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Persistent Provenance of South Asian Monsoon-Induced Silicate Weathering Over the Past 27 Million Years

The but our understanding of the interaction of tectonics, monsoon-driven erosion, silicate weathering and global Abstract The development of the South Asian monsoon (SAM) and Himalaya-Tibetan Plateau uplift were closely intertwined with some studies suggesting that uplift initiated the monsoon whereas others link tectonics with monsoon-controlled exhumation. Silicate weathering controls atmospheric CO 2 on geological timescales resulting in a large potential for monsoon strength and the Himalayan orogeny to influence global climate but detailed records of SAM-induced weathering on million year (Myr) timescales are lacking. Here, we present radiogenic Sr, Nd, and Pb isotope compositions of clay minerals produced by silicate weathering and transported to the central Bay of Bengal. The radiogenic isotope data exhibit a relatively small range and demonstrate a remarkably consistent mixture of sources dominated by Himalayan rocks and the Indo-Burman ranges, which consist of sediments derived from the Himalayas. This suggests that the spatial pattern of regional weathering, which today is highest in the regions of strongest monsoon rains, has persisted in a similar form for the last 27 Myrs. A pronounced increase in primary clay mineral abundance (from 9% to 22%) coincident with global cooling 13.9 Myrs ago points to a shift in the weathering regime given that the clay provenance did not change dramatically. Relatively weaker chemical weathering intensity during the mid and late Miocene cooling suggests increased aridity and changes in the large scale atmospheric circulation in the SAM domain. The establishment of the dry winter monsoon season during the mid and late Miocene may have caused this shift in the weathering regime and can reconcile much of the contrasting evidence for SAM initiation.

climate is limited by a lack of continuous records from the South Asian Monsoon (SAM) region with well-constrained age control extending back into the Oligocene (e.g., Clift & Webb, 2019).
The unique land-sea configuration of the Indian Ocean and the HTP is key to the evolution of the Asian monsoon system in that it controls the spatial pattern of atmospheric circulation and the regional hydrology of Asia (Clemens & Oglesby, 1992;Zhao & Moore, 2004). The vast majority of south and east Asian monsoon rain occurs during the SW summer monsoon from June to September (Figure 1). These feed the Asian rivers which deliver huge amounts of sediments (>50% of global fluxes) into the northern Indian Ocean and the South China Sea (Milliman & Syvitski, 1992). The Bay of Bengal (BoB) has received discharge and sediments from the Ganga and Brahmaputra rivers (G-B) draining the Himalayas since the Eocene  resulting in the largest accumulation of sediment on the planet, the Bengal Fan (Curray et al., 2003). The BoB also receives sediments from Indian peninsular rivers and the Irrawaddy and Salween rivers (I-S), which, although most of their load is deposited in the Andaman Sea, are significant sediment suppliers (I-S load ∼70% of G-B) (Chapman et al., 2015) draining geological formations similar to the Brahmaputra. The small rivers of the Arakan coast draining the Indo-Burman Ranges are poorly studied but the Sr and Nd isotope compositions of surface sediments reveal that they are an important source of material to the eastern BoB (Figures 1 and 2; Colin et al., 1999).
Radiogenic Sr ( 87 Sr/ 86 Sr), Nd ( 143 Nd/ 144 Nd, expressed as εNd) and Pb ( 206 Pb/ 204 Pb,207 Pb/ 204 Pb,208 Pb/ 204 Pb) isotope compositions reflect rock type and age and are widely used as provenance tracers (Frank, 2002;Hemming & McLennan, 2001). The geological formations of the continental areas surrounding the Bay of Bengal are characterized by large differences in radiogenic isotope compositions, which allow the detailed distinction of sediment sources (e.g., Galy & France-Lanord, 2001, Figures 1 and 2). Analyses of modern river sediments reveal that a disproportionally large fraction (compared to drainage area) of the sediments in the lower Meghna river, after the confluence of the Ganga and Brahmaputra, originate from the latter (Galy & France-Lanord, 2001). This has been attributed to higher monsoon rainfall over parts of the Brahmaputra catchment driving enhanced erosion ( Figure 1). Intense erosion and incision around the Namche Barwa syntax of the Siang tributary and the eastern tributaries (Dibang & Lohit), where average annual rainfall is > 3 m/yr, results in a high contribution from the rocks of the Transhimalayan plutonic belt to the downstream Brahmaputra sediments (Singh & France-Lanord, 2002). The isotope composition of BoB surface sediments exhibit a pronounced east-west divide (Colin et al., 1999; Figure 1a) with more radiogenic Nd isotope signatures in the eastern part reflecting input from the Indo-Burman Ranges, where monsoon rainfall is also particularly intense (Figure 1b; Damodararao et al., 2016).
The monsoon-related erosional history of the Himalayas has been reconstructed in the geological past based on the Sr and Nd isotope compositions of Bengal Fan sediments that accumulated over the last 12 (Galy et al., 2010) and 16.5 Myrs . However, these records do not include the postulated initiation or strengthening of the monsoon in the early Miocene (Clift et al., 2008;Guo, 2002) and the discontinuous deposition of the Fan sediments by turbidity currents and ALI ET AL. and other drill core sites discussed are marked. Nd isotope data of river sediments and marine sediments are shown in italics (sources and details in Data Set S4). Compiled endmember source values are taken from Damodararao et al. (2016). Major rivers are marked in blue: Gang., Ganges; Brah., Brahamaputra; Maha., Mahanadi; Goda., Godavari; Kris., Krishna Figure 1) on the Ninety East Ridge, which has a well-constrained stratigraphy that has recently been updated and improved based on results from a new drill Site (IODP Site U1443) at the same location (Clemens et al., 2016) (see Section 2). We reconstruct the sources of clay minerals, which are the product of silicate weathering in the core SAM region of the past 27 Myrs and find that the regions with the highest monsoon rainfall today have been weathered persistently over this time.

