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We have performed experimental investigations of methanol formation via the reactions of low energy $CH_{3}^{+}$ ions with an amorphous solid water (ASW) surface around 10 K. A newly developed experimental apparatus enabled irradiation of the ASW surface by several eV ions and detection of trace amounts of reaction products on the surface. It was found that methanol molecules were produced by low-energy $CH_{3}^{+}$ irradiation of the ASW surface and that hydroxy groups in produced methanol originated from water molecules in ASW, as predicted in a previous theoretical study. Little temperature dependence of observed methanol intensity is apparent in the temperature range 12 - 60 K. Ab-initio molecular dynamics simulations under constant temperature conditions of 10 K suggested that this reaction spontaneously produced a methanol molecule and an $H_{3}O^{+}$ ion, regardless of the contact point of $CH_{3}^{+}$ on the ASW surface. We have performed simulation with an astrochemical model under molecular-cloud conditions, where the reaction between $CH_{3}^{+}$ and $H_{2}O$ ice, leading to methanol formation, was included. We found that the impact of the reaction on methanol abundance was limited only at the edge of the molecular cloud (< 1 mag) because of the low abundance of $CH_{3}^{+}$ in the gas phase, whereas the reaction between the abundant molecular ion $HCO^{+}$ and $H_{2}O$ ice, which has not yet been confirmed experimentally, can considerably affect the abundance of a complex organic molecule. This work sheds light on a new type of reaction between molecular ions and ice surfaces that should be included in astrochemical models., Comment: 5 figures and Appendix, accepted to ApJ

Using a combination of photostimulated desorption and resonance-enhanced multiphoton ionization methods, the behaviors of OH radicals on the surface of interstellar ice analog was monitored at temperatures between 54 and 80 K. The OH number density on the surface of ultraviolet (UV)-irradiated compact amorphous solid water gradually decreased at temperatures above 60 K. Analyzing the temperature dependence of OH intensities with the Arrhenius equation, the decrease can be explained by recombination of two OH radicals, which is rate-limited by thermal diffusion of OH. The activation energy for surface diffusion was experimentally determined for the first time to be 0.14 +/- 0.01 eV, which is larger than or equivalent to those assumed in theoretical models. This value implies that the diffusive reaction of OH radicals starts to be activated at approximately 36 K on interstellar ice., Comment: 5 figures, Accepted to ApJL

Three structural isomers of the C2H4O2 molecule, namely, methyl formate (MF; HCOOCH3), acetic acid (AA; CH3COOH), and glycol aldehyde (GA; HOCH2CHO), have attracted considerable attention as targets for understanding pathways towards molecular complexity in the interstellar medium (ISM). Among these isomers, MF is decisively abundant in various astronomical objects. For various formation pathways of MF, surface reactions on cosmic dust would play an important role. However, when compared to observations, the formation of MF has been found to be relatively inefficient in laboratory experiments in which methanol (CH3OH)-dominant ices were processed by ultraviolet (UV) photons and cosmic-ray analogues. Here, we show experimental results on the effective formation of MF by the photolysis of CH3OH on water ice at 10 K. We found that the key parameter leading to the efficient formation of MF is the supply of OH radicals by the photolysis of H2O, which significantly differs from CH3OH-rich experimental conditions. Moreover, using an ultra-high-sensitivity surface analysis method, we succeeded in constraining the decisive formation pathway of MF via the photolysis of methoxymethanol (MM; CH3OCH2OH), which would improve our current understanding of chemical evolution in the ISM., Comment: Accepted in ApJL; 10 figures including 5 figures in Appendix

We present acoustic signatures of the electric quadrupolar degrees of freedom in the honeycomb-layer compound UNi$_4$B. The transverse ultrasonic mode $C_{66}$ shows softening below 30 K both in the paramagnetic phase and antiferromagnetic phases down to $\sim0.33$ K. Furthermore, we traced magnetic field-temperature phase diagrams up to 30 T and observed a highly anisotropic elastic response within the honeycomb layer. These observations strongly suggest that $\Gamma_6$(E$_{\rm 2g}$) electric quadrupolar degrees of freedom in localized $5f^2$ ($J = 4$) states are playing an important role in the magnetic toroidal dipole order and magnetic-field-induced phases of UNi$_4$B, and evidence some of the U ions remain in the paramagnetic state even if the system undergoes magnetic toroidal ordering., Comment: 6 pages, 4 figures + Supplemental Materials (11 pages, 9 figures)

