has high potential for design and production of NIR-MIR coatings.

Complementary Si/SiO2 dispersive mirrors for 2-4†µm spectral range.

Complementary pair of dispersive multilayers operating in the 2-4 µm spectral range were designed and produced for the first time. The mirrors comprise layers of Si and SiO2 thin-film materials. The pair exhibits unparalleled reflectance exceeding 99.7% and provides a group delay dispersion of (-200) fs2. The mirrors can be used in Cr:ZnS/Cr:ZnSe femtosecond lasers and amplifiers.

Directly diode-pumped, Kerr-lens mode-locked, few-cycle Cr:ZnSe oscillator.

Lasers based on Cr2+-doped II-VI material, often known as the Ti:Sapphire of the mid-infrared, can directly provide few-cycle pulses with octave-spanning spectra, and serve as efficient drivers for generating broadband mid-infrared radiation. It is expected that the wider adoption of this technology benefits from more compact and cost-effective embodiments. Here, we report the first directly diode-pumped, Kerr-lens mode-locked Cr2+-doped II-VI oscillator pumped by a single InP diode, providing average powers over 500 mW and pulse durations of 45 fs - shorter than six optical cycles at 2.4 µm. These correspond to a sixty-fold increase in peak power compared to the previous diode-pumped record, and are at similar levels with respect to more mature fiber-pumped oscillators. The diode-pumped femtosecond oscillator presented here constitutes a key step toward a more accessible alternative to synchrotron-like infrared radiation and is expected to accelerate research in laser spectroscopy and ultrafast infrared optics.

2/3 octave Si/SiO2 infrared dispersive mirrors open new horizons in ultrafast multilayer optics.

Dispersive mirrors operating in a broadband infrared spectral range are reported for the first time. The mirrors are based on Si/SiO2 thin-film materials. The coatings exhibit reflectance exceeding 99.6% in the spectral range from 2 to 3.2 µm and provide a group delay dispersion of -100 fs2 and -200 fs2 in this range. The fabricated mirrors are expected to be key elements of Cr:ZnS/Cr:ZnSe femtosecond lasers and amplifiers. The mirrors open a new avenue in the development of ultrafast dispersive optics operating in the infrared spectral range.

Efficient femtosecond mid-infrared generation based on a Cr:ZnS oscillator and step-index fluoride fibers.

Femtosecond light sources in the 3-5 µm region are highly sought after for numerous applications. While they can be generated by using nonlinear effects in optical fibers, the efficiencies and effectiveness of frequency conversion can be significantly enhanced by using ultrashort driving pulses. Here, we report on a few-cycle Cr:ZnS oscillator driving low-order soliton dynamics in soft-glass fibers. By selecting appropriate parameters, sub-two-cycle pulses or broad supercontinua spanning over 1.7 octaves from 1.6 to 5.1 µm can be generated at average power levels exceeding 300 mW. In the same setting, Raman-induced soliton self-frequency shifting has been exploited to generate sub-100-fs pulses continuously tunable from 2.3 to 3.85 µm with a conversion efficiency of ∼50%. These results demonstrate the vast potential of using Cr:ZnS or Cr:ZnSe lasers for powerful mid-infrared generation.

Broadband mid-infrared coverage (2-17 µm) with few-cycle pulses via cascaded parametric processes.

A myriad of existing and emerging applications could benefit from coherent and broadband mid-infrared (MIR) light. Yet, existing tabletop sources are often complex or sensitive to interferometric optical misalignment. Here we demonstrate a significantly simplified scheme of broadband MIR generation by cascading the intra-pulse difference-frequency generation process in a specific nonlinear crystal. This allows pulses generated directly from mode-locked lasers to be used without further nonlinear temporal compression. The system, together with the driving beam, can provide an ultra-broadband coherent radiation coverage ranging from 2 to 17 µm with femtosecond pulse durations. To the best of our knowledge, this is the first demonstration of cascaded DFG in the MIR range, which brings emerging time-domain spectroscopic techniques closer to real-world applications.

Broadband dispersive Ge/YbF3 mirrors for mid-infrared spectral range.

Broadband dispersive mirrors operating in the mid-infrared spectral range of 6.5-11.5 µm are developed for the first time, to the best of our knowledge. The mirrors comprise Ge and YbF3 layers, which have not been used before for manufacturing of multilayer dispersive optics. The design and production processes are described; mechanical stresses of the coatings are estimated based on experimental data; and spectral and phase properties of the produced mirrors are measured. The mirrors compensate group delay dispersion of ultrashort laser pulses accumulated by propagation through 4 mm ZnSe windows and additional residual phase modulation of an ultrashort laser pulse.

Mid-infrared long-pass filter for high-power applications based on grating diffraction.

A gold-coated silicon grating has been developed, enabling efficient spatial separation of broadband mid-infrared (MIR) beams with wavelengths >5 µm from collinearly propagating, broadband, high-power light in the near-infrared (NIR) spectral range (centered at 2 µm). The optic provides spectral filtering at high powers in a thermally robust and chromatic-dispersion-free manner such as that necessary for coherent MIR radiation sources based on parametric frequency downconversion of femtosecond NIR lasers. The suppression of a >20 W average-power, 2 µm driving pulse train by three orders of magnitude, while retaining high reflectivity of the broadband MIR beam, is presented.