Dataset Information

Band to Band Tunneling at the Zinc Oxide (ZnO) and Lead Selenide (PbSe) Quantum Dot Contact; Interfacial Charge Transfer at a ZnO/PbSe/ZnO Probe Device.

ABSTRACT: We provide a comprehensive understanding of interfacial charge transfer at the lead selenide (PbSe) quantum dot (QD)/zinc oxide (ZnO) interface, proposing band to band tunneling process as a charge transfer mechanism in which initial hopping of carriers from ZnO to PbSe QDs is independent of temperature. Using the transmission line method (TLM) in a ZnO/PbSe/ZnO geometry device, we measured the ZnO/PbSe electrical contact resistance, a measure of charge transfer efficiency. Fabrication of a highly conductive ZnO film through Al doping allows for the formation of ZnO source and drain electrodes, replacing conventional metal electrodes. We found that band to band tunneling at the PbSe QD/ZnO interface governs charge transfer based on temperature-independent PbSe QD/ZnO contact resistance. In contrast, the PbSe QD channel sheet resistance decreased as the temperature increased, indicating thermally activated transport process in the PbSe QD film. These results demonstrate that, at the ZnO/PbSe QD interface, temperature-independent tunneling process initiates carrier injection followed by thermally activated carrier hopping, determining the electrical contact resistance.

SUBMITTER: Kim M

PROVIDER: S-EPMC6678409 | biostudies-literature | 2019 Jul

REPOSITORIES: biostudies-literature

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Publications

Band to Band Tunneling at the Zinc Oxide (ZnO) and Lead Selenide (PbSe) Quantum Dot Contact; Interfacial Charge Transfer at a ZnO/PbSe/ZnO Probe Device.

Kim Minkyong M Han Chang-Yeol CY Yang Heesun H Park Byoungnam B

Materials (Basel, Switzerland) 20190717 14

We provide a comprehensive understanding of interfacial charge transfer at the lead selenide (PbSe) quantum dot (QD)/zinc oxide (ZnO) interface, proposing band to band tunneling process as a charge transfer mechanism in which initial hopping of carriers from ZnO to PbSe QDs is independent of temperature. Using the transmission line method (TLM) in a ZnO/PbSe/ZnO geometry device, we measured the ZnO/PbSe electrical contact resistance, a measure of charge transfer efficiency. Fabrication of a high ...[more]

PMID: 31319559

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Project description:The sensitive electronic environment at the quantum dot (QD)-dye interface becomes a roadblock to enhancing the energy conversion efficiency of dye-functionalized quantum dots (QDs). Energy alignments and electronic couplings are the critical factors governing the directions and rates of different charge transfer pathways at the interface, which are tunable by changing the specific linkage groups that connect a dye to the QD surface. The variation of specific anchors changes the binding configurations of a dye on the QD surface. In addition, the presence of a co-adsorbent changes the dipole-dipole and electronic interactions between a QD and a dye, resulting in different electronic environments at the interface. In the present work, we performed density functional theory (DFT)-based calculations to study the different binding configurations of N719 dye on the surface of a Cd33Se33 QD with a co-adsorbent D131 dye. The results revealed that the electronic couplings for electron transfer were greater than for hole transfer when the structure involved isocyanate groups as anchors. Such strong electronic couplings significantly stabilize the occupied states of the dye, pushing them deep inside the valence band of the QD and making hole transfer in these structures thermodynamically unfavourable. When carboxylates were involved as anchors, the electronic couplings for hole transfer were comparable to electron transfer, implying efficient charge separation at the QD-dye interface and reduced electron-hole recombination within the QD. We also found that the electronic couplings for electron transfer were larger than those for back electron transfer, suggesting efficient charge separation in photoexcited QDs. Overall, the current computational study reveals some fundamental aspects of the relationship between the interfacial charge transfer for QD@dye composites and their morphologies which benefit the design of QD-based nanomaterials for photovoltaic applications.

Dataset Information

Band to Band Tunneling at the Zinc Oxide (ZnO) and Lead Selenide (PbSe) Quantum Dot Contact; Interfacial Charge Transfer at a ZnO/PbSe/ZnO Probe Device.

Publications

Band to Band Tunneling at the Zinc Oxide (ZnO) and Lead Selenide (PbSe) Quantum Dot Contact; Interfacial Charge Transfer at a ZnO/PbSe/ZnO Probe Device.

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