Diffusing-Light Spectroscopies Beyond the Diffusion Limit: The Role of Ballistic Transport and Anisotropic Scattering

Diffuse transmission and diffusing-wave spectroscopy (DWS) can be used to probe the structure and dynamics of opaque materials such as colloids, foams, and sand. A crucial step is to model photon transport as a diffusion process. This approach is acceptable for optically thick samples, far into the limit of strong multiple scattering; however, it becomes increasingly inaccurate for thinner samples for several reasons. Here, we correct for two of these defects. By modeling photon propagation by a telegrapher equation with suitable boundary conditions, we can account for the ballistic transport of photons at finite speed between successive scattering events. By introducing a discontinuity in the photon concentration at the source point, and then averaging over a range of penetration depths, we can account for the fact that photons usually scatter anisotropically into the forward direction, rather than being completely randomized at each event. The accuracy of our approach is tested by comparison both with random walk computer simulations and with experiments on specially designed suspensions of polystyrene spheres. We find that our predictions extend the utility of diffuse transmission to slabs of all thicknesses and of DWS to slabs down to about two transport mean free paths. Disciplines Physical Sciences and Mathematics | Physics Comments At the time of publication, author Douglas J. Durian was affiliated with University of California, Los Angeles. Currently, he is a faculty member at the Physics Department at the University of Pennsylvania. This journal article is available at ScholarlyCommons: https://repository.upenn.edu/physics_papers/624 Diffusing-light spectroscopies beyond the diffusion limit: The role of ballistic transport and anisotropic scattering P.-A. Lemieux, M. U. Vera, and D. J. Durian Department of Physics and Astronomy, University of California, Los Angeles, California 90095-1547 ~Received 14 October 1997 ! Diffuse transmission and diffusing-wave spectroscopy ~DWS! can be used to probe the structure and dynamics of opaque materials such as colloids, foams, and sand. A crucial step is to model photon transport as a diffusion process. This approach is acceptable for optically thick samples, far into the limit of strong multiple scattering; however, it becomes increasingly inaccurate for thinner samples for several reasons. Here, we correct for two of these defects. By modeling photon propagation by a telegrapher equation with suitable boundary conditions, we can account for the ballistic transport of photons at finite speed between successive scattering events. By introducing a discontinuity in the photon concentration at the source point, and then averaging over a range of penetration depths, we can account for the fact that photons usually scatter anisotropically into the forward direction, rather than being completely randomized at each event. The accuracy of our approach is tested by comparison both with random walk computer simulations and with experiments on specially designed suspensions of polystyrene spheres. We find that our predictions extend the utility of diffuse transmission to slabs of all thicknesses and of DWS to slabs down to about two transport mean free paths. @S1063-651X~98!11604-5# PACS number ~s!: 82.70. 2y, 05.40. 1j, 42.62.Fi

[1]  D. Durian Two-stream theory of diffusing light spectroscopies , 1996 .

[2]  D. Durian,et al.  Angular distribution of diffusely transmitted light. , 1996, Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics.

[3]  D J Durian,et al.  Penetration depth for diffusing-wave spectroscopy. , 1995, Applied optics.

[4]  D. Durian,et al.  Accuracy of diffusing-wave spectroscopy theories. , 1995, Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics.

[5]  Kaplan,et al.  Diffuse-transmission spectroscopy: A structural probe of opaque colloidal mixtures. , 1994, Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics.

[6]  B. Ackerson,et al.  Correlation transfer: development and application. , 1994 .

[7]  Durian Influence of boundary reflection and refraction on diffusive photon transport. , 1994, Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics.

[8]  D. Pine,et al.  Geometric constraints for the design of diffusing-wave spectroscopy experiments. , 1993, Applied optics.

[9]  B. J. Ackerson,et al.  Correlation transfer - Application of radiative transfer solution methods to photon correlation problems , 1992 .

[10]  Müller,et al.  Scaling of transient hydrodynamic interactions in concentrated suspensions. , 1992, Physical review letters.

[11]  Clark,et al.  Effects of finite laser coherence in quasielastic multiple scattering. , 1991, Physical review. A, Atomic, molecular, and optical physics.

[12]  D. Weitz,et al.  Internal reflection of diffusive light in random media. , 1991, Physical Review A. Atomic, Molecular, and Optical Physics.

[13]  Middleton,et al.  Discrete scatterers and autocorrelations of multiply scattered light. , 1991, Physical review. B, Condensed matter.

[14]  Alfano,et al.  When does the diffusion approximation fail to describe photon transport in random media? , 1990, Physical review letters.

[15]  Zhu,et al.  Polarization memory of multiply scattered light. , 1989, Physical review. B, Condensed matter.

[16]  John,et al.  Diffusing-wave spectroscopy and multiple scattering of light in correlated random media. , 1989, Physical review. B, Condensed matter.

[17]  D. Weitz,et al.  Diffusing wave spectroscopy. , 1988, Physical review letters.

[18]  G. Maret,et al.  Multiple light scattering from disordered media. The effect of brownian motion of scatterers , 1987 .

[19]  C. Bohren Multiple scattering of light and some of its observable consequences , 1987 .

[20]  G. Batchelor,et al.  Brownian diffusion of particles with hydrodynamic interaction , 1976, Journal of Fluid Mechanics.

[21]  E. J. Hinch,et al.  Application of the Langevin equation to fluid suspensions , 1975, Journal of Fluid Mechanics.

[22]  Douglas J. Durian,et al.  Photon migration at short times and distances and in cases of strong absorption , 1997 .

[23]  Stephen,et al.  Temporal fluctuations in wave propagation in random media. , 1988, Physical review. B, Condensed matter.

[24]  P. Pusey,et al.  Particle diffusion in concentrated dispersions , 1987 .

[25]  H. Lekkerkerker,et al.  Brownian Diffusivities of interacting colloidal particles measured by dynamic light scattering , 1987 .

[26]  L. C. Henyey,et al.  Diffuse radiation in the Galaxy , 1940 .