Click Here JOURNAL OF GEOPHYSICAL RESEARCH, VOL. 113, F01014, doi:10.1029/2006JF000714, 2008 for Full Article Modeling weathering pathways and processes of the fragmentation of salt weathered quartz-chlorite schist T. Wells,1 G. R. Willgoose,1 and G. R. Hancock2 Received 19 October 2006; revised 5 August 2007; accepted 9 November 2007; published 29 February 2008. [1] The relationship between the rate of rock breakdown and environmental and geological factors must be understood in order to establish the conditions under which weathering limits erosion. In this study qualitative and quantitative models of the rock fragmentation process are fitted to previously published data obtained from laboratory salt weathering trials of quartz-chlorite schist. Weathering was modeled as a combination of (1) a fragmentation event that fragments the parent particle into a number of daughter particles while preserving mass, and (2) a fracture probability, that determines the probability that a fragmentation event will occur in a given time period. We show that observations of the complex breakdown of salt weathered schist are consistent with model assumptions of a simple fracture geometry model and an increase in fracture probability with time. For the fragmentation geometry the best fit to the experimental data was achieved by assuming that each fragmentation event involves splitting of the parent particle into two daughter fragments of equal volume. For the fragmentation rate the data could best be described with a fracture probability, and hence the weathering rate, that increased linearly with time. This paper shows that it is possible to use a physically based fragmentation model to infer the process of fragmentation for individual particles using a time evolving particle size distribution for the weathering rock fragments. Citation: Wells, T., G. R. Willgoose, and G. R. Hancock (2008), Modeling weathering pathways and processes of the fragmentation of salt weathered quartz-chlorite schist, J. Geophys. Res., 113, F01014, doi:10.1029/2006JF000714. 1. Introduction [2] The erodibility of the surface of newly constructed, man-made landforms can change dramatically in just a few decades [Moliere, 2001]. However, we are unable to predict with certainty the rate, or in some cases the dominant processes and pathways, of soil erodibility and soil production over design lifetimes (typically 100-1000 years). This is in large part due to the fact that current physically based erosion models assume that the surface properties do not evolve over time, or with cumulative erosion and deposition. Recent theoretical work with landscape evolution models has highlighted that weathering of the coarser, non-transportable rock material can act as the rate limiting step in the erosion process particularly over the medium to long-term (100s to 1000s of years) [Willgoose and Sharmeen, 2006; Sharmeen and Willgoose, 2006, 2007]. By adapting river armoring models [e.g., Parker and Klingeman, 1982] for erosion on hillslopes Willgoose and Sharmeen showed that hillslope erosion rates decline over time as fine material is selectively removed from the land surface until eventually a stable armor of coarse particles is formed. Thereafter the fine 1 School of Engineering, The University of Newcastle, Callaghan, New South Wales, Australia. 2 School of Environmental and Life Sciences, The University of Newcastle, Callaghan, New South Wales, Australia. Copyright 2008 by the American Geophysical Union. 0148-0227/08/2006JF000714$09.00 material generated by weathering of this armor is the only sediment available for transport so that erosion becomes weathering-limited. [3] To improve our predictions of the evolution of soil properties and weathering-limited erosion, we need to estimate not only the rate at which fine, transportable material is produced from the weathering of larger, nontransportable particles but also the resultant fragment size distribution and how that distribution evolves over time. This quantitative analysis of the rock weathering process represents a significant shift in emphasis from previous, more qualitative, work which concentrates on the pathways of breakdown rather than the rates of breakdown and the physical properties of the weathering products [McGreevy and Smith, 1982]. [4] Many studies [e.g., Cooke, 1979; Sperling and Cooke, 1985; Williams and Robinson, 1998, 2001; Rivas et al., 2003] utilize the change in mass of the largest (or collection of suitably large) fragment(s) to characterize the extent of the weathering process. Other studies [e.g., Davison, 1986] report only the total mass of debris produced. None of these studies provide information on the particle size distribution (PSD) of the weathering products. [5] Other studies examine the potential of salt weathering and other processes as possible sources of loess and silt sized particles, [Goudie et al., 1979; Pye and Sperling, 1983; Wright and Smith, 1993; Wright et al., 1998; Wright, 2001], and have presented a more detailed picture of the size distributions of rock debris produced. Fahey F01014 1 of 12 F01014 WELLS ET AL.: MODELING ROCK WEATHERING PATHWAYS [Fahey, 1983, 1985; Fahey and Dagesse, 1984] reports particle size distribution data for debris produced through the salt, freeze/thaw and wet/dry weathering of a variety of rock and aggregate materials including sandstone, dolomite, shale and schist. Unfortunately these studies report the fragment size distribution at only a few discrete times, such as at the beginning and end of weathering. Goudie [1986] and Wright et al. [1998] provide more detail with snapshots of sediment size distribution produced from sandstones samples after 40 and 60 salt weathering cycles. To develop fragmentation models suitable for input into erosion models, detailed PSD data have recently been collected by our research group for quartzchlorite schist cubes and fine aggregates undergoing salt weathering in a simulated tropical environment [Wells et al., 2006, 2007]. [6] The data presented in these latter studies are difficult to interpret directly because they involve the evolution of numerous interrelated sizes fractions. The change in one size fraction represents the net effect of population depletion due to breakdown into smaller size fractions and population increase due to the breakdown of larger size fractions. To allow