Acoustic signatures of the single-site quadrupolar Kondo effect in Y$_{0.966}$Pr$_{0.034}$Ir$_2$Zn$_{20}$ are presented. The elastic constant ($C_{11}-C_{12}$)/2, corresponding to the $\Gamma_3$(E)-symmetry electric-quadrupolar response, reveals a logarithmic temperature dependence of the quadrupolar susceptibility in the low-magnetic-field region below $\sim$0.3 K. Furthermore, the Curie-type divergence of the elastic constant down to $\sim$1 K indicates that the Pr ions in this diluted system have a non-Kramers ground-state doublet. These observations evidence the single-site quadrupolar Kondo effect, as previously suggested based on specific-heat and electrical resistivity data., Comment: 5 pages, 4 figures (+ Supplemental Material: 5 pages, 4 figures)

The elastic properties of URu$_2$Si$_2$ in the high-magnetic field region above 40 T, over a wide temperature range from 1.5 to 120 K, were systematically investigated by means of high-frequency ultrasonic measurements. The investigation was performed at high magnetic fields to better investigate the innate bare 5$f$-electron properties, since the unidentified electronic thermodynamic phase of unknown origin, so called `hidden order'(HO) and associated hybridization of conduction and $f$-electron ($c$-$f$ hybridization) are suppressed at high magnetic fields. From the three different transverse modes we find contrasting results; both the $\Gamma_4$(B$_{\rm 2g}$) and $\Gamma_5$(E$_{\rm g}$) symmetry modes $C_{66}$ and $C_{44}$ show elastic softening that is enhanced above 30 T, while the characteristic softening of the $\Gamma_3$(B$_{\rm 1g}$) symmetry mode $(C_{11}-C_{12})/2$ is suppressed in high magnetic fields. These results underscore the presence of a hybridization-driven $\Gamma_3$(B$_{\rm 1g}$) lattice instability in URu$_2$Si$_2$. However, the results from this work cannot be explained by using existing crystalline-electric field (CEF) schemes applied to the quadrupolar susceptibility in a local $5f^2$ configuration. Instead, we present an analysis based on a band Jahn-Teller effect., Comment: 11 pages, 6 figures

The magnetically ordered phase of body-centered tetragonal UAu$_2$Si$_2$ was explored through $^{29}$Si-NMR experiments. The field-swept NMR spectra show asymmetric peak splitting below magnetic phase transition temperature, $T_{\rm m}$ = 20 K. This splitting is well explained by the occurrence of a magnetic order with propagation vector of $q$ = (2/3, 0, 0) and magnetic moments pointing parallel to the tetragonal [001] axis, offering evidence for uncompensated "up-up-down"-type antiferromagnetic ordering with a spontaneous [001] magnetization component. A symmetry analysis of the hyperfine-coupling tensor with phenomenological corrections including orbital and dipolar-field contributions yields the magnitude of the ordered moment to be approximately 1.4 $\pm$ 0.2 Bohr magneton per uranium ion, and evaluates the site-dependent hyperfine-coupling constants.

We present high-frequency ultrasonic measurements on the filled skutterudite SmOs$_4$Sb$_{12}$ under hydrostatic pressure. The results clarify that the 4$f$ electrons in this compound transform from delocalized at ambient pressure to localized at high pressures with a crossover pressure of approximately 0.7 GPa. This drastic change in the 4$f$ electrons under pressure is apparently related to the non-Fermi liquid state, which appears in an intermediate-pressure range of 0.5-1.5 GPa. The results or our analysis strongly suggest that the ferro-octupolar interaction becomes dominant at high pressure. Moreover, we report the pressure dependence of the ultrasonic dispersion, which is due to rattling, over a wide range of ultrasonic frequencies up to 323 MHz. The drastic change in the ultrasonic dispersions and the frequency dependent elastic anomaly in the $C_{11}$ mode at lower temperatures imply a possible coupling between rattling phonons and 4$f$ electrons., Comment: 7 pages, 4 figures

We present a study of the alloying series of the non-centrosymmetric $f$-electron intermetallic CePt$_3$B$_{1-x}$Si$_x$ by means of muon spin rotation and relaxation measurements. In addition, we include a high pressure magnetization investigation of the stoichiometric parent compound CePt$_3$B. From our data we establish the nature of the magnetic ground state properties of the series, derive the ordered magnetic moment as function of stoichiometry and gain insight into the evolution of the symmetry of the ordered magnetic state with $x$. We thus can verify the notion that the behavior of the sample series can essentially be understood within the framework of the Doniach phase diagram. Further, our findings raise the issue of the role the Dzyaloshinskii-Moriya magnetic interaction plays in correlated electron materials, and its effect on magnetic fluctuations in such materials., Comment: 8 pages, 8 figures

