Comment on "Terahertz pump-probe of liquid water at 12.3 THz" by F. Novelli, C. Hoberg, E. M. Adams, J. M. Klopf and M. Havenith, , 2022, 24, 653-665.

The interpretation of the data presented by Novelli at al. as the nonlinear response of water is questioned.

Highly efficient THz four-wave mixing in doped silicon.

Third-order non-linearities are important because they allow control over light pulses in ubiquitous high-quality centro-symmetric materials like silicon and silica. Degenerate four-wave mixing provides a direct measure of the third-order non-linear sheet susceptibility χL (where L represents the material thickness) as well as technological possibilities such as optically gated detection and emission of photons. Using picosecond pulses from a free electron laser, we show that silicon doped with P or Bi has a value of χL in the THz domain that is higher than that reported for any other material in any wavelength band.

Spin preservation during THz orbital pumping of shallow donors in silicon.

We investigate the spin relaxation under conditions of optical excitation between the Rydberg orbital states of phosphorus donor impurities in silicon. Here we show that the spin relaxation is less than a few percent, even after multiple excitation/relaxation cycles. The observed high level of spin preservation may be useful for readout cycling or in quantum information schemes where coupling of neighbor qubits is via orbital excitation.

Acid solvation versus dissociation at "stardust conditions": Reaction sequence matters.

Chemical reactions at ultralow temperatures are of fundamental importance to primordial molecular evolution as it occurs on icy mantles of dust nanoparticles or on ultracold water clusters in dense interstellar clouds. As we show, studying reactions in a stepwise manner in ultracold helium nanodroplets by mass-selective infrared (IR) spectroscopy provides an avenue to mimic these "stardust conditions" in the laboratory. In our joint experimental/theoretical study, in which we successively add HO molecules to HCl, we disclose a unique IR fingerprint at 1337 cm that heralds hydronium (HO) formation and, thus, acid dissociation generating solvated protons.

Magnetoquantum Oscillations at THz Frequencies in InSb.

The ac magnetoconductance of bulk InSb at THz frequencies in high magnetic fields, as measured by the transmission of THz radiation, shows a field-induced transmission, which at high temperatures (≈100  K) is well explained with classical magnetoplasma effects (helicon waves). However, at low temperatures (4 K), the transmitted radiation intensity shows magnetoquantum oscillations that represent the Shubnikov-de Haas effect at THz frequencies. At frequencies above 0.

Coherent creation and destruction of orbital wavepackets in Si:P with electrical and optical read-out.

The ability to control dynamics of quantum states by optical interference, and subsequent electrical read-out, is crucial for solid state quantum technologies. Ramsey interference has been successfully observed for spins in silicon and nitrogen vacancy centres in diamond, and for orbital motion in InAs quantum dots. Here we demonstrate terahertz optical excitation, manipulation and destruction via Ramsey interference of orbital wavepackets in Si:P with electrical read-out.

Single-size thermometric measurements on a size distribution of neutral fullerenes.

We present measurements of the velocity distribution of electrons emitted from mass-selected neutral fullerenes, performed at the intracavity free electron laser FELICE. We make use of mass-specific vibrational resonances in the infrared domain to selectively heat up one out of a distribution of several fullerene species. Efficient energy redistribution leads to decay via thermionic emission.

Structures of the dehydrogenation products of methane activation by 5d transition metal cations.

The activation of methane by gas-phase transition metal cations (M(+)) has been studied extensively, both experimentally and using density functional theory (DFT). Methane is exothermically dehydrogenated by several 5d metal ions to form [M,C,2H](+) and H2. However, the structure of the dehydrogenation product has not been established unambiguously.

Scaling laws for photoelectron holography in the midinfrared wavelength regime.

Midinfrared strong-field laser ionization offers the promise of measuring holograms of atoms and molecules, which contain both spatial and temporal information of the ion and the photoelectron with subfemtosecond temporal and angstrom spatial resolution. We report on the scaling of photoelectron holographic interference patterns with the laser pulse duration, wavelength, and intensity. High-resolution holograms for the ionization of metastable xenon atoms by 7-16  μm light from the FELICE free electron laser are presented and compared to semiclassical calculations that provide analytical insight.

Influence of erroneous patient records on population pharmacokinetic modeling and individual bayesian estimation.

Background: Observational data sets can be used for population pharmacokinetic (PK) modeling. However, these data sets are generally less precisely recorded than experimental data sets. This article aims to investigate the influence of erroneous records on population PK modeling and individual maximum a posteriori Bayesian (MAPB) estimation.

[The 'paper-based' preoperative evaluation: non-optimal health care].

A nationwide preoperative assessment guideline was introduced in the Netherlands in 1997 at the advice of the Health Council of the Netherlands. The preoperative assessment should entail an appropriate interview, a physical examination, additional tests, risk assessment and informing the patient. Dutch and several international guidelines recommend a complete assessment under the responsibility of the anaesthesiologist.

Optimal sampling strategy development methodology using maximum a posteriori Bayesian estimation.

Maximum a posteriori Bayesian (MAPB) pharmacokinetic parameter estimation is an accurate and flexible method of estimating individual pharmacokinetic parameters using individual blood concentrations and prior information. In the past decade, many studies have developed optimal sampling strategies to estimate pharmacokinetic parameters as accurately as possible using either multiple regression analysis or MAPB estimation. This has been done for many drugs, especially immunosuppressants and anticancer agents.