the PSD evolution data to be used in landscape evolution and soil production models, such as SIBERIA [Willgoose et al., 1991] and ARMOUR [Willgoose and Sharmeen, 2006] we must model the evolution of the PSD. In this paper we will fit a physically based fragmentation model to the evolving PSD. The model we discuss here characterizes both the kinetics of the weathering process, (the probability of any single fragment fracturing per unit time, Pfr, or fragmentation rate), and the size distribution of the daughter particles produced by the fragmentation event, (i.e., the fragmentation geometry). [7] We determine if the fragmentation of schist due to salt weathering [Wells et al., 2006, 2007], can be successfully modeled using a range of simple fragmentation models. We also examine relationships for fracture probability with time. These models provide insights into the nature of the weathering process which are otherwise obscured by the complexity of the evolving size distribution data. 2. Rock Fragmentation Data [8] The rock fragmentation data we use were obtained from the salt weathering of quartz-chlorite schist specimens recovered from the Ranger Uranium Mine waste rock dumpsite located in the tropical monsoonal Kakadu region of the Northern Territory of Australia. The full details of the experimental procedures, chemical and mineralogical composition of the schist, and measured fragmentation data are reported elsewhere [Wells et al., 2005, 2006, 2007; hereafter collectively Wells]. [9] This study focuses on three data sets. We use data from Wells’ most aggressive salt weathering experiments because they produced a more complete picture of the weathering process than the less aggressive experiments which were terminated before complete conversion of the starting material to fines (particles of <1% of the original sample mass). This enabled a more rigorous testing of the different fragmentation models and comparison of competing weathering hypotheses to be undertaken. The experimental results may or may not be indicative of the dominant F01014 weathering process and/or post-weathering grading of less aggressive experiments or field behavior, but they are adequate for the purposes of this paper, that is, demonstrating that we can fit a physically based fragmentation model to an evolving particle size distribution, and that this evolving particle size distribution is sufficient to determine which weathering processes are responsible for the observed particle size distribution. Moreover, Wells et al. [2006] suggests, subject to the limited duration of their experiments, that the particle size distributions of the less and more aggressive experiments were indistinguishable, provided their timescale was adjusted to reflect the higher breakdown rates experienced by samples subjected to the harsher weathering regimes. [10] Two of the data sets pertain to the fragmentation of 1 cm schist cubes over 60 cycles of aggressive salt weathering; daily immersion in a 250 g/l MgSO4 solution coupled with either a 60° or 100°C temperature cycle. The critical temperatures for hydration of MgSO4 salts [Mellor, 1960] are 48.2°C for conversion from MgSO 4 .6H 2 O to MgSO4.7H2O (12% volume change) and 67.5°C for conversion from MgSO4.6H2O to MgSO4.H2O (135% volume change). As a result salt weathering is more aggressive over the 100°C weathering cycle which includes both hydration steps. We individually weighed each resulting fragment, grouping the mass distribution data into 5 categories; fragments >50% of the original block mass, 25– 50%, 10– 25%, 1 – 10% and <1%. Salt located both within and on the surface of the fragments was included in our weight determinations, however the salt contribution was found to be typically c. 5% by mass and consequently the trends indicated by the salt inclusive weights are indicative of the fragmentation processes [Wells et al., 2007]. The fragment mass distributions for the 9 replicates at 100°C (Figure 1) and 3 replicates at 60°C were then averaged to obtain the evolving fragment mass distribution. [11] The third data set relates to the salt weathering of a sub 500 mm powder generated by the crushing of the schist from the same parent material used for the cube experiments. Here we use data from one of the more aggressive salt weathering regimes; 45 cycles of daily immersion in 250 g/l MgSO4 solution with a 100°C temperature cycle. A laser particle sizer was employed to determine the PSD over time (Figure 2). [12] The rock samples used by Wells were chosen to reflect the typical rock type, and size, found on the surface of the Ranger Uranium Mine (RUM) waste rock dump. The RUM ore body lies in an area dominated by quartz-chlorite schists and the waste rock dump surface gravels are ‘. . .dominated by schist fragments, platy in shape, and largely 1 to 2 cm in diameter’ [Riley, 1994]. Wells used as their source material two quartz-chlorite schist samples collected from newly mined material deposited on the surface of the dumpsite. The two rock samples were retrieved within 10 m of each other at the dump site, and reflect the same mined stratigraphy and locality. Salt weathering was carried out on schist cubes cut from the interior of the two parent rocks well away from any obvious weathered rind or internal cracks. The chemical and mineralogical compositions of the parent rocks were determined by X-ray fluorescence and semi-quantitative X-ray diffraction [Wells et al., 2006]. XRD analysis revealed that the two samples 2 of 12 F01014 WELLS ET AL.: MODELING ROCK WEATHERING PATHWAYS F01014 breakdown and we believe that they may be indicative of field behavior [Wells et al., 2006]. 3. Description of Rock Fragmentation Models [14] The size and quantity of fragments produced by weathering is a product of the fragmentation geometry and rate of breakdown. We use four fragmentation models that we have computationally studied previously [Sharmeen and Willgoose, 2006]. Each of these fragmentation models consists of (1) a fragmentation geometry function describing the morphology (size and number) of fragments produced from a parent particle and, (2), a weathering rate expression, parameterized by a time varying probability of fracture per unit time for the parent particle. 