Sub-attosecond-precision optical-waveform stability measurements using electro-optic sampling.

The generation of laser pulses with controlled optical waveforms, and their measurement, lie at the heart of both time-domain and frequency-domain precision metrology. Here, we obtain mid-infrared waves via intra-pulse difference-frequency generation (IPDFG) driven by 16-femtosecond near-infrared pulses, and characterise the jitter of sub-cycle fractions of these waves relative to the gate pulses using electro-optic sampling (EOS). We demonstrate sub-attosecond temporal jitter at individual zero-crossings and sub-0.

Dynamic optical response of solids following 1-fs-scale photoinjection.

Photoinjection of charge carriers profoundly changes the properties of a solid. This manipulation enables ultrafast measurements, such as electric-field sampling, advanced recently to petahertz frequencies, and the real-time study of many-body physics. Nonlinear photoexcitation by a few-cycle laser pulse can be confined to its strongest half-cycle.

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.

Breast-cancer detection using blood-based infrared molecular fingerprints.

Background: Breast cancer screening is currently predominantly based on mammography, tainted with the occurrence of both false positivity and false negativity, urging for innovative strategies, as effective detection of early-stage breast cancer bears the potential to reduce mortality. Here we report the results of a prospective pilot study on breast cancer detection using blood plasma analyzed by Fourier-transform infrared (FTIR) spectroscopy - a rapid, cost-effective technique with minimal sample volume requirements and potential to aid biomedical diagnostics. FTIR has the capacity to probe health phenotypes via the investigation of the full repertoire of molecular species within a sample at once, within a single measurement in a high-throughput manner.

Infrared molecular fingerprinting of blood-based liquid biopsies for the detection of cancer.

Recent omics analyses of human biofluids provide opportunities to probe selected species of biomolecules for disease diagnostics. Fourier-transform infrared (FTIR) spectroscopy investigates the full repertoire of molecular species within a sample at once. Here, we present a multi-institutional study in which we analysed infrared fingerprints of plasma and serum samples from 1639 individuals with different solid tumours and carefully matched symptomatic and non-symptomatic reference individuals.

Molecular Origin of Blood-Based Infrared Spectroscopic Fingerprints*.

Infrared spectroscopy of liquid biopsies is a time- and cost-effective approach that may advance biomedical diagnostics. However, the molecular nature of disease-related changes of infrared molecular fingerprints (IMFs) remains poorly understood, impeding the method's applicability. Here we probe 148 human blood sera and reveal the origin of the variations in their IMFs.

Stability of person-specific blood-based infrared molecular fingerprints opens up prospects for health monitoring.

Health state transitions are reflected in characteristic changes in the molecular composition of biofluids. Detecting these changes in parallel, across a broad spectrum of molecular species, could contribute to the detection of abnormal physiologies. Fingerprinting of biofluids by infrared vibrational spectroscopy offers that capacity.

Multi-octave, CEP-stable source for high-energy field synthesis.

The development of high-energy, high-power, multi-octave light transients is currently the subject of intense research driven by emerging applications in attosecond spectroscopy and coherent control. We report on a phase-stable, multi-octave source based on a Yb:YAG amplifier for light transient generation. We demonstrate the amplification of a two-octave spectrum to 25 μJ of energy in two broadband amplification channels and their temporal compression to 6 and 18 fs at 1 and 2 μm, respectively.

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.

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 challenge. Here we show how broadband optical coherence opens up opportunities for fingerprinting complex molecular ensembles in their natural environment.

Complementary Si/SiO 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 SiO thin-film materials. The pair exhibits unparalleled reflectance exceeding 99.

Broadband dispersive Ge/YbF 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.

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

Lasers based on Cr-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 Cr-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.

Intra-pulse difference-frequency generation of mid-infrared (2.7-20 μm) by random quasi-phase-matching.

We present a mid-infrared (MIR) source based on intra-pulse difference-frequency generation under the random quasi-phase-matching condition. The scheme enables the use of non-birefringent materials whose crystal orientations are not perfectly and periodically poled, widening the choice of media for nonlinear frequency conversion. With a 2 μm driving source based on a Ho:YAG thin-disk laser, together with a polycrystalline ZnSe element, an octave-spanning MIR continuum (2.

