Enhanced molecular orientation via NIR-delay-THz scheme: Experimental results at room temperature.

Light-induced orientation of gas phase molecules is a long-pursued goal in physics and chemistry. Here, we experimentally demonstrate a six-fold increase in the terahertz-induced orientation of iodomethane (CHI) molecules at room temperature, provided by rotational pre-excitation with a moderately intense near-IR pulse. The paper highlights the underlying interference of multiple coherent transition pathways within the rotational coherence manifold and is analyzed accordingly. Our experimental and theoretical results provide desirable and practical means for all-optical experiments on oriented molecular ensembles.