Fluctuation dynamics of a single magnetic chain Adriana S. Silva, 1 Robert Bond, 1 Franck Plouraboue ´ , 2 and Denis Wirtz 1, * 1 Department of Chemical Engineering, The Johns Hopkins University, 3400 North Charles Street, Baltimore, Maryland 21218 2 Ecole Supe ´rieure de Physique et Chimie Industrielle de la Ville de Paris, Laboratoire PMMH, 10 rue Vauquelin, F-75231 Paris Cedex, France Received 27 March 1996 ‘‘Tunable’’ fluids such as magnetorheological MRand electrorheological ERfluids are comprised of paramagnetic or dielectric particles suspended in a low-viscosity liquid. Upon the application of a magnetic or electric field, these fluids display a dramatic, reversible, and rapid increase of the viscosity. This change in viscosity can, in fact, be tuned by varying the applied field, hence the name ‘‘tunable fluids.’’ This effect is due to longitudinal aggregation of the particles into chains in the direction of the applied field and the subsequent lateral aggregation into larger semisolid domains. A recent theoretical model by Halsey and Toor HTex- plains chain aggregation in dipolar fluids by a fluctuation-mediated long-range interaction between chains and predicts that this interaction will be equally efficient at all applied fields. This paper describes video- microscopy observations of long, isolated magnetic chains that test HT theory. The measurements show that, in contrast to the HT theory, chain aggregation occurs more efficiently at higher magnetic field strength ( H 0 ) and that this efficiency scales as H 0 1/2 . Our experiments also yield the steady-state and time-dependent fluc- tuation spectra C ( x , x ' ) [ h ( x ) -h ( x ' )] 2 1/2 and C ( x , x ' , t , t ' ) [ h ( x , t ) -h ( x ' , t ' )] 2 1/2 for the instanta- neous deviation h ( x , t ) from an axis parallel to the field direction to a point x on the chain. Results show that the steady-state fluctuation growth is similar to a biased random walk with respect to the interspacing | x -x ' | along the chain, C ( x , x ' ) | x -x ' | , with a roughness exponent =0.530.02. This result is partially con- firmed by Monte Carlo simulations. Time-dependent results also show that chain relaxation is slowed down with respect to classical Brownian diffusion due to the magnetic chain connectivity, C ( x , x ' , t , t ' ) | t -t ' | , with a growth exponent =0.350.05 1 2 . All data can be collapsed onto a single curve according to C ( x , x ' , t , t ' ) | x -x ' | ( | t -t ' | / | x -x ' | z ), with a dynamic exponent z =/ 1.42. S1063-651X9613911-8 PACS numbers: 47.50.+d, 83.80.Gv, 83.20.Jp I. INTRODUCTION Over the past decade, a great deal of attention has been focused on the development of a new class of fluids, termed ‘‘tunable’’ fluids 1,2. Electrorheological ERand magne- torheological MRfluids belong to this class. These fluids offer the promise of fast-response devices, which would ef- ficiently interface mechanical components with electronic controls. Advantages of such devices include fast switching speed, miniaturization, and continuously variable control. The inherent value of these materials lies in their ability to quickly and reversibly change from a liquidlike state to a semisolid state when subjected to an electric or magnetic field, with a response time on the order of a few milliseconds 3. This rapid ‘‘tunable’’ phase transition induces a rapid and drastic increase of the fluid viscosity 4. ER fluids are comprised of fine dielectric particles im- mersed in a medium of different dielectric constant i.e., sili- cone oil, water3. Due to particle chaining in the direction of the applied electric field, the fluid undergoes a change in viscosity 3,4. The development of ER fluids dates back to the 1940s, with the original work by Winslow 5. The sys- tem used was comprised of an ER fluid based on dispersed, moist silica gel. Winslow observed that, upon application of an electric field, particles suspended in oil formed fibrous structures aligned with the field. In addition, working with field strengths on the order of 3 kV/mm, he determined that the shear stress [ ( E ) -(0)] was dependent on the square of the applied voltage. Winslow postulated many applica- tions of ER fluids and described their use in clutches, brakes, and valves 3. After a brief period of intense interest, work in the field dwindled for almost 30 years. The next extensive work was carried out by Klass and Martinek 6,7, who reported their results from ER fluids comprised of silica and calcium titan- ate. In two landmark papers 6,7, these authors described the ( E ) -interdependence and how shear stress is ef- fected by several variables such as electric field strength ( E ), frequency ( f ), fluid composition , temperature ( T ), and shear rate ˙ . Klass and Martinek 7also presented bulk conductance measurements of the fluid as a whole and the consequent power demand of these typical ER systems under use. Our work focuses on the magnetic analogs of ER fluids, which are termed magnetorheological fluids MR fluids. Similar to ER fluids in many respects, MR fluids exhibit several key differences, among which are the absence of charge, higher strength, better stability over broader tempera- ture range, and less stringent manufacturing requirements 1. In addition, MR fluids are experimentally easier to work with as several potential difficulties are avoided such as elec- trode polarization and direct contact with the fluid. MR flu- ids, therefore, constitute model ‘‘tunable’’ fluids with prop- *Author to whom correspondence should be addressed. PHYSICAL REVIEW E NOVEMBER 1996 VOLUME 54, NUMBER 5 54 1063-651X/96/545/55029/$10.00 5502 © 1996 The American Physical Society