A. F. G. van der Meer

The Free-Electron-Laser user facility FELIX

Abstract The Free Electron Laser for Infrared eXperiments FELIX presents to its users a versatile source of radiation in the infrared and far-infrared spectral regions. Presently, the wavelength range of operation extends from 5 to 110 μm (2000−90 cm−1). The wavelength is continuously tunable over an octave in a few minutes. The output normally consists of macropulses of 5–10 μs duration, formed by a train of micropulses of a few ps length. Average power in the macropulses is of order 10 kW, peak power in the micropulses is in the MW range. The temporal and spectral characteristics of the micropulses can be controlled by varying the synchronism between the electron pulses and the optical pulses circulating in the laser cavity. Transform-limited pulse lengths in the range 2–20 ps can be generated. Long-range coherence has been induced by phase-locking successive micropulses, and narrow-band, essentially single-mode, radiation has been selected from the output.

Free electron laser-Fourier transform ion cyclotron resonance mass spectrometry facility for obtaining infrared multiphoton dissociation spectra of gaseous ions

A Fourier transform ion cyclotron resonance (FT-ICR) mass spectrometer has been installed at a free electron laser (FEL) facility to obtain infrared absorption spectra of gas phase ions by infrared multiple photon dissociation (IRMPD). The FEL provides continuously tunable infrared radiation over a broad range of the infrared spectrum, and the FT-ICR mass spectrometer, utilizing a 4.7Tesla superconducting magnet, permits facile formation, isolation, trapping, and high-mass resolution detection of a wide range of ion classes. A description of the instrumentation and experimental parameters for these experiments is presented along with preliminary IRMPD spectra of the singly-charged chromium-bound dimer of diethyl ether (Cr(C4H10O)2+) and the fluorene molecular ion (C13H10+). Also presented is a brief comparison of the fluorene cation spectrum obtained by the FT-ICR-FEL with an earlier spectrum recorded using a quadrupole ion trap (QIT).

Time-Resolved Holography with Photoelectrons

The intefererence pattern produced by photoelectrons provides holographic snapshots of the photoionization process. 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.

Free electron laser based biophysical and biomedical instrumentation

A survey of biophysical and biomedical applications of free-electron lasers(FELs) is presented. FELs are pulsed light sources, collectively operating from the microwave through the x-ray range. This accelerator-based technology spans gaps in wavelength, pulse structure, and optical power left by conventional sources.FELs are continuously tunable and can produce high-average and high-peak power. Collectively, FEL pulses range from quasicontinuous to subpicosecond, in some cases with complex superpulse structures. Any given FEL, however, has a more restricted set of operational parameters. FELs with high-peak and high-average power are enabling biophysical and biomedical investigations of infrared tissue ablation. A midinfrared FEL has been upgraded to meet the standards of a medical laser and is serving as a surgical tool in ophthalmology and human neurosurgery. The ultrashort pulses produced by infrared or ultraviolet FELs are useful for biophysical investigations, both one-color time-resolved spectroscopy and when coupled with other light sources, for two-color time-resolved spectroscopy.FELs are being used to drive soft ionization processes in mass spectrometry. Certain FELs have high repetition rates that are beneficial for some biophysical and biomedical applications, but confound research for other applications. Infrared FELs have been used as sources for inverse Compton scattering to produce a pulsed, tunable, monochromatic x-raysource for medical imaging and structural biology. FEL research and FEL applications research have allowed the specification of spin-off technologies. On the horizon is the next generation of FELs, which is aimed at producing ultrashort, tunable x rays by self-amplified spontaneous emission with potential applications in biology.

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. 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.

Rapamycin and MPA, but not CsA, impair human NK cell cytotoxicity due to differential effects on NK cell phenotype.

Cyclosporin A (CsA), rapamycin (Rapa) and mycophenolic acid (MPA) are frequently used for GVHD prophylaxis and treatment after allogeneic stem cell transplantation (SCT). As NK cells have received great interest for immunotherapeutic applications in SCT, we analyzed the effects of these drugs on human cytokine‐stimulated NK cells in vitro. Growth‐kinetics of CsA‐treated cultures were marginally affected, whereas MPA and Rapa severely prevented the outgrowth of CD56bright NK cells. Single‐cell analysis of NK cell receptors using 10‐color flow cytometry, revealed that CsA‐treated NK cells gained a similar expression profile as cytokine‐stimulated control NK cells, mostly representing NKG2A+KIR−NCR+ cells. In contrast, MPA and Rapa inhibited the acquisition of NKG2A and NCR expression and NK cells maintained an overall NKG2A−KIR+NCR+/− phenotype. This was reflected in the cytolytic activity, as MPA‐ and Rapa‐treated NK cells, in contrast to CsA‐treated NK cells, lost their cytotoxicity against K562 target cells. Upon target encounter, IFN‐γ production was not only impaired by MPA and Rapa, but also by CsA. Overall, these results demonstrate that CsA, MPA and Rapa each have distinct effects on NK cell phenotype and function, which may have important implications for NK cell function in vivo after transplantation.

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. 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.

Silicon as a model ion trap: Time domain measurements of donor Rydberg states

One of the great successes of quantum physics is the description of the long-lived Rydberg states of atoms and ions. The Bohr model is equally applicable to donor impurity atoms in semiconductor physics, where the conduction band corresponds to the vacuum, and the loosely bound electron orbiting a singly charged core has a hydrogen-like spectrum according to the usual Bohr–Sommerfeld formula, shifted to the far-infrared because of the small effective mass and high dielectric constant. Manipulation of Rydberg states in free atoms and ions by single and multiphoton processes has been tremendously productive since the development of pulsed visible laser spectroscopy. The analogous manipulations have not been conducted for donor impurities in silicon. Here, we use the FELIX pulsed free electron laser to perform time-domain measurements of the Rydberg state dynamics in phosphorus- and arsenic-doped silicon and we have obtained lifetimes consistent with frequency domain linewidths for isotopically purified silicon. This implies that the dominant decoherence mechanism for excited Rydberg states is lifetime broadening, just as for atoms in ion traps. The experiments are important because they represent a step toward coherent control and manipulation of atomic-like quantum levels in the most common semiconductor and complement magnetic resonance experiments in the literature, which show extraordinarily long spin lattice relaxation times—key to many well known schemes for quantum computing qubits—for the same impurities. Our results, taken together with the magnetic resonance data and progress in precise placement of single impurities, suggest that doped silicon, the basis for modern microelectronics, is also a model ion trap.

Quantum ratchet effects induced by terahertz radiation in GaN-based two-dimensional structures

Photogalvanic effects are observed and investigated in wurtzite (0001)-oriented GaN/AlGaN low-dimensional structures excited by terahertz radiation. The structures are shown to represent linear quantum ratchets. Experimental and theoretical analysis exhibits that the observed photocurrents are related to the lack of an inversion center in the GaN-based heterojunctions.

Vibrational ladder climbing in NO by ultrashort infrared laser pulses

Abstract The anharmonic vibrational ladder of nitric oxide (NO) is climbed by irradiating the molecule with femtosecond infrared (IR) pulses. The free-electron laser FELIX is tuned to λ = 5.3 μm with a bandwidth of Δλ = 0.3 μm, corresponding to a pulse duration of 150 femtoseconds. Transfer to the excited states of NO is monitored by 1 + 1 REMPI. Population is found up to ν″ = 5, the highest level within reach of the IR bandwidth. The average transfer per step of the ladder is found to be 17%.