We demonstrate a high-efficiency intermodal four-wave-mixing process in an all-fiber system, comprising a picosecond fiber laser and a high-order-mode (HOM) fiber. Two pump photons in the LP 01 mode of the fiber can generate an anti-Stokes photon in the LP 01 mode and a Stokes photon in the LP 02 mode. The wavelength dependent mode profiles of the HOM fiber produce significant spatial overlap between the modes involved. The anti-Stokes wave at 941 nm is generated with 20% conversion efficiency with input pulse energy of 20 nJ. The guidance of the anti-Stokes and Stokes waves in the HOM fiber enhances system stability. V C 2012 American Institute of Physics.[http://dx.doi.org/10.1063/1.4759038] Four-wave mixing (FWM) in optical fibers has been utilized for nonlinear frequency conversion. FWM has been studied in single-mode fibers, multimode fibers, and more recently, photonic crystal fibers (PCFs). [1][2][3][4][5][6][7][8] In most experiments, the red-shifted Stokes wave and the blue-shifted antiStokes wave are generated within the same mode as the pump light. In these cases, the phase-matching conditions require the pump to be in the vicinity of the zero dispersion wavelength (ZDW) of the propagating mode. 8,9 However, launching high power pump light near the ZDW can easily generate a supercontinuum (SC), which limits the conversion efficiency from the pump to the narrow-band Stokes and anti-Stokes waves. 10 High-efficiency FWM generation at 673 nm and 2539 nm has been achieved in an endlessly single-mode large-mode-area (LMA) PCF without having the pump light close to the ZDW. 11 However, this approach cannot be extended to generate light at other wavelengths, since the phase-matching condition is predominantly defined by the material dispersion. To overcome the limitation of FWM within a single spatial mode, an intermodal FWM approach has been proposed. 12 In this approach, pump light is launched in the normal dispersion region of the fundamental mode. The Stokes and the anti-Stokes waves can satisfy the phase-matching condition by propagating in other higher-order-modes (HOMs). This effect has been observed in conventional and Ge-doped multimode fibers at visible wavelengths, using a high power pump at 532 nm. 3,4 Recently, the effect has been studied more systematically in PCFs. [12][13][14] Intermodal FWM has several advantages over traditional single-mode FWM. This method can achieve high conversion efficiency without SC generation. 12 The wavelength of the Stokes and anti-Stokes light can be easily controlled by fiber design, such as changing the core diameter. 4,13 More importantly, intermodal FWM provides extra degrees of freedom, thus increased flexibility, in fiber designs to generate FWM, because the phase-matching condition can be fulfilled with more than one propagating mode. However, intermodal FWM demonstrations so far require a high-power laser source, such as a Q-switched Nd:YAG laser or a Ti:Sapphire regenerative amplifier. As a result, they are typically used to generate light with high pulse...