Ultrafast ps--TALIF and streak camera diagnostics of atomic hydrogen in a helium microplasma jet

Abstract: Picosecond two-photon absorption laser induced fluorescence (ps--TALIF) is combined with a streak camera ($\sim$1 ps highest temporal resolution) to probe the effective lifetime ($\tau_{eff_{H(n=3)}}$) and absolute density ($N_H$) of atomic hydrogen in the effluent of a helium atmospheric-pressure microplasma jet ($\mu$APPJ). This approach allows for improved temporal resolution compared to conventional nanosecond diagnostics, enabling measurements of $\tau_{eff_{H(n=3)}}$ as small as 50 ps, the corresponding $N_H$ reaching down to $10^{14} cm^{-3}$. Atomic densities are calibrated by performing identical ps--TALIF measurements in krypton gas contained in a custom-built low-pressure cuvette. Physical mechanisms that may be involved in the TALIF scheme such as photoionisation and/or stimulated emission are also assessed, ensuring reliable studies. The determined $\tau_{eff_{H(n=3)}}$ and $N_H$ increase with the helium flow rate ($Q_{He}$) in the range $Q_{He}=0.3-1$ slm. Both quantities are maximized near the exit nozzle of the $\mu$APPJ, obtaining values below 400 ps and $6x10^{14} cm^{-3}$, respectively. As the axial distance increases, $\tau_{eff_{H(n=3)}}$ declines with a rate of $\approx$65 ps/mm for $Q_{He}=1$ slm which is about 3 times smaller than for $Q_{He}=0.3$ slm. These findings reveal a strong correlation between the experimentally-measured $\tau_{eff_{H(n=3)}}$ and the local air entrainment into the jet as indicated by their comparison with calculated effective lifetimes based on published quenching rates. Furthermore, operating the $\mu$APPJ in the burst mode allows for the estimation of the residence time ($t_{res}$) of ground state H--atoms in the helium gas channel, which is larger for $Q_{He}=0.3$ slm ($t_{res} \approx 1.2 ms$) compared to $Q_{He}=1$ slm ($t_{res} \approx 0.5 ms$). H-atoms consumption in the gas channel can be affected by diffusion and mechanisms involving neutral ground-state and metastable species among others. Furthermore, based on an error propagation analysis, density uncertainty as high as 64% (depending on the operating condition) is revealed. This mainly originates in the ratio of the two-photon absorption cross sections of Kr and H atoms ( $\sigma^{(2)}Kr$ / $\sigma^{(2)}H$) which has not yet been measured in the picosecond regime. Nevertheless, the combined utilisation of ps--TALIF and streak camera diagnostics demonstrates high sensitivity and temporal resolution for directly probing key reactive species in atmospheric pressure microplasmas.