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The magnetoelectric coupling, i.e., cross-correlation between electric and magnetic orders, is a very desirable property to combine functionalities of materials for next-generation switchable devices. Multiferroics with spin-driven ferroelectricity presents such a mutual interaction concomitant with magneto-active and electro-active excitations called electromagnons. TbMnO3 is a paradigmatic material in which two electromagnons have been observed in the cycloidal magnetic phase. However, their observation in TbMnO3 is restricted to the cycloidal spin phase and magnetic ground states that can support the electromagnon excitation are still under debate. Here, we show by performing Raman spectroscopy measurements under pressure that the lower-energy electromagnon (4 meV) disappears when the ground state enters from a cycloidal phase to an antiferromagnetic phase (E-type). On the contrary, the magneto-electric activity of the higher-energy electromagnon (8 meV) increases in intensity by one order of magnitude. Using microscopic model calculations, we demonstrate that the lower-energy electromagnon, observed in the cycloidal phase, originates from a higher harmonic of the magnetic cycloid, and we determine that the symmetric exchange-striction mechanism is at the origin of the higher-energy electromagnon which survives even in the E-type phase. The colossal enhancement of the electromagnon activity in TbMnO3 paves the way to use multiferroics more efficiently for generation, conversion and control of spin waves in magnonic devices.Multiferroics: magneto-electric excitations survive outside cycloidal phaseTwo electromagnons are found to evolve differently when the ground state enters from a cycloidal phase to an antiferromagnetic phase in TbMnO3. An international team led by Maximilien Cazayous from Université Paris Diderot-Paris 7 performed Raman spectroscopy measurements and microscopic model calculations to understand how magneto-electric excitations evolve in TbMnO3 when hydrostatic pressure is applied. They found that two electromagnons, which are magneto-active and electro-active excitations, evolve differently when the ground state enters from a cycloidal phase to an antiferromagnetic phase. The lower-energy electromagnon only exists in the cycloidal phase, whereas the higher-energy one survives the phase transition and is enhanced by one order of magnitude in the antiferromagnetic phase. They attribute this to a symmetric exchange-striction mechanism, which may lead to a better use of multiferroics in magnonic devices.

Colossal electromagnon excitation in the non-cycloidal phase of TbMnO3 under pressure