Terahertz Vibrational Molecular Clock with Systematic Uncertainty at the 10^{-14} Level

Abstract

Neutral quantum absorbers in optical lattices have emerged as a leading platform for achieving clocks with exquisite spectroscopic resolution. However, the studies of these clocks and their systematic shifts have so far been limited to atoms. Here, we extend this architecture to an ensemble of diatomic molecules and experimentally realize an accurate lattice clock based on pure molecular vibration. We evaluate the leading systematics, including the characterization of nonlinear trap-induced light shifts, achieving a total systematic uncertainty of 4.6×10^{-14}. The absolute frequency of the vibrational splitting is measured to be 31 825 183 207 592.8(5.1) Hz, enabling the dissociation energy of our molecule to be determined with record accuracy. Our results represent an important milestone in molecular spectroscopy and THz-frequency standards, and may be generalized to other neutral molecular species with applications for fundamental physics, including tests of molecular quantum electrodynamics and the search for new interactions.