Interparticle Interaction Matters: Charge Carrier Dynamics in Hybrid Semiconductor–Metal Cryoaerogels

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Translated title of the contributionPartikelwechselwirkungen haben Einfluss: Ladungsträger Dynamiken in Hybrid Halbleiter-Metall Kryoaerogelen
Original languageEnglish
Article number2200055
JournalAdvanced Materials Interfaces
Volume9
Issue number12
Publication statusPublished - 22 Apr 2022

Abstract

Integration of noble metals into semiconductor-based nanoparticle gel structures facilitates the extraction of photoexcited charge carriers upon illumination. While charge carrier generation takes place in the semiconductor component, noble metals in contact to the semiconductor act as electron sinks. Thus, the nature of the interface between the components is of essential importance, as it dictates the characteristics of the interparticle contact. Here, the influence of the nanoscale building block design on the charge carrier dynamics in cryoaerogels consisting of CdSe/CdS nanorods and nanoplatelets as well as of gold or platinum is reported. It is shown that direct growth of noble metal domains onto the semiconductor prior to the gelation significantly facilitates charge carrier separation in their cryoaerogel structures compared to gels from the colloidal mixtures of semiconductor and noble metal nanoparticles, the latter ones having less defined metal/semiconductor boundaries and much more arbitrary component distributions. Although the structure of the different cryoaerogel systems is similar at the micro- and macroscale, nanoscale differences caused by the two synthetic routes drive essentially different behavior regarding the charge carrier dynamics efficiency. These effects are observed spectroelectrochemically via intensity-modulated photocurrent spectroscopy emphasizing the importance of the semiconductor–metal connection in the hybrid structures.

Keywords

    charge carrier separation, cryoaerogels, hybrid nanocrystal gels, semiconductor–metal hybrid gels, spectroelectrochemistry

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Cite this

Interparticle Interaction Matters: Charge Carrier Dynamics in Hybrid Semiconductor–Metal Cryoaerogels. / Schlosser, Anja; Schlenkrich, Jakob Cornelius; Zambo, Daniel et al.
In: Advanced Materials Interfaces, Vol. 9, No. 12, 2200055, 22.04.2022.

Research output: Contribution to journalArticleResearchpeer review

Schlosser, A., Schlenkrich, J. C., Zambo, D., Rosebrock, M., Graf, R. T., Escobar Cano, G. E., & Bigall, N.-C. (2022). Interparticle Interaction Matters: Charge Carrier Dynamics in Hybrid Semiconductor–Metal Cryoaerogels. Advanced Materials Interfaces, 9(12), Article 2200055. https://doi.org/10.1002/admi.202200055
Schlosser A, Schlenkrich JC, Zambo D, Rosebrock M, Graf RT, Escobar Cano GE et al. Interparticle Interaction Matters: Charge Carrier Dynamics in Hybrid Semiconductor–Metal Cryoaerogels. Advanced Materials Interfaces. 2022 Apr 22;9(12):2200055. doi: 10.1002/admi.202200055
Schlosser, Anja ; Schlenkrich, Jakob Cornelius ; Zambo, Daniel et al. / Interparticle Interaction Matters : Charge Carrier Dynamics in Hybrid Semiconductor–Metal Cryoaerogels. In: Advanced Materials Interfaces. 2022 ; Vol. 9, No. 12.
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title = "Interparticle Interaction Matters: Charge Carrier Dynamics in Hybrid Semiconductor–Metal Cryoaerogels",
abstract = "Integration of noble metals into semiconductor-based nanoparticle gel structures facilitates the extraction of photoexcited charge carriers upon illumination. While charge carrier generation takes place in the semiconductor component, noble metals in contact to the semiconductor act as electron sinks. Thus, the nature of the interface between the components is of essential importance, as it dictates the characteristics of the interparticle contact. Here, the influence of the nanoscale building block design on the charge carrier dynamics in cryoaerogels consisting of CdSe/CdS nanorods and nanoplatelets as well as of gold or platinum is reported. It is shown that direct growth of noble metal domains onto the semiconductor prior to the gelation significantly facilitates charge carrier separation in their cryoaerogel structures compared to gels from the colloidal mixtures of semiconductor and noble metal nanoparticles, the latter ones having less defined metal/semiconductor boundaries and much more arbitrary component distributions. Although the structure of the different cryoaerogel systems is similar at the micro- and macroscale, nanoscale differences caused by the two synthetic routes drive essentially different behavior regarding the charge carrier dynamics efficiency. These effects are observed spectroelectrochemically via intensity-modulated photocurrent spectroscopy emphasizing the importance of the semiconductor–metal connection in the hybrid structures.",
keywords = "charge carrier separation, cryoaerogels, hybrid nanocrystal gels, semiconductor–metal hybrid gels, spectroelectrochemistry",
author = "Anja Schlosser and Schlenkrich, {Jakob Cornelius} and Daniel Zambo and Marina Rosebrock and Graf, {Rebecca Tatjana} and {Escobar Cano}, {Giamper Eliseo} and Nadja-Carola Bigall",
note = "Funding Information: A.S. and J.S. contributed equally to this work. The authors would like to acknowledge the financial support from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (Grant Agreement No. 714429). In addition, this work was funded by the German Research Foundation (Deutsche Forschungsgemeinschaft, DFG) under Germany's excellence strategy within the cluster of excellence PhoenixD (EXC 2122, project ID 390833453) and the grant BI 1708/4‐1. D.Z. acknowledges the program financed by the National Research, Development and Innovation Office of the Ministry for Innovation and Technology, Hungary (TKP2021‐NKTA‐05). A.S. and R.T.G. are thankful for financial support from the Hannover School for Nanotechnology (hsn). The authors also thank Armin Feldhoff and J{\"u}rgen Caro for providing the SEM facility, and the LNQE for providing the TEM.",
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T1 - Interparticle Interaction Matters

