Characterization of Electronic Transport through Amorphous TiO2 Produced by Atomic Layer Deposition

Nunez, Paul; Richter, Matthias H.; Piercy, Brandon D.; Roske, Christopher W.; Cabán-Acevedo, Miguel; Losego, Mark D.; Konezny, Steven J.; Fermin, David J.; Hu, Shu; Brunschwig, Bruce S.; Lewis, Nathan S.

doi:10.1021/acs.jpcc.9b04434

Title: Characterization of Electronic Transport through Amorphous TiO₂ Produced by Atomic Layer Deposition

Journal Article · Wed Jun 19 00:00:00 EDT 2019 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.9b04434· OSTI ID:1599606

Nunez, Paul ^[1];

^[1]; Piercy, Brandon D. ^[2]; Roske, Christopher W. ^[1]; Cabán-Acevedo, Miguel ^[1];

^[2]; Konezny, Steven J. ^[3];

^[4];

^[3]; Brunschwig, Bruce S. ^[1];

^[1]

California Institute of Technology (CalTech), Pasadena, CA (United States)
Georgia Inst. of Technology, Atlanta, GA (United States)
Yale Univ., New Haven, CT (United States)
Bristol Univ. (United Kingdom)

Electrical transport in amorphous titanium dioxide (a-TiO₂) thin films, deposited by atomic layer deposition (ALD), and across heterojunctions of p⁺-Si|a-TiO₂|metal substrates that had various top metal contacts has been characterized by ac conductivity, temperature-dependent dc conductivity, space-charge-limited current spectroscopy, electron paramagnetic resonance (EPR) spectroscopy, X-ray photoelectron spectroscopy, and current density versus voltage (J–V) characteristics. Amorphous TiO₂ films were fabricated using either tetrakis(dimethylamido)-titanium with a substrate temperature of 150 °C or TiCl₄ with a substrate temperature of 50, 100, or 150 °C. EPR spectroscopy of the films showed that the Ti³⁺ concentration varied with the deposition conditions and increases in the concentration of Ti³⁺ in the films correlated with increases in film conductivity. Valence band spectra for the a-TiO₂ films exhibited a defect-state peak below the conduction band minimum (CBM) and increases in the intensity of this peak correlated with increases in the Ti³⁺ concentration measured by EPR as well as with increases in film conductivity. The temperature-dependent conduction data exhibited Arrhenius behavior at room temperature with an activation energy that decreased with decreasing temperature, suggesting that conduction did not occur primarily through either the valence or conduction bands. The information from all of the measurements are consistent with a Ti³⁺ defect-mediated transport mode involving a hopping mechanism with a defect density of 10¹⁹ cm^–3, a 0.83 wide defect band centered 1.47 eV below the CBM, and a free-electron concentration of 10¹⁶ cm^–3. The data are consistent with substantial room-temperature anodic conductivity resulting from the introduction of defect states during the ALD fabrication process as opposed to charge transport intrinsically associated with the conduction band of TiO₂.

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Research Organization:: California Institute of Technology (CalTech), Pasadena, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); UK Engineering and Physical Sciences Research Council; Tomkat Foundation

Grant/Contract Number:: SC0004993; EP/L017792/1

OSTI ID:: 1599606

Journal Information:: Journal of Physical Chemistry. C, Vol. 123, Issue 33; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 49 works

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