Inelastic electron tunneling spectroscopy of a single nuclear spin

Detection of a single nuclear spin constitutes an outstanding problem in different fields of physics such as quantum computing or magnetic imaging. Here we show that the energy levels of a single nuclear spin can be measured by means of inelastic electron tunneling spectroscopy (IETS). We consider two different systems, a magnetic adatom probed with scanning tunneling microscopy and a single Bi dopant in a silicon nanotransistor. We find that the hyperfine coupling opens new transport channels which can be resolved at experimentally accessible temperatures. Our simulations evince that IETS yields information about the occupations of the nuclear spin states, paving the way towards transport-detected single nuclear spin resonance.     

An inelastic electron tunneling spectroscopy study of the adsorption of CO on Rh

Inelastic Electron Tunneling Spectroscopy of CO adsorbed on alumina supported Rh allows the observation of the low frequency metal-carbon vibrational modes (~1000 cm^?1) that cannot be seen by Infrared Spectroscopy. We present a preliminary attempt to assign the modes observed, using istopic shifts $\text{C}{}^{16}\text{O}\text{C}{}^{18}\text{O}$.     

Inelastic electron tunneling spectroscopy: Intensity as a function of surface coverage

Inelastic election tunneling spectroscopy (IETS) is a sensitive technique for obtaining vibrational spectra of molecules adsorbed on an oxide surface and incorporated into a metal-oxide-metal tunnel junction. IETS energy data are used routinely. However, IETS intensities contain additional information which, for theoretical and experimental reasons, has not been used systematically. This paper examines the variation of IETS intensity with surface coverage of dopant molecules in the junction, a relationship of practical and theoretical importance. IET spectra are taken using standard experimental techniques and a liquid doping technique which allows the surface coverage to be determined independently. From an analysis of a large number of modes of benzoic acid on alumina, it is found that IETS intensity, defined in the usual way as the normalized change in conductance, $\text{Δ σ}\text{σ}$, is a nonlinear function of surface coverage. A physical model is presented which attributes this behavior to a difference in elastic tunneling conductances through empty or filled regions of the dopant layer in a junction with a fraction of a monolayer coverage. In addition, the liquid and vapor doping techniques in common use in IETS are discussed in terms of statistical mechanics and are shown to be manifestations of the same basic phenomenon.     

Inelastic electron tunneling spectroscopy evidence for a surface chemical reaction

The inelastic electron tunnel effect has been used to show the occurence of a surface chemical reaction between an organic molecule (benzoyl chloride) dopant and the tunnel barrier of a junction (Al-oxide-Pb).     

Inelastic electron tunneling spectroscopy on ultrahigh vacuum prepared tunnel junctions

Inelastic electron tunneling (IET) spectra of clean ultrahigh vacuum (UHV) prepared (Al/Al oxide/Pb) tunnel junctions are discussed. Microcrystalline Al oxide is shown to grow on these Al films. This is in contrast to the formation of amorphous Al oxide in the common high vacuum (HV) preparation process. The IET-spectra of UHV prepared tunnel junctions are free of peaks due to contaminations. Conclusions concerning the growth of oxides on Al films are drawn.     

Methane steam reforming in an annular microchannel with Rh/Al2O3 catalyst

Regularities of methane conversion in the presence of water steam were obtained experimentally while activating chemical conversions on the inner convex wall of an annular microchannel. The steam methane reforming was done on the Rh/Al₂O₃ nanocatalyst with the heat applied through the microchannel gap from the outer wall. Concentrations of the products of chemical reactions in the outlet gas mixture are measured at different temperatures of the outer microchannel wall. The range of channel wall temperatures at which the ratio of hydrogen and carbon oxide in the outlet mixture grows substantially is determined. Data on the composition of methane conversion products for the ratio H₂O/CH₄ = 1.77 and the activation energy of methane steam reforming at reactor outer wall temperatures of up to 880°C are obtained. The effect of the radiation heat exchange and the external diffuse limitation on the rate of chemical conversions in methane steam reforming in an annular microchannel with external heat supply is determined.     

Auger electron spectroscopy study on the Cr/Al2O3 interfacial reactions

Interfacial reactions of evaporated chromium with surface has been studied using Auger electron spectroscopy (AES). The results reveal that the interfacial region consists of a mixture, which is a double oxide of Cr and Al or two separated oxides. After annealing, the chromium oxide and the metallic Al produced by reduction of the Al³⁺ ions were easily detected by AES at the interface. We suggest that the interfacial reaction occurs mainly by the charge transfer from the 3d electrons of Cr atoms to O 2p orbitals of the Al₂O₃ substrate. The annealing at higher temperature (973 K) is favourable to promote the interfacial reaction between the surface oxygen and the initial few atomic monolayers of the deposited chromium. The results also showed that the change of the relative Auger peak-to-peak height (APPH(%)) of the Cr LMM group peaks can be used as an index to identify the oxidation states of chromium at the Cr/Al₂O₃ interface.     

