1. Max-Born-Institut, Max-Born-Strae 2A, 12489 Berlin, Germany
2. HISKP, Universität Bonn, Nussallee 14-16, 53115 Bonn, Germany
3. Department of Inorganic, Analytical and Applied Chemistry, University of Geneva, 30 quai Ernest-Ansermet, 1211 Geneva 4, Switzerland

Correspondence to: Manfred Fiebig^1,2 Correspondence and requests for materials should be addressed to M.F. (Email: fiebig@hiskp.uni-bonn.de).

Domains are of unparalleled technological importance as they are used for information storage and for electronic, magnetic and optical switches. They are an essential property of any ferroic material. Three forms of ferroic order are widely known: ferromagnetism, a spontaneous magnetization; ferroelectricity, a spontaneous polarization; and ferroelasticity, a spontaneous strain. It is currently debated whether to include an ordered arrangement of magnetic vortices as a fourth form of ferroic order, termed ferrotoroidicity. Although there are reasons to expect this form of order from the point of view of thermodynamics¹, a crucial hallmark of the ferroic state—that is, ferrotoroidic domains—has not hitherto been observed. Here ferrotoroidic domains are spatially resolved by optical second harmonic generation in LiCoPO₄, where they coexist with independent antiferromagnetic domains. Their space- and time-asymmetric nature relates ferrotoroidics to multiferroics with magnetoelectric phase control^{2, 3, 4, 5} and to other systems in which space and time asymmetry leads to possibilities for future applications.

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