PHYSICAL REVIEW E 80, 021111 共2009兲 Subdiffusive behavior in a trapping potential: Mean square displacement and velocity autocorrelation function M. A. Despósito1,2,* and A. D. Viñales1 1 Departamento de Física, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, 1428 Buenos Aires, Argentina 2 Consejo Nacional de Investigaciones Científicas y Técnicas, Buenos Aires, Argentina 共Received 16 February 2009; published 14 August 2009兲 A theoretical framework for analyzing stochastic data from single-particle tracking in viscoelastic materials and under the influence of a trapping potential is presented. Starting from a generalized Langevin equation, we found analytical expressions for the two-time dynamics of a particle subjected to a harmonic potential. The mean-square displacement and the velocity autocorrelation function of the diffusing particle are given in terms of the time lag. In particular, we investigate the subdiffusive case. Using a power-law memory kernel, exact expressions for the mean-square displacement and the velocity autocorrelation function are obtained in terms of Mittag-Leffler functions and their derivatives. The behaviors for short-, intermediate-, and long-time lags are investigated in terms of the involved parameters. Finally, the validity of usual approximations is examined. DOI: 10.1103/PhysRevE.80.021111 PACS number共s兲: 02.50.⫺r, 05.40.⫺a, 05.10.Gg, 05.70.Ln I. INTRODUCTION The viscoelastic properties of complex fluids, such as polymers, colloids, and biological materials, can be derived from the dynamics of individual spherical particles embedded in it 关1,2兴. Particle tracking microrheology experiments 关1–8兴 are based on the observation of the motion of individual tracer particles. In a typical microrheology experiment, particle positions are recorded in the form of a time sequence and information about the dynamics is essentially extracted by measuring the mean-square displacement 共MSD兲 of the probe particles 关9–11兴. On the other hand, during the last 2 decades, optical traps 共or “optical tweezers”兲 have been increasingly used for position detection, covering a wide range of applications in physics and biology 关3,12–17兴. In an optical trap, the interaction between the laser and the trapped particle can be approximated by a harmonic potential 关18兴. If the particle is embedded in a Newtonian fluid, the temporal behavior of its position X共t兲 is described by the standard Langevin equation mẌ共t兲 + ␥Ẋ共t⬘兲 + X = F共t兲, 共1兲 where m is the mass of the particle, ␥ is the friction coefficient, is the trap stiffness, and F共t兲 represents the random thermal force, which is zero centered and has a flat power spectrum 关19兴. From an experimental point of view, calibration of the trap stiffness is necessary to determine the trapping force at any position where the trapping potential is harmonic. A usually employed method for calibration in normal viscous fluids is the power spectrum method 关19兴. Quantitative measurements with optical traps in normal viscous fluids have been applied in numerous microrheology experiments. Optical tweezers microrheological technique was extended to measure the viscoelastic properties of complex fluids 关20–22兴. However, it has