Collisional quenching of metastable states of antiprotonic helium by hydrogen and deuterium molecules

The quenching of metastable states of antiprotonic helium by collisions with hydrogen and deuterium molecules was studied. A systematic investigation of the delayed annihilation time spectra at various H₂ and D₂ admixture ratios at the ppm level revealed characteristic changes of their shape, which indicated a strong principal and orbital quantum number dependent quenching of levels in both cases. Applying a laser spectroscopy technique to measure the lifetimes of individual states and cascades we deduced H₂ and D₂ quenching cross-sections for the states (n, l )= (39, 35) and (37, 34). These cross-sections establish for D₂ molecules the strong increase of the quenching efficiency with increasing principal quantum number n of the state under investigation previously reported for the case of H₂ admixtures. Our experiments indicate that the low-n state (37, 34) is somewhat less affected by D₂ than by H₂, while the high-n state (39, 35) is equally quenched by both isotopes. Received 2 October 2000     

Dichromatic squeezing generation

We propose a novel scheme for the joint generation of two squeezed beams at arbitrary frequencies ω ₁ and ω ₂. The scheme consists of two successive steps, both involving nonlinear interactions in χ⁽²⁾ crystals. The dynamics of the setup is analyzed both quantum mechanically and classically within the parametric approximation. An experimental implementation involving the fundamental and the harmonics of a Nd:YAG laser pulse, and β-BaB ₂ O ₄ nonlinear crystals is suggested. Received 17 May 2000 and Received in final form 9 October 2000     

Surface and flexoelectric polarization in a nematic liquid crystal 5CB

The temperature dependence of the surface polarization has been measured for both the planar and homeotropic orientation of a nematic liquid crystal at a solid substrate. A conventional liquid crystal 5CB, pure and doped with an azo-dye, was used in cells with controlled asymmetry for light absorption. The measurements have been made by a pyroelectric technique using short pulses of a YAG laser to create a temperature increment. The latter, in turn, was measured independently by a novel time-resolved “optical thermometer” technique monitoring temperature-dependent birefringence by a He- Ne laser beam. In accordance with the symmetry of the order parameter, the surface polarization has different sign for the two orientations, its magnitude ranges from -4 to +2pC/m. The same technique has been used for the measurement of the flexoelectric polarization in hybrid cells. The sum of the flexoelectric coefficients is e ₁ + e ₃ = - 13pC/m at 25°C. Received 28 February 2000 and Received in final form 5 September 2000     

Control of wavepacket dynamics in mixed alkali metal clusters by optimally shaped fs pulses

We have performed adaptive feedback optimization of phase-shaped femtosecond laser pulses to control the wavepacket dynamics of small mixed alkali-metal clusters. An optimization algorithm based on Evolutionary Strategies was used to maximize the ion intensities. The optimized pulses for NaK and Na₂K converged to pulse trains consisting of numerous peaks. The timing of the elements of the pulse trains corresponds to integer and half integer numbers of the vibrational periods of the molecules, reflecting the wavepacket dynamics in their excited states. Received 4 December 2001     

Solvation and chemical reaction of sodium in water clusters

Na_m(H₂O)_n Clusters ( n = 1...200, m = 1...50) are formed in a recently build pick-up arrangement. Preformed water clusters traverse a sodium oven, where sodium atoms are picked up. At low sodium vapour pressure ( < 1×10^-4 mbar) pure Na(H₂O)_n clusters are observed in the mass spectra. At high sodium vapour pressure ( > 1×10^-3 mbar) the water cluster pick up more than 50 Na atoms and reaction products Na(NaOH)_n ( n = 2, 4...50) dominate the mass spectra. The even number of NaOH units in the products indicate that also in a finite cluster the reaction occurs in pairs as in the macroscopic reaction. Received 4 December 2000     

