0018-9464 (c) 2016 IEEE. Personal use is permitted, but republication/redistribution requires IEEE permission. See http://www.ieee.org/publications_standards/publications/rights/index.html for more information. This article has been accepted for publication in a future issue of this journal, but has not been fully edited. Content may change prior to final publication. Citation information: DOI 10.1109/TMAG.2017.2699740, IEEE Transactions on Magnetics >FOR CONFERENCE-RELATED PAPERS, REPLACE THIS LINE WITH YOUR SESSION NUMBER, E.G., AB-02 (DOUBLE-CLICK HERE)< 0018-9464 © 2015 IEEE. Personal use is permitted, but republication/redistribution requires IEEE permission. See http://www.ieee.org/publications_standards/publications/rights/index.html for more information. (Inserted by IEEE.) 1 New multiferroic composite materials consisting of ferromagnetic, ferroelectric and polymer components Liudmila A. Makarova 1 , Valeria V. Rodionova 2 , Yuliya A. Alekhina 1 , Tatiana S. Rusakova 1 , Aleksander S. Omelyanchik 2 and Nikolai S. Perov 1 1 Faculty of Physics, Lomonosov MSU,Moscow, 119991,Russian Federation 2 Immanuel Kant Baltic Federal University, Kaliningrad, 236041, Russian Federation The multiferroic ferroelectric-ferromagnetic-polymer composite systems, consisting of ferroelectric PZT particles, ferromagnetic NdFeB (or barium ferrite) particles and silicone matrix, were investigated. The influence of the polymer Young’s modulus on the properties was determined. The coercivity of elastomers with the same magnetic fillers in different matrices differ by a factor of 7. The influence of magnetic field on electric properties was investigated. Magnetodielectric effect in three-phase samples was found to be non-monotonic. The influence of electric field on magnetic properties of elastomers was investigated. The magnetoelectric effect under an applied electric field in new three-phase material was discovered. Keywords— multiferroic materials, composite materials, magneto-elastic, hard magnetic particles, magnetorheological elastomers, magnetoelectric effect, magnetodielectric effect, tunable properties. I. INTRODUCTION ultiferroic materials are of a great interest now [1- 5].Such innovative technological devices as magnetic field detectors, miniature magnetoelectric transducer, four-stage memory devices, spintronic devices, devices for information storage and processing and other applications make the investigation of multiferroic materials more prospective [6-8]. Magnetoelectric effect in multiferroic composites consisting of ferroelectric and ferromagnetic components is the result of combination of mechanical connection between components, magnetostriction and piezoelectric effects. Currently, the most studied are the multilayer multiferroic composites. But other types of composite materials could be investigated as well. Magnetorheological (magnetoactive) elastomers are so-called “smart” materials. Various parameters of composites based on elastic polymers are tunable by magnetic field. Magnetic field can change Young’s modulus, deformation and other mechanical parameters by 1000% and more [9-12]. The dielectric permittivity of magnetic elastomers also can be changed by magnetic field which is known as magnetodielectric effect (MDE)[13]. It is assumed that the increase in the permittivity of the elastomer in the external magnetic field is due to the rotation of the filling particles [14- 17] and their displacement in the elastic matrix because of the interaction of the magnetic moment with magnetic field. Thus, the displacement of magnetic particles leads to internal stresses in the elastic matrix. Probably the same effect could be observed when the external electric field applied to the elastomer with ferroelectric particles [18], namely, the particles could shift and the internal stresses appeared. The research of multiferroic materials based on elastomers was also carried out: ferromagnetic particles are usually embedded in elastic matrix or similar ferroelectric polymer takes the role of an interlayer between ferromagnetic thin films [19-23]. All these facts make probable, that the combination of ferromagnetic and ferroelectric filling particles can lead to a new material, which properties can be changed both by external electric and magnetic field. The new multifunctional material, consisting of ferromagnetic, ferroelectric filling particles in the elastic matrix was studied in this work. It is assumed that the changes in orientation of polarization vectors of the ferroelectric particles in the material would occur due to the mechanical stresses in the matrix, not due to magnetostrictive properties of ferromagnetic particles as in the case regular multiferroics. It is also assumed that the magnetic properties of the composite material will be affected by the external electric field. The aim of the work was to study the features of the magnetoelectric transformation in the composite multiferroic materials based on ferromagnetic and ferroelectric fillers, including the development of new multi-functional materials and structures with magnetoelectric and magnetorheological properties. II. MATERIALS AND METHODS A. Materials 1. NdFeB powder. The initial powder size exceeded 100 μm. The powder was ground using the Ball mill at 1500 rpm for 5 minutes and sorted into three sets using sieve system: smaller than 29 μm, from 29 to 46 μm, larger than 46 μm. 2. Barium ferrite (BF) powder. Bulk polycrystalline barium ferrite was split and ground using the Ball mill at 1500 rpm for 5 min. The average size of the particles (about 7 μm) was determined using optical microscope. The sample of bulk barium ferrite crystal was also prepared as a flat disc with the M Manuscript received April 1, 2015; revised May 15, 2015 and June 1, 2015; accepted July 1, 2015. Date of publication July 10, 2015; date of current version July 31, 2015. (Dates will be inserted by IEEE; “published” is the date the accepted preprint is posted on IEEE Xplore®; “current version” is the date the typeset version is posted on Xplore®). Corresponding author: F. A. Author (e-mail: f.author@nist.gov). If some authors contributed equally, write here, “F. A. Author and S. B. Author contributed equally.” IEEE TRANSACTIONS ON MAGNETICS discourages courtesy authorship; please use the Acknowledgment section to thank your colleagues for routine contributions. Color versions of one or more of the figures in this paper are available online at http://ieeexplore.ieee.org. Digital Object Identifier (inserted by IEEE).