Neutral Barium in Solid Neon: Optical Spectroscopy and First Excited State Lifetime

TL;DR

This study investigates neutral barium atoms in solid neon using optical spectroscopy, measuring energy level shifts, linewidths, and the first lifetime of the 5d6s 3D1 state, advancing the understanding for electron dipole moment experiments.

Contribution

It provides the first lifetime measurement of barium's 5d6s 3D1 state in neon and explores matrix-induced effects on barium energy levels and relaxation channels.

Findings

Measured the 5d6s 3D1 state lifetime as 0.39 ± 0.02 s in neon.

Observed matrix-induced shifts and linewidths of barium energy levels.

Confirmed multiple radiative pathways and relaxation channels in neon matrices.

Abstract

Matrix isolation spectroscopy enables probing atomic properties in controlled cryogenic environments. We present a spectroscopic study on neutral barium atoms embedded in a neon cryogenic crystal at 6.8 K, extending previous investigations performed in other noble gas hosts. The visible and near-infrared emission spectra were recorded under two different laser excitation schemes. First, 10-ns laser pulses at 355 nm were used to directly excite high-lying energy levels of barium, enabling the observation of fluorescence cascades. Second, a tunable continuous-wave laser operating between 700 nm and 900 nm allowed us to determine the matrix-induced shifts of barium energy levels relative to their vacuum values, as well as the inhomogeneous linewidths of the observed transitions and to perform lifetime measurements. Our results confirm multiple radiative pathways and matrix-induced relaxation channels affecting the 5d6s and 6s6p barium manifolds. Furthermore, we present the first lifetime measurement of the barium 5d6s 3D1 state in a neon crystal, yielding 0.39 \pm 0.02 s, with a predicted increase of about 10% at 2 K. The study of fluorescence and spectroscopic properties of barium isolated in neon represents an important step toward future searches for the electron electric dipole moment using barium monofluoride in neon matrices, where neutral barium atoms may act as unavoidable impurities and potential sources of background and systematic limitations.