Determination of the helium-4 mass in a Penning trap

The determination of the rotational quadrupole alignment of diatomic molecules via REMPI detection is investigated. In this process a high focal intensity usually increases the detection probability. At high intensities the AC Stark effect may cause a splitting of the normally degenerate m_J sublevels of a rotational state J beyond the spectral width of the exciting radiation. This leads to a selective detection of only certain m_J states with the consequence that deduced alignment factors can be misleading. From the theoretical considerations line profiles are explicitly calculated for dynamic polarizabilities which represent the B ¹Σ⁺ _u←X ¹Σ⁺ _g transition of H₂, in order to fit an experimental (3+1) REMPI spectrum and to predict (1+1') line shapes as a function of laser intensity. It is further shown that the deduced quadrupole alignment factor A ₀ ⁽²⁾ is significantly changed by the second order AC Stark effect when the intensities are chosen high enough to observe asymmetric broadened line profiles. Different combinations of relative linear polarizations of the exciting and ionizing laser beams are discussed. Received 1st August 2000 and Received in final form 2 May 2001     

General theory of population transfer by adiabatic rapid passage with intense, chirped laser pulses

We present a general theory of adiabatic rapid passage (ARP) with intense, linearly chirped laser pulses. For pulses with a Gaussian profile and a fixed bandwidth, we derive a rigorous formula for the maximum temporal chirp rate that can be sustained by the pulse. A modified Landau-Zener formula displays clearly the relationships among the pulse parameters. This formula is used to derive the optimal conditions for efficient, robust population transfer. As illustrations of the theory, we present results for two- and four-level systems, and selective vibronic excitation in the I₂ molecule. We demonstrate that population transfer with chirped pulses is more robust and more selective than population transfer with transform-limited pulses. Received 6 September 2000 and Received in final form 25 September 2000     

Fragmentation of water clusters: Molecular-dynamics simulation study

The fragmentation of water clusters, [(H ₂ O)_n;n = 2-8], have been investigated by using molecular-dynamics simulation method. In the simulations a polarizable-dissociable potential energy function for water has been used. Particular attention has bee paid to investigate the effect of structural properties and cluster size on the fragmentation. Received 27 April 2000 and Received in final form 6 October 2000     

Self- and foreign-broadening and shift coefficients for C2H2 lines at 1.54 μm

In this article we present experimental data for line parameters measurements of several transition lines of overtone bands of C₂H₂ at 1540 nm. The measurements were done with a spectrometer based on a semiconductor diode laser and a direct absorption spectroscopy scheme. Broadening and shift coefficients have been measured for the pure gas or in mixtures with N₂, O₂ and CO₂ as perturbing gas. Received 6 November 2000 and Received in final form 13 March 2001     

High-order harmonic generation from organic molecules in ultra-short pulses

We have studied high-order harmonic generation (HHG) from organic molecules irradiated with near-infrared high intensity laser pulses of 70 fs and 240 fs duration. The molecular systems studied were the aromatics benzene and naphthalene and the alkanes cyclopropane and cyclohexane (cyclic) and n-hexane (linear). Harmonic intensities were measured both as a function of laser intensity (in the range 5×10¹³-5×10¹⁵ W cm^-2) and as a function of ellipticity of the laser field polarisation. The results were compared with those from the xenon atom. For 70 fs pulses, harmonic generation from the organic systems was similar to that of xenon, revealing an atom-like behaviour for molecules when the laser pulse duration is shorter than the fragmentation timescale of the molecule. We note significant differences between molecules with respect to HHG efficiencies and the suppression of HHG in larger species. We discuss these differences in the context of the molecular properties, electronic structure and behaviour of ionisation and fragmentation that result in enhancement of field ionisation in larger systems. Study of the polarisation ellipticity dependence of HHG shows that the harmonic yield in molecules is less sensitive to the polarisation than for atoms (xenon). This is consistent with the expected behaviour given the larger recollision cross-section presented by the core in the molecular system compared to the atom. Our results suggest that study of HHG from molecules exposed to ultra-short pulses is potentially a powerful tool for understanding the electron dynamics of molecules exposed to an intense field. Received 14 September 2000 and Received in final form 6 December 2000     

