Stuart R. Burns, Oliver Paull, J.M. Le Breton, Manuel Bibes, Maximilien Cazayous, Yann Gallais, Laurent Bellaiche, Jean Juraszek, Vincent Garcia, Alain Sacuto, Bertrand Dupé, Valanoor Nagarajan, Brahim Dkhil, Florian Appert, Daniel Sando, C. Carrétéro, Bin Xu, Agnès Barthélémy, School of Materials Science and Engineering [Sydney], University of New South Wales [Sydney] (UNSW), Groupe de physique des matériaux (GPM), Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Université de Caen Normandie (UNICAEN), Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS), Tsinghua University [Beijing] (THU), Unité mixte de physique CNRS/Thales (UMPhy CNRS/THALES), THALES [France]-Centre National de la Recherche Scientifique (CNRS), Laboratoire Structures, Propriétés et Modélisation des solides (SPMS), Institut de Chimie du CNRS (INC)-CentraleSupélec-Centre National de la Recherche Scientifique (CNRS), Laboratoire Matériaux et Phénomènes Quantiques (MPQ (UMR_7162)), Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), DAM Île-de-France (DAM/DIF), Direction des Applications Militaires (DAM), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Department of Physics Department [Fayetteville], University of Arkansas [Fayetteville], Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU), Tsinghua University [Beijing], Unité mixte de physique CNRS/Thalès (UMP CNRS/THALES), THALES-Centre National de la Recherche Scientifique (CNRS), CentraleSupélec-Centre National de la Recherche Scientifique (CNRS), and Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Université de Rouen Normandie (UNIROUEN)
BiFeO3 thin films have attracted considerable attention by virtue of their potential application in low-energy spintronic and magnonic devices. BiFeO3 possesses an intricate magnetic structure, characterized by a spin cycloid with period ∼62 nm that governs the functional magnonic response, and which can be modulated or even destroyed by strain, magnetic and electric fields, or chemical doping. The literature on (110)-oriented BiFeO3 films is not explicit in defining the conditions under which this cycloid persists, as its presence depends on synthesis method and thin-film boundary conditions, especially in the sub-100 nm thickness regime. This report aims to end “trial and error” approaches in determining the conditions under which this cycloid and its associated functional magnonic response exist. We show that in specific crystallographic orientations of epitaxial BiFeO3, an unexplored strain parameter—the distortion in the ab plane of the monoclinic unit cell—significantly influences the spin structure. Combining Mossbauer spectroscopy and low-energy Raman spectroscopy with first-principles-based effective Hamiltonian calculations, we show that both average strain and this distortion destroy the cycloid. For films grown on (110)-oriented SrTiO3 substrates, if the BiFeO3 lattice parameters a and b differ by more than about 1.2%, the cycloid is destabilized, resulting in a pseudocollinear magnetic order ground state. We are thereby able to construct a phase diagram of the spin structure for nanoscale epitaxial BiFeO3 films, which aims to resolve long-standing literature inconsistencies and provide powerful guidelines for the design of future magnonic and spintronic devices.BiFeO3 thin films have attracted considerable attention by virtue of their potential application in low-energy spintronic and magnonic devices. BiFeO3 possesses an intricate magnetic structure, characterized by a spin cycloid with period ∼62 nm that governs the functional magnonic response, and which can be modulated or even destroyed by strain, magnetic and electric fields, or chemical doping. The literature on (110)-oriented BiFeO3 films is not explicit in defining the conditions under which this cycloid persists, as its presence depends on synthesis method and thin-film boundary conditions, especially in the sub-100 nm thickness regime. This report aims to end “trial and error” approaches in determining the conditions under which this cycloid and its associated functional magnonic response exist. We show that in specific crystallographic orientations of epitaxial BiFeO3, an unexplored strain parameter—the distortion in the ab plane of the monoclinic unit cell—significantly influences the spin structure...