1 Methods 2 We numerically simulated groundwater age in a wide range of steady-state, regional-scale (1- 3 100s km) groundwater systems (see Table S1 for range of parameter values). We simulate mean 4 groundwater age mass as a tracer subject to advection, diffusion and dispersion using a yearly 5 production of one unit of conservative solute within the fluid (Bethke and Johnson, 2002; Goode, 6 1996; Voss and Wood, 1994). Over 1000 simulations were conducted with SUTRA, a US 7 Geological Survey numerical groundwater model that uses the finite element method (Voss, 8 2002). Recently, the full distribution of groundwater age (Cornaton, 2011) and the moments of 9 age distribution (Ginn et al., 2009) have been quantified but we focus on mean age that represent 10 first-order patterns of groundwater age within a basin. The model domain consists of a 11 rectangular cross-section of a generic basin with an imposed linear hydraulic gradient at the 12 upper boundary and no flow boundaries on all other sides (Figure 1b). The basin contains three 13 layers, an upper aquifer, a low permeability unit and a lower aquifer. Each unit is assumed to be 14 homogeneous and isotropic. Parameters other than permeability such as diffusivity and porosity 15 are kept constant within the whole domain. Values of dispersivity at the regional scale are 16 uncertain (Freeze and Cherry, 1979). We chose to assign the dispersivity at the minimum value 17 that allows numerical stability, and we studied the effect of dispersivity on groundwater ages in a 18 separate set of model simulations (Figure S3). Longitudinal dispersivity is set to one fourth of the 19 local element dimension (αL = 5m) and transversal dispersivity at one tenth of longitudinal 20 dispersivity(Voss, 2002) (αT = 0.5m). We explored the effects of a large range of values of the 21 key parameters that control groundwater age, including the permeability of the low-permeability 22 unit (k2) and the high permeability unit (k1), basin size and aspect ratio, hydraulic gradient and 23 lateral continuity of the low-permeability layer. The continuity of the low-permeability unit is 24 defined as the lateral extent of the low-permeability unit divided by the total length of the basin, 25 and the layer is equally cut off at the recharge and discharge ends. The parameter ranges 26 (Table S1) are intended to capture the variability observed in natural hydrogeological systems. 27 We define ‘high age zone’ as a zone within the low permeability layer where the maximum 28 groundwater age is at least twice that of surrounding water. The width of this high age zone was 29 determined as the horizontal distance where the groundwater age is more than half the maximum 30 age (Figure S4b). If groundwater age remained above 50% of the maximum on one side of the 31 layer, we considered that the high age zone did not form (Figure S4a, S4c) which excludes cases 32 where the whole low permeability unit has a higher groundwater age. The value of 50% of the 33 maximum age is arbitrary; other cut offs such as 90% were also examined and result in similar 34 patterns of high age zones. In many simulations, groundwater age also is high in the discharge- 35 side of the domain within and below the low permeability layer (i.e. lower left hand corner of 36 Figure 2c). This is the natural result of longer flow paths and has been documented previously 37 (Jiang et al., 2010), but is not considered as a high age zone, since the zone is not surrounded on 38 both sides by younger water. 39 Table S1. Overview of parameter values. Parameter Range of variation Related figure Permeability k1 of the aquifer k1 = 10-8 m² to 10-17 m² Figure 2, Figure 3 Permeability k2 of the low-permeability unit k2 = 10-8.5 m² to 10-20 m² Figure 2, Figure 3 Hydraulic gradient 0.001, 0.005, 0.01, 0.1 Figure 2 Depth of the low-k layer 0.1 to 0.9 Figure 4a Thickness of the low-k layer 0.05 to 0.95 Figure 4b Continuity of the low-k layer 0.05 to 1 Figure 4c Length of the basin L 1 to 100 km Figure 4d Depth of the basin Z 100 m to 10km Figure 4d Aspect ratio of the basin 1:1 to 1:100 Figure 4e Porosity 0.1, 0.3 All figures with n = 0.3 except for Figure S5. 40 41 Longitudinal dispersivity αL 5, 50, 500 m Figure S3 Transversal dispersivity αT 0.005, 0.05, 0.5, 5, 50 m Figure S3 Horizontal grid spacing 20 m Vertical grid spacing 5m 42 43 Table S2. Parameter values for Figure 2a-c. Parameter Value Permeability k1 of the aquifer k1 = 10-13 m² Permeability k2 of the low-permeability unit (a) k2 = 10-14 m², (b) k2 = 10-15.4 m², (c) k2 = 10-16 m² 44 45 Hydraulic gradient 0.01 Depth of the low-k layer 0.5 Thickness of the low-k layer 0.2 Continuity of the low-k layer 1 Length of the basin L 10 km Depth of the basin Z 1 km Porosity 0.3 Longitudinal dispersivity αL 5m Transversal dispersivity αT 0.5 m 46 47 48 49 Table S3. Parameter values for Figure 3. Parameter Value Permeability k1 of the aquifer k1 = 10-8 m² to 10-18 m² Permeability k2 of the low-permeability unit k2 = 10-8.5 m² to 10-18 m² Hydraulic gradient 0.01 Depth of the low-k layer 0.5 Thickness of the low-k layer 0.2 Continuity of the low-k layer 1 Length of the basin L 10 km Depth of the basin Z 1 km