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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. We show milliradian control over the wavefunction phase for the two-level system formed by the 1s and 2p states. The results have been verified by all-optical echo detection methods, sensitive only to coherent excitations in the sample. The experiments open a route to exploitation of donors in silicon for atom trap physics, with concomitant potential for quantum computing schemes, which rely on orbital superpositions to, for example, gate the magnetic exchange interactions between impurities.

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. Two types of structures have been considered: a carbene structure where an intact CH2 fragment is bound to the metal (M(+)-CH2) and a carbyne (hydrido-methylidyne) structure with both a CH and a hydrogen bound to the metal separately (H-M(+)-CH). For metal ions with empty d-orbitals, an agostic interaction can occur that could influence the competition between carbene and carbyne structures. In this work, the gas phase [M,C,2H](+) (M = Ta, W, Ir, Pt) products are investigated by infrared multiple-photon dissociation (IR-MPD) spectroscopy using the Free-Electron Laser for IntraCavity Experiments (FELICE). Metal cations are formed in a laser ablation source and react with methane pulsed into a reaction channel downstream. IR-MPD spectra of the [M,C,2H](+) species are measured in the 300-3500 cm(-1) spectral range by monitoring the loss of H (2H in the case of [Ir,C,2H](+)). For each system, the experimental spectrum closely resembles the calculated spectrum of the lowest energy structure calculated using DFT: for Pt, a classic C(2v) carbene structure; for Ta and W, carbene structures that are distorted by agostic interactions; and a carbyne structure for the Ir complex. The Ir carbyne structure was not considered previously. To obtain this agreement, the calculated harmonic frequencies are scaled with a scaling factor of 0.939, which is fairly low and can be attributed to the strong redshift induced by the IR multiple-photon excitation process of these small molecules. These four-atomic species are among the smallest systems studied by IR-FEL based IR-MPD spectroscopy, and their spectra demonstrate the power of IR spectroscopy in resolving long-standing chemical questions.

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. Time-resolved electron kinetic energy distributions measured give information on the decay rate of the selected fullerene. This method is generally applicable to all neutral species that exhibit thermionic emission and provides a unique tool to study the stability of mass-selected neutral clusters and molecules that are only available as part of a size distribution.

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., Methods: A total of 1123 patient records of neonates who were administered vancomycin were used for population PK modeling by iterative 2-stage Bayesian (ITSB) analysis. Cut-off values for weighted residuals were tested for exclusion of records from the analysis. A simulation study was performed to assess the influence of erroneous records on population modeling and individual MAPB estimation. Also the cut-off values for weighted residuals were tested in the simulation study., Results: Errors in registration have limited the influence on outcomes of population PK modeling but can have detrimental effects on individual MAPB estimation. A population PK model created from a data set with many registration errors has little influence on subsequent MAPB estimates for precisely recorded data. A weighted residual value of 2 for concentration measurements has good discriminative power for identification of erroneous records., Conclusions: ITSB analysis and its individual estimates are hardly affected by most registration errors. Large registration errors can be detected by weighted residuals of concentration.

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.

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. In addition, Dutch law states that patients should be clearly informed about any medical procedure that is to be performed, including the possible risks and alternatives. All of the above is not possible with a paper-based assessment. A complete assessment may reduce health care costs by reducing the number of consultations by other specialists, additional tests, cancellations and length of stay. The assessment also reduces patient anxiety and improves patient satisfaction. In conclusion, a complete preoperative assessment is required by guidelines and law and does offer many advantages.

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. Methods of development for optimal sampling strategies (OSS) are diverse and heterogeneous. This review provides a comprehensive overview of OSS development methodology using MAPB pharmacokinetic parameter estimation, determines the transferability of published OSSs, and compares sampling strategies determined by MAPB estimation and multiple regression analysis. OSS development has the following components: 1) prior distributions; 2) reference value determination; 3) optimal sampling time identification; and 4) validation of the OSS. Published OSSs often lack all data necessary for the OSS to be clinically transferable. MAPB estimation is similar to multiple regression analysis in terms of predictive performance but superior in flexibility.

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.