3.1. Weathering Geometry [15] The geometry of the weathering process governs the grading of the (fine) transportable material generated, and the subsequent rate of erosion on the landform surface being weathered. Sharmeen and Willgoose [2006] showed, for instance, that a mass of rock which weathers via the granular disintegration of fine surface particles will produce a markedly different erosion history from one where parent fragments split into two equal sized daughter fragments. In our study four simple weathering geometries were investigated, three involving the fracturing of the rock along a cracked surface, and one involving the flaking of fine particles from a thin surface layer (Figure 3). These models, summarized below, are discussed in detail in Sharmeen and Willgoose [2006, 2007]. 3.1.1. Symmetric Fragmentation [16] A parent fragment, volume V, fractures into Nfr daughter particles of equal volume (Model 1 in Figure 3) such that: Vfr ¼ Figure 1. Fragment mass distribution profiles of schist samples subjected to an aggressive salt weathering regime. [Daily immersion in 250 g/l MgSO4 solution and 100°C drying cycle; average of 9 samples. Error bars represent ±1 standard deviation]. were mineralogically similar, both being quartz-chlorite schists. Thin section analysis indicated that both source rocks were originally quartz-biotite schists that had been strongly altered by infiltration of a low temperature hydrothermal fluid, which converted the original biotite content to chlorite and a white mica. [13] The aim of this study was primarily to test the validity and applicability of using simple physically based rock fragmentation models to simulate observed rock fragmentation. The question of how representative the laboratory fragmentation results are of field behavior is not the central focus of this paper. However, the analysis that follows will highlight the advantages and limitations of laboratory weathering data as a means of parameterizing a physically based model of rock fragmentation. Accordingly, data from more aggressive weathering regimes were used. These regimes produced the greatest level of fragment V Nfr ð1Þ Figure 2. Particle size distribution of unweathered schist powder (.) and schist powder after 45 cycles of daily immersion in 250 g/l MgSO4 followed by drying at 100°C (6). 3 of 12 WELLS ET AL.: MODELING ROCK WEATHERING PATHWAYS F01014 F01014 Figure 3. The four fragmentation geometries examined in this study. [17] The number of daughter particles, Nfr, can be constant or a function of parent size [Lerman, 1979]: Nfr ¼ d dmin b ¼ V Vmin b=3 ð2Þ where d is the diameter of the parent particle, and dmin and Vmin are the minimum threshold parent fragment diameter and volume (in this paper nominally fixed at 0.1% of the initial particle volume). Constant b was varied between 0.005 and 1. 3.1.2. Asymmetric Fragmentation [18] The parent particle splits into two daughter particles of unequal volumes (Model 2 in Figure 3): Nfr ¼ 2 Vfr;1 ¼ aV ; Vfr;2 ¼ ð1 aÞV ð3Þ where a is the ratio of the daughter fragment volumes, and Vfr,1, Vfr,2 are the volumes of the two daughter fragments. Values of a ranging from a = 0.5 (i.e., symmetric fragmentation model, Nfr = 2) to a = 0.01 (i.e., granular surface disintegration) were examined. In all cases a was assumed to be independent of time and parent fragment size. 4 of 12 WELLS ET AL.: MODELING ROCK WEATHERING PATHWAYS F01014 3.1.3. Whitworth Fragmentation [19] A parent particle is broken into Nfr daughter particles with a volume distribution proposed by W.A. Whitworth [Lerman, 1979] (Model 3 in Figure 3): Nfr V X 1 or Vfr;j j¼1;Nfr ¼ Nfr j¼1 Nfr j þ 1 V 1 V 1 1 ;...; ; þ Nfr Nfr Nfr Nfr Nfr 1 V 1 1 1 þ þ ...: ...: þ 1 Nfr Nfr Nfr 1 Nfr i þ 1 ð4Þ [20] Fragmentation numbers of Nfr = 2, 3, 4 were used for the rock cube data, while a range from 2 to 10 was used for the powder. 3.1.4. Granular Surface Disintegration [21] A thin surface layer encompassing the parent particle breaks down to produce a collection of equal sized spherical daughter particles of diameter equal to the layer thickness, and a single large daughter particle with a diameter equal to the parent particle diameter less twice the layer thickness (Figure 3). The number of fine particles generated was calculated from volume continuity (Model 4 in Figure 3): Nfr;fine 6d 2 12d ¼8þ 2 dr dr ð5Þ where Nfr,fine is the number of fine daughter particles spalled from each parent particle, dr is the surface layer thickness, and once again d represents the parent particle diameter. For small parent particles (d < 2dr) the parent particle splits into 2 particles of equal volume. [22] The surface layer thickness, dr, was assumed to be either (a) a constant or (b) vary with time as [Bland and Rolls, 1998]: 1 dr ðnÞ ¼ kr nr ð6Þ where kr and r are constants (r 1), and n is the cumulative number of elapsed weathering cycles (a surrogate for elapsed time). 3.2. Weathering Rate [23] The weathering rate is parameterized by the fracture probability, Pfr, the likelihood of a parent fragment fracturing per unit time. Our unit of time is one weathering cycle. Three fracture probability models were considered: 3.2.1. Constant Rate [24] The probability of fragment fracturing in a single weathering cycle is constant and independent of time or fragment size. 3.2.2. Rate as a Function of Volume [25] The fracture probability decreases with particle volume. The relationship was derived from Weibull statistics of brittle failure. Weibull proposed that the survival probability, Ps, for a specimen of volume, V, under tensile stress, s, is [McDowell and Bolton, 1998]: m V s Ps ¼ exp Vref sT F01014 where s is the stress applied to the fragment in the current weathering cycle, sT is the tensile stress that causes failure in 63% of rock samples, Vref is the reference particle volume at which 63% of the samples fail, and m is the Weibull modulus which decreases with increasing variability in tensile strength. For chalk, stone pottery and cement m 5 [McDowell and Bolton, 1998]. We assumed that the applied stress, s, (in our experiments caused by hydration and/or crystallization during the salt weathering process), is independent of particle size. Lee [1992, as cited by McDowell and Bolton, 1998] observed that the mean tensile strength of the rock particles, sM, was related to particle diameter, d, in the following fashion: sM / d c ð8Þ where c is an exponent varying with rock type. Lee observed values of c from 0.35 to 0.42 for some sands and limestones. Assuming that the fragment is spherical with a density independent of size, sT / sM and s is constant, then equation (7) can be re-written as: Pfr ¼ 1 exp k1 V k2 ð9Þ where Pfr is the probability of fracture, Pfr = (1 Ps), k1 is a 1 , and is therefore depenfragmentation constant (/ smVref dent on the rock material and environmental conditions), and k2 is an exponent (=1 mc/3). In this study we fit k1 and k2. Using the data of Lee, and McDowell and Bolton k2 lies in the range 1.55 – 1.70, but for generality in this study k2 is restricted to a range of 1 – 2. 