T2 - Charge Carrier Dynamics in Hybrid Semiconductor–Metal Cryoaerogels

AU - Schlosser, Anja

AU - Schlenkrich, Jakob Cornelius

AU - Zambo, Daniel

AU - Rosebrock, Marina

AU - Graf, Rebecca Tatjana

AU - Escobar Cano, Giamper Eliseo

AU - Bigall, Nadja-Carola

N1 - Funding Information: A.S. and J.S. contributed equally to this work. The authors would like to acknowledge the financial support from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (Grant Agreement No. 714429). In addition, this work was funded by the German Research Foundation (Deutsche Forschungsgemeinschaft, DFG) under Germany's excellence strategy within the cluster of excellence PhoenixD (EXC 2122, project ID 390833453) and the grant BI 1708/4‐1. D.Z. acknowledges the program financed by the National Research, Development and Innovation Office of the Ministry for Innovation and Technology, Hungary (TKP2021‐NKTA‐05). A.S. and R.T.G. are thankful for financial support from the Hannover School for Nanotechnology (hsn). The authors also thank Armin Feldhoff and Jürgen Caro for providing the SEM facility, and the LNQE for providing the TEM.

PY - 2022/4/22

Y1 - 2022/4/22

N2 - Integration of noble metals into semiconductor-based nanoparticle gel structures facilitates the extraction of photoexcited charge carriers upon illumination. While charge carrier generation takes place in the semiconductor component, noble metals in contact to the semiconductor act as electron sinks. Thus, the nature of the interface between the components is of essential importance, as it dictates the characteristics of the interparticle contact. Here, the influence of the nanoscale building block design on the charge carrier dynamics in cryoaerogels consisting of CdSe/CdS nanorods and nanoplatelets as well as of gold or platinum is reported. It is shown that direct growth of noble metal domains onto the semiconductor prior to the gelation significantly facilitates charge carrier separation in their cryoaerogel structures compared to gels from the colloidal mixtures of semiconductor and noble metal nanoparticles, the latter ones having less defined metal/semiconductor boundaries and much more arbitrary component distributions. Although the structure of the different cryoaerogel systems is similar at the micro- and macroscale, nanoscale differences caused by the two synthetic routes drive essentially different behavior regarding the charge carrier dynamics efficiency. These effects are observed spectroelectrochemically via intensity-modulated photocurrent spectroscopy emphasizing the importance of the semiconductor–metal connection in the hybrid structures.

AB - Integration of noble metals into semiconductor-based nanoparticle gel structures facilitates the extraction of photoexcited charge carriers upon illumination. While charge carrier generation takes place in the semiconductor component, noble metals in contact to the semiconductor act as electron sinks. Thus, the nature of the interface between the components is of essential importance, as it dictates the characteristics of the interparticle contact. Here, the influence of the nanoscale building block design on the charge carrier dynamics in cryoaerogels consisting of CdSe/CdS nanorods and nanoplatelets as well as of gold or platinum is reported. It is shown that direct growth of noble metal domains onto the semiconductor prior to the gelation significantly facilitates charge carrier separation in their cryoaerogel structures compared to gels from the colloidal mixtures of semiconductor and noble metal nanoparticles, the latter ones having less defined metal/semiconductor boundaries and much more arbitrary component distributions. Although the structure of the different cryoaerogel systems is similar at the micro- and macroscale, nanoscale differences caused by the two synthetic routes drive essentially different behavior regarding the charge carrier dynamics efficiency. These effects are observed spectroelectrochemically via intensity-modulated photocurrent spectroscopy emphasizing the importance of the semiconductor–metal connection in the hybrid structures.

KW - charge carrier separation

KW - cryoaerogels

KW - hybrid nanocrystal gels

KW - semiconductor–metal hybrid gels

KW - spectroelectrochemistry

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JO - Advanced Materials Interfaces

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SN - 2196-7350

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ER -

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