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The notion of ``conformal sets'' of aromatic and other conjugated compounds is introduced. To a good approximation, it is found that the sum of the heats of combustion of the compounds in one set equals the sum for the compounds in the other set. Similar additivity occurs for their LCAO‐calculated total π‐electron energies, LCAO bond orders and free valences. Bond lengths and dissociation energies are also considered. Conformal sets are defined in terms of their number and quality of self‐returning random walks on the atoms of the conjugated compounds. Even‐electron nonalternant and alternant compounds are included, as are, in certain cases, radicals. Some insight into the additivity for LCAO properties is obtained by relating the coefficients in LCAO secular equations to random walks and using contour integral formulas connecting LCAO properties with secular determinants.

Additivity of Heats of Combustion, LCAO Resonance Energies, and Bond Orders of Conformal Sets of Conjugated Compounds