Abstract
Transition metals, characterised by their partially filled d orbitals, provide the basis for many of the most relevant processes in chemistry, biology, and physics. Embedded as single atoms or in small clusters, they give rise to exceptional optical, chemical, and magnetic properties. So far, it has proven impossible to disentangle the complex network of excited quantum states, which greatly hinders prediction and control of material properties. Here, we apply two-colour resonant four-wave mixing to quantitatively resolve the quantum states of the neutral copper dimer. This allows us to unwind the individual spectral lines by isotopic composition and rotational quantum number and reveals a rich network of bright and perturbing dark states. While this work presents a road map for the experimental study of the bonding between and with transition metal atoms, it also provides experimental reference data for prospective quantum chemical approaches on handling systems with a high density of states.
Highlights
Transition metals, characterised by their partially filled d orbitals, provide the basis for many of the most relevant processes in chemistry, biology, and physics
While catalysis yields products like fertilisers, which are indispensable to feed the current world population[5], the lack of knowledge about the active transition metal sites obstructs the rational design of new catalysts, which are necessary for the transition towards green chemistry[6]
Two-Colour Resonant Four-Wave mixing (TC-RFWM) spectroscopy allows overcoming the hindrances that have so far prevented experimental access to systems exhibiting a high density of states
Summary
Transition metals, characterised by their partially filled d orbitals, provide the basis for many of the most relevant processes in chemistry, biology, and physics. It has been demonstrated that the highest activity, and the largest adjustability of chemical and physical properties, can be found in the quantum size regime, which spans the size range between a single atom[7] and several nanometres[8] In this regime, the partially filled d orbitals of transition metals lead to a very large number of electronic states. Perturbation-induced mixing of energetically close states is abundant Such vibronic coupling, which is neglected in the BornOppenheimer approximation, along with spin–orbit interaction combines with coherence phenomena to enhance function in chemical and biophysical systems[9], but obstructs the understanding of such systems. We provide a solution to this problem by partitioning these spectra into components of defined rotational quantum states, which can be assigned
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