TY - JOUR

T1 - One-Step Formation of Hybrid Nanocrystal Gels

T2 - Deposition of Metal Domains on CdSe/CdS Nanorod and Nanoplatelet Networks

AU - Zámbó, Dániel

AU - Schlosser, Anja

AU - Graf, Rebecca T.

AU - Rusch, Pascal

AU - Kißling, Patrick A.

AU - Feldhoff, Armin

AU - Bigall, Nadja C.

N1 - Funding Information: The project leading to these results was funded by the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (grant agreement 714429). The authors acknowledge the financial support from the German Federal Ministry of Education and Research (BMBF) within the framework of the program NanoMatFutur, support code 03X5525.?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. A.S. and R.T.G. are thankful for financial support from the Hannover School for Nanotechnology (HSN). The authors moreover thank the Laboratory of Nano and Quantum Engineering (LNQE) for providing the TEM facility. Open Access funding enabled and organized by Projekt DEAL.

PY - 2021/9/6

Y1 - 2021/9/6

N2 - Hybrid semiconductor-based nanocrystals (NCs) are generally synthesized in organic media prior to their assembly into catalytically promising nanostructures via multistep methods. Here, a tunable, easy-to-adapt and versatile approach for the preparation of hybrid nanoparticle networks from aqueous nanocrystal solutions is demonstrated. The networks consist of interconnected semiconductor NC backbones (made of CdSe/CdS dot-in-rods or core/crown nanoplatelets) decorated with noble metal (Au and Pt) or with metal-based domains (Co2+ and Ni2+) demonstrating a powerful synthetic control over a variety of hybrid nanostructures. The deposition of the domains and the formation of the network take place simultaneously (one-step method) at room temperature in dark conditions without any external trigger. Beside the in-depth structural characterization of the gel-like hybrid networks, the wavelength-dependent optical features are studied to reveal an efficient charge carrier separation in the systems and a controllable extent of fluorescence quenching through the domain sizes. Photoluminescence quantum yields and decay dynamics highlight the importance of fine-tuning the conduction band/Fermi level offset between the semiconductors and the various deposited metals playing central role in the electron–hole separation processes. This procedure provides a novel platform toward the preparation of photo(electro)catalytically promising hybrid nanostructures (acetogels and xerogels) without the need of presynthetic hybrid particle design.

AB - Hybrid semiconductor-based nanocrystals (NCs) are generally synthesized in organic media prior to their assembly into catalytically promising nanostructures via multistep methods. Here, a tunable, easy-to-adapt and versatile approach for the preparation of hybrid nanoparticle networks from aqueous nanocrystal solutions is demonstrated. The networks consist of interconnected semiconductor NC backbones (made of CdSe/CdS dot-in-rods or core/crown nanoplatelets) decorated with noble metal (Au and Pt) or with metal-based domains (Co2+ and Ni2+) demonstrating a powerful synthetic control over a variety of hybrid nanostructures. The deposition of the domains and the formation of the network take place simultaneously (one-step method) at room temperature in dark conditions without any external trigger. Beside the in-depth structural characterization of the gel-like hybrid networks, the wavelength-dependent optical features are studied to reveal an efficient charge carrier separation in the systems and a controllable extent of fluorescence quenching through the domain sizes. Photoluminescence quantum yields and decay dynamics highlight the importance of fine-tuning the conduction band/Fermi level offset between the semiconductors and the various deposited metals playing central role in the electron–hole separation processes. This procedure provides a novel platform toward the preparation of photo(electro)catalytically promising hybrid nanostructures (acetogels and xerogels) without the need of presynthetic hybrid particle design.

KW - charge carrier separation

KW - gel networks

KW - hybrid nanostructures

KW - metal domain

KW - semiconductor nanoplatelets

KW - semiconductor nanorods

UR - http://www.scopus.com/inward/record.url?scp=85106754820&partnerID=8YFLogxK

U2 - 10.1002/adom.202100291

DO - 10.1002/adom.202100291

M3 - Article

AN - SCOPUS:85106754820

VL - 9

JO - Advanced Optical Materials

JF - Advanced Optical Materials

SN - 2195-1071

IS - 17

M1 - 2100291

ER -