H 2 Molecule / Vibrationally Excited / 2+1 REMPI / Rotational AnisotropyWe report the spectroscopic detection of vibrationally excited molecular hydrogen using 2ϩ1 resonantly enhanced multiphoton ionization (REMPI) via the I 1 Π g (v′ ϭ 0) Ϫ X 1 Σ ϩ g (v″ ϭ 3) band ca. 198 nm. Vibrationally excited H 2 was produced by passing roomtemperature hydrogen over a hot ion gauge filament in a high-vacuum chamber. The internal energy distributions were characterized spectroscopically by use of the EF 1 Σ ϩ g ϪX 1 Σ ϩ g 2ϩ1 REMPI detection scheme. We have identified band origins for the S, Q, R, and P rotational branches of the I-X (0,3) band, as well as isolated lines corresponding to two-photon transitions into other nearby H 2 gerade states, including EF 1 Σ ϩ g (v′ ϭ 2, 3, 4), GK 1 Σ ϩ g (v′ ϭ 1), and J 1 ∆g (v′ ϭ 0). We propose the I-X transition as a suitable candidate for the determination of the rotational anisotropy of vibrationally excited ground-state H2 molecules. We support this contention with a calculation of the line strength moments and sensitivities to the second-(quadrupolar) and fourth-rank (hexadecapolar) moments of the rotational angular momentum distributions, which is compared against the well-established Q-branch members of the EF 1 Σ ϩ g ϪX 1 Σ ϩ g two-photon transition.