An asymmetric mechanism for correlated motion occurring in noninteracting pairs of adjacent orthogonal 1,4-bis(carboxyethynyl)bicyclo[1.1.1]pentane (BCP) rotators 1 in the solid state is unraveled and shown to play an important role in understanding the dynamics in the crystalline rotor, Bu4N+[1-]·H2O. Single crystal X-ray diffraction and calculation of rotor-rotor interaction energies combined with variable-temperature, variable-field 1H spin-lattice relaxation experiments led to the identification and microscopic rationalization of two distinct relaxation processes.

Departament de Química Física i Inorgànica Universitat Rovira i Virgili Marcel·lí Domingo 1 43007 Tarragona Spain

Department of Chemistry and Biochemistry University of Colorado Boulder Boulder Colorado 80309 0215 United States

Institut de Ciència de Materials de Barcelona Campus de la UAB 08193 Bellaterra Spain

Institute of Organic Chemistry and Biochemistry Academy of Sciences of the Czech Republic Flemingovo nam 2 Prague 6 16610 Prague Czech Republic

Laboratoire de Physique des Solides CNRS and Université de Paris Sud 91405 Orsay France

Laboratoire MOLTECH Anjou CNRS UMR 6200 Université d'Angers 49045 Angers France

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Chlorinated Cubane-1,4-dicarboxylic Acids