been recently noted that the Langevin equation 共1兲 fails to describe the stochastic mo- tion of the trapped bead when it is embedded in a viscoelastic medium 关20,21兴. In this case, the dynamics of the particle differs from that in a pure viscous media because the stochastic process exhibits an anomalous diffusive behavior 关2,11,22–24兴. As a consequence, the use of a trapping complicates the analysis of the obtained data, since the interactions with the viscoelastic environment overlap with the influence of the trapping force 关1,22,25兴. Moreover, calibration by power spectrum method becomes invalid because it based on the assumption that a bead is trapped in a purely viscous fluid. For example, in the application of optical traps in living cells, it is necessary to take into account the a priori unknown viscoelastic properties of the medium to properly calibrate the trap 关20兴. When particles diffuse through a soft complex fluids or biological materials, the mean-square displacement exhibits a slow relaxation with a power-law decay in the range of large times. In absence of external forces, a theoretical description is now well established. A quantitative analysis of the resulting subdiffusive behavior enables one to extract the rheological properties of the material 关1兴. Based on a generalized Langevin equation 共GLE兲, Mason and co-workers 关5,6兴 obtained a direct relation in the Laplace domain between the mean-square displacement of free tracer particles and the viscoelastic parameters of the medium. On the other hand, if the anomalously diffusing particle is subjected to an external harmonic well, the decay of the position autocorrelation function is strongly nonexponential 关17,26,27兴. For example, the corresponding GLE for a particle in a viscoelastic medium and subjected to a harmonic potential was recently investigated by us in Ref. 关27兴, where analytical expressions for the evolution of mean values and variances in terms of Mittag-Leffler functions were obtained for any temporal range and involved parameters. Nevertheless, from an experimental point of view, it is necessary to get expressions for the two-time correlation functions. For instance, the mean-square displacement can be expressed as 共兲 = lim 具关X共t + 兲 − X共t兲兴2典, t→⬁ *[email protected] 1539-3755/2009/80共2兲/021111共7兲 共2兲 where 兩X共t + 兲 − X共t兲兩 is the particle displacement between 021111-1 ©2009 The American Physical Society PHYSICAL REVIEW E 80, 021111 共2009兲 M. A. DESPÓSITO AND A. D. VIÑALES two time points, t denotes the absolute time, while is the so-called lag time 关28兴. Alternative information about the experimentally observed diffusive behavior can be extracted from the normalized velocity autocorrelation function 共VACF兲 关29兴 defined as 关27,30兴 CV共兲 = lim t→⬁ 具V共t + 兲V共t兲典 . 