Force Generation in Confined Active Fluids: The Role of Microstructure.

We experimentally determine the force exerted by a bath of active particles onto a passive probe as a function of its distance to a wall and compare it to the measured averaged density distribution of active particles around the probe. Within the framework of an active stress, we demonstrate that both quantities are-up to a factor-directly related to each other. Our results are in excellent agreement with a minimal numerical model and confirm a general and system-independent relationship between the microstructure of active particles and transmitted forces.

Work fluctuation relation of an active Brownian particle in a viscoelastic fluid.

We experimentally investigate the work fluctuations of an active Brownian particle (ABP) during its self-propelled motion in a viscoelastic medium. Under such conditions, ABPs display a persistent circular motion which allows the determination of the orientational work fluctuations along its trajectory. Due to the nonlinear coupling to the non-Markovian bath, we find strong deviations from the work fluctuation theorem (WFT) due to observed increased rotational ABP dynamics. Taking this enhanced rotational diffusion into account, the orientational work distributions can be recasted to be in accordance with the WFT by considering an effective temperature of about two orders of magnitude larger than k_{B}T. This approach is confirmed by the good agreement of the torque exerted by the viscoelastic bath on the ABP obtained from the WFT with the value obtained from the mean angular velocity and the friction coefficient of the ABP.

Bayesian inference of the viscoelastic properties of a Jeffrey's fluid using optical tweezers.

Bayesian inference is a conscientious statistical method which is successfully used in many branches of physics and engineering. Compared to conventional approaches, it makes highly efficient use of information hidden in a measured quantity by predicting the distribution of future data points based on posterior information. Here we apply this method to determine the stress-relaxation time and the solvent and polymer contributions to the frequency dependent viscosity of a viscoelastic Jeffrey's fluid by the analysis of the measured trajectory of an optically trapped Brownian particle. When comparing the results to those obtained from the auto-correlation function, mean-squared displacement or the power spectrum, we find Bayesian inference to be much more accurate and less affected by systematic errors.

A quantitative analysis of memory effects in the viscously coupled dynamics of optically trapped Brownian particles.

We provide a quantitative description of the memory effects existing in the apparently random Markovian dynamics of a pair of optically trapped colloidal microparticles in water. The particles are trapped in very close proximity to each other such that the resultant hydrodynamic interactions lead to non-Markovian signatures manifested by the double exponential auto-correlation function for the Brownian motion of each particle. In connection with the memory effects, we quantify the storage of energy in terms of various system parameters and demonstrate that a pair of Markovian particles - confined in individual optical traps in a viscous fluid - can be described in the framework of a single Brownian particle in a viscoelastic medium. We define and quantify the equivalent storage and loss moduli of the two-particle system, and show experimentally that the memory effects are maximized at a certain trap stiffness ratio, and reduce with increasing particle separation. The technique can be generally used to determine the effective viscoelastic parameters of any such fluid-particle systems, and can thus help understand the interactions between active particles mediated by simple or complex fluids.

Dynamics of hydrodynamically coupled Brownian harmonic oscillators in a Maxwell fluid.

It has been shown recently that the coupled dynamics of micro-particles in a viscous fluid has many interesting aspects including motional resonance which can be used to perform two-point micro-rheology. However, it is expected that this phenomenon in a viscoelastic fluid is much more interesting due to the presence of the additional frequency-dependent elasticity of the medium. Thus, a theory describing the equilibrium dynamics of two hydrodynamically coupled Brownian harmonic oscillators in a viscoelastic Maxwell fluid has been derived which appears with new and impressive characteristics. Initially, the response functions have been calculated and then the fluctuation-dissipation theorem has been used to calculate the correlation functions between the coloured noises present on the concerned particles placed in a Maxwell fluid due to the thermal motions of the fluid molecules. These correlation functions appear to be in a linear relationship with the delta-correlated noises in a viscous fluid. Consequently, this reduces the statistical description of a simple viscoelastic fluid to the statistical representation for an extended dynamical system subjected to delta-correlated random forces. Thereupon, the auto and cross-correlation functions in the time domain and frequency domain and the mean-square displacement functions of the particles have been calculated which are perfectly consistent with their corresponding established forms in a viscous fluid and emerge with exceptional features.

Single-shot phase-sensitive wideband active microrheology of viscoelastic fluids using pulse-scanned optical tweezers.

