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Published in Soil Sci. Soc. Am. J. 67:1334-1343 (2003).
© 2003 Soil Science Society of America
677 S. Segoe Rd., Madison, WI 53711 USA

DIVISION S-1—SOIL PHYSICS

Scale- and Rate-Dependent Solute Transport within an Unsaturated Sandy Monolith

M. Javaux* and M. Vanclooster

Dep. of Environmental Sciences and Land Use Planning, Université Catholique de Louvain (UCL), Croix du Sud, 2 Bte 2, B-1348 Louvain-la-Neuve, Belgium

* Corresponding author (javaux{at}geru.ucl.ac.be).


    ABSTRACT
 TOP
 ABSTRACT
 INTRODUCTION
 THEORY
 MATERIALS AND METHODS
 RESULTS AND ANALYSIS
 CONCLUSIONS
 APPENDIX 1
 Appendix 2
 REFERENCES
 
Solute transport in unsaturated soil is a scale- and flow rate-dependent process, and high quality experimental studies are needed to introduce scaling relationships in the governing flow and transport models. Within this paper, we present an experimental study to characterize the solute transport for an unsaturated and undisturbed subsoil monolith sampled in a sandy aquifer. Leaching experiments were performed at different flow rates, and solute breakthrough at different positions in the monolith was measured by time domain reflectometry (TDR) probes. At TDR probe scale, the transport is assessed as being a convective-dispersive process with mixing lengths <0.3 m. At the scale of the monolith, that is, the meso-scale, transport is rather a stochastic-convective process with mixing lengths >1 m. At the bottom of the monolith, the meso-scale dispersivity is at least two times larger than the local-scale dispersivity. In addition, this meso-scale dispersivity can be successfully predicted using a stream tube model in combination with a local scale convective-dispersive process. Important scale effects are also observed in the relationship between the square coefficient of variation of the local velocities and the dispersivity. In contrast to previous studies, we do not observe a significant difference in transport properties for different flow rates (from 1.05 to 54.16 cm d-1). We attribute this insignificance either to a balance between the decrease of the tortuosity and the increase of the coefficient of variation of the velocity with the flow rate or a non-dependency of both terms on the flow rate.

Abbreviations: BTC, breakthrough curve • CD, convective dispersive • CDE, CD equation • EC, electrical conductivity • superscript [l], local scale • LSM, least square method • superscript [m], meso-scale • MM, moment method • NTC, negative temperature coefficient • PVC, polyvinyl chloride • SC, stochastic convective • TDR, time domain reflectometry


    INTRODUCTION
 TOP
 ABSTRACT
 INTRODUCTION
 THEORY
 MATERIALS AND METHODS
 RESULTS AND ANALYSIS
 CONCLUSIONS
 APPENDIX 1
 Appendix 2
 REFERENCES
 
THE HYDRODYNAMIC DISPERSIVITY {lambda} (L) is a key parameter for describing solute transport in natural porous media. However, the link between this parameter and basic soil properties for a given flow regime is still poorly understood. Much evidence shows that hydrodynamic dispersivity depends on the scale and the flow conditions and is therefore not a material constant of the porous medium. Scale-dependent dispersivity has been studied in saturated porous media at the laboratory and the field scale, both in homogeneous as well as in heterogeneous formations (Pickens and Grisak, 1981) and has been related to the variability of the microscale flow field (Huang et al., 1995; Pang and Hunt, 2001). Similarly, scale-dependent dispersivity has been studied in partially saturated media where velocity and water content variations as well as structural variability of the porous medium complicate the study of the scale effect. Diverging scaling behaviors of the hydrodynamic dispersivity were obtained from solute transport experiments, using different experimental soil types, different experimental scales and different boundary conditions. At the scale of an undisturbed soil column (21.8- to 87-cm length, 10- to 20-cm i.d.), Khan and Jury (1990) observed an increasing hydrodynamic dispersivity with the column length when high flow conditions were imposed. In contrast, a constant dispersivity was obtained for lower flow rate or when the material was disturbed. Similar results were obtained by Porro et al. (1993) in uniform and layered soil columns of 0.95-m diam. and 6-m depth. In an undisturbed layered lysimeter (0.8-m i.d., 2-m depth), Vanclooster et al. (1995) observed a nearly linear increase of the hydrodynamic dispersivity with depth. Vanderborght et al. (2001), studying solute transport on small Regosol lysimeters (0.3-m i.d., 0.8-m depth), reported constant dispersivity with depth at low flow rates but depth dependent dispersivity at high flow rates. Studying solute transport through two undisturbed Spodosols monoliths (0.8-m i.d., 1-m depth), Seuntjens et al. (2001) obtained opposite depth scaling behaviors of the dispersivity, and related this to the different morphological characteristics of the two peds.