具V2共t兲典 共3兲 Then, to calculate the MSD and the VACF, one must know the behavior of the two-time correlations 具X共t + 兲X共t兲典 and 具V共t + 兲V共t兲典. The aim of this paper is to obtain analytical expressions for the MSD 共2兲 and VACF 共3兲 for a harmonically bounded particle immersed in a viscoelastic environment. This enables us to provide a theoretical framework to analyze the data obtained by particle tracking microrheology experiments in viscoelastic media and using a trapping potential. For this purpose, in Sec. II, we present the corresponding GLE. The two-time dynamics is obtained, which enables us to calculate the MSD and VACF for arbitrary memory kernels. Section III is devoted to the study of the subdiffusive case. The complete analytical solutions are obtained and approximate expressions for different temporal ranges are given. Moreover, the validity of the overdamped approximation is analyzed. Finally, a summary of our results is presented in Sec. IV. of the general form f = −共XX + Y Y + ZZ兲 and assuming that the local environment surrounding the sphere is isotropic. However, our model could also be used to investigate the case of a trapped particle close to a limiting wall, where the motion becomes anisotropic but the drag term can be separated into components parallel and perpendicular to the surface 关32兴. The GLE 共4兲 can be formally solved by means of the Laplace transformation. Taking into account the deterministic initial conditions x0 = X共0兲 and v0 = Ẋ共0兲, the evolution of the Laplace transform of the position X共t兲 reads X̂共s兲 = x0 冉 冊冉 冊 1 1 − 20Î共s兲 + v0 + F̂共s兲 Ĝ共s兲, s m 共7兲 where F̂共s兲 is the Laplace transform of the noise. The relaxation function G共t兲 is the Laplace inversion of Ĝ共s兲 = 1 , ˆ s + s␥共s兲 + 20 2 共8兲 where ␥ˆ 共s兲 is the Laplace transform of the damping kernel and Ĝ共s兲 s Î共s兲 = 共9兲 is the Laplace transform of I共t兲 = II. DIFFUSION IN A HARMONIC WELL 冕 t dt⬘G共t⬘兲. 共10兲 0 A. Formal solution for the GLE In what follows, we consider the dynamics of a spherical bead of mass m immersed in a complex or viscoelastic environment and simultaneously trapped in a harmonic potential. The resulting motion can be described by the following GLE: mẌ共t兲 + m 冕 t dt⬘␥共t − t⬘兲Ẋ共t⬘兲 + m20X = F共t兲, where 0 = 冑 / m is the frequency of the trap, ␥共t兲 is the dissipative memory kernel representing the viscoelastic friction, and the thermal force F共t兲 is a zero-centered and stationary random force with a correlation function of the form 共11兲 where ĝ共s兲 = sĜ共s兲. 共12兲 From Eqs. 共7兲 and 共11兲, a formal expression for the displacement X共t兲 and the velocity V共t兲 can be written as X共t兲 = 具X共t兲典 + V共t兲 = 具V共t兲典 + 1 m 冕 1 m 冕 t dt⬘G共t − t⬘兲F共t⬘兲, 共13兲 dt⬘g共t − t⬘兲F共t⬘兲, 共14兲 0 t 0 where 共6兲 where T is the absolute temperature and kB is the Boltzmann constant. Although we consider the one-dimensional GLE 共4兲, our results can be extrapolated to the two- or three-dimensional case, assuming that the resulting motion can be described by two or three uncoupled equations for independent coordinates. This can be achieved if the trap exerts an elastic force 冊 1 F̂共s兲 ĝ共s兲 − x020Ĝ共s兲, m 共5兲 The integral term in Eq. 共4兲 represents the dependence of the viscous force on the velocity history and the memory kernel ␥共t兲 is related to the noise correlation function C共t兲 via the second fluctuation-dissipation theorem 关31兴 C共t兲 = kBTm␥共t兲, 冉 V̂共s兲 = v0 + 共4兲 0 具F共t兲F共t⬘兲典 = C共兩t − t⬘兩兲. On the other hand, the Laplace transform of the velocity V共t兲 = Ẋ共t兲 satisfies that 具X共t兲典 = x0关1 − 20I共t兲兴 + v0G共t兲, 共15兲 具V共t兲典 = v0g共t兲 − x020G共t兲 共16兲 are the position and velocity mean values evolution, respectively. B. Expressions for the MSD and VACF To calculate the two-time properties of the dynamical variables involved in the expressions of the MSD 共2兲 and 021111-2 PHYSICAL REVIEW E 80, 021111 共2009兲 SUBDIFFUSIVE BEHAVIOR IN A TRAPPING… VACF 共3兲, we will make use of the double Laplace transform technique 关33兴. Then, from Eqs. 