We present a fast phase sensitive active microrheology technique exploring the phase response of a microscopic probe particle trapped in a linear viscoelastic fluid using optical tweezers under an external perturbation. Thus, we experimentally determine the cumulative response of the probe to an entire repertoire of sinusoidal excitations simultaneously by applying a spatial square pulse as an excitation to the trapped probe. The square pulse naturally contains the fundamental sinusoidal frequency component and higher odd harmonics, so that we measure the phase response of the probe over a wide frequency band in a single shot, with the band being tunable over the spectrum by choosing suitable experimental parameters. We then determine the responses to individual harmonics using a lock-in algorithm, and compare the phase shifts to those obtained theoretically by solving the equation of motion of the probe particle confined in a harmonic potential in the fluid in the presence of a sinusoidal perturbation. We go on to relate the phase response of the probe to the complex shear modulus [Formula: see text], and proceed to verify our technique in a mixture of polyacrylamide and water, which we compare with known values in literature and obtain very good agreement. Our method increases the robustness of active microrheology in general and ensures that any drifts in time are almost entirely ruled out from the data, with the added advantage of high speed and ease of use.

Free and confined Brownian motion in viscoelastic Stokes-Oldroyd B fluids.

We linearize the Stokes-Oldroyd B model for small perturbations and instantaneous hydrodynamic friction to simulate the environment for a free and confined Brownian particle. We use the standard Green's function approach to determine the viscoelasticity, and show that the expression obtained for the frequency dependent viscosity is similar to that given by the Jeffrey's model, though the latter describes viscoelasticity by the bulk storage and loss moduli that is represented by a complex elastic modulus [Formula: see text] of the fluid concerned. In contrast, we consider the characteristics of the polymer chains and the Newtonian solvent of the complex fluid individually, and determine an expression for frequency-dependent viscosity that would be useful for microrheology performed from Brownian trajectories measured in experiments. Finally, we evaluate the trajectory of a free Brownian particle in a viscoelastic environment using our formalism, and calculate various important parameters quantifying Brownian dynamics, which we then extend to the particle confined in a harmonic potential as provided by optical tweezers.

Two-point active microrheology in a viscous medium exploiting a motional resonance excited in dual-trap optical tweezers.

Two-point microrheology measurements from widely separated colloidal particles approach the bulk viscosity of the host medium more reliably than corresponding single-point measurements. In addition, active microrheology offers the advantage of enhanced signal to noise over passive techniques. Recently, we reported the observation of a motional resonance induced in a probe particle in dual-trap optical tweezers when the control particle was driven externally [Paul et al., Phys. Rev. E 96, 050102(R) (2017)2470-004510.1103/PhysRevE.96.050102]. We now demonstrate that the amplitude and phase characteristics of the motional resonance can be used as a sensitive tool for active two-point microrheology to measure the viscosity of a viscous fluid. Thus, we measure the viscosity of viscous liquids from both the amplitude and phase response of the resonance, and demonstrate that the zero crossing of the phase response of the probe particle with respect to the external drive is superior compared to the amplitude response in measuring viscosity at large particle separations. We compare our viscosity measurements with those using a commercial rheometer and obtain an agreement ∼1%. The method can be extended to viscoelastic material where the frequency dependence of the resonance may provide further accuracy for active microrheological measurements.

Fast Bayesian inference of optical trap stiffness and particle diffusion.

Bayesian inference provides a principled way of estimating the parameters of a stochastic process that is observed discretely in time. The overdamped Brownian motion of a particle confined in an optical trap is generally modelled by the Ornstein-Uhlenbeck process and can be observed directly in experiment. Here we present Bayesian methods for inferring the parameters of this process, the trap stiffness and the particle diffusion coefficient, that use exact likelihoods and sufficient statistics to arrive at simple expressions for the maximum a posteriori estimates. This obviates the need for Monte Carlo sampling and yields methods that are both fast and accurate. We apply these to experimental data and demonstrate their advantage over commonly used non-Bayesian fitting methods.

Direct verification of the fluctuation-dissipation relation in viscously coupled oscillators.

The fluctuation-dissipation relation, a central result in nonequilibrium statistical physics, relates equilibrium fluctuations in a system to its linear response to external forces. Here we provide a direct experimental verification of this relation for viscously coupled oscillators, as realized by a pair of optically trapped colloidal particles. A theoretical analysis, in which interactions mediated by slow viscous flow are represented by nonlocal friction tensors, matches experimental results and reveals a frequency maximum in the amplitude of the mutual response which is a sensitive function of the trap stiffnesses and the friction tensors. This allows for its location and width to be tuned and suggests the utility of the trap setup for accurate two-point microrheology.