From a theoretical point of view, the dispersion process in a soil can be viewed as the result of the concomitant movement of a high number of dissolved solute particles, each one having its own velocity and direction, which continuously change along its trajectory. The regime of lateral mixing of solute between vertically oriented stream tubes therefore defines the transport process. To evaluate the mixing process, a mixing time t* has been introduced by different authors (Dagan, 1984; Scheidegger, 1960; Taylor, 1953). Vanderborght et al. (2001) defined t* as "the time interval during which a particle travels with a constant velocity or ‘remembers’ its velocity" (Vanderborght et al., 2001). If the mean solute arrival time is much lower than t*, the solute particles spread longitudinally by virtue of differences in their convective velocities, resulting in an overall dispersion increasing linearly with depth. This process is called stochastic-convective (SC). In contrast, if t* is much lower than the mean solute arrival time, the concentration differences normal to the direction of flow are smoothed out by transverse mixing (Khan and Jury, 1990). In this case, dispersion remains constant with depth and solute transport is convective dispersive (CD).

At a given depth, any medium discontinuity can affect the solute particles velocity distribution at that depth by changing (increasing or decreasing) the transverse mixing between adjacent regions having different velocities. So, transverse layering, structural or textural change of the porous medium along the flow path and non-uniform distribution of the moisture in the partially saturated porous medium may change the lateral mixing regime and hence the longitudinal dispersion (Koch and Flühler, 1994).

In addition, the dispersion process can also be affected by the flow rate. However, two antagonistic effects have to be considered. If flow rate increases, the pores domain encompassed into the transport process becomes larger and therefore the mixing time variance of the solute particles velocity increases. In this case, {lambda} should increase. This was observed by Vanderborght et al. (1997), amongst others. On the other hand, increase of the soil water content related to a higher flow rate can lead to reduced tortuosity then the flow paths will be shorter and this will narrow the arrival time distribution (Maciejewski, 1993). In that case, {lambda} diminishes.

Within that context, the experimental protocol or set-up affects the mixing regime of a surface applied solute in a partially saturated soil. Column length, flow rates, and structural heterogeneity of the porous medium within the flow domain influence the solute transport process, and subsequently, the solute transport parameters. It implies that well-conducted experiments are needed to identify the governing transport concept and to assess the solute transport parameters. It also implies that appropriate scaling relationships are needed to introduce solute transport parameters, identified under specific experimental conditions, in predictive solute transport models operational under variable boundary conditions. This is of paramount importance given the influence of the hydrodynamic dispersivity in predicting chemical concentrations in soil and subsoil, especially at the low concentration front end of the pollutant breakthrough curve. In addition, for engineering applications, parameter generation techniques need to be developed which allow the hydrodynamic dispersion to be identified for different porous media in a practical way and this in terms of the scale of application and flow conditions. Unfortunately, the experimental database supporting the development of generic scaling relationships for hydrodynamic dispersion in natural porous media is still small. In addition, the experimental studies reported above have mostly been collected in surface soils and little experimental data are available for the solute transport behavior in subsoil vadose zone. The understanding of the mixing regime in these formations is therefore needed to predict large-scale solute transport in practical applications.

The objective of this study was to investigate the scale- and flow rate-dependency of the solute transport process within an undisturbed sandy soil core at the scale of a TDR sampling window (called ‘local scale’ hereafter) and the scale of the soil column (called ‘meso-scale’ hereafter). We especially focused our attention on the respective contribution of the coefficient of variation of the velocity and the mixing length on the longitudinal apparent dispersivity.


    THEORY
 TOP
 ABSTRACT
 INTRODUCTION
 THEORY
 MATERIALS AND METHODS
 RESULTS AND ANALYSIS
 CONCLUSIONS
 APPENDIX 1
 Appendix 2
 REFERENCES
 
If the travel time is much greater than the mixing time t*, the vertical transport of inert solutes into a homogeneous partially saturated soil can be modeled by means of convection-dispersion equation (CDE) written as:

[1]
with C (M L-3) the concentration, DL (L2 T-1) the longitudinal dispersion coefficient, (L T-1) the average solute velocity, and t (T), z (L) the time and space coordinates. Neglecting chemical diffusion, the longitudinal hydrodynamic dispersivity {lambda}L can be formulated as:

[2]

As pointed out by Vanderborght et al. (2001), {lambda}L is a descriptor for the mixing regime in soils. That means that, even if the mixing regime is not CD, {lambda}L can be used as an apparent coefficient but its definition of travel-time distribution will be different (see Eq. [9] and [10] hereafter). Mixing regimes can be defined in terms of the autocorrelation of the solute transport velocities in time and the variance of the solute travel distances. Following Scheidegger (1960), the solute mixing time t* (T) is:

[3]
where rv is the dimensionless coefficient of correlation between the transport velocity v at time t and v at time t + {tau}, where {tau} is the time lag. The mixing time, also called autocorrelation time (Bear, 1972), is therefore a threshold value discriminating between a process for which the particle velocities at time t and t + {tau} are not correlated (if {tau} >> t*) and another one for which every particle progresses with its velocity without random effect (when {tau} << t*).

