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Project supported by the National Natural Science Foundation of China (Grants Nos. 11705064, 11675060, and 91730301).
Significant and persistent trajectory-to-trajectory variance are commonly observed in particle tracking experiments, which have become a major challenge for the experimental data analysis. In this theoretical paper we investigate the ergodicity recovery behavior, which helps clarify the origin and the convergence of trajectory-to-trajectory fluctuation in various heterogeneous disordered media. The concepts of self-averaging and ergodicity are revisited in the context of trajectory analysis. The slow ergodicity recovery and the non-Gaussian diffusion in the annealed disordered media are shown as the consequences of the central limit theorem in different situations. The strange ergodicity recovery behavior is reported in the quenched disordered case, which arises from a localization mechanism. The first-passage approach is introduced to the ergodicity analysis for this case, of which the central limit theorem can be employed and the ergodicity is recovered in the length scale of diffusivity correlation.
Particle tracking experiments on various disordered systems, including the living cells,[1–4] colloidal[5,6] and granular[7] systems have provided numerous trajectories with rich dynamic details. This has been utilized to infer the latent dynamics of the tracer[8] and also the disordered feature of the environments,[3,9] which calls for careful statistics analysis[10,11] on random walks.
The commonly observed significant trajectory-to-trajectory variance is one of the major challenges in the trajectory analysis. Due to the stochastic nature of random walks, it exists even in the normal Brownian motion in the homogeneous media. In this simple case the fluctuation is depressed in the longer trajectories, hence the ergodicity recovers. It has been observed in experiments, however, the trajectory-to-trajectory variance can sustain in disordered media over the whole experiments,[1,2] which has been considered as a consequence of the heterogeneity of dynamics in the media. In the case of strong disorder, the heterogeneity leads to sub-diffusive continuous time random walk (CTRW).[12,13] The ergodicity would not recover in such a case.[14,15] In the case of moderate heterogeneity, one may also observe slow ergodicity recovery while the random diffusivity correlates along the trajectory. In this case the non-Gaussian diffusion has been intensively studied.[2,16–18] In recent studies on the non-Gaussian diffusion,[9,19] a localization mechanism has been discovered in the quenched disordered media with locally correlated diffusivity. The population splitting[19,20] due to the localization introduces strange and ultra-slow recovery of ergodicity. The similar behavior has also been reported in the molecular dynamics simulation.[17] It is currently unclear whether and how the ergodicity recovers in the quenched disordered case.[19,21]
In this paper, we crystalize the idea of self-averaging and ergodicity recovery by the model study in the fashion of experimental trajectory analysis, where the trap model[13,22,23] is employed as a theoretical framework containing the random walks in the homogeneous media, in the annealed disordered media with temporally correlated diffusivity, and in the quenched disordered media with spatially correlated diffusivity. One will see that the central limit theorem (CLT) plays a key role in most of the materials dealt in this paper, which is also connected to the non-Gaussian diffusion. We suggest that the first-passage time would be a proper observable for the investigation on the ergodicity recovery in the quenched disordered system.
This paper is arranged as follows. We introduce in Section
Let us consider the trap dynamics on a two-dimensional square lattice with lattice constant a, of which a particle jumps from site i evenly to its nearest-neighbour site j with the transition rate w. The stochastic processes can then be considered as a normal random walk on the lattice subordinated to a time series defined by the waiting time for each jump, {ti}, where ti follows exponential distribution
The dynamics defined above is often called the continuous time random walk in literature, which is discrete in space and continuous in time. The particle tracking experiment data is, however, in a different style that the particle positions are recorded at fixed time intervals. For better guidance to the experiment data analysis, the trajectories from the trap dynamics are discretized into the series of the particle positions {xi} with the constant time interval tbin = ti − ti − 1 as shown in Fig.
In the simulation on the homogeneous case, we are sure that the trajectories are similar due to the same and constant transition rate. It is, however, not trivial to verify the similarity of the trajectories obtained in experiments, where the underlying mechanism is usually unknown. For more rigorous analysis, one may turn to the concept of ergodicity, which refers that the observable averaged along each trajectory equals to that averaged over the ensemble of the trajectories. The most commonly used observable in the particle tracking experiments is the time-averaged mean squared displacement (TAMSD),[11,15] which is a trajectory-wise version of mean squared displacement (MSD). The TAMSD averages the square of the head-to-tail displacement of the short segments from single trajectory by
We estimate here the distribution of trajectory-wise TAMSD defined by Eq. (
The so-called ergodicity breaking parameter[15] is introduced as the square of relative standard deviation of
In this section, we study the case that the instantaneous diffusivity fluctuates along the trajectory, which has been commonly observed in experiments. The classical CTRW[12,23,25] offers a way to capture the feature by sampling the waiting time for every jump from a non-exponential distribution P(t), which has been a successful model to explain the anomalies in sub-diffusion. In the framework of trap dynamics defined above, it is equivalent to the case that the transition rate w is resampled after each jump from the distribution P(w).[26]
It has been realized in recent years that the diffusivity can be a stochastic process independent of the jumps in the case with certain latent dynamics, such as the fluctuating configuration of the protein tracer or the transient interaction between the protein and the cell membrane.[8] To include this case, one may modify the classical CTRW model by introducing an additional latent dynamics, of which w is resampled from the distribution P(w) by a rate wD = 1/tD. w is then correlated to the time scale tD. When the correlation time of the diffusivity, tD, is in a moderate scale, i.e. Δt < tD < T, one may observe the non-Gaussian distribution of the head-to-tail displacement |δ| = |x(t+ Δt) − x(t)| of the short segments. Noting that the latent dynamics fluctuates over time and is independent of the particle location, one can see that it is an annealed model for the non-Gaussian diffusion, which can also be understood as a lattice version of the diffusing diffusivity model introduced by Chubynsky and Slater.[27] In this section, we study the case that w follows the generalized Gamma distribution
In this annealed disordered model, the trajectory-to-trajectory variance sustains in the time scale of τD, which vanishes for longer observation time. Figure
One can start from Eq. (
In the long time limit with T ≫ tD, one can regroup the summation terms in Eq. (
In this section, we study the random walk in the quenched disordered media, of which the diffusivity depends on the local structures of the environments. In the case that the structures relax in a quite long time scale, the local diffusivity can be assumed unchanged over the experiments. In the framework of trap dynamics, the quenched trap model (QTM)[22] assigns the random transition rates {wi} to sites {i} in the lattice. In the experiment with spatial resolution high enough to reveal the local structures, the measured local diffusivity is usually correlated in the scale of the structure size. To include the locally correlated dynamics, we study the trap dynamics on the extreme landscape,[9,19] which is an extension of QTM with the locally correlated {wi}.