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.

Multi-mW, few-cycle mid-infrared continuum spanning from 500 to 2250 cm.

The demand for and usage of broadband coherent mid-infrared sources, such as those provided by synchrotron facilities, are growing. Since most organic molecules exhibit characteristic vibrational modes in the wavelength range between 500 and 4000 cm, such broadband coherent sources enable micro- or even nano-spectroscopic applications at or below the diffraction limit with a high signal-to-noise ratio. These techniques have been applied in diverse fields ranging from life sciences, material analysis, and time-resolved spectroscopy.

Nonlinear pulse compression in a gas-filled multipass cell.

We present an efficient method for compressing sub-picosecond pulses at 200 W average power with 2 mJ pulse energy in a multipass cell filled with different gases. We demonstrate spectral broadening by more than a factor of five using neon, argon, and nitrogen as nonlinear media. The 210 fs input pulses are compressed down to 37 fs and 35 GW peak power with a beam quality factor of 1.

Multi-watt, multi-octave, mid-infrared femtosecond source.

Spectroscopy in the wavelength range from 2 to 11 μm (900 to 5000 cm) implies a multitude of applications in fundamental physics, chemistry, as well as environmental and life sciences. The related vibrational transitions, which all infrared-active small molecules, the most common functional groups, as well as biomolecules like proteins, lipids, nucleic acids, and carbohydrates exhibit, reveal information about molecular structure and composition. However, light sources and detectors in the mid-infrared have been inferior to those in the visible or near-infrared, in terms of power, bandwidth, and sensitivity, severely limiting the performance of infrared experimental techniques.

Synthesis, fabrication and characterization of a highly-dispersive mirrors for the 2 µm spectral range.

We report a challenging design, fabrication and post-production characterization problem of a dispersive mirror supporting the spectral range from 2000 nm to 2200 nm and providing a group delay dispersion of -1000 fs. The absolute reflectance in the working range is over 99.95%.

1 kW, 200 mJ picosecond thin-disk laser system.

We report on a laser system based on thin-disk technology and chirped pulse amplification, providing output pulse energies of 200 mJ at a 5 kHz repetition rate. The amplifier contains a ring-type cavity and two thin Yb:YAG disks, each pumped by diode laser systems providing up to 3.5 kW power at a 969 nm wavelength.

Near-PHz-bandwidth, phase-stable continua generated from a Yb:YAG thin-disk amplifier.

We report on the generation of a multi-octave, phase-stable continuum from the output of a Yb:YAG regenerative amplifier delivering 1-ps pulses with randomly varying carrier-envelope phase (CEP). The intrinsically CEP-stable spectral continuum spans from 450 nm to beyond 2500 nm, covering a spectral range of about 0.6 PHz.

Direct regenerative amplification of femtosecond pulses to the multimillijoule level.

We present a compact femtosecond nonlinear Yb:YAG thin-disk regenerative amplifier delivering pulses carried at a wavelength of 1030 nm with an average power of >200  W at a repetition rate of 100 kHz and an energy noise value of 0.46% (rms) in a beam with a propagation factor of M<1.4.

Powerful 100-fs-scale Kerr-lens mode-locked thin-disk oscillator.

We have recently demonstrated a simple power scaling procedure for Kerr-lens mode-locked thin-disk oscillators. Here we report on the extension of this scheme to a broadband high-peak-power thin-disk oscillator, delivering 140-fs pulses with a peak and average power of 62 MW and 155 W, respectively. This result shows that reaching the emission bandwidth of the gain material in Kerr-lens mode-locked thin-disk oscillators is feasible without sacrificing output power, efficiency, or stability by relying on high intracavity nonlinearities.

Atomic-scale diffractive imaging of sub-cycle electron dynamics in condensed matter.

For interaction of light with condensed-matter systems, we show with simulations that ultrafast electron and X-ray diffraction can provide a time-dependent record of charge-density maps with sub-cycle and atomic-scale resolutions. Using graphene as an example material, we predict that diffraction can reveal localised atomic-scale origins of optical and electronic phenomena. In particular, we point out nontrivial relations between microscopic electric current and density in undoped graphene.