By definition, the longitudinal dispersion is defined as

[4]
with {sigma}2z (L2) the variance of solute travel distance. Depending on the travel time, {sigma}2z can be simplified as (Bear, 1972):

[5]

[6]
with {sigma}2v (L2 T-2) the variance of the solute velocities. Actually, in a porous medium, the mixing regime is dependent on the connectivity of the pore space. Thus, it is rather in terms of length than in term of time that we could define a mixing characteristic value. So, we can define a mixing length l* (L) corresponding to the distance traveled during a time t*, assuming that the mixing time t* = l*/ (Skopp and Gardner, 1992; Vanderborght et al., 2001). From Eq. [4], [5], and [6], and given the definition of l*, the following expressions for DL are obtained:

[7]

[8]

Combining Eq. [7] and [8] with Eq. [2] yields:

[9]

[10]
with CV2v, the coefficient of variation of solute velocities. The apparent longitudinal hydrodynamic dispersivity can therefore be defined in two ways depending on the mixing regime. Equations [5], [7], and [9] are only suitable if the solute travel depth of the considered transport event is larger than the mixing length. In this case, the travel depth variance grows linearly with time and the dispersivity is independent of depth as long as CV2v is constant. Considering that the solute travel depth probability density function is normal, this transport process can be modeled with the CDE. In Eq. [10], the {lambda}L is related to the depth by the z and the CVv terms. It can be shown (see Appendix 1) that the condition to have a SC process is that CVv/ is constant with depth. Furthermore, if is constant, the process can be modeled, for instance, by the convective-lognormal transfer function (CLT) (Jury, 1982). In this case, the {lambda}L scales linearly with depth.

Equations [9] and [10] also indicate that, even in a homogeneous soil, flow rate changes can affect {lambda}L by modifying the CVv (Vanderborght et al., 2001). As pointed out in the introduction, this is caused by two antagonistic effects: (i) a change of the tortuosity affecting the length of flow paths and (ii) a modification in the range of pores explored by the flow paths. Moreover, although it is not explicit from the previous equations, it is worth noting that l* can also be influenced by the flow rate or the water content (Matsubayashi et al., 1997). Indeed, when the soil water content increases, flow paths are better connected, which may improve the mixing and reduce the mixing length. However, in the other hand, higher water content may also result in a higher mixing length if continuous macropores are activated.

The spatial scale effect on {lambda}L, both horizontally and vertically, is generated by the scale dependence of CVv and l*. Indeed, if more heterogeneity is encompassed in the flow domain when scale changes, the CVv will increase because of a broader pore water velocity distribution. In addition, complete mixing between flow paths will take more time if the scale is larger. Consequently, l* should increase with scale.


    MATERIALS AND METHODS
 TOP
 ABSTRACT
 INTRODUCTION
 THEORY
 MATERIALS AND METHODS
 RESULTS AND ANALYSIS
 CONCLUSIONS
 APPENDIX 1
 Appendix 2
 REFERENCES
 
Subsoil Sampling and Monolith Equipment
One undisturbed monolith (1-m height by 0.8-m i.d.) was extracted from a sand quarry (Mont-Saint-Guibert, Belgium) at 10-m depth below the ground surface using the method as described by Vanclooster et al. (1995). The subsoil is a Tertiary marine sandy deposit being characteristic for the aquifer material of the region. Since it is the result of a sedimentation process, this subsoil exhibits a series of small horizontal layers (<5 cm thick), inversely size-graded, possibly cross-bedded. Disturbed samples were collected with kopecki rings near the monolith-sampling hole to characterize the grain-size distribution of the material at different depths. As can be seen in Table 1, the texture of the subsoil seems rather homogeneous with roughly 95% of coarse material. It is important to note that some coarse siliceous concretions (max. 100 cm3) were present in the formation, which for obvious reasons, were not considered in the granulometric analysis. The apparent contradiction between the layering and the textural homogeneity is due to kopecki ring volume, which was too large compared with the layer thickness.


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Table 1. Grain-size distribution of the subsoil at five depths.

