Elucidation of a Photothermal Energy Conversion Mechanism in Hydrogenated Molybdenum Suboxide: Interplay of Trapped Charges and Their Dielectric Interactions

• Published in: The journal of physical chemistry letters Vol. 14; no. 6; pp. 1528 - 1534
• Main Authors: Nishikubo, Ryosuke, Kuwahara, Yasutaka, Naito, Shintaro, Kusu, Kazuki, Saeki, Akinori
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 16.02.2023
• Subjects: Physical Insights into Materials and Molecular Properties
• ISSN: 1948-7185; 1948-7185
• DOI: 10.1021/acs.jpclett.3c00080

Hydrogenated molybdenum suboxide (H x MoO3–y ) is a promising photothermal energy conversion (PEC) material. However, its charge carrier dynamics and underlying mechanisms remain unclear. Utilizing flash-photolysis time-resolved microwave conductivity, we investigated charge carrier–dielectric interactions in the Pt/H x MoO3–y composite. The charge recombination of H2-reduced Pt/H x MoO3–y was 2–3 orders of magnitude faster than that of Pt/MoO3, indicating efficient PEC. A complex photoconductivity study revealed that Pt/H x MoO3–y has two types of trapping mechanisms, Drude–Zener (DZ) and negative permittivity effect (NPE) modes, depending on the reduction temperature. Pt/H x MoO3–y reduced at 100 °C exhibited a dominant NPE owing to the electrical interaction of trapped charges with the surrounding ions and/or OH base. This polaronic trapped state retarded the PEC process. We found Pt/H x MoO3–y reduced at 200 °C to be optimal owing to the balanced suppression of the NPE and charge diffusion. This is the first report revealing the charge dynamics in hydrogenated metal oxides and their impacts on PEC processes.