Although the frequency shift and odd-even intensity modulation in high-order harmonic generation (HHG) have both been observed for asymmetric laser-target systems, they are typically studied as two separate effects. In this Letter we provide a comprehensive picture of these two nonlinear optical phenomena, unifying them through a common origin: asymmetry of the laser-target system. By tuning asymmetric laser-target systems, we discover a transition from the harmonic frequency shift to the odd-even intensity modulation upon increasing the duration of the driving laser pulse. Specifically, these phenomena are observed simultaneously for laser pulses with intermediate pulse duration. For numerical evidence, we solve the time-dependent Schrödinger equation, while insight into the underlying physics is obtained from a simplified analytically tractable model. Understanding the asymmetric characteristics reflected in the HHG as provided is crucial for retrieving laser-target information, sampling external fields, and probing molecular dynamics.

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• High-order harmonic generation
• Light-matter interaction
• Nonlinear optics