 
In the laboratory, 12 horizontal TDR probes were placed in the monolith with a specific spatial configuration allowing the breakthrough curves at different scales to be measured. The TDR probes were inserted in three vertical transects spaced 120° apart, two of them with 3 probes (at 0.15-, 0.45-, and 0.75-m depth) and the third with six probes (at 0.15-, 0.30-, 0.45-, 0.60-, 0.75-, and 0.90-m depth, see Fig. 1) . The probes consist in three parallel 0.425-m length and 0.005-m i.d. stainless steel rods, embedded in an epoxy head. The distance between the horizontally aligned rods is 0.025 m, yielding an estimated sampling volume of 2.1 x 10-3 m3. The probes were connected to a TDR multiplexer (Campbell SDMX50, Campbell Scientific Lt., UK), which is controlled by a fully automatic data logger and personal computer. Time domain reflectometry signals are generated and recorded by means of a Tektronix 1502B device (Tektronix, Beaverton, OR). The dielectric constant as well as the medium conductance 1/Z within the TDR sampling volumes are recorded at fixed time steps (max. 15 min.) during the transport experiments. Four negative temperature coefficient (NTC) thermistors (numbered from 1 to 4 in Fig. 1) and four tensiometers (T1 to T4 in Fig. 1) were introduced horizontally and allowed the time course of the temperature and suction head at different depths in the soil monolith to be monitored. Positions of the instruments are given in Fig. 1. The central outlet of the bottom plate was connected to an electrical conductivity probe (Aquasys, type SON-10-25, Aquasys, Belgium) coupled with a NTC temperature probe. Drainage rate at the outlet was measured by means of tipping bucket device (GME, type PR12). The NTC, the electrical conductivity probe at the bottom of the soil column, and the tipping bucket were automatically recorded (GME-Easylog datalogger, GME, Belgium). For controlling the incoming flow rate during the experiments, a specific irrigation system was designed consisting of a square reservoir of 0.8-m depth and 1-cm height, having 280 needles (i.d. 0.5-mm) inserted regularly in a 5-cm grid at the bottom surface of the reservoir. Depending on the flow rate, one or two pulse pumps (Prominent, type 1001N, Prominent, Germany) were connected at the top of the reservoir, imposing a constant flow rate at the inlet of the irrigation device. The irrigation plate was placed on the top of a polyvinyl chloride (PVC) cylinder extending the monolith for another 30 cm from the soil surface and sealed to prevent evaporation during the experiments. To avoid surface sealing by the falling raindrops, 0.5 cm of fine gravel was spread on top of the soil surface. The soil column was put on top of a 5-cm layer of fine gravel. The closing bottom system was constituted of one 1-cm PVC plate stuck on a 1-cm thick stainless steel plate with an outlet gate imbedded at the center. A draining tube connected to the outlet gate conducts the leachate of the monolith to the tipping bucket and the electrical conductivity (EC)-meter.



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Fig. 1. Schematic of the equipped column (perspective and top view).

 
Transport Experiments
To analyze the flow rate effect on solute transport, 11 inert solute transport experiments were conducted on the monolith at different flow rates ranging from 1- to 55-cm d-1. Partially saturated experiments were performed as follows. First, a constant flow rate Jw of unloaded water (EC = 500 µS cm-1) was imposed at the soil surface until steady-state flow rate was obtained. The steady-state regime was controlled by a constant moisture and tension reading. Subsequently, the irrigation system was removed and CaCl2–loaded water (from 0.15 to 0.3 mol L-1) was applied uniformly and constantly with a hand-sprayer. The duration of application was adapted to Jw to be negligible compared with the total duration of the experiment so that we could mathematically interpret it as a Dirac delta function. After solute application, unloaded water was irrigated with the same Jw. Details of the experiments can be found in Table 2. Since no suction could be applied at the lower face of the column, the bottom water boundary condition was always a seepage face.


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Table 2. Features of solute transport experiments.

 
For the saturated flow experiments, the monolith was previously saturated from the bottom (for 2 d). During the steady-state flow, a small ponding depth of 0.1 cm was maintained at the soil surface. The solute was applied by removing the irrigation system and, once the ponding has disappeared, by adding a given volume of CaCl2–loaded water (see Table 2).

Because of technical problems with the data logger, TDR breakthrough curves (BTCs) could not be recorded for the Exp.1 and outlet BTC for the Exp. 7 (Table 2). They therefore do not appear in the following graphics and tables.

The water content during the leaching experiments was estimated from the TDR readings using the Topp calibration equation (Topp et al., 1980). The steady-state flow rate was estimated both from the tipping bucket measurements at the outlet of the monolith as well as from the measurement of the mean volume of the top reservoir.

Estimating Solute Transport Properties at Local and Meso-Scale
The time-integral normalized resident concentration Crt*(z,x,t) at time t of a surface applied solute within the TDR sampling volume positioned at location x and at depth z is defined as (Vanderborght et al., 1996):

[11]

By relating Cr(z,x,t) to the impedance of a soil sample Z(z,x,t) ({Omega}) (Eq. [A8]), Crt*(z,x,t) is directly derived from the TDR readings as follows (Vanderborght et al., 1996):

[12]
with 1/Z*(z,x,t) = 1/Z(z,x,t) - 1/Z0(z,x), where Z0(z,x) ({Omega}) is the TDR load at infinity before the solute pulse is added and TC, the temperature correction factor at 25°C. The TC is considered uniform at a given depth z and is calculated as (Heimovaara et al., 1995):

[13]
in which T(z) is the temperature (°C) measured at the same depth z at which the bulk electrical conductivity is measured and {alpha}C (°C-1) is a temperature correction coefficient. Mean time-integral normalized resident concentration at each depth z was obtained by averaging time series (see Appendix 2):

[14]

Outlet ECw(z,t) (µS cm-1) were transformed to time-integral-normalized flux concentration Cft*(z,t) by:

[15]
which equals the travel time probability density function ff(z,t) when the solute input is a narrow pulse when steady-state flow occurs (Jury and Roth, 1990).

