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Item type:Item, Effect of Fe2O3 coating on ZnO nanowires in photoelectrochemical water splitting: A synchrotron x-ray spectroscopic and spectromicroscopic investigation(2020-06-01) ;Lu, Y. R. ;Wang, Y. F. ;Chang, H. W. ;Huang, Y. C.Chen, J. L.An array of ZnO/Fe2O3 core-shell nanowires (NW) for the highly efficient absorption of light and carrier collection is developed for use in photoelectrochemical (PEC) water-splitting. The oriented NW architecture favors physical matching, providing a direct electron conduction pathway and reducing the diffusion length of photogenerated holes. This work involves a combination of spectral imaging, spectromicroscopy and in situ x-ray absorption spectroscopy; spectra are obtained under operando conditions. Direct investigation of oriented nanowires using polarization-dependent x-ray spectromicroscopy enables the determination of the relationship between anisotropic electronic orbitals and charge carrier water-splitting efficiency. The results of O K-edge STXM demonstrated that the ZnO/Fe2O3 core-shell NW exhibits strong anisotropy and thus provides higher electron-hole transport efficiency than bare ZnO. In situ XAS revealed that interfacial charge transfer between Fe 3d and Zn 4p states enhances the photoelectrochemical reaction in the ZnO/Fe2O3 core-shell NW. The photogenerated electrons of Fe2O3 are transferred from Fe 3d states to the Zn 4p state under photoelectrochemical conditions.Item type:Item, Time-resolved photoluminescence of isoelectronic traps in ZnSe1-xTex semiconductor alloys(2008-12-15) ;Lin, Y. C. ;Chou, W. C. ;Fan, W. C. ;Ku, J. T.Ke, F. K.Kohlrausch's stretched exponential law correlates well with the photoluminescence (PL) decay profiles of ZnSe1-xTex. As the Te concentration increases, the stretching exponent beta initially declines and then monotonically increases. This result can be understood using the hopping-transport and energy transfer model. The increase in the number of isoelectronic Te localized traps can reduce the PL decay rate and increase the linewidth, whereas the hybridization of the Te localized states with the valence-band edge states causes a reduction in both the lifetime and linewidth.Item type:Item, A comprehensive study of temperature-dependent reflectance and photoluminescence of Zn1-xMnxO thin films grown on c-Al2O3(2009-03-01) ;Lin, D. Y. ;Lin, H. J. ;Wu, J. S. ;Chou, W. C.Yang, C. S.We present a systematic study of temperature-dependent reflectance (R) and photoluminescence (PL) measurements on ZnMnO films grown by plasma-assisted molecular beam epitaxy. For the first time, the three free-exciton transitions FXA (Gamma(7c)-Gamma(u)(7v)), FXB (Gamma(7c)-Gamma(9v)), and FXC (Gamma(7c)-Gamma(l)(7v)) and the longitudinal-optical phonon replicas of FXB and FXC of ZnMnO films have been clearly observed in the R spectra. The parameters describing the activation energy and the temperature dependence of the transition energy and broadening have been extracted by fitting the experimental R and PL spectra. The spectral data of ZnMnO films not only show the deterioration of crystalline quality with increasing Mn composition fraction but also indicate the Mn clustering caused by Mn atom segregation.Item type:Item, Lattice Dynamics and Crystalline Properties of Wurtzite Zn1-xMgxO Powders under High Pressure(2011-10-13) ;Lin, Y. C. ;Tseng, C. L. ;Chou, W. C. ;Chia, C. H.Han, T. C.This investigation systematically studies the lattice dynamics and crystalline properties in Zn1-xMgxO using high-pressure Raman spectroscopy. The incorporation of Mg and the application of external pressure cause distinct phonon vibrational behaviors in ZnO. Accordingly, the 202.7, 332.7, and 511.5 cm(-1) phonons, which have been controversially assigned, can be conclusively identified. Detailed Raman spectra reveal that the metallic phase transition of ZnO is complete by around 13.2 GPa, which pressure is found to decrease as the Mg content increases. Upon pressure release, an unusual hysteresis effect (>10.0 GPa) in Zn1-xMgxO is observed. The degree of crystal ionicity and anisotropy importantly affects the phase transition pressure of Zn1-xMgxO. Under ambient conditions, ZnO becomes more ionic upon the incorporation of Mg and becomes more covalent under higher pressure. These results are caused by the interplay between the pressure dependence of the high-frequency dielectric constant and Born's transverse dynamical effective charge. The E-1-A(1) splitting of the longitudinal and transverse optical phonons is analyzed, yielding insight into the pressure-dependent crystal anisotropy of Zn1-xMgxO.Item type:Item, Optical characterization of isoelectronic ZnSe1-xOx semiconductors(2011-05-15) ;Lin, Y. C. ;Chung, H. L. ;Ku, J. T. ;Chen, C. Y.Chien, K. F.We have studied the temperature dependence of the band gap and the decay dynamics of isoelectronic ZnSe1-xOx (x=0-0.053) semiconductors, using photoluminescence (PL) and time-resolved PL spectroscopy. The temperature dependence of the band gap of ZnSe1-xOx decreases with the increase in 0 concentration. The Kohlrausch law is in good agreement with the O-induced complex decay profiles. As temperature increases, the mechanism of carrier decay undergoes a complicated change from trapped to free excitons. These findings are consistent with the temperature dependence of the stretching exponent beta. (C) 2010 Elsevier B.V. All rights reserved.Item