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nanomaterials Article Supported Ultra-Thin Alumina Membranes with Graphene as Efficient Interference Enhanced Raman Scattering Platforms for Sensing Montserrat Aguilar-Pujol 1, Rafael Ramírez-Jiménez 1,2, Elisabet Xifre-Perez 3, Sandra Cortijo-Campos 1, Javier Bartolomé 1,4, Lluis F. Marsal 3 and Alicia de Andrés 1,* 1 2 3 Instituto de Ciencia de Materiales de Madrid, Consejo Superior de Investigaciones Científicas Cantoblanco, 28049 Madrid, Spain; xochitl.aguilarpujol@gmail.com (M.A.-P.); ramirez@fis.uc3m.es (R.R.-J.); s.cortijo@csic.es (S.C.-C.); jbvilchez@gmail.com (J.B.) Departamento de Física, Escuela Politécnica Superior, Universidad Carlos III de Madrid, Avenida Universidad 30, Leganés, 28911 Madrid, Spain Department of Electronic Engineering, Universitat Rovira i Virgili, Avda. Països Catalans 26, 43007 Tarragona, Spain; elisabet.xifre@urv.cat (E.X.-P.); lluis.marsal@urv.cat (L.F.M.) Departamento de Física de Materiales, Universidad Complutense de Madrid, Plaza Ciencias 1, 28040 Madrid, Spain 4 * Correspondence: ada@icmm.csic.es; Tel.: +34-913-349016 Received: 6 April 2020; Accepted: 23 April 2020; Published: 27 April 2020 Abstract: The detection of Raman signals from diluted molecules or biomaterials in complex media is still a challenge. Besides the widely studied Raman enhancement by nanoparticle plasmons, interference mechanisms provide an interesting option. A novel approach for amplification platforms based on supported thin alumina membranes was designed and fabricated to optimize the interference processes. The dielectric layer is the extremely thin alumina membrane itself and, its metallic aluminum support, the reflecting medium. A CVD (chemical vapor deposition) single-layer graphene is transferred on the membrane to serve as substrate to deposit the analyte. Experimental results and simulations of the interference processes were employed to determine the relevant parameters of the structure to optimize the Raman enhancement factor (E.F.). Highly homogeneous E.F. over the platform surface are obtained, typically 370 ± (5%), for membranes with ~100 nm pore depth, ~18 nm pore diameter and the complete elimination of the Al2O3 bottom barrier layer. The combined surface enhanced Raman scattering (SERS) and interference amplification is also demonstrated by depositing ultra-small silver nanoparticles. This new approach to amplify the Raman signal of analytes is easily obtained, low-cost and robust with useful enhancement factors (~400) and allows only interference or combined enhancement mechanisms, depending on the analyte requirements. Keywords: interference; enhanced Raman scattering; alumina membrane; graphene; nanoparticles; optical simulations; AFM; SEM 1. Introduction The search of novel platforms for the amplification of Raman signal is still an objective since Raman spectroscopy is one of the most powerful techniques to identify analytes through the characteristic vibration modes of molecules and crystals. The detection and imaging of extremely diluted and/or complex materials still require further research and development to get cheap, reliable, reproducible and stable over time systems that can be easily reused several times. The enhancement achieved using localized plasmons, the so-called surface enhanced Raman scattering (SERS) [1–4] is definitely the most efficient process allowing to reach single molecule detection through complex structures Nanomaterials 2020, 10, 830; doi:10.3390/nano10050830 www.mdpi.com/journal/nanomaterialsPDF Image | Supported Ultra-Thin Alumina Membranes with Graphene
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