Time-resolved holography with photoelectrons.

Ionization is the dominant response of atoms and molecules to intense laser fields and is at the basis of several important techniques, such as the generation of attosecond pulses that allow the measurement of electron motion in real time. We present experiments in which metastable xenon atoms were ionized with intense 7-micrometer laser pulses from a free-electron laser. Holographic structures were observed that record underlying electron dynamics on a sublaser-cycle time scale, enabling photoelectron spectroscopy with a time resolution of almost two orders of magnitude higher than the duration of the ionizing pulse.

Coherent control of Rydberg states in silicon.

Laser cooling and electromagnetic traps have led to a revolution in atomic physics, yielding dramatic discoveries ranging from Bose-Einstein condensation to the quantum control of single atoms. Of particular interest, because they can be used in the quantum control of one atom by another, are excited Rydberg states, where wavefunctions are expanded from their ground-state extents of less than 0.1 nm to several nanometres and even beyond; this allows atoms far enough apart to be non-interacting in their ground states to strongly interact in their excited states.

Intensity-resolved IR multiple photon ionization and fragmentation of C60.

The sequential absorption of multiple infrared (IR) photons by isolated gas-phase species can lead to their dissociation and/or ionization. Using the newly constructed "Free-Electron Laser for IntraCavity Experiments" (FELICE) beam line at the FELIX facility, neutral C(60) molecules have been exposed to an extremely high number (approximately 10(23)) of photons/cm(2) for a total time duration of up to 5 micros. At wavelengths around 20 microm, resonant with allowed IR transitions of C(60), ionization and extensive fragmentation of the fullerenes are observed.

Structures of neutral Au7, Au19, and Au20 clusters in the gas phase.

The catalytic properties of gold nanoparticles are determined by their electronic and geometric structures. We revealed the geometries of several small neutral gold clusters in the gas phase by using vibrational spectroscopy between 47 and 220 wavenumbers. A two-dimensional structure for neutral Au7 and a pyramidal structure for neutral Au20 can be unambiguously assigned.

Two-color facility based on a broadly tunable infrared free-electron laser and a subpicosecond-synchronized 10-fs-Ti:sapphire laser.

Subpicosecond synchronization between a mirror-dispersion-controlled 10-fs Ti:sapphire laser and the Free-Electron Laser for Infrared Experiments has been achieved. The measured intensity cross correlation between the two lasers is consistent with a jitter of only 400 fs rms. The wide and continuous tunability of the free-electron laser (FEL; 4.

Mid-infrared (2.75-6.0-microm) second-harmonic generation in LiInS(2).

Phase-matched second-harmonic generation is obtained in various LiInS(2) crystals by use of the tunable picosecond output of the free-electron laser for infrared experiments (FELIX) as the pump source in the mid-IR range from 2.75 to 6.0 microm.

Benchmarking of electro-optic monitors for femtosecond electron bunches.

The longitudinal profiles of ultrashort relativistic electron bunches at the soft x-ray free-electron laser FLASH have been investigated using two single-shot detection schemes: an electro-optic (EO) detector measuring the Coulomb field of the bunch and a radio-frequency structure transforming the charge distribution into a transverse streak. A comparison permits an absolute calibration of the EO technique. EO signals as short as 60 fs (rms) have been observed, which is a new record in the EO detection of single electron bunches and close to the limit given by the EO material properties.

Spin relaxation by transient monopolar and bipolar optical orientation.

We have used two-color time-resolved spectroscopy to measure the relaxation of electron spin polarizations in a bulk semiconductor. The circularly polarized pump beam induces a polarization either by direct excitation from the valence band, or by free-carrier (Drude) absorption when tuned to an energy below the band gap. We find that the spin relaxation time, measured with picosecond time resolution by resonant induced Faraday rotation in both cases, increases in the presence of photogenerated holes.

Electro-optic technique with improved time resolution for real-time, nondestructive, single-shot measurements of femtosecond electron bunch profiles.

Electro-optic detection of the Coulomb field of a relativistic electron bunch combined with single-shot cross correlation of optical pulses is used to enable single-shot measurements of the shape and length of femtosecond electron bunches. This method overcomes a fundamental time-resolution limit of previous single-shot electro-optic measurements, which arises from the inseparability of time and frequency properties of the probing optical pulse. Using this new technique we have made real-time measurements of a 50 MeV electron bunch, observing the profile of 650 fs FWHM ( approximately 275 fs rms) long bunches.

Single-shot electron-beam bunch length measurements.

We report subpicosecond electro-optic measurements of the length of individual relativistic electron bunches. The longitudinal electron-bunch shape is encoded electro-optically on to the spectrum of a chirped laser pulse. The electron-bunch length is determined by analyzing individual laser-pulse spectra obtained with and without the presence of an electron bunch.

Excited-state lifetimes of far-infrared collective modes in proteins.

Vibrational excitations of low frequency collective modes are essential for functionally important conformational transitions in proteins. Here we report the first direct measurement on the lifetime of vibrational excitations of the collective modes at 87 microm (115 cm(-1)) in bacteriorhodopsin, a transmembrane protein. The data show that these modes have extremely long lifetime of vibrational excitations, over 500 ps, accommodating 1500 vibrations.