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Fast kinetic laser spectroscopy of the exciton dynamics during photocatalytic ZnCdS/ZnCdS/ZnS QDs mediated hydrogen production

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Abstract

The alloys of Zn0.34Cd0.66S QDs show a high photocatalytic activity when mediating the hydrogen production from water with a reaction rate of 233 ± 9 µmol h−1 g−1. The reaction is carried out in the presence of ascorbic acid as sacrificial electron donor. The alloy Zn0.34Cd0.66S/ZnS QDs with a ZnS shell showed a yield about seven times lower for the same process compared to the ZnCdS/ZnS alloy. The dynamics of the exciton reactions in the initial stages of the reaction mediated by these QDs was studied by femtosecond laser spectroscopy. Femtosecond transient absorption spectra is reported in a detailed and comprehensive way describing dynamics of the absorption peak A1 near the bleach band of edge exciton B1. This A1 absorption peak is attributed to the Stark shift due to exciton–exciton interactions due to the trapping of a hole or an electron on the QDs surface. In shell-less ZnCdSQDs, the A1 peak presented two kinetic components: the damping of the A1 peak amplitude due to the relaxation of “hot” excitons and the concomitant growth of the A1 peak at later delay times. We suggest that this was due to due to the carrier capture charge by surface traps leading to electric field redistribution in the QDs. The relaxation/decay of “hot” electrons in alloys of ZnCdS and ZnCdS/ZnS QDs occur with characteristic times of τZnCdS = 153 fs for ZnCdS and τZnCdS/ZnS = 193 fs.

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Dynamics of the TA spectra demonstrated in Figures 4, 6, and 8 suggests that holes are captured at the surface traps.

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Funding

Ministry of Science and Higher Education of the Russian Federation Grant #075-15-2022-255.

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Authors and Affiliations

  1. N. N. Semenov Federal Research Center for Chemical Physics, Russian Academy of Sciences, Kosygin St. 4, Moscow, 119991, Russian Federation

    Victor Nadtochenko, Andrei Kostrov, Fedor Gostev, Ivan Shelaev, Arseniy Aybush, Alexandr Vasin & Andrei Titov

  2. Department of Chemistry, Lomonosov Moscow State University, Leninskiye Gory 1-3, Moscow, 119991, Russian Federation

    Victor Nadtochenko

  3. A. N. Nesmeyanov Institute of Organoelement Compounds, Russian Academy of Sciences, Vavilova St. 28, Moscow, 119991, Russian Federation

    Sergei Kochev & Yurii Kabachii

  4. Ecole Polytechnique Fédérale de Lausanne (EPFL), 1015, Lausanne, Switzerland

    John Kiwi

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  1. Victor Nadtochenko
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Nadtochenko, V., Kochev, S., Kabachii, Y. et al. Fast kinetic laser spectroscopy of the exciton dynamics during photocatalytic ZnCdS/ZnCdS/ZnS QDs mediated hydrogen production. Appl. Phys. A 129, 155 (2023). https://doi.org/10.1007/s00339-023-06453-z

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