3.2.3. Rate as a Function of Time [26] Wells et al. [2006] observed that weathered cubes were increasingly susceptible to fracture as weathering progressed. To model this affect we assumed that each rock fragment possesses a fixed number of sites, S, which ensure the structural integrity of the rock sample, but which are vulnerable to weathering. After n cycles a fraction, (wS), of those sites have failed. If the rate at which vulnerable sites are weathered is proportional to the number of S sites remaining then d ðwS Þ ¼ k3 ðS wS Þ dn ð10Þ or dw ¼ k3 dn ð1 wÞ solving for w while noting that w = 0 when n = 0 leads to: w ¼ 1 expðk3 nÞ where k3 parameterizes the rate of decrease of vulnerable sites. [27] If it is assumed that the probability of fragmentation is linearly related to the fraction of weathered sites then: ð7Þ 5 of 12 Pfrn¼n ¼ Pfrn¼0 þ 1 Pfrn¼0 w ð11Þ F01014 WELLS ET AL.: MODELING ROCK WEATHERING PATHWAYS Figure 4. A comparison of the evolving fragment mass distribution from (1) an analytical solution and (2) a Monte Carlo simulation (200 simulations). Symmetric fragmentation, Nfr = 2, Pfr = 0.5. —: Analytical prediction; Monte Carlo Prediction: 6, >50%; &, 25– 50%; 4, 10 –25%; u, 1 – 10%; 5, <1%. n=n where Pn=0 are the probabilities of fracture at the fr , Pfr commencement, and cycle n, of the weathering sequence respectively. The fracture probability can then be expressed as the following function of elapsed weathering cycles: Pfrn ¼ Pfrn¼0 þ 1 Pfrn¼0 ð1 expðk3 nÞÞ ð12Þ [28] In this study both k3 and w were fit. [29] It should be noted that this model parameterizes weathering rate as a function of time by one particular mechanism. Other physical mechanisms that lead to a time varying weathering rate, (e.g., cumulative build up of crystallized salt in the rock fragment), can be postulated and they may yield different trends with time. We have not investigated alternative mechanisms for temporal trends because we believe that our data are insufficient to differentiate competing hypotheses for time varying weathering rates. 4. Fragmentation Model Validation Procedure 4.1. Cube Experiments [30] For the simpler weathering geometries and fracture probability scenarios, the mass distributions of fragments generated in the rock cube experiments were determined directly from analytical expressions (Appendix A, Figure 4). For more complex models, the rock material was partitioned into 400 size classes and a Monte Carlo simulation performed to determine an average temporal evolution of fragmentation. Figure 4 shows a comparison between one of the analytic solutions and a Monte-Carlo simulation. At the commencement of each weathering cycle a uniformly F01014 distributed random number (Prand = U(0, 1)) was used to decide whether a fragment would be fractured (i.e., when Prand < Pfr). After processing all volume fractions, the new volume distribution was recalculated. The process was repeated for each weathering cycle. The average of 200 Monte-Carlo simulations was used to determine the ‘‘average’’ fragmentation. Comparison of analytical profiles with the averaged numerical simulations suggested that 200 simulations were sufficiently accurate (Figure 4). [31] The fragment mass distribution profiles for the different breakdown models were then compared to the experimental data. There were insufficient data to do a statistical comparison, so we qualitatively assessed each model’s ability to predict the following key features: [32] 1. The dominance of large (>25%) fragments in the first 10 cycles. [33] 2. The lack of fines (<1%) production during the first 20 cycles. [34] 3. The successive ‘‘waves’’ of the intermediate volume fractions (25 – 50%, 10– 25% and 1 –10%) in the middle cycles. [35] 4. The peaking of the intermediate volume fraction at approximately 30– 60% of the original rock volume. [36] 5. The presence, or otherwise, of the ‘S’ shaped fines curve in the latter part of the trial. [37] 6. The relative positions of the coarse (>50%), and fine (<1%), fragment curves (important for erosion modeling). 4.2. Powder Experiments [38] The unweathered PSD (Figure 2) was used as the initial PSD in the powder weathering simulations. The experimental PSD profiles (Figure 2) show a depletion of particles in the 183– 224 mm and larger size categories, and a corresponding increase for particles smaller than 183 mm. Maximum depletion occurred in the 332 – 404 mm size fraction and maximum increase in the 124 – 151 mm size fraction. To improve model accuracy the experimental data were interpolated into 2000 finer size fractions. At the commencement of each weathering cycle the probability of fracture, (Pfr), of material in each of the size classes was determined, and a fraction of the material equal to Pfr was fragmented. Once each size fraction was calculated the new PSD was recalculated and used as input for the next cycle. After the final cycle the volume distribution was aggregated into the original experimental size fractions classes. [39] Each fragmentation model was assessed qualitatively by their ability to: [40] 1. Match the form, location, and width of the PSD profile of the coarse material (>100 mm). [41] 2. Reproduce the ‘debris tail’ (PSD < 50 mm). [42] 3. Match the cumulative volume distribution curve. [43] 4. Not produce bimodal, or higher modalities, which were absent in the experimental data. 5. Results 5.1. Cube Experiments 5.1.1. Symmetric Fragmentation [44] Table 1 summarizes the performance of each fragmentation model. The best fit to the experimental data was obtained using symmetric fragmentation with a low fracture 6 of 12 WELLS ET AL.: MODELING ROCK WEATHERING PATHWAYS F01014 F01014 Table 1. Goodness of Fit Ratings Achieved by the Various Rock Breakdown Modelsa Probability of Fracture Function Geometry 1.Symmetric