Attosecond Compression of Relativistic Electron Pulses via Continuous Harmonic Undulator Resonance

Extending megaelectronvolt ultrafast electron diffraction (MeV UED) into the attosecond regime is essential for resolving intrinsic structural dynamics, yet requires simultaneously controlling electron-pulse duration and arrival-time stability. Here, we propose a generalized harmonic laser-electron interaction that extends beam modulation into a continuous harmonic regime. We demonstrate that highly detuned, non-integer harmonic modulation via a single-period undulator achieves stronger coupling efficiency than conventional integer-harmonic resonance. Driven by a mid-infrared seed laser whose wavelength is a small fraction of the nominal resonant wavelength, this mechanism enables effective longitudinal phase space manipulation. It facilitates attosecond compression with minimal laser-induced energy spread, preserving the beam quality required for high-fidelity diffraction. Furthermore, deriving both the modulation and experimental pump lasers from a common source intrinsically locks their relative timing. Simulations demonstrate 680-as pulse durations and 470-as arrival-time jitter, establishing a viable route to attosecond MeV UED for resolving coupled electron-nuclear dynamics.