共7兲 and 共11兲, we have 具V共t + 兲V共t兲典 = 冉 具X̂共s兲X̂共s⬘兲典 = x20ˆ 共s兲ˆ 共s⬘兲 + v20Ĝ共s兲Ĝ共s⬘兲 + x0v0关ˆ 共s兲Ĝ共s⬘兲 + ˆ 共s⬘兲Ĝ共s兲兴 + 冉 + 20 x2020 − 1 Ĝ共s兲Ĝ共s⬘兲具F̂共s兲F̂共s⬘兲典, m2 冊 k BT k BT g共兲 + v20 − g共t + 兲g共t兲 m m 冊 k BT G共t + 兲G共t兲 m − x0v020关g共t + 兲G共t兲 + g共t兲G共t + 兲兴. 共23兲 共17兲 具V̂共s兲V̂共s⬘兲典 = v20ĝ共s兲ĝ共s⬘兲 + x2040Ĝ共s兲Ĝ共s⬘兲 − x0v020关ĝ共s兲Ĝ共s⬘兲 + ĝ共s⬘兲Ĝ共s兲兴 + 1 ĝ共s兲ĝ共s⬘兲具F̂共s兲F̂共s⬘兲典, m2 共18兲 where ˆ 共s兲 = 1 − 20Î共s兲 s 共19兲 lim ␥共t兲 = lim s␥ˆ 共s兲 = 0. t→⬁ is the Laplace transform of 共t兲 = 1 − 20I共t兲. In the Appendix, we show how the last term of Eqs. 共17兲 and 共18兲 can be calculated. Inserting expressions 共A4兲 and 共A5兲 into Eqs. 共17兲 and 共18兲 and making a double Laplace inversion, we arrive at 冉 It is important to notice that the analytical expressions 共22兲 and 共23兲 are valid for all absolute times t and time lags . They enable us to obtain the two-time dynamics for an arbitrary memory kernel provided that the fluctuationdissipation theorem 共6兲 is satisfied. Nevertheless, to evaluate the relevant experimental magnitudes 共2兲 and 共3兲, we must take the limit t → ⬁. In this case, these expressions could be simplified as follows. Taking into account the usual assumption that the time-dependent frictional coefficient ␥共t兲 goes to zero when t → ⬁ 关34兴 and using the final value theorem 关35兴, one gets 冊 Noticing that the Laplace transform of the relaxation function I共t兲 defined through Eq. 共9兲 is Î共s兲 = 共20兲 冊 冊 共21兲 CV共兲 = g共兲. 共⬁兲 = 具关X共t + 兲 − X共t兲兴 典 2kBT I共兲 − 2x0v020关G共t + 兲 − G共t兲兴关I共t + 兲 − I共t兲兴 m 冉 冊 k BT 关G共t + 兲 − G共t兲兴2 m + 20 x2020 − 冊 k BT 关I共t + 兲 − I共t兲兴2 , m 共28兲 共22兲 共29兲 Taking into account Eqs. 共26兲 and 共27兲, the equilibrium value of the MSD is given by 2 冉 2kBT I共兲 m and Finally, by considering time lags ⬎ 0, from Eqs. 共20兲 and 共21兲 we have + v20 − 共27兲 Applying these conditions in order to take the limit t → ⬁ in Eqs. 共22兲 and 共23兲 and using the definitions 共2兲 and 共3兲, one finally obtains the simpler expressions 共兲 = k BT G共t兲G共t⬘兲 m − x0v020关g共t兲G共t⬘兲 + g共t⬘兲G共t兲兴. = 共26兲 G共⬁兲 = g共⬁兲 = 0. k BT k BT g共t兲g共t⬘兲 g共兩t − t⬘兩兲 + v20 − m m 冉 共25兲 and using Eqs. 共9兲 and 共12兲 gives k BT k BT 2 + 关I共t兲 + I共t⬘兲 − I共兩t − t⬘兩兲兴 − I共t兲I共t⬘兲, m m 0 + 20 x2020 − s−1 , s + s␥ˆ 共s兲 + 20 2 I共⬁兲 = 1/20 + x0v0关共t兲G共t⬘兲 + 共t⬘兲G共t兲兴 冉 共24兲 the application of the final value theorem and the use of condition 共24兲 yield 关34兴 k BT G共t兲G共t⬘兲 具X共t兲X共t⬘兲典 = x20共t兲共t⬘兲 + v20 − m 具V共t兲V共t⬘兲典 = s→0 2kBT m20 , 共30兲 while, as expected, the VACF decays to zero, i.e., CV共⬁兲 = 0. It is worth pointing out that in experimental realizations, the time lag is min ⱕ ⱕ max, being min the acquisition time interval and max the measurement time. Moreover, if N is the number of steps n taken at intervals min, only small values of n共n ⬍ N / 10兲 are used. Therefore, it is important to obtain valid expressions for all observational time scales instead of getting only its behavior to large times. 