296 research outputs found
Mixing Effects in the Crystallization of Supercooled Quantum Binary Liquids
By means of Raman spectroscopy of liquid microjets we have investigated the
crystallization process of supercooled quantum liquid mixtures composed of
parahydrogen (pH) diluted with small amounts of up to 5\% of either neon or
orthodeuterium (oD), and of oD diluted with either Ne or pH. We
show that the introduction of Ne impurities affects the crystallization
kinetics in both the pH-Ne and oD-Ne mixtures in terms of a significant
reduction of the crystal growth rate, similarly to what found in our previous
work on supercooled pH-oD liquid mixtures [M. K\"uhnel et {\it al.},
Phys. Rev. B \textbf{89}, 180506(R) (2014)]. Our experimental results, in
combination with path-integral simulations of the supercooled liquid mixtures,
suggest in particular a correlation between the measured growth rates and the
ratio of the effective particle sizes originating from quantum delocalization
effects. We further show that the crystalline structure of the mixture is also
affected to a large extent by the presence of the Ne impurities, which likely
initiate the freezing process through the formation of Ne crystallites.Comment: 19 pages, 7 figures, submitted to J. Chem. Phy
Observation of crystallization slowdown in supercooled para-hydrogen and ortho-deuterium quantum liquid mixtures
We report a quantitative experimental study of the crystallization kinetics
of supercooled quantum liquid mixtures of para-hydrogen (pH) and
ortho-deuterium (oD) by high spatial resolution Raman spectroscopy of
liquid microjets. We show that in a wide range of compositions the
crystallization rate of the isotopic mixtures is significantly reduced with
respect to that of the pure substances. To clarify this behavior we have
performed path-integral simulations of the non-equilibrium pH-oD liquid
mixtures, revealing that differences in quantum delocalization between the two
isotopic species translate into different effective particle sizes. Our results
provide first experimental evidence for crystallization slowdown of quantum
origin, offering a benchmark for theoretical studies of quantum behavior in
supercooled liquids.Comment: 6 pages, 3 figure
Layer- and bulk roton excitations of 4He in porous media
We examine the energetics of bulk and layer-roton excitations of 4He in
various porous medial such as aerogel, Geltech, or Vycor, in order to find out
what conclusions can be drawn from experiments on the energetics about the
physisorption mechanism. The energy of the layer-roton minimum depends
sensitively on the substrate strength, thus providing a mechanism for a direct
measurement of this quantity. On the other hand, bulk-like roton excitations
are largely independent of the interaction between the medium and the helium
atoms, but the dependence of their energy on the degree of filling reflects the
internal structure of the matrix and can reveal features of 4He at negative
pressures. While bulk-like rotons are very similar to their true bulk
counterparts, the layer modes are not in close relation to two-dimensional
rotons and should be regarded as a third, completely independent kind of
excitation
Crystallographic and NMR Investigation of Ergometrine and Methylergometrine, Two Alkaloids from Claviceps purpurea
Ergometrine and methylergometrine are two alkaloids that are used as maleate salts for the prevention and control of postpartum hemorrhage. Although the two molecules have been known for a long time, few and discordant crystallographic and NMR spectroscopic data are available in the literature. With the aim of providing more conclusive data, we performed a careful NMR study for the complete assignment of the 1H, 13C, and 15N NMR signals of ergometrine, methylergometrine, and their maleate salts. This information allowed for a better definition of their conformational equilibria. In addition, the stereochemistry and the intermolecular interactions in the solid state of the two maleate salts were deeply investigated by means of single-crystal X-ray diffraction, showing the capability of these derivatives to act as both hydrogen-bond donors and acceptors, and evidencing a correlation between the number of intermolecular interactions and their different solubility
Experimental verification of the Heisenberg uncertainty principle for hot fullerene molecules
The Heisenberg uncertainty principle for material objects is an essential
corner stone of quantum mechanics and clearly visualizes the wave nature of
matter. Here we report a demonstration of the Heisenberg uncertainty principle
for the most massive, complex and hottest single object so far, the fullerene
molecule C70 at a temperature of 900 K. We find a good quantitative agreement
with the theoretical expectation: dx * dp = h, where dx is the width of the
restricting slit, dp is the momentum transfer required to deflect the fullerene
to the first interference minimum and h is Planck's quantum of action.Comment: 4 pages, 4 figure
(S)-Pramipexole and Its Enantiomer, Dexpramipexole : a New Chemoenzymatic Synthesis and Crystallographic Investigation of Key Enantiomeric Intermediates
A new chemoenzymatic method has been developed for the synthesis of (S)- and (R)-N-(6-hydroxy-4,5,6,7-tetrahydrobenzo[d]thiazol-2-yl) acetamide, two key synthons for the preparation of (S)-pramipexole, an anti-Parkinson drug, and its enantiomer dexpramipexole, which is currently under investigation for the treatment of eosinophil-associated disorders. These two building blocks have been obtained in good yields and high enantiomeric excess (30% and >98% ee for the R-enantiomer, and 31% and >99% ee for the S- one) through a careful optimization of the reaction conditions, starting from the corresponding racemic mixture and using two consecutive irreversible transesterifications, catalyzed by Candida antarctica lipase type A. Single crystal X-ray analysis has been carried out to unambiguously define the stereochemistry of the two enantiomers, and to explore in depth their three-dimensional features
Interatomic Coulombic Decay following Photoionization of the Helium Dimer: Observation of Vibrational Structure
Using synchrotron radiation we simultaneously ionize and excite one helium
atom of a helium dimer (He_2) in a shakeup process. The populated states of the
dimer ion (i.e. He^[*+](n = 2; 3)-He) are found to deexcite via interatomic
coulombic decay. This leads to the emission of a second electron from the
neutral site and a subsequent coulomb explosion. In this letter we present a
measurement of the momenta of fragments that are created during this reaction.
The electron energy distribution and the kinetic energy release of the two He^+
ions show pronounced oscillations which we attribute to the structure of the
vibrational wave function of the dimer ion.Comment: 8 pages, 5 figure
Single photon double ionization of the helium dimer
We show that a single photon can ionize the two helium atoms of the helium
dimer in a distance up to 10 {\deg}A. The energy sharing among the electrons,
the angular distributions of the ions and electrons as well as comparison with
electron impact data for helium atoms suggest a knock-off type double
ionization process. The Coulomb explosion imaging of He_2 provides a direct
view of the nuclear wave function of this by far most extended and most diffuse
of all naturally existing molecules.Comment: 10 pages, 5 figure
Diffraction of complex molecules by structures made of light
We demonstrate that structures made of light can be used to coherently
control the motion of complex molecules. In particular, we show diffraction of
the fullerenes C60 and C70 at a thin grating based on a standing light wave. We
prove experimentally that the principles of this effect, well known from atom
optics, can be successfully extended to massive and large molecules which are
internally in a thermodynamic mixed state and which do not exhibit narrow
optical resonances. Our results will be important for the observation of
quantum interference with even larger and more complex objects.Comment: 4 pages, 3 figure
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