Equation [12] defines local scale time series and Eq. [14] and [15] are assumed to define time series representative at the scale of the cross-section of the monolith, called hereafter ‘meso-scale’.

Apparent dispersion and velocity were obtained from the CDE definition through adequate resolution of Eq. [1] in two different ways: (i) fitting the calculated time series of Crt* and <Crt*> inferred from the TDR readings to the analytical solution of the CDE in terms of Crt* by minimizing the mean square error (least squared method, LSM) and (ii) equaling the theoretical and experimental central time moments (method of moments, MM). All calculations were done in a Matlab environment (Matlab 5.3, The Mathworks Inc., Natick, MA). To determine the mixing regime, an apparent longitudinal hydrodynamic dispersivity was obtained by Eq. [2].

The analytical solutions of the CDE and time moments in terms of Crt* for a Dirac delta input pulse and a semi-infinite medium, assuming that there is no solute present in the system initially, were obtained from Jacques et al. (1998). For the outlet BTC, we used the travel time probability density function for a 3rd type input function (Jury and Roth, 1990).

Local scale solute transport parameters (at the scale of the TDR sampling window) will be denoted with the superscript l (e.g., {lambda}lL and l for, respectively, apparent dispersivity and velocity) whereas the meso-scale solute transport parameters resulting from the mean of three local BTCs or from the outlet BTCs will be denoted with superscript m.

Statistical Analysis
To discriminate the effect of the location and the depth on the parameters at the local scale (the scale of the TDR sampling window) and meso-scale (the scale of the soil core), analyses of variance (ANOVA1 or ANOVA2) were performed using the statistical toolbox of Matlab. Statistical significance was assessed at the 0.01 and.05 probability levels.

Given the small sampling points, standard deviation estimates were calculated following the equation (Dagnelies, 1998):

[16]


    RESULTS AND ANALYSIS
 TOP
 ABSTRACT
 INTRODUCTION
 THEORY
 MATERIALS AND METHODS
 RESULTS AND ANALYSIS
 CONCLUSIONS
 APPENDIX 1
 Appendix 2
 REFERENCES
 
Spatial Scale and Flow Rate Dependency of the Local Scale Solute Transport Parameters
Spatial Scale Dependency
For each TDR probe, 11 local scale apparent dispersivities, {lambda}lL, and velocities, l, were estimated by inversion of the CDE, one for each experiment/flow rate. In general, BTCs were unimodal and CDE equations fit the experimental curves pretty well with a determination coefficient (r2) between 0.9 and 1 (see Fig. 2) . At that local scale, the LSM and the MM gave very similar results. To simplify the discussion, we show in the subsequent part only the results obtained by the LSM.



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Fig. 2. Local scale (top) and meso-scale (bottom) breakthrough curves (BTCs) during Exp. 7 (see Table 2). The six local scale BTCs were measured by time domain reflectometry (TDR) Probes 1 to 6 (see Fig. 1). Gray line shows the fitted BTC.

 
For each position where a TDR probe is located, we obtained a set of local scale solute parameters, corresponding to the different flow rate experiments. Figure 3 shows the mean and standard deviation of the apparent dispersivity. We observe that {lambda}lL is quite small compared with local scale dispersivity values reported by Beven et al. (1993). This can be explained by different factors. First, these values are similar to those obtained by Maraqa et al. (1997) for soils of comparable texture ({lambda}lL from 0.99 to 1.6 cm). In addition, this low value can also be related to the layering of our sample, which can inhibit preferential flows and increase the mixing as reported by Porro et al. (1993).



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Fig. 3. Local-scale dispersivity as a function of soil depth obtained by using the LSM method (Probes 1 to 6: squares, Probes 7 to 9: circles, and probes 10 to 12: triangles). Error bars show the standard deviation. For improving readability, the {lambda}L values obtained from time domain reflectometry (TDR)-readings positioned at the same depth have been a slightly shifted on the depth-axis.