021111-3 PHYSICAL REVIEW E 80, 021111 共2009兲 M. A. DESPÓSITO AND A. D. VIÑALES ⬁ To conclude this section, we will find the extension for a trapped particle of the widely used Mason formula 关5,6兴. Taking the Laplace transform of Eq. 共28兲 and using the definition 共25兲 of the relaxation function I共t兲, one gets s␥ˆ 共s兲 = 2kBT 1 − s2 − 20 , m sˆ 共s兲 共32兲 where R is the radius of the spherical tracer particle, ˆ 共s兲 is the bulk frequency-dependent viscosity of the medium, and Ĝ共s兲 is the Laplace-transformed shear modulus of the viscoelastic fluid. Equation 共32兲 is based on the implicit assumption that Stokes drag for viscous fluids 共no-slip boundary conditions兲 can be generalized to viscoelastic fluids at all s 关6兴. 共− 1兲k 2kBT 共k兲 共0兲2k2E2−,3+k 共− ␥2−兲, 兺 m k=0 k! 共37兲 ⬁ 共31兲 which gives a direct relation between the mean-square displacement of the particle and the memory kernel. Finally, expression 共31兲 can be related with the viscoelastic parameters of the complex fluid using the generalized StokesEinstein equation 关1,5,6兴 s␥ˆ 共s兲 = 6Rsˆ 共s兲 = 6RĜ共s兲, 共兲 = C V共 兲 = 兺 k=0 C共t兲 = C t− , ⌫共1 − 兲 共33兲 where ⌫共z兲 is the gamma function 关38兴. The exponent for a viscoelastic medium is taken as 0 ⬍ ⬍ 1. The proportionality coefficient C is independent of time but depends on the exponent . Using the fluctuation-dissipation relation 共6兲, the memory kernel ␥共t兲 can be written as ␥ ␥共t兲 = t− , ⌫共1 − 兲 ⬁ E␣,共y兲 = 兺 j=0 s−1 . s2 + ␥s + 20 共39兲 共40兲 Using the series expansions 共39兲 and 共40兲, one can realize that the short-time behavior of the MSD reads 共兲 ⬇ 再 冎 2 2␥ k BT 2 − 4− − 0 4 , 12 m ⌫共5 − 兲 共41兲 where the first term shows that the particle undergoes ballistic motion when time is very small 关39兴. The second term comes from the influence of the viscoelastic medium while the third term corresponds to the fact that the particle begins to “see” the trap. The short-time behavior of the VACF can be obtained in a similar way. In this case, we get 2 ␥ 2− − 0 2 . 2 ⌫共3 − 兲 C V共 兲 ⬇ 1 − 共42兲 On the other hand, for ␥2− Ⰷ 1, the MSD and VACF can be obtained introducing the asymptotic behavior of the Mittag-Leffler function 关38兴 E␣,共− y兲 ⬃ 1 , y⌫共 − ␣兲 y⬎0 共43兲 into Eqs. 共37兲 and 共38兲. After some calculations, we have 共兲 ⬇ 2kBT m20 再 冉 冊冎 1 − E − 冉 20 ␥ 共44兲 , 冊 20 1 d2 E − , ␥ 20 d2 共45兲 where E共y兲 = E,1共y兲 denotes the one-parameter MittagLeffler function 关38兴. It is worth pointing out that these expressions can be also obtained discarding the inertial term s2 in Eq. 共36兲. In this case, we get 共36兲 Î共s兲 = The complete temporal behavior of the relaxation functions I共t兲, G共t兲, and g共t兲 was previously obtained by us in Ref. 关27兴. Using those results in Eqs. 共28兲 and 共29兲, we have ⬎0 共j + k兲 ! y j dk . = k E␣,共y兲 = 兺 dy j=0 j ! ⌫共␣共j + k兲 + 兲 C V共 兲 ⬇ − 共35兲 ␣ ⬎ 0, ⬁ E␣共k兲,共y兲 共34兲 In this situation, the Laplace transform of the relaxation function Î共s兲 reads Î共s兲 = yj , ⌫共␣ j + 兲 and E␣共k兲,共y兲 is the derivative of the Mittag-Leffler function where ␥ = C / kBT. Then, its Laplace transform reads ␥ˆ 共s兲 = ␥s−1 . 