We theoretically discover purely electronic polarization modes in THz frequency region in dimer Mott insulators κ-(BEDT-TTF)2X. The unusual low-frequency modes arise from the coupling between the oscillation of intradimer electric dipole moments and that of alternating interdimer bond orders. These collective motions play an important role in the dynamical dielectric properties of the dimer Mott insulators. Near the phase boundary of the dimer Mott transition, the ferroelectric ground state is realized by introducing electron-lattice coupling.PACS numbers: 71.30.+h, 78.30.Jw Low-dimensional strongly correlated electron systems with a quarter-filled band have recently attracted much attention. BEDT-TTF salts are typical two-dimensional systems with anisotropic triangular lattices, and the strong correlation and frustration act cooperatively to generate exotic phases. Among the BEDT-TTF salts, κ-(BEDT-TTF) 2 X (X: a counter anion) exhibit the Mott insulator phase [1][2][3][4][5], exotic superconducting phase [6], spin liquid phase [7][8][9], and so on. The BEDT-TTF molecular lattice is distorted to form dimers in κ-(BEDT-TTF) 2 X. Hybridized two sites can be effectively treated as a single site, and the valence band is regarded as a half-filled one. As a result, κ-(BEDT-TTF) 2 X exhibits the Mott insulator phase if the effective on-site Coulomb energy is large enough. The state is called the dimer Mott insulator.Recently quite interesting charge excitation phenomena have been observed in the dimer Mott insulators: photoinduced phase transition to a metallic state [10], and anomaly in dielectric properties [11]. In particular, the latter suggests that low-energy charge excitation exists in the dimer Mott insulators in contrast to the case of the Mott insulators.In this letter, we show for the first time that the dimer Mott insulator has THz electric polarization, which purely arises from the electron dynamics. The ferroelectricity which arises from the electron dynamics has been observed in some materials, and these ferroelectrics have unconventional origins such as charge order generation [12][13][14][15][16]. We propose another new origin of ferroelectricity in this paper.We adopt the 1/4-filled extended Hubbard Hamiltonian for holes on the two-dimensional anisotropic triangular lattice, which includes the degrees of freedom in a dimer. It is given by H = (β n,mpn,m + V n,m n n n m ) + U n n n,↑ n n,↓ , (1) where < n, m > denotes the neighbor site pairs, c n,σ (c † n,σ ) is the annihilation (creation) operator for a hole of spin σ at the site n, β n,m (V n,m ) is the transfer integral (the Coulomb interaction energy) between the sites n and m,p n,m = σ (c † m,σ c n,σ + c † n,σ c m,σ ), U is the on-site Coulomb interaction energy, n n,σ = c † n,σ c n,σ , and n n = σ n n,σ . The 4 × 4 cluster of the system size N = 16 with the periodic boundary condition is used.We calculate the quantum state excited by light pulse expressed by the vector potential A(t) = eA exp(−(t/D)2 ) cos(ω p t) of a Gaussian profile....