 
The {lambda}lL situates around 0.7 cm for the three upper probes located at 0.15-m depth (TDR5, TDR8, and TDR11), and further down in the soil profile, it increases suddenly to 1 cm where it remains fairly constant. Thus, the transport process at the local scale is CD from at least 0.30-m depth and, consequently, Eq. [9] should be used to characterize {lambda}lL below this depth. Similar observations of an increase of the dispersivity at shallow depths at the meso-scale were made by Seuntjens et al. (2001). The increase of the shallow depth dispersivity in this study was related to the presence of a Spodic horizon, which enhanced the lateral mixing. In our case, similar effect due to layering is also likely, even if the scale of this layering (<5 cm thick) and the relatively small textural difference is not as important (see Table 1). However a gradual effect is also possible. In any case, the observed scale effect at shallow depths depends on the micro-scale variability of the flow field within the porous medium at the local scale inducing a SC process. Therefore, the l* indicating the apparent depth discriminating between a SC and a CD process (see Eq. [9] and [10]) should be situated between 0.10- and 0.30-m depth. Below this depth, constant {lambda}lL may be attributed either to a uniform subsoil or to a stabilization effect due to the layering, as observed by Porro et al. (1993).

We also note a remarkably small variations of {lambda}lL in terms of flow rate (see further) and in terms of the horizontal position within the monolith. This high uniformity of the local scale dispersivity should be emphasized.

Figure 4 shows the local scale mean solute velocities l estimated from the local scale BTCs observed with the three upper TDR probes (TDR6, TDR9, and TDR12). For a given flow rate, l differs at each location. However, the velocity pattern seems consistent for the different flow rates. The l estimated for TDR9 are systematically lower than those estimated for the other positions. Since the position of the irrigation device was changed for each new experiment, the constant velocity patterns reflect the intrinsic physical behavior of the porous medium. A constant velocity pattern was also observed by Buchter et al. (1995) in a stony soil monolith, when carrying out two consecutive BTC experiments at the same flow rate.



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Fig. 4. Local-scale velocities estimated at TDR6, TDR9, and TDR12, represented respectively by the first, second, and third bar for each experiment.

 
Flow Rate Dependency
Figure 5 shows the mean and standard deviation of {lambda}lL versus log(Jw). The flow rate effect on {lambda}lL was insignificant as confirmed by a ANOVA2 test statistic (P = 0.017). This is in contrast to the studies of Jardine et al. (1993), Padilla et al. (1999), and Maciejewski (1993) who showed an increase of the dispersivity with a decrease of the water content and to the study of Vanderborght et al. (1997) showing an increase of {lambda}lL with the flow rate.



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Fig. 5. Local-scale dispersivities in terms of flow rate. Error bar shows the standard deviation obtained from observations at 12 different probe locations.

 
This could be attributed to the slight layering of our sample. Indeed, this could prevent the activation of continuous macropores which would have increased the both CVv and l*. On the other hand, layering make the flow paths converge or diverge at the interfaces (Koch and Flühler, 1994). It may increase the tortuosity whatever the flow rate, which could counterbalance a possible reduction of the tortuosity within the different layers. This will also result in rate-independent CVv and l*.

Figure 6 shows the observation of l in terms of depth and flow rates. As for the horizontal pattern, the vertical pattern of distribution of l is consistent for the different flow rates. This elucidates the persistency of the transport process in the different ‘stream tubes’.



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Fig. 6. Local-scale velocity for TDR1 to 6 for 12 different flow rates. Figures refer to experiments number.

 
Spatial Scale and Flow Rate Dependency of the Meso-Scale Parameters
Spatial Scale Dependency
As described before, meso-scale parameters were obtained from two types of measurement: horizontally averaged local scale BTCs <Crt*(z,t)> at three depths (0.15-, 0.45- and 0.75-m depth), and flux concentration ff(z,t) at the outlet of the column at 1-m depth. Because of larger variation between curves (see Fig. 2), we also used the MM to estimate the parameters.

Figure 7 illustrates the depth dependency of the mean and standard deviation of the meso-scale dispersivity {lambda}mL. We observe that the two methods, the MM and LSM, yield similar results, except for a depth of 0.4 m where MM overestimates {lambda}mL as compared with LSM. This is probably because the velocity variation at that depth is quite large, which produces multi-modal averaged BTCs from some flow rate. It appears also that the dispersivity value obtained from the outlet time series is remarkably similar to the dispersivity estimates from the meso-scale time series from TDR probes. This confirms the assumption made at the beginning of equivalence of scale between those two types of meso-scale time series.



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Fig. 7. Meso-scale dispersivity versus depth. Circles represent the dispersivity obtained by the least square method (LSM) while squares those obtained by moment method (MM). Error bars show the standard deviation.

 
Although the local scale dispersivity did not significantly scale with depth, the meso-scale dispersivity significantly increases with depth, as confirmed by an ANOVA2 test statistic (P = 3.5 x 10-7). In contrast to {lambda}lL, {lambda}mL seems not to reach a constant value at 1-m depth. Therefore, one may deduce that the mixing regime at that scale is SC and that l* is larger than 1 m. Contrary to what we observed at local scale, non-uniform layering and higher scale heterogeneities (siliceous concretions, for instance) prevent a complete mixing between flow paths at least above 1-m depth. Hence, l* depends very much on the scale of observation.