共38兲 where E␣,共y兲 is the generalized Mittag-Leffler function 关38兴 defined by the series expansion III. SUBDIFFUSIVE BEHAVIOR Notice that the previous results are valid for any memory kernel that satisfies condition 共24兲. On the other hand, it is well known that in the absence of active transport, the dynamics of the particle in a viscoelastic fluid or complex media is subdiffusive and thus the stochastic process presents a long-time tail noise. The most utilized model to reproduce a subdiffusive behavior is characterized by a noise correlation function exhibiting a power-law time decay 关27,36,37兴 共− 1兲k 共k兲 共0兲2kE2−,1+k 共− ␥2−兲, k! 冉 冊 1 1 s−1 s−1 = , − ␥s + 20 20 s s + 20/␥ 共46兲 and using that the Laplace transform of the Mittag-Leffler function 关38兴 021111-4 PHYSICAL REVIEW E 80, 021111 共2009兲 SUBDIFFUSIVE BEHAVIOR IN A TRAPPING… 1 1.4 0.75 1.2 0.5 CV Τ ΡΤΡ 1 0.8 0.6 0.25 0 0.25 0.4 0.5 0.2 0.75 2 4 6 Τ 8 FIG. 1. 共Color online兲 MSD vs time lag for = 1 / 2, ␥ = 1, and 0 = 1.4. Solid line corresponds to the exact solution 共37兲, dotted line to the approximate solution 共44兲, and dashed line to the asymptotic behavior 共48兲. 冕 ⬁ e−stE␣共− ␥t␣兲dt = 0 s␣−1 , s␣ + ␥ 共47兲 one obtains expressions 共44兲 and 共45兲. Finally, if Ⰷ ␥ / 20, the behaviors of the MSD and VACF can be obtained using again the approximation 共43兲. In this case, we get 共兲 ⬇ 2kBT m20 再 C V共 兲 ⬇ − 1− 2 10 冎 1 ␥ − , 2 0 ⌫共1 − 兲 共48兲 ␥ 共 + 1兲 −共+2兲 , 40 ⌫共1 − 兲 共49兲 showing a pure power-law decay. In Figs. 1 and 2, we have plotted the MSD vs time lag using the exact solution 共37兲 and the approximations 共44兲 and 共48兲. Note that the exact solution exhibits a nonmonotonic approach to 共⬁兲, while the approximations always present a monotonic behavior. More pronounced differences occur in the behavior of CV共兲 as is evidenced in Figs. 3 and 4. Note that the approximate solutions exhibit a negative velocity autocorrelation for 6 Τ 8 10 FIG. 3. 共Color online兲 CV vs time lag for = 1 / 2, ␥ = 1, and 0 = 1.4. Solid line corresponds to the exact solution 共38兲, dotted line to the approximate solution 共45兲, and dashed line to the asymptotic behavior 共49兲. all times, whereas the exact solutions alternate between positive and negative values. This behavior is related to the socalled whip-back effect 关27,37兴. These behaviors can be understood taking into account that the approximations 共44兲 and 共45兲 only depend on the one-parameter Mittag-Leffler function E共−20 / ␥兲. It is known that the function E共−t兲 is a completely monotone function and tends to zero from above as t tends to infinity for 0 ⬍ ⬍ 1 关40兴. Then, the approximate solutions are always monotonic for every value of 0 and 0 ⬍ ⬍ 1. However, the exact solutions 共37兲 and 共38兲 are expressed as infi共k兲 2− 兲 functions. In this case, the nite sums of E2−, 共−␥ solutions can exhibit a nonmonotonic behavior as is displayed in the previous figures. Then, the overdamped approximation must be used with care in the analysis of the short- and intermediate-time dynamics where the MSD and VACF exhibit a relaxation plus an oscillatory behavior. Interestingly, Burov and Barkai 关41兴 recently arrived to a similar conclusion using a fractional Langevin equation. Solving the corresponding fractional differential equation in terms of roots of regular polynomials, they analyze the position correlation 具X共t兲X共0兲典. As in our case, they found that the exact solution can exhibit a nonmonotonic decay, while the overdamped approximation gives a monotonic decay. 