Absolute measurement of enhanced fluctuations in assemblies of biomolecules by ultrasonic techniques

By expressing the fluctuation-dissipation theorem explicitly, equations are obtained for the ultrasonic relaxation amplitudes that contain one single molecular parameter, i.e., the fluctuation, or the sum of fluctuations. The absolute measurement of this parameter is therefore possible. The equations apply to a two-state system, to a multistate system and to a linear Ising chain as well. In an aqueous medium, where molar volume changes are important, the ultrasonic relaxation amplitudes are proportional to the volume fluctuations. For assemblies of biomolecules that exhibit enhanced ultrasonic absorption on assembly it is possible to measure the increase on assembly of the sum of fluctuations. In view of application to tobacco mosaic virus protein aggregates, examples are given in which the fluctuations associated with two normal modes of relaxation are equally enhanced when the difference of conformational stability of the states is reduced. The corresponding observable changes of the ultrasonic spectra are described.