Control of molecular ultracold plasma relaxation dynamics by mm-wave Rydberg-Rydberg transitions

Resonant mm-wave fields drive $n_0f(2) \rightarrow (n_0 \pm 1)g(2)$ transitions in a state-selected $n_0f(2)$ Rydberg gas of NO. This transformation produces a clear signature in the selected field ionization spectrum and dramatically increases the intensity of corresponding features in the spectrum of the $n_0f(2)$ Rydberg series observed in UV-UV double resonant transitions via the $A ~^2\Sigma^+, ~N'=0$ state. Here, $n_0$ refers to the principal quantum number of an $f$ Rydberg state converging to the $N^+=2$ rotational state of NO$^+ X~ ^1\Sigma^+$. Enhancement owing to transitions from $\ell=3$ ($f$) to $\ell=4$ ($g$) appears both in the electron signal detected at early time by the field ionization of Rydberg molecules and, 40 $\mu$s later, as the late-peak signal of plasma in a state of arrested relaxation. Similar stabilization and enhanced intensity also occurs for shorter-lived interloping complex resonances, $44p(0) - 43d(1)$ and $43p(0) - 42d(1)$. We conclude from these observations that avalanche alone does not guarantee a plasma state of arrested relaxation. But rather, the formation of an arrested phase requires both avalanche-produced NO$^+$ ions and a persistent population of long-lived Rydberg molecules.