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Abstract

Ultracold diatomic molecules have achieved significant breakthroughs in recent years, enabling the exploration of quantum chemistry, precision measurements, and strongly correlated many-body physics. Extending ultracold molecular complexity to polyatomic molecules, such as triatomic and tetratomic molecules, has attracted considerable interest. However, the realization of ultracold polyatomic molecules remains technically challenging due to their complex energy-level structures. While only a few experiments have successfully demonstrated the formation of polyatomic molecules by magnetoassociation or electroassociation, here we present the first step toward producing tetratomic molecules through the development of a microwave association technique combined with microwave dressing. When the two lowest rotational states of the molecules are dressed by a microwave field, weakly bound tetramer states emerge in the entrance channel with free dark excited states $\ket{0}$ and a dressed state $\ket{+}$. The spectroscopy of these weakly bound tetramers is probed by another microwave field that drives transitions from the populated dressed states $\ket{+}$. By precisely discriminating the complex hyperfine structure of the dark excited level $\ket{0}$ from the dressed-state spectroscopy, the binding energy of the tetratomic molecules is measured and characterized. Our work contributes to the understanding of complex few-body physics within a system of microwave-dressed molecules and may open an avenue toward the creation and control of ultracold polyatomic molecules.