fragmentation a) Nbr = 2,4,6,8 b) Nfr = fn(size) 2. Asymmetric fragmentation a = 0.005-0.5 3. Whitworth fragmentation Nfr = 2,3,4 4. Surface disintegration a) dr = constant b) dr = fn (time) Pf = 1 Pf = constant (<1) Pf = F (size) Pf = F (time) very poor very poor very good poor poor not tested excellent good very poor very good poor excellent poor poor poor very good very poor very poor very poor very poor very poor very poor very poor very poor a Each model was evaluated by assessing the number of criteria listed in the fragmentation model validation procedure which are achieved by the model: Very Poor: No criteria achieved; Poor: 1 to 2 criteria achieved; Good: 3 criteria achieved; Very Good: 4 to 5 criteria achieved; Excellent: all criteria achieved. number, Nfr = 2, coupled with a fracture probability that increased with time (Figure 5). The model was able to simultaneously fit both the decline of the coarse (>50%) fraction, and the rise of the fine (<1%) fraction. The position and magnitude of the intermediate size fractions was also superior to the other models. Higher fracture numbers, (up to Nfr = 8), produced less realistic simulations. Simulations with Nfr > 4 did not yield any material in the 25– 50% size fraction and overestimated early levels of fines (Figure 5). [45] Less satisfactory fits were obtained when using a constant fracture probability term. Best fits occurred when Pfr = 0.20 – 0.25 (Figure 5), however the timing of large fragment breakdown and the appearance of the intermediate size fractions was poorly modeled. [46] Symmetric fragmentation models with a size dependent fracture number Nfr, (equation (2)), also yielded unsatisfactory fits. The relative percentage of the coarse and fine fraction curves could not be reproduced without predicting unrealistically high values for the intermediate, (particularly the 1 – 10%), size fractions. [47] The inclusion of a size dependent fracture probability (equation (9)) resulted in poorer fits, with late fragmentation rates being drastically reduced (Figure 5) as particles became finer. 5.1.2. Asymmetric Fragmentation [48] This model was assessed for a values from a = 0.5, (equivalent to symmetric fragmentation, Nfr = 2), to a = 0.01, (more akin to surface disintegration). The best match to the data was obtained for a = 0.5 (Figure 6), indicating that symmetric fragmentation (Nfr = 2) was a more appropriate model. As for symmetric fragmentation, both constant and size dependent fracture probability produced poor fits. Best results were obtained with a fracture probability that increased with time. 5.1.3. Whitworth Fragmentation [49] Fracture numbers, (Nfr), of 2, 3 and 4 were investigated. Fragmentation distributions were dominated by the smaller size fractions (1 – 10% and <1%, Figure 6). Increasing the fracture number increased both the weathering rate and the dominance of finer fractions. [50] Low fracture number values and a fracture probability increasing with time again produced the best fit. The fit, however, was poorer than that observed for the symmetric and asymmetric fragmentation. While the coarse and fine fractions were well reproduced, there was a tendency for the 10– 25% and 25 –50% fractions to be under predicted. 5.1.4. Granular Surface Disintegration [51] All surface disintegration models performed poorly. Mass distribution profiles were characterized by the early development of a large amount of fine material (Figure 6) with intermediate size fractions almost completely absent. Figure 5. Fit of symmetrical fragmentation model to the experimental fragmentation data. —: Averaged experimental data; —: Time dependent fracture probability (Nfr = 2, Pfrn=0 = 0.03, k3 = 0.0105) – excellent fit. ——: Constant fracture probability, high fracture number (Nfr = 8, Pfr = 0.1) – poor fit. — —: Constant fracture probability, low fracture number (Nfr = 2, Pfr = 0.22) – good fit. >>>>: Size dependent fracture probability (Nfr = 2, k1 = 0.1, k2 = 1) – poor fit. 7 of 12 F01014 WELLS ET AL.: MODELING ROCK WEATHERING PATHWAYS F01014 [54] A constant fracture probability, Pfr = 0.03, resulted in the correct positioning of the particle distribution peak (183– 224 mm). Increasing the fracture probability simply shifted the peak to lower particle sizes at any given time. A size dependent fracture number increased the proportion of finer material but also created multiple peaks (Figure 7). A time dependent fracture probability, which improved the modeling of the cube weathering, did not improve the fit to the powder data. 5.2.2. Asymmetric Fragmentation [55] The performance of the asymmetric model, (for 0.01 a 0.5), was similar to the symmetric model with the best fit achieved when 0.2 < a < 0.5. As in the case of symmetric fragmentation, the main peak was well modeled while the tail was under predicted. Size and time dependent fracture probabilities did not produce any significant improvement. 5.2.3. Whitworth Fragmentation [56] The main deficiency of the above models was an under prediction of the fine debris tail. Employing a high fracture number, Nfr, in equation (4) generates a large range of particle sizes, and hence should perform better. For instance Nfr = 10 produces particles ranging in size from 0.3% to 97.5% of the volume of the parent particle. Nfr values from 2 to 10 were examined. In general a high fracture number gave a better fit to the fines data (<20 mm), however the intermediate size particles were over predicted and coarse particles under predicted (Figure 7). Figure 6. Fit of asymmetric, Whitworth fragmentation and granular surface disintegration models to the experimental fragmentation data. —: Averaged experimental data. —: Asymmetric model with time dependent fracture term (Pfrn=0 = 0.03, k3 = 0.010) for various a values, (a = 0.5). The case for a = 0.4 is also shown (— . —) – excellent fit in both cases. — —: Whitworth fragmentation model with time dependent fracture probability, (Nfr = 2, Pfrn=0 = 0.03, k3 = 0.01) – good fit. . . . .: Granular surface disintegration model, (Pfr = 1, dr/d0 = 0.025) – poor fit. 5.2. Powder Experiments [52] No model fulfilled all the criteria for fitting the powder data although several satisfied 3 out of the 4 conditions. As observed above for modeling cube breakdown, the three cracking models (symmetric, asymmetric and Whitworth models) all performed better than the surface disintegration model. 