Porosity 0.3 Longitudinal dispersivity αL 5m Transversal dispersivity αT 0.5 m 50 51 52 53 Table S4. Parameter values for Figure 4. Parameter Value Permeability k1 of the aquifer k1 = 10-13 m² Permeability k2 of the low-permeability unit k2 = 10-14 m² to 10-16 m² Hydraulic gradient 0.01 Depth of the low-k layer (a) 0.1 to 0.9 Thickness of the low-k layer (b) 0.05 to 0.95 Continuity of the low-k layer (c) 0.05 to 1 Length of the basin L (d) 1 to 100 km Depth of the basin Z (e) 100 m to 10km Aspect ratio of the basin (e) 1:1 to 1:100 Porosity 0.3 Longitudinal dispersivity αL 5m Transversal dispersivity αT 0.5 m 54 55 Details on why high age zones form (with figures) 56 Our results suggest that two mechanisms lead to the formation of a zone of high groundwater 57 ages. First, high age zones are caused by mixing of groundwater from flow paths that travel 58 through only the upper two layers and flow paths that travel through all three layers. For a wide 59 range of permeabilities of the low permeability unit (k2), the groundwater velocity in the lower 60 aquifer is high enough for the groundwater to travel faster than the groundwater flowing only 61 through the overlying low-permeability unit (Figure S1). Upward flow of the younger 62 groundwater near the discharge zone leads to rejuvenation of groundwater age within the low- 63 permeability unit. High age zones are formed upgradient of the intersection of flow paths going 64 through the lower aquifer and the low-permeability unit, and through the low-permeability unit 65 only. Second, the high age zones are controlled by the flow velocities in the low-permeability 66 unit (Figure S2). The lowest velocities are found near the middle of the basin and coincide with 67 the location of the high age zone. 68 Which of these two mechanisms is dominant controls the location of the high age zone and is 69 predictable from the permeability contrast between the aquifer and the low-permeability unit. At 70 low permeability contrasts the velocity is relatively constant over most of the low-permeability 71 unit, and the high age zone is mainly controlled by the rejuvenation of groundwater below the 72 discharge zone due to upflowing groundwater from the lowest aquifer (Figure S2a). At high 73 permeability contrast the location of the high age zone follows the narrow zone of low flow 74 velocities that is located in the middle of the basin (Figure S2b-c). Model simulations confirm 75 that high age zones are not necessarily stagnation points, zones where groundwater velocity is 76 zero or/and flow is in opposite directions (Jiang et al., 2011). In our model simulation flow 77 velocities maintain values of 10-4 m/yr or higher (Figure S2). However, high age zones develop 78 in areas of low velocities. 79 80 81 82 83 84 85 86 Figure S1. The permeability of the low-permeability unit controls the velocity of the lower aquifer. Distribution of velocity (m/yr) within the aquifer under a 0.01 hydraulic gradient for sedimentary rocks (k1 = 10-13 m²) and a layer permeability of (a) k2 = 10-14 m², (b) k2 = 10-15.4 m² and (c) k2 = 10-16 m². 87 88 89 90 91 92 93 94 95 Figure S2. High age zones are not hydraulic stagnation points. Cross-section of groundwater age (blue) and velocity (red) at the middle of the low-permeability unit under a 0.01 hydraulic gradient for sedimentary rocks (k1 = 10-13 m²) and a layer permeability of (a) k2 = 10-14 m², (b) k2 = 10-15.4 m² and (c) k2 = 10-16 m². 96 97 98 99 Figure S3. Zones of high groundwater age are common for diverse values of dispersivity. Location of high age zone vs. k2 for sedimentary rocks (k1 = 10-13 m²) under a gradient of 0.01 with a longitudinal and transversal dispersivity of (a) αL = 5 m and αT = 0.5 m, (b) αL = 50 m and αT = 5 m, and (c) αL = 5 m and αT = 0.005 m. 100 101 102 103 104 105 Figure S4. Determination of high age zone location. Cross-section of groundwater age and location of maximum age (xmax) and points where groundwater age is 50% of the maximum (x1 < xmax < x2) at the middle of the low-permeability unit under a 0.01 hydraulic gradient for sedimentary rocks (k1 = 10-13 m²) and a layer permeability of (a) k2 = 10-13.6 m², (b) k2 = 10-14 m² and (c) k2 = 10-16.4 m². High age zone forms in case b but not in cases a and c. 106 107 108 109 110 111 112 113 114 115 116 117 118 119 Figure S5. Location of zones of high groundwater age for a 0.1 porosity. (a-c). Distribution of groundwater age within the aquifer under a 0.01 hydraulic gradient for sedimentary rocks (k1 = 10-13 m²) and a layer permeability of (a) k2 = 10-14 m², (b) k2 = 10-15.4 m² and (c) k2 = 10-16 m². (d-f). Location of high age zone vs. k2 for sedimentary rocks (k1 = 10-13 m²) under a gradient of (d) 0.1, (e) 0.01 and (f)0.001. (g-i). Location of high age zone vs. k2 for unconsolidated sediments (k1 = 10-11 m²) under a gradient of (g) 0.1, (h) 0.01 and (i) 0.001. Circles represent the location of the maximum groundwater age; lines represent the area where groundwater ages are higher than 50% of the maximum age. For each case, simulations have been run for values of k2 from k1 to 10-18 m². Values not specified mean that a high age zone does not form for this set of parameters.