The extreme landscape {vi} is generated by the extreme statistics as follows. First, generate the uncorrelated auxiliary potential {ui} following the distribution with a finite expectation and variance, such as the exponential distribution
Without loss of generality, we investigate the ergodicity recovery in the quenched disordered case with α = 1.2. Extensive simulations are performed for 160 trajectories of a quite long time (T = 107) to guarantee that the landscape is fully sampled. Figure
To clarify the self-averaging behavior in the quenched case, one may turn to another observable, i.e., the trajectory-wise mean first-passage time (FPT). In the first-passage approach, the trajectory {x(t)} is divided into several segments determined by the successive first-passage events with radius r at time {tk}. The events can be formally defined by the conditions
The trajectory-to-trajectory fluctuation can be measured by the scaled variance of
Two origins of the trajectory-to-trajectory variance have been analysed in this study: the intrinsic stochastic feature of the random walk and the heterogeneity of the disordered environments, both for the annealed and quenched cases. In an ideal case, the ergodicity would eventually recover when the self-averaging over both origins is achieved in each trajectory. It is, however, the rare case in the experiments with limited observation time on the living cells. As shown in the study, the fluctuation introduced by the disordered environments persists much longer than that by the intrinsic random feature of the walk. One may expect for the long observation, the trajectory-to-trajectory variance is mainly contributed by the heterogeneity of the media. In this sense, the variance encodes the structure information of the environments. One may utilize the information and visualize the structures by the diffusion map (see Ref. [1] for example) and other ways.
This theoretical study may provide guidance on the data analysis for the particle tracking experiments on the living cells and the colloidal systems.
Living cells Due to the heterogeneity of the cellular environments, the behaviors of diffusion in different parts of the cells vary significantly.[29] The cytoplasm of eukaryotic cells is rather dynamical.[30] The nano-particles tracked in such systems are expected to follow the dynamics with fluctuating diffusivity, which has already been investigated in Section
Colloidal systems In the colloidal systems, the tracer can be easily tracked and the environment structure also can be manipulated and imaged (see e.g., Ref. [5]). They are hence good proving grounds for the diffusion theories. In the dense colloidal liquids, the tracer is obstructed by the colloidal particles. Since the liquid structure changes over time, the annealed disordered model may be employed in this case. As the counterpart, the quenched effects are expected in static disordered colloidal matrices.
In this work, we study the ergodicity recovery of random walk in various disordered media, which concerns how the mean of the random observable converges along the elongating trajectory to its expected value. The trajectory-wise TAMSD is chosen as the observable following the convention. The ergodicity recovery in the homogeneous media is revisited in the fashion of the experimental trajectory analysis with the constraints of finite time–space resolution. It offers the first taste on how the CLT would lead to self-averaging in a series of uncorrelated random variables. In more complicated cases with the annealed dynamic heterogeneity, we have shown that the ergodicity recovers only when the observation time is much longer than the relaxation time of the temporal correlated diffusivity. In such a case, the coarse-graining in time can cancel the correlation in the summands of the TAMSD. The CLT can then be applied, which leads to the EB ∼ 1/T behavior.
There has been a puzzle whether and how the ergodicity recovers in the quenched disordered media, where the whole particle populations are usually split into the localized state and mobile one. In the localized state, the particle is frozen in the area with small diffusivity, which can hardly escape the area since it walks slowly. Our extensive simulation shows that the localized particles delay the ergodicity recovery for a very long time, which provides insights into the slow decay of EB parameter observed in the particle tracking experiments. It also explains the abnormal TAMSD behavior that previously observed in the molecular dynamics simulation (see Fig. 8 in Ref. [17]).
The first-passage approach is further introduced for the analysis of trajectories in the quenched disordered media, of which the trajectory is decomposed into segments of the fixed head-to-tail distance. The ergodicity recovery analysis is generalized by choosing the FPT of the segment as the observable. Since the diffusivity is locally correlated, the CLT can be applied to the mean FPT when the space scale of the trajectory is much larger than the correlation length. The variance of the mean FPT is then depressed by VT ∼ 1/L2, where L is the head-to-tail distance of the whole trajectory. This approach may be employed in the future analysis on the trajectories from the particle tracking experiments, especially in the case that the disordered environments are static over the experiment time scale and the particle dynamics is correlated in space but not in time.
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