We propose an ultrafast way to generate spin chirality and spin current in a class of multiferroic magnets using a terahertz circularly polarized laser. Using the Floquet formalism for periodically driven systems, we show that it is possible to dynamically control the Dzyaloshinskii-Moriya interaction in materials with magnetoelectric coupling. This is supported by numerical calculations, by which additional resonant phenomena are found. Specifically, when a static magnetic field is applied in addition to the circularly polarized laser, a large resonant enhancement of spin chirality is observed resembling the electron spin resonance. Spin current is generated when the laser is spatially modulated by chiral plasmonic structures and could be detected using optospintronic devices. DOI: 10.1103/PhysRevLett.117.147202 Introduction.-Control of emergent collective phenomena by external fields is an important problem in condensed matter. Multiferroic magnets (for a review, see Refs. [1][2][3]) are opening new possibilities in this direction since the local spins are coupled not only to magnetic fields but to electric fields through the magnetoelectric (ME) coupling. Laser control of materials is attracting interest with a goal of realizing ultrafast and noncontact manipulation [4][5][6][7][8][9][10][11][12][13][14]. In the research community of magnetic systems, control of magnetism using a laser is being studied in the context of spin-pumping and spintronics [4][5][6][7]. On the other hand, in the field of electronic systems, periodically driven quantum systems draw the interest of many researchers. When the Hamiltonian is time periodic, the system can be described by the so-called Floquet states [15,16], a temporal analog of the Bloch states, and it is possible to control their quantum nature. For noninteracting systems, the control of the band topology has been studied theoretically [8][9][10] and experimentally [13,14]. It is possible to understand the effect of a laser through a mapping from the time-dependent Hamiltonian to a static effective Hamiltonian using the Floquet theory, and the change of quantum state, e.g., topology and symmetry, is attributed to the emergent terms in the static effective Hamiltonian. This framework can also be applied to quantum magnets. Laser-induced magnetization growth in general quantum magnets [17,18] as well as laser-driven topological spin states [18,19], a quantum spin versions of Floquet topological insulators, were proposed recently.In the current work, we apply the Floquet theory to quantum multiferroics and study the synthetic interactions appearing in the effective Floquet Hamiltonian