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

Molecular hydrogen isotopes adsorbed on krypton-preplated graphite: Quantum Monte Carlo simulations

Adsorption of ortho-deuterium and para-hydrogen films on a graphite substrate, pre-plated with a single atomic layer of krypton, is studied theoretically by means of quantum Monte Carlo simulations at low temperature. Our model explicitly includes substrate corrugation. Energetic and structural properties of these adsorbed films are computed for a range of hydrogen coverages. Thermodynamically stable adsorbed films are solid, with no clear evidence of any liquid-like phase. Quantum exchanges of ortho-deuterium and para-hydrogen are essentially absent in this system, down to zero temperature; consequently, this system displays no superfluidity in this limit. Our simulations provide evidence of a stable domain wall fluid at low temperature, consistently with recent experimental observations.Comment: 7 pages, 7 figure

Low temperature phase diagram of condensed para-Hydrogen in two dimensions

Extensive Path Integral Monte Carlo simulations of condensed para-Hydrogen in two dimensions at low temperature have been carried out. In the zero temperature limit, the system is a crystal at equilibrium, with a triangular lattice structure. No metastable liquid phase is observed, as the system remains a solid down to the spinodal density, and breaks down into solid clusters at lower densities. The equilibrium crystal is found to melt at a temperature close to 7 K

Melting of a p-H2 monolayer on a lithium substrate

Adsorption of para-hydrogen films on Alkali metals substrates at low temperature is studied theoretically by means of Path Integral Monte Carlo simulations. Realistic potentials are utilized to model the interaction between two para-hydrogen molecules, as well as between a para-hydrogenmolecule and the substrate, assumed smooth. Results show that adsorption of para-hydrogen on a Lithium substrate, the most attractive among the Alkali, occurs through completion of successive solid adlayers. Each layer has a two-dimensional density approximatley equal 0.070 inverse square Angstroms. A solid para-hydrogen monolayer displays a higher degree of confinement, in the direction perpendicular to the substrate, than a monolayer Helium film, and has a melting temperature of about 6.5 K. The other Alkali substrates are not attractive enough to be wetted by molecular hydrogen at low temperature. No evidence of a possible superfluid phase of para-hydrogen is seen in these systems.Comment: Scales on the y-axis in Figs. 4,5 and 7 are off by a factor 2 in published version; corrected her

Excitations in confined helium

We design models for helium in matrices like aerogel, Vycor or Geltech from a manifestly microscopic point of view. For that purpose, we calculate the dynamic structure function of 4He on Si substrates and between two Si walls as a function of energy, momentum transfer, and the scattering angle. The angle--averaged results are in good agreement with the neutron scattering data; the remaining differences can be attributed to the simplified model used here for the complex pore structure of the materials. A focus of the present work is the detailed identification of coexisting layer modes and bulk--like excitations, and, in the case of thick films, ripplon excitations. Involving essentially two--dimensional motion of atoms, the layer modes are sensitive to the scattering angle.Comment: Phys. Rev. B (2003, in press

Superfluid 4He dynamics beyond quasiparticle excitations

The dynamics of superfluid 4He at and above the Landau quasiparticle regime is investigated by high precision inelastic neutron scattering measurements of the dynamic structure factor. A highly structured response is observed above the familiar phonon-maxon-roton spectrum, characterized by sharp thresholds for phonon-phonon, maxon-roton and roton-roton coupling processes. The experimental dynamic structure factor is compared to the calculation of the same physical quantity by a Dynamic Many-body theory including three-phonon processes self-consistently. The theory is found to provide a quantitative description of the dynamics of the correlated bosons for energies up to about three times that of the Landau quasiparticles.Comment: 5 pages, 3 figure

Quantum sticking, scattering and transmission of 4He atoms from superfluid 4He surfaces

We develop a microscopic theory of the scattering, transmission, and sticking of 4He atoms impinging on a superfluid 4He slab at near normal incidence, and inelastic neutron scattering from the slab. The theory includes coupling between different modes and allows for inelastic processes. We find a number of essential aspects that must be observed in a physically meaningful and reliable theory of atom transmission and scattering; all are connected with multiparticle scattering, particularly the possibility of energy loss. These processes are (a) the coupling to low-lying (surface) excitations (ripplons/third sound) which is manifested in a finite imaginary part of the self energy, and (b) the reduction of the strength of the excitation in the maxon/roton region

Application of inelastic epithermal neutron scattering to the vibrational spectroscopy of adsorbed molecules: Butane physisorbed on graphite (0001) surfaces

doi:10.1063/1.448924Inelastic epithermal neutron scattering (IENS) has been used to investigate the intramolecular vibrations of butane [CH3(CH2)2CH3] physisorbed on the (0001) surfaces of a graphite powder. The purpose of these studies was to assess IENS as a vibrational spectroscopy for adsorbed species by using a relatively well‐characterized substrate (Carbopack B). The experiments were performed on the IN1 spectrometer located on a beam from the ''hot'' source at the Institut Laue‐Langevin reactor in Grenoble. Film coverages of 1.0 and 3.6 layers were investigated at a temperature of 78 K. The IENS spectra are rich in structure, containing eight vibrational bands in the energy‐transfer range from 280-3470 cm−1 (35-430 meV). The similarity in the spectra at the two coverages investigated indicates that in this energy‐transfer range the butane intramolecular modes are not strongly perturbed by physisorption on graphite. A detailed comparison is made between the monolayer IENS spectrum and those calculated from models of a free and adsorbed molecule. Both models employ a previously derived intramolecular force field in the normal mode calculation. A third calculation assumes the displacement eigenvectors of the free molecule but replaces the mode eigenfrequencies by their measured Raman and IR values. It reproduces the observed IENS spectra very well. The large number of vibrational bands observed and the close agreement with the calculated spectra suggest butane as a desirable adsorbate for similar experiments on catalytic substrates.This work was supported in part by National Science Foundation Grants DMR-1905958, INT- 8012228, and DMR-8304366 and by a grant of the Petroleum Research fund, administered by the American Chemical Society

Magnetic Structure in Fe/Sm-Co Exchange Spring Bilayers with Intermixed Interfaces

The depth profile of the intrinsic magnetic properties in an Fe/Sm-Co bilayer fabricated under nearly optimal spring-magnet conditions was determined by complementary studies of polarized neutron reflectometry and micromagnetic simulations. We found that at the Fe/Sm-Co interface the magnetic properties change gradually at the length scale of 8 nm. In this intermixed interfacial region, the saturation magnetization and magnetic anisotropy are lower and the exchange stiffness is higher than values estimated from the model based on a mixture of Fe and Sm-Co phases. Therefore, the intermixed interface yields superior exchange coupling between the Fe and Sm-Co layers, but at the cost of average magnetization.Comment: 16 pages, 6 figures and 1 tabl