We have measured the elastic constant (C11-C12)/2 in URu2Si2 by means of high-frequency ultrasonic measurements in pulsed magnetic fields H || [001] up to 61.8 T in a wide temperature range from 1.5 to 116 K. We found a reduction of (C11-C12)/2 that appears only in the temperature and magnetic field region in which URu2Si2 exhibits a heavy-electron state and hidden-order. This change in (C11-C12)/2 appears to be a response of the 5f-electrons to an orthorhombic and volume conservative strain field \epsilon_xx-\epsilon_yy with {\Gamma}3-symmetry. This lattice instability is likely related to a symmetry-breaking band instability that arises due to the hybridization of the localized f electrons with the conduction electrons, and is probably linked to the hidden-order parameter of this compound., Comment: 5 pages, 4 figures

We report detailed studies of the upper critical field and low-temperature specific heat in the two-gap superconductor Lu$_{2}$Fe$_{3}$Si$_{5}$. The anisotropy of the upper critical field suggests that the active band is quasi-one-dimensional. Low-temperature specific heat in magnetic fields reveals that the virtual $H_{c2}$ in the passive band is almost isotropic. These results strongly indicate that the two bands have two different anisotropies, similar to the typical two-gap superconductor MgB$_{2}$, and their interplay may be essential to the two-gap superconductivity in Lu$_{2}$Fe$_{3}$Si$_{5}$., Comment: 5 pages, 5 figures

The present study experimentally demonstrated that solid H2O is formed through the surface reaction OH + H2 at 10 K. This is the first experimental evidence of solid H2O formation using hydrogen in its molecular form at temperatures as low as 10 K. We further found that H2O formation through the reaction OH + H2 is about one order of magnitude more effective than HDO formation through the reaction OH + D2. This significant isotope effect results from differences in the effective mass of each reaction, indicating that the reactions proceed through quantum tunneling., Comment: 12 pages, 10 figures

The nature of competition between incommensurate (IC) and commensurate (C) antiferromagnetic (AF) orders in UPd2Si2 was investigated by performing elastic neutron scattering experiments under uniaxial stress sigma. It is found that applying sigma along tetragonal [010] direction reduces the IC-AF order, and then stabilizes the C-AF order. The transition temperature from IC- to C-AF phases T_Nl is enhanced from 109 K (sigma=0) to 112.5 K (0.8 GPa), while the onset of IC-AF transition T_Nh is unchanged from 132 K under sigma. In addition, c-axis component q_z of the IC-AF modulation at 115 K also increases from 0.736 (sigma=0) to 0.747 (0.8 GPa). The magnitude of C-AF moment at 5 K is estimated to be 2.2 mu_B/U in the entire sigma range presently investigated (sigma <= 0.8 GPa). These features are similar to those obtained from the investigations using hydrostatic pressure p, indicating that applications of p and sigma||[010] commonly induce the crystal strains which inherently affect a delicate balance of frustrated magnetic interactions between uranium 5f moments., Comment: 4 pages, 2 figures

Experiments on the hydrogenation of CO on crystalline and amorphous ice at 15 K were carried out to investigate the structural effects of the ice surface. The effective rate of H atom addition to CO on the amorphous ice was found to be larger than that on the crystalline ice, while CO depletion on crystalline ice became larger after long exposure.We demonstrated that the CO-coverage on the ice surfaces dominates the effective reaction rate rather than the surface structure. The larger depletion of CO on crystalline ice, as compared to amorphous ice, suggests easier desorption of CO and/or products by the heat of the reaction., Comment: 11 pages, 4 figures

The reactions of cold H atoms with solid O2 molecules were investigated at 10 K. The formation of H2O2 and H2O has been confirmed by in-situ infrared spectroscopy. We found that the reaction proceeds very efficiently and obtained the effective reaction rates. This is the first clear experimental evidence of the formation of water molecules under conditions mimicking those found in cold interstellar molecular clouds. Based on the experimental results, we discuss the reaction mechanism and astrophysical implications., Comment: 12 pages, 3 Postscript figures, use package amsmath, amssymb, graphics