We further observe that {lambda}mL at 0.75-m depth is at least two times larger than {lambda}lL. This can be related to the higher heterogeneity encompassed in the solute flow domain at the meso-scale, which increases the CVv. It will have, of course, significant consequences for the real world predictions of solute transport. From a practical point of view, these experiments justify the use of at least three TDR probes at the same depth to obtain a valuable estimation of the meso-scale dispersivity.

Flow Rate Dependency
Figure 8 shows the estimated {lambda}mL estimated from <Crt*(z,t)> at z = 0.75 m and ff(z,t) at z = 1 m. As confirmed by a ANOVA2 test statistic, the {lambda}mL remained in the same order of magnitude for all flow rates and are nearly twice as high as {lambda}mL. No significant differences between MM and LSM estimates could be discerned. In addition, the differences between parameters for the 0.75-m soil depth and the 1-m soil depth are small, showing that flow rate does not affect {lambda}mL. This could again be attributed the layering, which stabilize the CVv. To have an estimation of the CVv, a coefficient of variation of l, CVl (z,Jw), was calculated at each depth and flow rate (with only three replicates). Indeed, it was observed (not shown here) that CVV was completely independent of l and Jw.



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Fig. 8. Meso-scale dispersivity at 0.75-m depth estimated by least square method (LSM) (squares), by moment method (MM) (triangles) and dispersivity estimated from outlet breakthrough curves (BTCs) at 1-m depth estimated by LSM (time sign) and MM (plus sign).

 
However, this could also be partly explained by the bottom boundary condition used in our experiments (seepage face), which did not allow the observation of a wide range of different water content (see Table 2). Consequently, the soil water content increase when higher flow rates were imposed did not activate enough new pore domains (or reduce the tortuosity) to increase (or decrease) the CVv significantly.

Linking the Meso- and Local-Scale Parameters Relationship between CVl and {lambda}mL
To evaluate the contribution of the apparent local velocity variation to the meso-scale apparent dispersivity, we will compare the CVl (z,Jw) to {lambda}lL. For the sake of simplicity, the notation ‘CVV’ will be used, instead of CVl (z,Jw).

Figure 9 shows the {lambda}mL–CVV relationship for the {lambda}mL estimated by the LSM. This figure shows a clear linear and depth dependent relationship. At 0.15- and 0.75-m depth, the scattering of the points is small. Hence, for these depths, the local-scale velocity variations explain the meso-scale dispersivity to a large extent. At 0.45-m depth, however, the meso-scale dispersivity could not be explained by this CVV (r2 = 0.10), probably because velocity variations were too small. The linear regressions between {lambda}mL and CVV yields slopes of 11.4 and 18.1 cm for the 0.15- and 0.75-m depth respectively. The increase of this slope parameter with depth is consistent with an identified SC transport process at the meso-scale level.



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Fig. 9. Meso-scale dispersivity vs. coefficient of variation of the local scale velocities squared. Triangles, squares and plus signs stand respectively for dispersivity estimated at 0.15-, 0.45-, and 0.75-m depth.

 
Using Eq. [10], and assuming that the CVV is an acceptable estimator of CVv, the travel depths are respectively, 23 and 36 cm, which differ from the actual transport depth (0.15- and 0.75-m depth). This difference could be explained by the fact that CVV is based on a sample of three local scale BTC measurements that may introduce bias and that the pore-scale velocity variation is not considered when the TDR sampling methodology is used (Seuntjens et al., 2001; Vanderborght et al., 1997). In addition, the intercept in Fig. 9 is inconsistent with the theory leading to Eq. [9] and [10]. Similar observations were obtained by Vanderborght et al. (2001).

It is worth noting that the CVV is completely independent of l (not shown here). This could confirm our assumption that this reflects a intrinsic characteristic of our subsoil sample. However, as already said, our CVV estimate is may be too rough to show the actual dependence.

Meso-Scale {lambda}mL Estimated from Lognormal Distribution of Local Scale {lambda}lL
From our results, it appears that the mixing regime is CD at the local scale and SC at the meso-scale. Therefore, we can model transport at the meso-scale by considering the monolith as an ensemble of parallel stream tubes through which the solute is transported following a CD process. Assuming that l and Dl are independent and log-normally distributed, Jury and Roth (see problem 4.7. in Jury and Roth, 1990) defined {lambda}mL for such a system as:

[17]
with µ the mean and {sigma}2 the variance of Dl or l. We estimated µD, {sigma}2D, µV and {sigma}2V from the Dl and l distribution. Note that, for a log-normal distribution, the term in Eq. [17] is the square root of the coefficient of variation of ln. The second term therefore reflects the variability in the local velocity field and is depth dependent.