Inelastic electron tunneling spectroscopy of an alkanethiol self-assembled monolayer using scanning tunneling microscopy

We report inelastic electron tunneling spectroscopy (IETS) of a C8 alkanethiol self-assembled monolayer using a scanning tunneling microscope (STM). High-resolution STM IETS spectra show clear features of the C-H bending and C-C stretching modes in addition to the C-H stretching mode, which enables a precise comparison with previously reported vibrational spectroscopy, especially electron energy loss spectroscopy data. Intensity variation of vibrational peaks with tip position is discussed with the STM IETS detection mechanism.     

Inelastic electron tunneling spectroscopy of carboxylic acids on alumina at low coverage

The difficulties in assigning certain modes of carboxylic acids adsorbed on alumina are discussed. The study of the spectra of marked acetic acid CH₃C¹⁸O¹⁸OH adsorbed on alumina has allowed us to clarify the assignments of the acetate ion formed. Then an examination of the spectra at very low coverages has enabled us to propose a model for the adsorption, which occurs on (at least) two different sites.     

Inelastic electron tunneling spectroscopy on MOS structures with very thin oxide films

Inelastic electron tunneling spectroscopy at 4.2 K was used to investigate the defect structure of MOS capacitors with very thin SiO₂ films. Samples were degeneratelyP-andB-doped Si substrates, oxidized in O₂ at 600°C and provided with evaporated Pb, Au, In, Al or Mg electrodes. The observed peaks in the second derivative of theI-U characteristic were assigned to the excitation of phonons and of vibrational modes of the dopants and impurities. The results were found to correlate with infrared data. In addition, a distinct effect of Si/SiO₂ interface states on the characteristic was found.     

Carbonate formation on Al2O3 thin film model catalyst supports

The formation of carbonate species on alumina upon CO and CO₂ exposure was studied by PM-IRAS and XPS, utilizing the model system of an ultrathin alumina film grown on NiAl(110). No carbonates were detected under UHV conditions, even after exposures up to 100.000 L of the gasses. In contrast, in a 100 mbar CO₂ atmosphere the formation of monodentate carbonates was identified. The surface concentration of the carbonates increased after generating defects on the alumina film by Ar⁺ ion bombardment. It is suggested that this kind of carbonate species is produced by reaction of coordinatively unsaturated O^2? ions of alumina with the C-atom of the CO₂ molecule. This is corroborated by the observation that the amount of carbonates further increased when CO₂ and oxygen were dosed simultaneously. In agreement with the “water gas shift” mechanism previously proposed for carbonate formation on high surface area alumina powders, no carbonates were detected from CO even upon mbar exposure, consistent with the absence of the required OH-groups on the model alumina support.     

Study on ultrasound-assisted precipitation for preparing Ni/Al2O3 catalyst

With the rapid development of oil hydrogenation industry, the development of oil hydrogenation catalyst has also become a research hotspot. In this paper, ultrasound-assisted precipitation technique is used to prepare Ni/Al₂O₃ catalyst. The effect of ultrasonic output power on catalyst performance is investigated. The prepared catalyst is applied to the hydrogenation reaction of castor oil. It is found that the prepared catalyst shows the best hydrogenation performance when ultrasonic output power, frequency and ultrasonic treatment time are 80 W, 40 kHz and 600 min respectively. It also indicates that ultrasound-assisted precipitation technique can reduce the particle size and increase the specific surface area of Ni/Al₂O₃ catalyst so that its activity is improved. In addition, six important elements that should be considered in the development of industrial oil refining catalysts are discussed, and the effects of these factors on the catalyst performance are discussed. Finally, new way for improving catalyst performance is given, and the application of some new materials and methods in oil refining is introduced.     

Magnetism in a UNi2/3Rh1/3Al single crystal

We report a magnetization, magnetostriction, electrical resistivity, specific heat and neutron scattering study of a UNi_2/3Rh_1/3Al single crystal, a solid solution of an antiferromagnet UNiAl and a ferromagnet URhAl. The huge uniaxial magnetic anisotropy confining the principal magnetic response to the c axis in the parent compounds persists also for the solid solution. The magnetization curve at 1.6 K has a pronounced S shape with an inflection at 12 T. The temperature dependence of magnetic susceptibility exhibits a maximum around 10 K and is magnetic history dependent at lower temperatures where the resistivity increases linearly with decreasing temperature. The low-temperature ρ(T) anomaly is removed in a magnetic field applied along c, which yields a large negative magnetoresistance amounting to m46 zin 14T (at 2 K). The C/T values exhibit a minimum around 12 K and below 8 K they become nearly constant (about 250 mJ mol^?1 K^?2), which is strongly affected by magnetic fields. Neutron scattering data confirm a non-magnetic ground state of UNi_2/3Rh_1/3Al. The bulk properties at low temperatures are tentatively attributed to the freezing of U magnetic moments with antiferromagnetic correlations. The additional intensities detected on top of nuclear reflections in neutron diffraction in a magnetic field applied along c are found to be proportional to the field-induced magnetization, which reflects field-induced ferromagnetic coupling of U magnetic moments. This scenario is corroborated also by finding low-temperature magnetostriction data that also scale with the square of magnetization.     