type:Item, Interrelation of transport and optical properties in gold nanoclusters(2010-09-20) ;Shu, G. W. ;Chen, T. Y. ;Shen, J. L. ;Lin, C. A. J.Chang, W. H.Temperature dependence of the electrical conductivity and photoluminescence (PL) in Au nanoclusters (NCs) is investigated. The correlation of the conductivity and PL in Au NCs at different temperatures is evident: (i) for T < 50 K, both the conductivity and PL intensity decrease with temperature, which suggests thermal structural fluctuations; (ii) for 50 K < T < 90 K, conductivity and PL are explained by variable range hopping; (iii) for 90 K < T < 170 K, simple thermal activated hopping dominates in conductivity, with a rate-equation model proposed to analyze the carrier transfer in PL. (C) 2010 American Institute of Physics. [doi: 10.1063/1.3491288]Item type:Item, Effects of rapid thermal annealing on the structural properties of TiO2 nanotubes(2011-10-15) ;Lin, J. Y. ;Chou, Y. T. ;Shen, J. L. ;Yang, M. D.Wu, C. H.The structural properties of TiO2 nanotubes with rapid thermal annealing (RTA) and traditional thermal annealing in O-2 were studied by X-ray diffraction (XRD) and Raman scattering measurements. From analyzing the line width of XRD and the correlation length of the Raman peak, we demonstrate that RTA can be an effective tool for amorphous-anatase transformation in TiO2 nanotubes. The Raman peak redshifts and reduces its line width after thermal annealing and RTA, which may involves the reduction of oxygen-related defects. (C) 2011 Elsevier B. V. All rights reserved.Item type:Item, Carrier dynamics in isoelectronic ZnSe1-xOx semiconductors(2010-07-26) ;Lin, Y. C. ;Chung, H. L. ;Chou, W. C. ;Chen, W. K.Chang, W. H.This study explores the effects of both Oxygen and temperature on the carrier dynamics of isoelectronic ZnSe1-xOx (x=0.027 and 0.053) semiconductors using photoluminescence (PL) and time-resolved PL spectroscopy. We find that the Kohlrausch law is highly consistent with the complex decay traces induced by isoelectronic O traps, and the mechanism of carrier recombination undergoes a complicated change from trapped to free excitons with the increase in temperature. Complex recombination processes are clarified using the relaxation model based on various decay channels. These findings are consistent with the initial fall in the stretching exponent beta followed by its monotonic increase with increasing temperature. (C) 2010 American Institute of Physics. [doi:10.1063/1.3473776]Item type:Item, Light-induced and holographic properties of ruthenium and manganese co-doped Bi4Ge3O12 crystals(2010-07-01) ;Lin, S. H. ;Marinova, V. ;Lin, Y. C. ;Petrova, D.Chou, W. C.The effect of Ru + Mn co-doping on the light-induced properties of Bi4Ge3O12 (BGO) crystals is studied and compared with single Ru- and Mn-doped crystals. Optical absorption spectra of Ru + Mn co-doped crystal demonstrates a photosensitivity shift to the visible spectral range. In addition, a strong photochromic effect, being fully reversible by thermal annealing is observed. It is verified by photoluminescence emission that charge traps could be manipulated under ultraviolet (UV) excitation, as the photoluminescence intensity decreases revealing the existence of the state filling effect. Ru + Mn doping leads to a faster response time during holographic recording at 633 nm and a prolonged read-out process, especially after a preliminary exposure to UV light. The ability to modify the defect structure and corresponding absorption bands suggests the future potential for optical fixing using a two-step sensitization method.Item type:Item, Eco-friendly luminescent solar concentrators with low reabsorption losses and resistance to concentration quenching based on aqueous-solution-processed thiolate-gold nanoclusters(2017-09-15) ;Huang, H. Y. ;Cai, K. B. ;Chang, L. Y. ;Chen, P. W.Lin, T. N.Heavy-metal-containing quantum dots (QDs) with engineered electronic states have been served as luminophores in luminescent solar concentrators (LSCs) with impressive optical efficiency. Unfortunately, those QDs involve toxic elements and need to be synthesized in a hazardous solvent. Recently, biocompatible, eco-friendly gold nanoclusters (AuNCs), which can be directly synthesized in an aqueous solution, have gained much attention for promising applications in 'green photonics'. Here, we explored the solid-state photophysical properties of aqueoussolution- processed, glutathione-stabilized gold nanoclusters (GSH-AuNCs) with a ligand-tometal charge-transfer (LMCT) state for developing 'green' LSCs. We found that such GSH-AuNCs exhibit a large Stokes shift with almost no spectral overlap between the optical absorption and PL emission due to the LMCT states, thus, suppressing reabsorption losses. Compared with GSH-AuNCs in solution, the photoluminescence quantum yields (PL-QYs) of the LSCs can be enhanced, accompanied with a lengthened PL lifetime owing to the suppression of non-radiative recombination rates. In addition, the LSCs do not suffer from severe concentration-induced PL quenching, which is a common weakness for conventional luminophores. As a result, a common trade-off between light-harvesting efficiency and solid-state PL-QYs can be bypassed due to nearly-zero spectral overlap integral between the optical absorption and PL emission. We expect that GSH-AuNCs hold great promise for serving as luminophores for 'green' LSCs by further enhancing solid-state PL-QYs.