Developing molecular circuits that can function as the active components in electrical devices is an ongoing challenge in molecular electronics. It demands mechanical stability of the single-molecule circuit while simultaneously being responsive to external stimuli mimicking the operation of conventional electronic components. Here, we report single-molecule circuits based on spiropyran derivatives that respond electrically to chemical and mechanical stimuli. The merocyanine that results from the protonation/ ring-opening of the spiropyran form showed single-molecule diode characteristics, with an average current rectification ratio of 5 at ±1 V, favoring the orientation where the positively charged end of the molecule is attached to the negative terminal of the circuit. Mechanical pulling of a single spiropyran molecule drives a switch to a more conducting merocyanine state. The mechanical switching is enabled by the strong Au−C covalent bonding between the molecule and the electrodes, which allows the tensile force delivered by the STM piezo to break the molecule at its spiropyran C−O bond.
An open-cage fullerene incorporating phosphorous ylid and carbonyl group moieties on the rim of the orifice can be filled with gases (H 2 ,He, Ne) in the solid state,and the cage opening then contracted in situ by raising the temperature to complete an intramolecular Wittig reaction, trapping the atom or molecule inside.K nown transformations complete conversion of the product fullerene to C 60 containing the endohedral species.A sw ell as providing an improved synthesis of large quantities of 4 He@C 60 ,H 2 @C 60 ,and D 2 @C 60 ,the method allows the efficient incorporation of expensive gases such as HD and 3 He,t op repare HD@C 60 and 3 He@C 60 .T he method also enables the first synthesis of Ne@C 60 by molecular surgery,and its characterization by crystallography and 13 CNMR spectroscopy.
The interactions between atoms and molecules may be described by a potential energy function of the nuclear coordinates. Nonbonded interactions between neutral atoms or molecules are dominated by repulsive forces at a short range and attractive dispersion forces at a medium range. Experimental data on the detailed interaction potentials for nonbonded interatomic and intermolecular forces are scarce. Here, we use terahertz spectroscopy and inelastic neutron scattering to determine the potential energy function for the nonbonded interaction between single He atoms and encapsulating C 60 fullerene cages in the helium endofullerenes 3 He@C 60 and 4 He@C 60 , synthesized by molecular surgery techniques. The experimentally derived potential is compared to estimates from quantum chemistry calculations and from sums of empirical two-body potentials.
Synthesis of Ar@C60 is described, using a route in which high-pressure argon filling of an open-fullerene and photochemical desulfinylation are the key steps for >95% encapsulation of the noble gas....
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