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This study investigates the influence of BaTiO3 layer thickness (50\u2013220 nm) on the films\u2019 structural, magnetic, and dielectric properties. The dense, polycrystalline films exhibited a tetragonal BaTiO3 phase and a cubic spinel CoFe2O4 layer. Structural analysis revealed compression of the CoFe2O4 unit cell along the growth direction, while the BaTiO3 layer showed a tetragonal distortion, more pronounced in thinner BTO layers. These strain effects, attributed to the mechanical interaction between both layers, induced strain-dependent wasp-waisted behavior in the films\u2019 magnetic hysteresis cycles. The strain effects gradually relaxed with increasing BaTiO3 thickness. Raman spectroscopy and second harmonic generation studies confirmed BTO\u2019s non-centrosymmetric ferroelectric structure at room temperature. The displayed dielectric permittivity dispersion was modeled using the Havriliak\u2013Negami function combined with a conductivity term. This analysis yielded relaxation times, DC conductivities, and activation energies. The observed BTO relaxation time behavior, indicative of small-polaron transport, changed significantly at the BTO ferroelectric Curie temperature (Tc), presenting activation energies E\u03c4 in the 0.1\u20130.3 eV range for T &lt; Tc and E\u03c4 &gt; 0.3 eV for T &gt; Tc. The BTO thickness-dependent Tc behavior exhibited critical exponents \u03bd ~ 0.82 consistent with the 3D random Ising universality class, suggesting local disorder and inhomogeneities in the films. This was attributed to the composite structure of BTO grains, comprising an inner bulk-like structure, a gradient strained layer, and a disordered surface layer. DC conductivity analysis indicated that CoFe2O4 conduction primarily occurred through hopping in octahedral sites. These findings provide crucial insights into the dynamic dielectric behavior of multiferroic bilayer thin films at the nanoscale, enhancing their potential for application in emerging Si electronics-compatible magneto-electric technologies.<\/jats:p>","DOI":"10.3390\/ma17235707","type":"journal-article","created":{"date-parts":[[2024,11,22]],"date-time":"2024-11-22T06:41:48Z","timestamp":1732257708000},"page":"5707","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Structural, Magnetic, and Dielectric Properties of Laser-Ablated CoFe2O4\/BaTiO3 Bilayers Deposited over Highly Doped Si(100)"],"prefix":"10.3390","volume":"17","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-7538-6847","authenticated-orcid":false,"given":"Jo\u00e3o","family":"Oliveira","sequence":"first","affiliation":[{"name":"Center of Physics of Minho and Porto Universities (CF-UM-UP), Laboratory for Materials and Emergent Technologies (LaPMET), Departamento de F\u00edsica, Universidade do Minho, Campus de Gualtar, 4710-057 Braga, Portugal"},{"name":"Nanostructured Materials Group, International Iberian Nanotechnology Laboratory (INL), Avenida Mestre Jos\u00e9 Veiga, 4715-330 Braga, Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8408-8235","authenticated-orcid":false,"given":"Bruna M.","family":"Silva","sequence":"additional","affiliation":[{"name":"Center of Physics of Minho and Porto Universities (CF-UM-UP), Laboratory for Materials and Emergent Technologies (LaPMET), Departamento de F\u00edsica, Universidade do Minho, Campus de Gualtar, 4710-057 Braga, Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8887-3591","authenticated-orcid":false,"given":"Tiago","family":"Rebelo","sequence":"additional","affiliation":[{"name":"Electron Microscopy for Materials Science (EMAT), University of Antwerp, Campus Groenenborger, Groenenborgerlaan 171, 2020 Antwerpen, Belgium"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0397-8808","authenticated-orcid":false,"given":"Pedro V.","family":"Rodrigues","sequence":"additional","affiliation":[{"name":"Institute for Polymers and Composites (IPC), Polymer Engineering Department, University of Minho, Campus de Azur\u00e9m, 4804-533 Guimar\u00e3es, Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5380-9212","authenticated-orcid":false,"given":"Rosa M. F.","family":"Baptista","sequence":"additional","affiliation":[{"name":"Center of Physics of Minho and Porto Universities (CF-UM-UP), Laboratory for Materials and Emergent Technologies (LaPMET), Departamento de F\u00edsica, Universidade do Minho, Campus de Gualtar, 4710-057 Braga, Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4758-1151","authenticated-orcid":false,"given":"Manuel J. L. F.","family":"Rodrigues","sequence":"additional","affiliation":[{"name":"Center of Physics of Minho and Porto Universities (CF-UM-UP), Laboratory for Materials and Emergent Technologies (LaPMET), Departamento de F\u00edsica, Universidade do Minho, Campus de Gualtar, 4710-057 Braga, Portugal"},{"name":"Integrated Micro and Nanotechnologies (IMiNa) Group, International Iberian Nanotechnology Laboratory (INL), Avenida Mestre Jos\u00e9 Veiga, 4715-330 Braga, Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7968-5038","authenticated-orcid":false,"given":"Michael","family":"Belsley","sequence":"additional","affiliation":[{"name":"Center of Physics of Minho and Porto Universities (CF-UM-UP), Laboratory for Materials and Emergent Technologies (LaPMET), Departamento de F\u00edsica, Universidade do Minho, Campus de Gualtar, 4710-057 Braga, Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7552-8534","authenticated-orcid":false,"given":"Neenu","family":"Lekshmi","sequence":"additional","affiliation":[{"name":"Institute of Physics of Advanced Materials, Nanotechnology and Photonics (IFIMUP), Department of Physics and Astronomy, Faculty of Sciences, University of Porto, Rua Campo Alegre, 4169-007 Porto, Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1646-7727","authenticated-orcid":false,"given":"Jo\u00e3o P.","family":"Ara\u00fajo","sequence":"additional","affiliation":[{"name":"Institute of Physics of Advanced Materials, Nanotechnology and Photonics (IFIMUP), Department of Physics and Astronomy, Faculty of Sciences, University of Porto, Rua Campo Alegre, 4169-007 Porto, Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8357-6608","authenticated-orcid":false,"given":"Jorge A.","family":"Mendes","sequence":"additional","affiliation":[{"name":"Center of Physics of Minho and Porto Universities (CF-UM-UP), Laboratory for Materials and Emergent Technologies (LaPMET), Departamento de F\u00edsica, Universidade do Minho, Campus de Gualtar, 4710-057 Braga, Portugal"},{"name":"Instituto Superior de Engenharia do Porto, Instituto Polit\u00e9cnico do Porto, Rua Dr. Ant\u00f3nio Bernardino de Almeida, 4249-015 Porto, Portugal"}]},{"given":"Francis Leonard","family":"Deepak","sequence":"additional","affiliation":[{"name":"Nanostructured Materials Group, International Iberian Nanotechnology Laboratory (INL), Avenida Mestre Jos\u00e9 Veiga, 4715-330 Braga, Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7604-0111","authenticated-orcid":false,"given":"Bernardo G.","family":"Almeida","sequence":"additional","affiliation":[{"name":"Center of Physics of Minho and Porto Universities (CF-UM-UP), Laboratory for Materials and Emergent Technologies (LaPMET), Departamento de F\u00edsica, Universidade do Minho, Campus de Gualtar, 4710-057 Braga, Portugal"}]}],"member":"1968","published-online":{"date-parts":[[2024,11,22]]},"reference":[{"key":"ref_1","doi-asserted-by":"crossref","first-page":"203","DOI":"10.1038\/s41563-018-0275-2","article-title":"Advances in magnetoelectric multiferroics","volume":"18","author":"Spaldin","year":"2019","journal-title":"Nat. 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