The dynamical behavior of small particles has been observed by high resolution electron microscopy. Spontaneous structural fluctuations, between various orientations, were observed and quantified. Clear transitions involving appearance and vanishing of twins were detected. Measurements of the angle change between succeeding configurations of the ͗111͘ atomic plane reveal the existence of several preferred angular changes. Twin related transformations give a good fit to the observed angular correlation, which excludes complete particle melting during the transition between successive configurations. It was also found that the particles rotate by a few degrees during this transformation.[S0031-9007(97)02816-0] PACS numbers: 61.46.+w, 61.16.Bg, 61.72.Mm, 63.90.+t The structure of atomic clusters is interesting because they present a state of matter that is intermediate between single atoms and the bulk state. In ultrafine particles ͑R , 10 nm͒, new phenomena may be expected, especially due to the high ratio between surface area and volume.Previous studies performed on small particles revealed a structure which is characterized by multiple twinned domains in many fcc metals [1-3].High resolution electron microscopy (HREM) studies in ultrafine particles revealed instability in the particles structure [4] which was defined as quasimelting phenomenon. A comprehensive review on the structure and instability of small clusters has been presented by Marks [5]. Several models were proposed to explain the dynamical evolution in the cluster structure. These models can be divided into two categories. The first one relates the restructuring of the particle to a short but complete melting period, followed by recrystallization of a new structure [6][7][8]. The second approach suggests that due to the small energy barrier between the various particle configurations, there can be random fluctuations between the different structures without melting [9].Previous study of lead particles reveals a definite range of particle size in which the structure is unstable, while in the solid state [10]. In this Letter, we report the first quantitative analysis of the fluctuations which occur in lead particles. This analysis reveals a definite angular correlation between successive structures.The samples are lead particles embedded in an amorphous SiO matrix. The samples were prepared by successive evaporation of 10 nm of SiO, 5 nm of Pb, 10 nm of SiO on a copper grid covered by a thin film of carbon. The embedded case ensures better thermal coupling, which defines good thermodynamical variables and prevents oxidation, migration, and evaporation [11]. During deposition, the substrate was held at a temperature of 200 ± C, causing the particles to coalesce in the liquid state, and resulting in an equilibrium spherical shape. The specimens were observed at room temperature in a HREM (JEOL 4000-EX) at 400 kV. The structure evolution of the particles was video recorded via a low level video CCD camera with a time resolution of 25 frames͞sec. The re...