Comparison between {lambda}mL calculated from Eq. [17] and {lambda}mL estimated from averaged BTC and outflow BTC is given at Fig. 10 for three depths and 11 flow rates. Mean local scale dispersivity values <{lambda}lL> are also given to show the specific contribution of local scale to {lambda}mL. Note that, from Eq. [17], three outliers came from a bad estimation of the variance. Those are not shown in Fig. 10 and the determination coefficient calculated without those three points was significant (r2 = 0.66). This confirms that the stream tube theory allows the scaling of the observed solute transport in the monolith to a reasonable extent.



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Fig. 10. Meso-scale dispersivity estimated from Eq. [17] (closed circles, right axis) versus meso-scale dispersivity obtained from averaged BTCs. On the left axis, open circles represent the local scale dispersivity.

 

    CONCLUSIONS
 TOP
 ABSTRACT
 INTRODUCTION
 THEORY
 MATERIALS AND METHODS
 RESULTS AND ANALYSIS
 CONCLUSIONS
 APPENDIX 1
 Appendix 2
 REFERENCES
 
Through a series of 11 solute breakthrough experiments, flow rate, and scale dependencies of the solute transport process have been elucidated in a monolithic subsoil sampled in an aquifer deposit. We observed that:
  1. The mixing length l*, and therefore the apparent transport process, depends on the measurement scale. At the local scale (4 x 10-2 m2), l* was lower than 0.3 m whereas at the meso-scale (0.5 m2) l* exceeded 1 m. It confirms that both l* and the mixing regime depend on the scale;
  2. The flow rate does not affect {lambda}mL or {lambda}lL. We attribute this insignificance to the slight layering which prevents the formation of preferential flow paths and stabilize both the CVv and the l*. However, the adopted experimental protocol, in particular the control of the bottom boundary condition during the BTC experiments, did not permit us to explore a large range of water content (see Table 2);
  3. The local scale dispersivity deviates from the meso-scale {lambda}mL by a factor of 2 at 0.75-m depth. This can be related to the higher heterogeneity encompassed in the solute flow domain at the meso-scale, which increases the CVv. Hence several TDR probes at a given horizontal depth need to be installed in large soil columns if a reliable estimate of the meso-scale dispersivity is needed;
  4. The meso-scale {lambda}mL can be linearly related to an estimate of the coefficient of variation of the apparent velocity with a slope proportional to the depth. This is characteristic of a SC mixing process;
  5. The meso-scale solute transport in an undisturbed soil monolith could be reasonably well described by a stream tube model in which transport in each stream tube follows a CD process;
  6. However quantitative relationships between structure, flow rate, and dispersivity have still to be found and more research is needed to assess the transport regime at a larger scale and relate the mixing length to the scale of interest.


    APPENDIX 1
 TOP
 ABSTRACT
 INTRODUCTION
 THEORY
 MATERIALS AND METHODS
 RESULTS AND ANALYSIS
 CONCLUSIONS
 APPENDIX 1
 Appendix 2
 REFERENCES
 
Constraints on CVV(z) for a Stochastic-Convective Process
Considering the spread of arrival time {sigma}2t around the average value E(t) at a given depth z, an alternative definition of the longitudinal dispersion is (Simmons, 1982):

[A1]
where {sigma}2t the variance of the solute travel time pdf. Combining with Eq. [8], it yields:

[A2]

For a SC process, the solute travel time pdf scales with depth as follows (Jury and Roth, 1990):

[A3]

Inserting Eq. [A3] in [A2] yields:

[A4]
and hence:

[A5]


    Appendix 2
 TOP
 ABSTRACT
 INTRODUCTION
 THEORY
 MATERIALS AND METHODS
 RESULTS AND ANALYSIS
 CONCLUSIONS
 APPENDIX 1
 Appendix 2
 REFERENCES
 
Mean Time-Integrated Normalized Resident Concentrations
Large scale resident concentration at a depth z can be obtained by averaging n local BTCs at locations x and depth z as (Vanderborght et al., 1996):

[A6]

By inserting Eq. [A6] in the definition of Crt* (Eq. [11]), if n = 3, it yields:

[A7]

Cr(z,x,t) is usually defined as (see e.g., in Vanclooster et al., 1995)

[A8]
with K(z) a calibration constant and TC, the temperature correction factor at 25°C. After plugging Eq. [A8] in [A7], it gives Eq. [14].

Received for publication May 28, 2002.


    REFERENCES
 TOP
 ABSTRACT
 INTRODUCTION
 THEORY
 MATERIALS AND METHODS
 RESULTS AND ANALYSIS
 CONCLUSIONS
 APPENDIX 1
 Appendix 2
 REFERENCES
 




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