5.2.1. Symmetric Fragmentation [53] We examined fracture numbers, Nfr, from 2 to 8. Symmetric fragmentation scenarios with constant fracture probabilities and low fracture numbers (2 to 3) reproduced the weathered fragment PSD > 100 mm with a slightly broader peak width, however the fine debris distribution was not reproduced (Figure 7). To reproduce the finer particle population, higher fragmentation numbers were required. However, multiple peaks were then predicted, a feature not observed in the experimental data. Figure 7. A comparison of experimentally derived PSD —) with that predicted from several the fragmentation (— model. — + —: Symmetric fragmentation model with constant fracture probability (Nfr = 2, Pfr = 0.03). .....: Symmetric fragmentation model with size dependent Nfr term (b = 0.9, Vmin = 10, Pfr = 0.01). — . —: Whitworth fragmentation model with constant probability of fracture (Nfr = 10, Pfr = 0.03). — —: Granular surface disintegration model with time dependent fracture probability (dr = 10 um, Pfr = 0.01). 8 of 12 F01014 WELLS ET AL.: MODELING ROCK WEATHERING PATHWAYS 5.2.4. Granular Surface Disintegration [57] Once again the surface disintegration models performed poorly (Figure 7). Surface disintegration generated a localized peak of fine material at 10 mm with very little material in the 10– 100 mm range. Again, this reflects the propensity of the surface disintegration mechanism to create weathered daughter particles in a very narrow size range that is determined by the depth of the disintegrating surface layer. 6. Discussion [58] The results of this study show that the evolution of the fragment mass distribution produced during the salt weathering of a quartz-chlorite schist can be well represented using a simple fracture geometry and probability model. The geometry model indicates the mechanics of the fragmentation process. The probability term indicates how the weathering rate varies over time. Characterizing rock weathering in this fashion allows us to test the applicability of various rock weathering models using complex PSD data, which otherwise would be difficult to interpret. 6.1. Cube Experiments [59] The best fit was achieved by simply assuming that the rock fragments split in half, (symmetric fragmentation, Nfr = 2). The schistose nature of the samples [Wells et al., 2005, 2006] governs the breakdown geometry. Consequently the results obtained in this study may not be applicable to other rock types. Salt weathering of rocks types exhibiting more granular structures, (e.g., sandstones for example), might be better modeled with granular surface disintegration or Whitworth fragmentation geometries. [60] Two conclusions can be drawn. First, the entire fragmentation process, from weathering of the initial rock sample to the final production of fines, was satisfactorily described using a single fragmentation geometry, hinting at scale invariant behavior. From the limited study here it is impossible to say whether this is a general finding or specific to our rock and weathering regime. Data over a greater range of materials and weathering conditions are needed to draw more general conclusions. Secondly, the fragmentation geometry which best described the fracture process was one of the simplest examined; splitting the parent fragment into two daughter particles of equal volume. This is not simply a result of the average daughter particle size for Nfr = 2 being half that of the parent particle. We used the best fit parameters for the 50/50 split and simulated the case where the ratio a randomly varied from 0.1 to 0.9 at any time, while maintaining a long term average value of 0.5. This simulation gave a poorer fit to the data than when a constant value of a = 0.5 was employed. [61] We can also draw conclusions as to how the rate of weathering changes over time. Like Goudie [1986] and Davison [1986], we observed salt weathering rates accelerating with time, possibly as a result of increasing surface roughness, increasing pore volume, improved access for salt bearing fluids to the rock interior, and/or salt build up within the rock particles. In contrast, Goudie and Viles [1995] noted many factors that may decelerate the fragmentation rate. Wright et al. [1998], found that >90% of debris produced during a 60 cycle sandstone weathering trial was liberated in the first 40 cycles. A slowdown over time of the F01014 deepening of tafoni [Matsukura and Matsuoka, 1991], and the weathering of coastal bedrock [Mottershead, 1989], has also been reported. Rivas et al. [2003] and Williams and Robinson [1998] witnessed a linear reduction over time of the largest remaining fragment mass, after an initial period with little change. The deceleration of weathering observed in these studies may be attributable to pore plugging or preferential removal of more easily weathered rock in the early stages of the weathering process. Finally, Cooke [1979] observed a three stage salt weathering disintegration curve: (1) a initial phase with little or no observable change, (2) a longer period of rapid disintegration; and (3) a final phase in which the rate of weathering slows appreciably. [62] Wells et al. [2006] qualitatively concluded that acceleration/deceleration depended in part on the criteria used to characterize the weathering process. In Figure 1 the largest mass fraction (>50%) decreases linearly with time, while the production of fines (<1%) shows an initial period of acceleration (0-30 cycles) followed by a deceleration (30 cycles onwards). Consequently, in this paper we have used a more general approach to describe the weathering rate, characterizing the weathering rate by the fracture probability, Pfr. When modeling the schist fragmentation data shown in Figure 1, an adequate fit could only be obtained when the fracture probability increases with time (equation (12)). One explanation for this behavior arises from the Wells experimental procedure. In the Wells experiments salt solution was added after each drying phase, possibly leading to a build up of salt crystals in the particle. There was evidence of surface efflorescence on some of the larger particles in the laboratory as well as in the field, however smaller particles did not show this behavior. Another explanation is that the detrimental effects of previous weathering of the particle structure