Optical and electrical properties of hydrogenated yttrium nanoparticles

We studied the effect of hydrogen in yttrium nanoparticles on a quartz substrate, using optical spectroscopy and electrical resistance measurements. Pulsed laser deposition is used to obtain the Y clusters in an UHV environment. We show, that these clusters are highly sensitive to monoatomic H₁ produced from ambient hydrogen gas pressures, ranging from 10^-5 to 50 mbar with our experimental arrangement. The changes of optical and electrical properties due to the chemical reaction within the particles are sufficient to consider this material as a possible sensor for low concentrations of hydrogen. Received 29 November 2000     

Coupling and dissociation in artificial molecules

We show that the spin-and-space unrestricted Hartree-Fock method, in conjunction with the companion step of the restoration of spin and space symmetries via Projection Techniques (when such symmetries are broken), is able to describe the full range of couplings in two-dimensional double quantum dots, from the strong-coupling regime exhibiting delocalized molecular orbitals to the weak-coupling and dissociation regimes associated with a Generalized Valence Bond combination of atomic-type orbitals localized on the individual dots. The weak-coupling regime is always accompanied by an antiferromagnetic ordering of the spins of the individual dots. The cases of dihydrogen (H₂, 2e) and dilithium (Li₂, 6e) quantum dot molecules are discussed in detail. Received 19 December 2000     

Systematic field-theory for the hard-core one-component plasma

A continuous liquid flow in a vacuum (a liquid beam) of an aqueous solution of adenine salt containing hydrochloric acid or sodium hydroxide was irradiated with an intense pulsed IR laser at 3 μm, which is resonant to a vibrational mode related to the OH stretch vibration of H₂O. Neutral species isolated into the vacuum were ionized by a pulsed UV laser at 270 nm, and the product ions were mass-analyzed by a time-of-flight mass spectrometer. It is found that AH ₂ ^{2 + .} 2Cl^- and [A-iH] ^{i - .} iNa⁺ (i = 1-3) are isolated in the vacuum from the aqueous acidic and alkaline solutions, respectively, under irradiation of the IR laser, and undergo four-photon ionization involving decomposition and proton transfer of the intermediate species under irradiation of the UV laser. Received 1st May 2002 Published online 13 September 2002     

High energy collisions of protonated water clusters

We have measured attenuation cross sections and fragmentation cross sections for protonated water clusters H(H₂O)_n ⁺ (n = 1 to 100) colliding with noble gas atoms (He and Xe) at a laboratory energy of 50 keV. In collisions with He, a transparency effect in the attenuation cross section was observed. For the case of fragmentation in collisions with Xe, a strong enhancement of small clusters was observed which we attribute to multifragmentation. Received 30 November 2000     

Alternating magneto-birefringence of ionic ferrofluids in crossed fields

A dynamic probing of magnetic liquids is performed experimentally, using a static magnetic field modulated by another smaller field, normal and alternating. The optical magneto-birefringence under these crossed magnetic fields is recorded as a function of the frequency for different field intensities and different sizes of the magnetic nanoparticles. A general reduced behavior is found for the in-phase and the out-of-phase optical response which is well-described by a simple mechanical model. Depending on the value H _ani of the anisotropy field of the nanoparticles, we can distinguish two different high magnetic field regimes: - a rigid dipole regime (large anisotropy energy with respect to k _B T) for cobalt ferrite nanoparticles with a relaxation time inversely proportional to the field intensity H _C(H _C < H _ani), - a soft dipole regime (anisotropy energy of the order of k _B T) for maghemite nanoparticles with a relaxation time independent of the field intensity H _C(H _C > H _ani). Received 5 June 2000 and Received in final form 8 January 2001     

Hydrogen atom transfer in indole clusters: formation dynamics of , n = 1-6, fragments