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. For eventual application of such states, a solid-state implementation is very desirable. Here we demonstrate the coherent control of impurity wavefunctions in the most ubiquitous donor in a semiconductor, namely phosphorus-doped silicon. In our experiments, we use a free-electron laser to stimulate and observe photon echoes, the orbital analogue of the Hahn spin echo, and Rabi oscillations familiar from magnetic resonance spectroscopy. As well as extending atomic physicists' explorations of quantum phenomena to the solid state, our work adds coherent terahertz radiation, as a particularly precise regulator of orbitals in solids, to the list of controls, such as pressure and chemical composition, already familiar to materials scientists.

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. The resulting photofragment distributions are attributed to absorption in fragmentation products formed once C(60) is excited to internal energies at which fragmentation or ionization takes place within the duration of the laser pulse. The high IR intensities available combined with the large interaction volume permit spatially resolved detection of the ions inside the laser beam, thereby disentangling the contributions from different IR intensities. The use of spatial imaging reveals intensity dependent mass distributions that are substantially narrower than what has been observed previously, indicating rather narrow energy distributions. A simple rate-equation modeling of the excitation process supports the experimental observations.

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. The reduction of the symmetry when a corner atom is cut from the tetrahedral Au20 cluster is directly reflected in the vibrational spectrum of Au19.

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.

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. In the case of the material chosen, n-InSb, the increase was from 14 to 38 ps.

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.

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. Since the length of the chirped laser pulse can be easily changed, the electron bunch can be visualized on different time scales. This single-shot imaging technique is a promising method for real-time electron-bunch diagnostics.

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. We suggest that there is a connection between this relatively slow anharmonic relaxation rate of approximately 10(9) sec(-1) and the similar observed rate of conformational transitions in proteins, which require multilevel vibrational excitations.

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. Deviations from the phase-matching curve calculated from Boyd's refractive-index data are observed. Furthermore, the optical damage threshold of the crystals has been measured to be 1.1. J/cm(2)(>6 GW/cm(2)) at the 5-microm wavelength. LiInS(2) holds great promise for parametric interaction in the 1-13-microm range.

Time-resolved measurements of the transverse electric field associated with relativistic electron bunches are presented. Using an ultrafast electro-optic sensor close to the electron beam, the longitudinal profile of the electric field was measured with subpicosecond time resolution and without time-reversal ambiguity. Results are shown for two cases: inside the vacuum beam line in the presence of wake fields, and in air behind a beryllium window, effectively probing the near-field transition radiation. Especially in the latter case, reconstruction of the longitudinal electron bunch shape is straightforward.

The detailed shape of picosecond optical pulses from a free-electron laser (FEL) oscillator has been studied for various cavity detunings. For large values of the cavity detuning the optical pulse develops an exponential leading edge, with a time constant proportional to the applied cavity detuning and the quality factor of the resonator. This behavior has been observed at two separate FELs that have completely different resonator layouts and electron beam characteristics, and using different methods of optical pulse length measurement. The optical pulses have a full width at half maximum time-bandwidth product Deltat(FWHM)Deltaf(FWHM) of 0.2-0.3. The results presented here can be used to predict the optical pulse length and corresponding minimum spectral width that can be generated in a FEL pumped by short electron bunches. This is important for the design of new infrared free-electron laser user facilities, which need to make a balanced choice between short pulses for high temporal resolution and narrow bandwidth for linear and nonlinear spectroscopy.

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; 4.2-300mum) combined with ultrashort pulse duration of six optical cycles and high pulse energy of several tens of microjoules makes a series of two-color experiments possible in a previously inaccessible wavelength range. We demonstrate these capabilities by performing a two-color pump-probe experiment to study carrier cooling in GaAs. A FEL tuned from 8 to 17mum is used as the pump, and a synchronized Ti:sapphire laser pulse serves as the probe.

We report measurements of the toroidal plasma current in the high-beta tokamak SPICA II using a magnetooptic current sensor. Both the sine and cosine components of the angle of rotation are recorded during the current pulse. In this way, the overall accuracy is increased and a computer algorithm can be employed to calculate the value of the current. The effect of linear birefringence is taken into account. The system has a resolution of 1 kA, and a frequency range of DC to 1 MHz. The measured values of the plasma current (up to 350 kA) are in good agreement with the results of a Rogowski coil.