Retrieving Angular Distributions of High-Order Harmonic Generation from a Single Molecule

We present a novel method to retrieve angular distributions of high-order harmonic generation from a single molecule. This technique uses an iterative procedure based only on experimental results of time and angle-dependent harmonic signals, and no actual shape of molecular orbital is assumed. The molecular axis distribution in a target gas can simultaneously be deduced in this procedure. The angle-dependent signal retrieved for a single N-2 and O-2 molecule is demonstrated to reflect the highest occupied molecular orbital, excluding the ambiguity due to the imperfect alignment.