SOLUTION —
$ \mathbf{b} \times(\mathbf{a} \times \mathbf{b})=\frac{2}{3} \mathbf{a} \Rightarrow(\mathbf{b} \cdot \mathbf{b}) \mathbf{a}-(\mathbf{b} \cdot \mathbf{a}) \mathbf{b}=\frac{2}{3} \mathbf{a}\\ \Rightarrow \quad \mathbf{a} \cdot \mathbf{b}=0 \Rightarrow \mathbf{a} \perp \mathbf{b}$
So, The correct option of this question will be (C).