outweighed the increased resistance to fragmentation assumed for smaller particles. In both cases weathering history is important. [63] Finally, the modeling methodology in this paper can also be used to analyze the effect of changes in environmental conditions on the fragmentation process. For instance, Wells et al. [2006] showed that lowering the temperature cycle from 100°C to 60°C significantly slowed the fragmentation of schist rock cubes. Geometry parameters obtained from the modeling of the 100°C data in conjunction with a reduced weathering rate term were used = 0.03 and k3 = to model the 60°C data, (Nfr = 2, Pn=0 fr 0.001; Figure 8). The good fit achieved suggests that while the fracture probability was lower for the 60°C weathering cycle, the fragmentation geometry was unaffected by the change in temperature cycle. This result hints at the tantalizing conclusion that an increase in the temperature range may be a viable method of accelerating weathering experiments if all that is desired is the PSD produced by the weathering process. The weathering rate, however, would still need to be determined by other means. This is consistent with the qualitative conclusions of Wells et al. [2006]. 6.2. Comparing Cube and Powder Experiments [64] As noted earlier, the material used in the rock cube and powder experiments originated from the same source material and were weathered under similar conditions. Particle volumes examined in the two studies however differed by many orders of magnitude, (rock cube fragments 9 of 12 F01014 WELLS ET AL.: MODELING ROCK WEATHERING PATHWAYS F01014 an additional (second order) fragmentation process is operating which produces a range of very fine debris (perhaps via a surface disintegration process) when the finer schist powder is weathered. [66] A final point of contrast between the two studies is the role of fracture probability. For the rock cube fracturing, the initial fracture probabilities of about 0.03 increased over time to approximately 0.4 after 45 100°C weathering cycles. Fracture probabilities for the schist powders were of the order 0.01 – 0.03 and remained constant over 45 cycles. This represents about a 10 fold decrease in fragmentation rates for the powder. This reduction is most likely a consequence of the smaller particle size (equation (9)). The large disparity in particle sizes examined in the two studies (3 to 12 orders of magnitude) relative to the weathering rate (1 order of magnitude) suggests however that any size dependence of the fracture probability term is weak, which would explain why a size dependent fracture probability term did little to improve the fit of the fragmentation models. A more definitive conclusion would require further experimental data for size ranges intermediate between those of the cubes and powders examined here. Figure 8. Fit of symmetric fragmentation model to experimental fragmentation data obtained at lower drying temperature (60°C max). —: Averaged experimental data. — — —: Symmetric fragmentation model with time dependent fracture probability (Nfr = 2, Pfrn=0 = 0.03, k3 = 0.001). 0.03 to 3.3 cm3; powder fragments 6 1014 to 6 105 cm3). Despite this large difference, symmetric fragmentation with low fragmentation number (Nfr = 2) was found to provide the best model of the fragmentation process in both cases. This suggests that the dominant weathering mechanism was a scale invariant cleavage. [65] The symmetric fragmentation model however, was unable to characterize the <100 mm particle population for the powders. This may simply be a consequence of the dramatically differing size scales and measurement techniques employed in the two experimental studies. The powders were sized with a laser diffraction device while throughout the cube experiments the individual fragment masses were determined manually. One problem with laser sizing is that it returns the diameter of an equivalent spherical particle, so that it can be unreliable for non spherical particles such as the platy particles generated in the weathering of schist. It is also possible that very fine (<100 mm) material was generated in the cube experiments but was not observed or recorded. Finally, it is possible that 6.3. Implications for Future Work [67] A key finding of this study is that the rate of weathering, (modeled by the probability of fragmentation), and the grading of the weathering products, (modeled by the fragmentation geometry), can be separated. This result is consistent with the qualitative conclusions reached by Wells et al. [2006] who suggested that two sets of his experiments were consistent, one done using a field temperature range and one using a more extreme temperature range. The more extreme experiments produced more rapid weathering, however the PSD at early times was similar to that which occurred at later times in the lower temperature experiment. This tantalizing result suggests it may be possible to perform accelerated experiments in the laboratory to yield data on the evolution of the particle size distribution of the fragmentation products. Sharmeen and Willgoose [2006] showed that the particle size distribution was essential to the correct modeling of the impact of weathering on erosion. [68] The rate of weathering, which is difficult to determine in the laboratory even with realistic experimental conditions, might then be determined from field studies of weathered products (e.g., old mine waste dumps). This would yield a snapshot of weathering products at a given time rather than the evolution through time. This combination of laboratory and field data may eliminate the need to mimic field conditions in the laboratory to determine weathering rates. [69] We do not believe that all weathering model parameters can be determined from field data. Different models can yield the same end-weathering product, (i.e., exhibit equifinality), but have different temporal evolution. This suggests that field data from a material of one age of weathering exposure is unlikely to provide sufficient data to calibrate the weathering model. Thus both laboratory and field data are required to fully characterize the weathering process. 