High dielectric constant and capacitance in ultrasmall (2.5 nm) SrHfO3 perovskite nanoparticles produced in a low temperature non-aqueous sol-gel route

resumo

Strontium hafnium oxide (SrHfO3) has great potential as a high-k gate dielectric material, for use in memories, capacitors, CMOS and MOSFETs. We report for the first time the dielectric properties (relative permittivity and capacitance) of SrHfO3 nanoparticles (NPs), as opposed to thin films or sintered bulk ceramics. These monodisperse, ultra-small, perovskite-type SrHfO3 nanocrystals were synthesised through a non-aqueous sol-gel process under solvothermal conditions (at only 220 degrees C) using benzyl alcohol as a solvent, and with no other capping agents or surfactants. Advanced X-ray diffraction methods (whole powder pattern modelling, WPPM), CS-corrected high-resolution scanning transmission electron microscopy (HRSTEM), dielectric spectroscopy, and optical (UV-vis, Raman) and photoluminescent spectroscopy were used to fully characterise the NPs. These SrHfO3 NPs are the smallest reported and highly monodisperse, with a mean diameter of 2.5 nm, a mode of 2.0 nm and a small size distribution. The formation mechanism of the NPs was determined using NMR and GC-MS analysis of the species involved. Our SrHfO3 nanoparticles had a dielectric constant of 17, which is on par with literature data for bulk and thin film samples, and they also had a relatively large capacitance of 9.5 nF cm(-2). As such, they would be suitable for applications as gate dielectrics for capacitors and in metal-oxide semiconductor field-effect transistor (MOSFET) technology.

palavras-chave

PBNM ORTHORHOMBIC SRHFO3; OPTICAL-PROPERTIES; COMBUSTION TECHNIQUE; PHASE-TRANSITIONS; CRYSTAL-STRUCTURE; FUEL-CELLS; OXIDE; NANOSTRUCTURES; DIFFRACTION; POWDER

categoria

Chemistry

autores

Karmaoui, M; Ramana, EV; Tobaldi, DM; Lajaunie, L; Graca, MP; Arenal, R; Seabra, MP; Labrincha, JA; Pullar, RC

nossos autores

agradecimentos

Mohamed Karmaoui thanks Fundacao para a Ciencia e a Tecnologia (FCT) for Grant no. SFRH/BPD/74477/2010. Robert C. Pullar acknowledges the support of FCT grant SFRH/BPD/97115/2013. This work was developed in the scope of the project CICECO-Aveiro Institute of Materials (Ref. FCT UID/CTM/50011/2013), financed by national funds through the FCT/MEC and when applicable co-financed by FEDER under the PT2020 Partnership Agreement. Mohamed Karmaoui thanks Prof. Artur Silva for NMR measurements and fruitful discussions. Dr Carla Andrea Vilela is acknowledged for helpful discussions regarding the GC-MS (University of Aveiro, Portugal). Authors also acknowledge the PEstC/CTM/LA0011/2013 programme. E. Venkata Ramana would like to acknowledge the financial support from FCT, Portugal (SFRH/BPD/75582/2010). The HRSTEM work was conducted in the Laborario de Microscopias Avanzadas (LMA) at the Instituto de Nanociencia de Aragon (INA) - Universidad de Zaragoza (Spain). Some of the research leading to these results has received funding from the European Union Seventh Framework Program under Grant Agreement 312483 - ESTEEM2 (Integrated Infrastructure Initiative - I3). Raul Arenal also acknowledges funding from the Spanish Ministerio de Economia y Competitividad (FIS2013-46159-C3-3-P).

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