Emotion, an essential aspect in inferring human psychological states, is featured by entangled oscillators operating at multiple frequencies and montages. However, the dynamics of mutual interactions among rhythmic activities in EEGs under various emotional expressions are unclear. To this end, a novel method named variational phase-amplitude coupling is proposed to quantify the rhythmic nesting structure in EEGs under emotional processing. The proposed algorithm lies in variational mode decomposition, featured by its robustness to noise artifacts and its merit in avoiding the mode-mixing problem. This novel method reduces the risk of spurious coupling compared to that with ensemble empirical mode decomposition or iterative filter when evaluated by simulations. An atlas of cross-couplings in EEGs under eight emotional processing is established. Mainly, α activity in the anterior frontal region serves as a critical sign for neutral emotional state, whereas γ amplitude seems to be linked with both positive and negative emotional states. Moreover, for those γ-amplitude-related couplings under neutral emotional state, the frontal lobe is associated with lower phase-given frequencies while the central lobe is attached to higher ones. The γ-amplitude-related coupling in EEGs is a promising biomarker for recognizing mental states. We recommend our method as an effective tool in characterizing the entangled multifrequency rhythms in brain signals for emotion neuromodulation.