7. Conclusions [70] This study has shown that it is possible to model the breakdown of schist rock subjected to an aggressive salt 10 of 12 F01014 WELLS ET AL.: MODELING ROCK WEATHERING PATHWAYS weathering regime using a simple fragmentation geometry function coupled with a time dependent fracture probability. The approach adopted by the authors of using a fragmentation geometry coupled to a fracture probability term enabled some insight into the fragmentation process to be gained which would otherwise be lost in the complexities of the particle size distribution data. [71] Application of the model to the schist fragmentation data suggests the following: [72] (1) The fragmentation geometry is best described by assuming that each fragment splits into two daughter fragments of equal volume. [73] (2) Smaller particles, currently unidentified, with diameters of the order of the schist layer thickness or less, weather via another mechanism. [74] (3) The rate of weathering, (as represented by the probability of fragmentation), increased over time for the weathering of larger particles. [75] (4) The fracture probability showed a very weak scale dependence, with deceases in particle diameter of 3 – 12 orders of magnitude producing approximately 1 order of magnitude decrease in fracture probability. [76] (5) The rate of weathering, (in this study represented by the probability of fragmentation), and the grading of the weathering products, (modeled using the fragmentation geometry), can be separated. This suggests that it may be possible to determine PSD evolution from accelerated laboratory experiments while using field studies of weathered products to determine rates of weathering. [77] As stated earlier, the experimental results, (and hence the model outcomes), may or may not be indicative of less aggressive experiments, weathering involving other rock types or field behavior. The main purpose of this paper is to demonstrate a methodology for quantification of the effects of weathering in erosion. We have shown that it is possible to use these data to interpret and develop a systematic model of the fragmentation process. Sharmeen and Willgoose [2006] showed how this information can then be used to examine the relative effect of weathering, armouring and erosion, as well as the effect of the fragmentation process on erosion rate, and finally the possible erosion characteristics of a weathering slope. [78] There remain significant unresolved issues. These include: (1) the effect of environmental conditions on the weathering rate, and (2), the extent to which fragmentation characteristics are rock type dependent. Nevertheless, we feel that the approach described here points the way forward in assessing the long term evolution of the surface erodibility of disturbed hillslopes (e.g., rehabilitated mine sites) and engineered covers for encapsulation of waste (e.g., hazardous and nuclear waste dumps). F01014 volume, Vfr. If the rock population begins with a single rock fragment of volume, Vn=0 then the following analytical expressions are applicable. [108] Case 1. 0 < Pfr = constant < 1, Nfr = constant [109] When both the fracture probability, Pfr, and the break up number, Nfr, are constant, symmetric fragmentation of a solitary initial rock sample will produce fragments of n + 1 different individual volumes after n cycles of weathering. The volumes of the different fragments produced after n weathering cycles (Vnj ), and the total volume, Wnj , of fragments in each of the n + 1 volume fractions are: V n¼0 Vjn ¼ j ; j ¼ 0 ! n Nfr Wjn ¼ nj n¼0 n! j V ;j ¼ 0 ! n Pfr 1 Pfr ðn iÞ! ðA2Þ [110] Case 2. Nnfr,j = fn(Vnj ), 0 < Pfr = constant < 1 [111] Where the fracture number is a function of particle volume, (equation (2)), the volumes of the fragments produced and the total volume of each volume fraction are: d Vjn ¼ V n¼0 ðVmin Þe ; j ¼ 0 ! n where d = (1 3c)j and e = Wjn ¼ c 3 j1 P k¼0 ðA3Þ (1 3c)k nj n¼0 n! j V Pfr 1 Pfr ðn jÞ! ðA4Þ A2. Model 2. Asymmetric Fragmentation [112] A rock fragment of volume, V, fractures along a cracked surface to produce 2 sub-fragments of volumes, aV and (1 a)V. [113] Case 2. 0 < Pfr = constant < 1, a = constant [114] When both the fracture probability, Pfr, and the fracture ratio, a, are constant, asymmetric fragmentation of j¼nþ1 P a solitary initial rock sample will produce fragments of j j¼1 different individual volumes after n cycles of weathering. The volumes of the different individual fragments are: Vjn ¼ ai ð1 aÞj V n¼0 ; j ¼ 0 ! n; i ¼ 0 ! ðn jÞ ðA5Þ with the total volume of fragments in each volume fraction being nji ðnjÞ n¼0 n! ; a V 1 Pfr ðn j iÞ!j!i! j ¼ 0 ! n; i ¼ 0 ! ðn jÞ Wjn ¼ Appendix A [106] For simpler fragmentation geometries we directly determined the fragment distribution after a number of weathering cycles, n, using analytic expressions. ðA1Þ Notation A1. Model 1. Symmetric Fragmentation [107] A rock fragment of volume, V, fractures along a cracked surface to produce Nfr sub-fragments of equal 11 of 12 a ratio of daughter fragment volumes in asymmetric fragmentation model (1) b fitting exponent in symmetric fragmentation model, (1) c exponent used to determine particle tensile strength (1) d diameter of parent particle (L3) ðA6Þ F01014 WELLS ET AL.: MODELING ROCK WEATHERING PATHWAYS dmin minimum particle diameter (L) dr layer thickness for surface disintegration (L) kr coefficient in granular surface disintegration model (L) k1 fitting coefficient used in determining fracture probability as a function of particle volume (L3) k2 fitting coefficient used in determining fracture probability as a function of particle volume (1) k3 fitting coefficient used in determining fracture probability as a function of time (1) m Weibull modulus (1) Nfr number of particles formed when parent particle fractures (1) n cumulative number of elapsed weathering cycles (1) Pfr probability of a particle fracturing (1) Ps probability of a particle surviving intact (1) r exponent in granular surface disintegration model (1) S number of potential failure sites within particle (1) V parent particle volume (L3) Vfr fractured particle volume (L3) Vmin minimum particle volume (L3) Vref reference particle volume at which 63% fracture (L3) W total volume of particles possessing a given individual volume (L3) w fraction of potential failure sites which have failed (1) s stress applied to particle (M L1 T2) sM mean tensile strength of particles (M L1 T2) sT tensile stress required to fracture 63% of particle (M L1 T2) References Bland, W., and D. 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