Catalytic ignition of light hydrocarbons over Rh/Al2O3 studied in a stagnation-point flow reactor

The ignition (light-off) temperatures of catalytic oxidation reactions provide very useful information for understanding their surface reaction mechanism. In this study, the ignition behavior of the oxidation of hydrogen (H₂), carbon monoxide (CO), methane (CH₄), ethane (C₂H₆), and propane (C₃H₈) over Rh/alumina catalysts is examined in a stagnation-point flow reactor. The light-off temperatures are identified by means of the sudden increase of the catalyst temperature when linearly heating the catalyst for various fuel/oxygen ratios. For hydrogen and all hydrocarbons studied, the results show a rise of ignition temperature with increasing fuel/oxygen ratio, whereas the opposite trend is observed for the light-off of CO oxidation. Hydrogen oxidation, however, shows an opposite trend compared to previous investigations, performed on platinum [1], [2].     

Hydrogen production over a commercial Pd/Al2O3 catalyst for fuel cell utilization

In order to produce a hydrogen stream for fuel cell utilization, the study of the ethanol steam reforming process over an alumina supported palladium commercial catalyst was carried out. The effect of the reaction temperature, the H₂O/C₂H₆O molar ratios and the contact time on catalytic activity and stability was studied. It was found that even at very low temperature values complete ethanol conversion was possible. Hydrogen selectivities up to 98% were obtained at temperature values close to 625 °C. It was also observed that for different reactant molar ratios carbon monoxide concentration exhibits a minimum at a temperature value close to 450 °C. Furthermore, carbon formation was found to be negligible even for H₂O/C₂H₆O molar ratios equal to the stoichiometric one. Paper presented at the 9th EuroConference on Ionics, Ixia, Rhodes, Greece, Sept. 15–21, 2002     

Co-Mo/Al2O3加氢脱硫催化剂的CO吸附原位红外光谱表征及应用研究

燃油的无硫化成为车用燃料发展的必然趋势.为开发高性能的柴油超深度加氢脱硫催化剂,文章采用CO吸附原位红外光谱法对系列还原态Co-Mo/Al2O3催化剂和高活性工业剂进行了表征,并将表征结果与微反加氢脱硫活性评价结果进行了关联分析.结果表明:随金属负载量的变化CO吸附的光谱特征发生变化,当MoO3负载量达20%、助剂CoO量为4.16%时,在2 179 cm-1出现一个新的CO特征吸收峰,该活性中心的出现明显有利于加氢脱硫(HYD)的反应.在相同金属负载量的情况下,与采用化学处理法制备的催化剂相比较,后者对应的2179 cm-1的特征吸收明显增强,微反评价显示该催化剂的催化活性特别是HYD反应活性明显提高.     

CuO/Al2O3、CuO/CeO2-Al2O3和CuO/La2O3-Al2O3催化剂中CuO物种被CO氧化的比较

用浸渍法制备了CuO/Al2O3 (Cu/Al)、CuO/CeO2- Al2O3 (Cu/CeAl)和CuO/La2O3-Al2O3(Cu/LaAl)催化剂. 通过原位XRD、Raman和H2-TPR方法， 对催化剂中的CuO物种以及CuO-Al2O3的固-固相反应进行了表征. 结果表明，对于Cu/Al催化剂，CuAl2O4存在于CuO与Al2O3层之间，CuO以高分散和晶相两种相态存在于催化剂的表层；对于Cu/CeAl催化剂，除了少量高分散和晶相的CuO存在于表层外，大部分CuO迁移到了CeO2的内层，     

Ion beam mixing at Fe:Al2O3 interface: A conversion electron Mössbauer spectroscopy study

The effect of ion beam induced atomic mixing and subsequent thermal transformations at the Fe:Al₂O₃ interface have been investigated by means of conversion electron Mössbauer spectroscopy [CEMS]. It is shown that the asdeposited and ion beam mixed samples exhibit distinctly different features. In particular, the ion beam mixed sample in as-mixed state shows the presence of FeAl₂O₄ along with non-stoichiometric FeO. Upon annealing at 600°C it shows precipitation of α-Fe with reduced contribution of FeAl₂O₄. The study of dose dependence of ion beam mixing has also revealed interesting features regarding the ion beam induced interface reactions.