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    Study of the Bulk Charge Carrier Dynamics in Anatase and Rutile TiO2 Single Crystals by Femtosecond Time Resolved Spectroscopy

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    Type
    Article
    Authors
    Maity, Partha cc
    Mohammed, Omar F. cc
    Katsiev, Khabiboulakh
    Idriss, Hicham cc
    KAUST Department
    Chemical Science Program
    KAUST Solar Center (KSC)
    Physical Science and Engineering (PSE) Division
    SABIC - Corporate Research and Innovation Center (CRI) at KAUST
    Ultrafast Laser Spectroscopy and Four-dimensional Electron Imaging Research Group
    Date
    2018-04-02
    Online Publication Date
    2018-04-02
    Print Publication Date
    2018-04-26
    Permanent link to this record
    http://hdl.handle.net/10754/627541
    
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    Abstract
    Understanding of the fundamentals behind charge carriers of photo-catalytic materials are still illusive hindering progress in our quest for renewable energy. TiO2 anatase and rutile are the most understood phases in photo-catalysis and serve as the best model for fundamental studies. Their ultrafast charge carrier dynamics especially on TiO2 anatase single crystal (the most active phase) are unresolved. Here femtosecond time resolved spectroscopy (TRS) was carried out to explore the dynamics of photo-excited charge carriers’ recombination in anatase single crystal, for the first time using pump fluence effects, and compares it to that of the rutile single crystal. A significant difference in charge carrier recombination rates between both crystals is observed. We found that the time constants for carrier recombination are two orders of magnitude slower for anatase (101) when compared to those of rutile (110). Moreover, bulk defects introduced by reduction of the samples via annealing in ultra-high vacuum resulted in faster recombination rates for both polymorphs. Both states (fresh and reduced) probed by pump fluence dependence measurements revealed that the major recombination channel in fresh and reduced anatase and reduced rutile is the first-order Shockley–Reed mediated. However, for fresh rutile, third-body Auger recombination was observed, attributed to the presence of higher density of intrinsic charge carriers. At all excitation wavelengths and fluence investigated, anatase (101) single crystal show longer charge carrier lifetime when compared to rutile (110) single. This may explain the superiority of the anatase phase for the electron transfer H+ reduction to molecular hydrogen.
    Citation
    Maity P, Mohammed OF, Katsiev K, Idriss H (2018) Study of the Bulk Charge Carrier Dynamics in Anatase and Rutile TiO2 Single Crystals by Femtosecond Time-Resolved Spectroscopy. The Journal of Physical Chemistry C. Available: http://dx.doi.org/10.1021/acs.jpcc.8b00256.
    Publisher
    American Chemical Society (ACS)
    Journal
    The Journal of Physical Chemistry C
    DOI
    10.1021/acs.jpcc.8b00256
    Additional Links
    https://pubs.acs.org/doi/10.1021/acs.jpcc.8b00256
    ae974a485f413a2113503eed53cd6c53
    10.1021/acs.jpcc.8b00256
    Scopus Count
    Collections
    Articles; Physical Science and Engineering (PSE) Division; Chemical Science Program; KAUST Solar Center (KSC)

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