Electromagnetic wave emission based on optical rectification at terahertz (THz) wavelengths was observed from surface-immobilized gold nanospheres (SIGNs) above a gold surface. Although the excitation wavelength is offresonant with the localized surface plasmons, the THz emission field was observed to be approximately 4.8 times greater than that from a percolated gold thin film of 10 nm thickness. A theoretical calculation predicts that the light electric field is enhanced in the SIGN system, even at off-resonance wavelengths. The observed THz field amplitude was quadratic with the illumination light field, suggesting that the THz generation is due to a second-order nonlinear optical process. showed THz generation at gold and silver surfaces [3]. A metallic surface shows second-order NLO activity because of the lack of an inversion center near the surface. Later they reported OR-based THz generation in thick metal films (100-200 nm thick), and attributed the optical nonlinearity to nonlocal effects [4]. On the other hand, Ramakrishnan and Planken have reported THz emission from a thin percolated gold film of 10 nm thickness, having localized surface plasmon (LSP) hot spots [5]. Recently Ramakrishnan et al. observed THz emission from ordered NLO chromophores in a molecular monolayer at the surface plasmon resonance condition [6]. In these studies, the THz emission amplitude is quadratic in the excitation field, suggesting that the THz emission is based on the second-order NLO process. On the contrary, Welsh et al. [7] and Polyushkin et al.[8] observed a non-quadratic dependence of the THz emission amplitude on the incident electric field. They attributed the THz emission from the metallic surface to multiphoton ionization and ponderomotive acceleration of electrons in the evanescent field produced by surface plasmons. This process may be called gindirect OR. These different observations suggest that different THz generation mechanisms are possible at gold surfaces.In this letter, we report THz emission from surfaceimmobilized gold nanospheres (SIGNs) above a gold surface with a gap distance of less than 1 nm. The SIGN structure is schematically illustrated in Fig. 1(a). The gap between the SIGN and the surface is supported by an aminoundecanethiol (AUT) self-assembled monolayer (SAM). The SIGNs show an intense resonance of LSPs, as a result of the EM interaction between the SIGNs and the gold surface [9][10][11][12][13]. Second-order NLO optical phenomena, second-harmonic generation (SHG) [10,11], OR and the Pockels effect [12], have been observed from the SIGNs, since the SIGN structure is noncentrosymmetric. Here, THz emission was observed from the SIGNs and its amplitude was found to be quadratic in the excitation field amplitude. This indicates that the THz generation is due to a second-order NLO process.The SIGN sample was prepared by the following procedure: As a substrate, a 100 nm thick thin gold film was vacuum-evaporated on a glass slide. The surface was covered with an AUT SAM, by dipping the gold subs...