1 1 0.8 0.8 0.6 0.4 0.6 CV Τ ΡΤΡ 4 0.4 0.2 0 0.2 0.2 0.4 2 4 6 Τ 8 10 12 14 FIG. 2. 共Color online兲 Idem Fig. 1 for 0 = 0.8. 2 4 6 Τ 8 10 12 FIG. 4. 共Color online兲 Idem Fig. 3 for 0 = 0.8. 021111-5 14 PHYSICAL REVIEW E 80, 021111 共2009兲 M. A. DESPÓSITO AND A. D. VIÑALES IV. SUMMARY In this work, we have obtained the mean-square displacement and the velocity autocorrelation function for a trapped particle and immersed in a complex or viscoelastic media. For this purpose, and starting from a suitable generalized Langevin equation, we have been able to derive analytic expressions for the two-time dynamics of the processes, valid for all absolute times and times lags. We have showed that the MSD and VACF can be expressed as a simple expression when the memory kernel goes to zero for large times. Furthermore, we have presented a generalization of the Mason formula valid when a trapping potential is present. In particular, we have examined the subdiffusive case, which is a representative example of passive transport in viscoelastic media. Using a power-law memory kernel, exact expressions and valid for all time lags have been obtained in terms of Mittag-Leffler functions and their derivatives. The behavior for short-, intermediate-, and long-time lags are given in terms of the involved parameters. Finally, we have showed that the usual approximations cannot reproduce the nonmonotonic dynamics present in the exact solutions. In summary, we have presented a theoretical method to account for the effects of the trapping potential in the anomalous behavior of the mean-square displacement and the normalized velocity autocorrelation function of a particle embedded in a complex or viscoelastic environment. We believe that the presented results will be useful to analyze the obtained data from microrheology experiments in viscoelastic media using trapping potentials. 31980/05 from Agencia Nacional de Promoción Científica y Tecnológica and Grant No. X099 from Universidad de Buenos Aires, Argentina. APPENDIX To calculate the last term of Eqs. 共17兲 and 共18兲, we make use of a relation given in Ref. 关33兴. Given any stationary correlation function of the form 具⌿共t兲⌿共t⬘兲典 = Af共兩t − t⬘兩兲, the corresponding double Laplace transform writes 具⌿̂共s兲⌿̂共s⬘兲典 = A f̂共s兲 + f̂共s⬘兲 . s + s⬘ 共A2兲 Then, the Laplace domain version of the fluctuationdissipation relation 共6兲 reads 关33兴 具F̂共s兲F̂共s⬘兲典 = kBTm ␥ˆ 共s兲 + ␥ˆ 共s⬘兲 . s + s⬘ 共A3兲 After some algebra and using the relations between the kernels I共t兲G共t兲 and g共t兲, one can find that Ĝ共s兲Ĝ共s⬘兲具F̂共s兲F̂共s⬘兲典 = kBTm 冋 Î共s兲 Î共s⬘兲 Î共s兲 + Î共s⬘兲 − + s⬘ s s + s⬘ 册 − kBTm关Ĝ共s兲Ĝ共s⬘兲 + 20Î共s兲Î共s⬘兲兴, 共A4兲 ĝ共s兲ĝ共s⬘兲具F̂共s兲F̂共s⬘兲典 ACKNOWLEDGMENTS We would like to thank the anonymous referee for his suggestions, which were very useful to the final form of the paper. This work was performed under Grant No. PICT 关1兴 T. A. Waigh, Rep. Prog. Phys. 68, 685 共2005兲. 关2兴 M. T. Valentine, P. D. Kaplan, D. Thota, J. C. Crocker, T. Gisler, R. K. Prud’homme, M. Beck, and D. A. Weitz, Phys. Rev. E 64, 061506 共2001兲. 关3兴 S. Yamada, D. Wirtz, and S. C. Kuo, Biophys. 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