Transition films from amorphous (a-) to microcrystalline (μc-) silicon were prepared by hot-wire chemical vapor deposition using silane decomposition with either varied hydrogen-to-silane ratio, R, or with fixed R=3 but a varied substrate temperature, Ts. Raman results indicate that there is a threshold for the structural transition from a- to μc-Si:H in both cases. The onset of the structural transition is found to be R≈2 at Ts=250 °C and Ts≈200 °C at R=3. The properties of the material were studied by infrared absorption, optical absorption, photoluminescence (PL), and conductivity temperature dependence. We observed that the peak frequency of the SiH wag mode remains at 630−640 cm−1 for all the films, but the hydrogen content shows two regimes of fast and slow decreases separated by the onset of microcrystallinity. When microcrystallinity increased, we observed that (a) the SiO vibration absorption at 750 cm−1 and 1050−1200 cm−1 appeared, (b) the relative intensity of the 2090 cm−1 absorption increased, (c) the low-energy optical absorption at photon energy <1.4 eV increased one to two orders of magnitude, (d) the low-energy PL band at ∼1.0 eV emerged with a decrease of total PL intensity, and (e) the conductivity activation energy decreased. The aforementioned changes correlated well with the crystallinity of the material. We attribute the observations mainly to the formation of the c-Si gain boundaries during crystallization.
Films were prepared by hot wire chemical vapor deposition at ∼240 °C with varied hydrogen dilution ratios R=H2:SiH4 from 1 to 20. The optical and electronic properties as a function of microcrystallinity were studied. We found: (a) At low H dilution R⩽2, there is no measurable crystallinity by Raman spectroscopy and x-ray diffraction in the a-Si:H matrix, but an optical absorption peak at ∼1.25 eV appears; when R=2, the film shows the lowest subgap absorption, the highest photosensitivity, and the largest optical gap. (b) When R⩾3, the c-Si phase is measurable by Raman and a low-energy photoluminescence (PL) band (0.84–1.0 eV) appears in addition to the high-energy band (1.3–1.4 eV). Meanwhile, all the absorption spectra show a featureless line shape. (c) An energy redshift is observed for both PL peaks as the film grows thicker. Finally, (d) the conductivity activation energy first decreases from 0.68 to 0.12 eV, then increases with increasing microcrystallinity. A mode of two sets of energy bands of electronic states for these two-phase materials is suggested.
Thin films of guest-free type-II Si clathrate (Si136) were fabricated on Si(111) wafers in two steps: NaxSi136 thin-film formation by thermal decomposition of NaSi precursor films and Na removal from the NaxSi136 film by a heat treatment with iodine. Cross-sectional TEM observation and XRD and Raman measurements verified the formation of 1-µm-thick Si136 films on the Si wafer. Since the prepared films showed n-type conduction, pn junction devices were developed by a Si136/p-type Si structure. This device showed a photovoltaic (PV) response under white light illumination. The thin film formation and the PV response of Si136 indicated this Si allotrope to be the next-generation platform for semiconductor technology.
Deep localized electronic states are created by O2 intercalation into C60 films and C70 films, which causes the Fermi level to shift down to the middle of gap. The states act as a trap level for charge carriers and as nonradiative recombination centers. It seems that prepared C60 films and C70 films have a shallow localized state. The shallow state is located at ∼0.2 eV under the conduction band and affects the electrical and optical properties. Furthermore, the photoirradiation of C60 films and C70 films causes polymerization of the O2-free sample and oxidization of the O2-intercalated sample. The quasistable electronic states at room temperature are created as a result of photo-oxidization of C60 films. C60 oxides create deep localized electronic states which cannot disappear under thermal annealing. The photoluminescence intensity of O2-free samples increases with photoirradiation for 1 h. It is found for the first time that this increase occurs along with a decrease of localized state density.
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