Temperature dependence of three-point correlation functions of viscous liquids: the case of glycerol

What causes the dramatic slowing down of flow and relaxation that leads to glass formation in liquids as temperature decreases is hardly understood so far and is the subject of intensive research work. It is tempting to ascribe the strong temperature dependence of the dynamics, irrespective of molecular details, to a collective or cooperative behavior characterized by a length scale that grows as one approaches the glass transition. To access this length experimentally, we use the recently introduced three-point dynamic susceptibility, from which the number of molecules dynamically correlated during the structural relaxation, N-corr, can be extracted. The three-point functions are related to the sensitivity of the averaged two-time dynamics to external control parameters, such as temperature and density. We studied Ncorr values in an important temperature range for a large number of liquids, and found that it systematically grows when approaching the glass transition. Here we specially emphasize the case of glycerol for which we combined dielectric and neutron spin echo spectroscopy to cover more than 16 decades in relaxation time.