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Creators/Authors contains: "Zare, Richard N."

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  1. Free, publicly-accessible full text available February 1, 2024
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  5. Interference observed in a double-slit experiment most conclusively demonstrates the wave properties of particles. We construct a quantum mechanical double-slit interferometer by rovibrationally exciting molecular deuterium (D 2 ) in a biaxial ( v = 2, j = 2) state using Stark-induced adiabatic Raman passage, where v and j represent the vibrational and rotational quantum numbers, respectively. In D 2 ( v = 2, j = 2) → D 2 ( v = 2, j ′ = 0) rotational relaxation via a cold collision with ground state helium, the two coherently coupled bond axis orientations in the biaxial state act as two slits that generate two indistinguishable quantum mechanical pathways connecting initial and final states of the colliding system. The interference disappears when we decouple the two orientations of the bond axis by separately constructing the uniaxial states of D 2 , unequivocally establishing the double-slit action of the biaxial state. This double slit opens new possibilities in the coherent control of molecular collisions.
  6. Although synthetic organic electrochemistry (EC) has advanced significantly, net redox neutral electrosynthesis is quite rare. Two approaches have been employed to achieve this type of electrosynthesis. One relies on turnover of the product by the reactant in a chain mechanism. The other involves both oxidation on the anode and reduction on the cathode in which the radical cation or the radical anion of the product has to migrate between two electrodes. Herein, a home-built electrochemistry/mass spectrometry (EC/MS) platform was used to generate an N -cyclopropylaniline radical cation electrochemically and to monitor its reactivity toward alkenes by mass spectrometry (MS), which led to the discovery of a new redox neutral reaction of intermolecular [3 + 2] annulation of N -cyclopropylanilines and alkenes to provide an aniline-substituted 5-membered carbocycle via direct electrolysis (yield up to 81%). A chain mechanism, involving the regeneration of the substrate radical cation and the formation of the neutral product, is shown to be responsible for promoting such a redox neutral annulation reaction, as supported by experimental evidence of EC/MS.