Dissociative excitation processes of HCOOH in the vacuum ultraviolet (VUV) region were studied by single-VUV photon with synchrotron radiation source and by two-ultraviolet (UV) photon with KrF excimer laser. In the VUV dissociation, fluorescence excitation cross sections for the OH(A) and HCOO* were separately determined in the 106–155 nm region. The branching fraction was found to be a function of the VUV excitation wavelength. The magnitude is σOH(A)/[σOH(A)+σHCOO*]=0.13 at 124.5 nm and gradually increases to 0.39 at 110 nm. In the UV multiphoton dissociation at 249 nm, OH(A) and HCOO* fragments were also identified by a fluorescence spectrum. The production of OH(A) was shown to take place in the two-UV photon absorption of HCOOH. Nascent rotational and vibrational (V/R) state distributions of OH(A 2Σ+) produced via the photodissociation at a single excitation energy of 9.96 eV (124.5×1/249 nm×2), HCOOH+nhν(n=1,2)→HCO+OH(A 2Σ+), were determined by simulation analysis of the dispersed fluorescence spectra. The internal state distributions were found to be of the relaxed type, and rotational distribution could be approximated by a Boltzmann distribution. One-VUV photon excitation gave the best-fit rotational temperature Tr(v′=0)=3000 K and vibrational population ratio Nv′=1/Nv′=0=0.14, while two-UV photon excitation showed Tr(v′=0)=2000 K with Nv′=1/Nv′=0=0.12. Possible mechanisms for the OH(A) formation by both excitation sources were examined based on simple theoretical models. The degree of internal excitation is not consistent with a direct dissociation on a repulsive surface, and neither is a dissociation from a long-lived intermediate state. The formation of OH(A 2Σ+) is interpreted as dissociation of an electronically excited intermediate state, leading to the formation of OH(A)+CHO, populated competitively via an electronic predissociation process. The substantially different V/R distributions observed are dependent on the excited precursor state initially accessed, and may result from the constraint in the competing predissociation step that follows.
Highly insulating tantalum pentoxide (Ta2O5) capacitor films were obtained by dry O3 annealing at low temperatures ranging from 350 to 500 °C. Typical leakage current density and resistivity of a 10-nm-thick Ta2O5 film measured at 2 MV/cm were 2.5×10−8 A/cm2 and 4.8×1013 Ω cm, respectively, obtained by dry O3 annealing at 450 °C, while leakage current density of the as-deposited film was about 10−1 A/cm2. It was confirmed that the mechanism which improves the insulating properties after dry O3 annealing involves the reduction of the leakage current due to the reduction of the concentration of such impurities as hydrogen and carbon, and the reduction of oxygen vacancies in Ta2O5 films. In addition, amorphous Ta2O5 films annealed in dry O3 show much better insulating properties than polycrystalline films. This can be attributed to the suppression of leakage current at the grain boundaries. Regarding dielectric properties, Ta2O5 films have an average dielectric constant of 28, and the typical SiO2 equivalent thickness of a 10-nm-thick Ta2O5 film was 2.4 nm. Results of the time dependent dielectric breakdown measurement, the calculation of the storage node height of a capacitor, and the frequency dependence of the capacitance value suggest that the above Ta2O5 film is applicable to an integrated capacitor for next generation devices, replacing conventional capacitor films.
This letter reports on highly insulating amorphous-Ta2O5 (a-Ta2O5) films with ultrathin SiO2 effective thickness [teff(SiO2)]. Insulating properties were improved using dry-O3 annealing at 450 °C, in which the typical leakage current density and resistivity at 1.5 MV/cm were 3×10−8 A/cm2 and 5×1013 Ω cm, respectively. Typical teff(SiO2) of 1.2 nm was obtained for the a-Ta2O5 film formed on a Ru/TiN/Ti/n+-Si substrate, where a Ru layer can act as an effective barrier against oxidation as well as interdiffusion during annealing. In contrast, the teff(SiO2) of the Ta2O5 film prepared on a conventional TiN/Ti/n+-Si substrate was increased by interfacial degradation. Technology employing Ru bottom electrodes and dry-O3 annealing will open a new era of logic embedded memory for 1 Gbit generation.
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