The H atom transfer reaction in electronically excited indole(NH ₃ ) _n clusters is studied in pump-probe experiments with femtosecond laser pulses. By applying different probe photon energies we are able to detect the dissociation products (NH ₃ ) _{n - 1} NH ₄ for n = 1-6. Furthermore we show that the analysis of the corresponding ion signals is not distorted by contributions from larger cluster ions due to evaporation of NH ₃ molecules. The formation times of the products are ca. 140ps for n = 2-4 and about 80ps for n = 5, 6. Received 30 April 2002 / Received in final form 29 May 2002 Published online 13 September 2002     

Second harmonic generation in Ga nanoparticle monolayers

Ga nanoparticle monolayers formed by evaporation-condensation in ultrahigh vacuum and embedded in a transparent SiO_x matrix generate second harmonic (SH) signals in transmission and reflection when illuminated by a 150 fs, 800 nm laser pulses. The observed SH light exhibits a critical dependence on input and output polarizations, angle of incidence and azimuthal orientation of the samples. The results lead to a consistent picture of shape and orientation of the nanoparticles. Linear transmittance spectra in the visible range support these findings and the observed size dependence of the SH signal. Received 29 November 2000     

Magnetoquantum de Haas-van Alphen oscillations in spin-split two-dimensional Fermi liquid

Theory of magnetoquantum oscillations with spin-split structure in strongly anisotropic (two-dimensional (2D)) metal is developed in the formalism of level approach. Parametric method for exact calculation of oscillations wave forms and amplitudes, developed earlier for spin degenerate levels is generalized on a 2D electron system with spin-split levels. General results are proved: 1) proportionality relation between magnetization and chemical potential oscillations accounting for spin-split energy levels and magnetic field unperturbed levels (states of reservoir), 2) basic equation for chemical potential oscillations invariant to various models of 2D and 1D energy bands (intersecting or overlapping) and localized states. Equilibrium transfer of carriers between overlapping 2D and 1D bands, characterizing the band structure of organic quasi 2D metals, is considered. Transfer parameter, calculated in this model to be of the order of unity, confirms the fact that the wave form of oscillations in organic metals should be quasisymmetric up to ultralow temperature. Presented theory accounts for spin-split magnetization oscillations at magnetic field directions tilted relative to the anisotropic axis of a metal. Theoretical results are compared with available experimental data on organic quasi-2D metal α-(BEDT-TTF)₂KHg(SNC)₄ explaining the appearance of clear split structure under the kink magnetic field and absence above by the corresponding change in the electron g-factor rather than cyclotron mass. Received 20 December 2000 and Received in final form 13 July 2001     

Influence of laser pulse width on absolute EUV-yield from Xe-clusters

Using 50 fs ( ∼ 2×10¹⁸ W/cm²) and 2 ps ( ∼ 5×10¹⁶ W/cm²) pulses from a Ti:Sa multi-TW laser at 800 nm wavelength large Xe-clusters ( 10⁵...10⁶ atoms per cluster) have been excited. Absolute yield measurements of EUV-emission in a wavelength range between 10 nm and 15 nm in combination with cluster target variation were carried out. The ps-laser pulse has resulted in about 30% enhanced and spatially more uniform EUV-emission compared to fs-laser excitation. Circularly polarized laser light instead of linear polarization results in enhanced emission which is probably caused by electrons gaining higher energies by the polarization dependent optical field ionization process. An absolute emission efficiency at 13.4 nm of up to 0.8% in 2π sr and 2.2% bandwidth has been obtained. Received 11 January 2001 and Received in final form 27 March 2001     

Ultrafast multidimensional dynamics of strong hydrogen bonds

The laser driven dynamics of the OH(D) stretching vibration in phthalic acid monomethylester is investigated. The combination of a 55-dimensional all-Cartesian reaction surface Hamiltonian and the time-dependent self-consistent field approach is shown to provide a microscopic picture of intramolecular vibrational energy redistribution taking place upon interaction with an external laser field. Choosing suitable zeroth-order vibrational states and combinations thereof a quasi-periodic in-phase and out-of-phase oscillatory behavior is observed manifesting energy flow on different time scales. The fingerprints of this behavior in transient absorption spectroscopy are also discussed. Received 24 August 2000 and Received in final form 11 October 2000