Materials and Methods
Ocean Drilling Program (ODP) Site 758 is located on the southeastern side of one of the large en echelon blocks that characterize the Ninety East Ridge between the equator and 10°N. The core was retrieved from a water depth of 2,924 m, about 1,000 m above the Bengal Fan in the southern Bay of Bengal (5° 23.05′ N, 90° 21.67′ E; Figure 1b). Site 758 was cored to 677 m below seafloor and recovered Upper Cretaceous to recent sediments (Pierce et al., 1989). Here, we only focus on the upper 234 m to reconstruct the SAM history from the Oligocene to the present. In December 2014 International Ocean Discovery Program (IODP) Expedition 353 drilled Site U1443 close to ODP Site 758. The continuous recovery enabled by multiple holes into the Oligocene at Site U1443 allowed significant improvement of the ODP Site 758 age model, especially during the early and middle Miocene. To import the new Site U1443 calcareous nannofossil and paleomagnetic age constraints, ODP Site 758A cores were correlated to Site U1443 A at the meter scale using color line scan data from U1443 A and RGB data extracted from composite core images of ODP Site 758 ( Figure S3) with macros written by Roy Wilkens (https:// www.codd-home.net/) for Igor ProTM (https://www.wavemetrics.com/index.html). During the middle Miocene (8.5-14 Ma), we use the age tie points from the high-resolution benthic foraminifer carbon and oxygen isotope stratigraphy from Site U1443 (Lübbers et al., 2019). Linear sedimentation rates fitted through all the age points were employed from the Pleistocene to Mid-Miocene and again in the early Miocene to Oligocene ( Figure S4). Further details of the new age model are provided in the supplement.
In total, 38 samples (Table S3), were selected for the analysis of radiogenic Sr, Nd, and Pb isotopes of the clay-size fraction and for the determination of clay mineral assemblages following Ali et al. (2015). Sediment samples were first freeze dried and then wet sieved over 63 µm and the <63 µm size fraction were further processed to separate clays (<2 µm). Carbonates and organic matter were removed by leaching for 12 h (with 30 min in an ultrasonic bath) with 1.5 M acetic acid and 10% H 2 O 2 . This was repeated several times until all carbonates were removed and no further reaction was observed. In a second step 0.05 M hydroxylamine hydrochloride and 2.6 M acetic acid solution buffered to pH 3.6 with NaOH was used to remove Fe-Mn oxyhydroxide coatings by leaching for 1 h in an ultrasonic bath and for 2 h on a shaker. This was followed by a triple rinse with de-ionized water to remove the soluble fraction. A centrifuge based Atterberg method was used to separate the clay-size fraction (<2 µm) which was confirmed by analyzing a subset of samples with a laser diffraction particle size analyzer (Beckman Coulter) LS I3 320. Finally, the separated clay samples were freeze-dried before total dissolution or X-Ray Diffractometer (XRD) analysis.
About 100 mg of the dried clays were completely dissolved using mixtures of concentrated HF-HNO3-HClO4. The separation and purification of Sr, Nd, and Pb followed previously established procedures in our lab (e.g., Ali et al., 2015). Sr, Nd, and Pb isotope compositions were measured on a Nu Plasma MC-ICP-MS at GEOMAR. Mass bias for 87 Sr/ 86 Sr was corrected with an 88 Sr/ 86 Sr of 0.1194 and values normalized to the accepted value of NIST NBS987 of 0.710245. The 2σ reproducibility for 87 Sr/ 86 Sr of NBS987 was ±0.00004 and repeated processing and analysis of USGS marine sediment reference material MAG-1 (n = 20) gave a mean 87 Sr/ 86 Sr value of 0.722873 ± 0.00003 (2σ) which agrees well with the values reported ALI ET AL.   (Galy et al., 2010;Hein et al., 2017): Generally plot in the HHC field but hemipelagic sediments (yellow squares) from the fan plot with the Ninety East Ridge bulk detrital silicates and clay size fraction confirming that these values are representative for the entire basin. Bulk detrital silicate isotope compositions of ODP Site 758 sediments are also shown and the offset between these values and the clay size data allows estimation of the grain size effect (see Figure S1). The fields for three major Himalayan rock formations are after Gourlan et al. (2010). by Nath et al. (2009) (0.722739). 143 Nd/ 144 Nd ratios were mass-bias corrected with 146 Nd/ 144 Nd = 0.7219 and normalized to the accepted value of the JNdi-1 standard of 0.512115 (Tanaka et al., 2000). Repeated measurements of an in-house Nd standard "SPEX" gave a reproducibility of ±0.20 εNd units (2σ). Repeated processing and analyses of reference material MAG-1 (n = 21) gave a mean εNd value of −11.2 ± 0.2, agreeing with the values reported by Nath et al. (2009). Blanks were typically below 60 pg for Nd and 1.8 ng for Sr and hence well below 1% of the sample mass. A standard-sample bracketing method was used to determine the Pb isotope ratios. The 2σ reproducibility for the Pb NIST NBS981 standard was ±0.0152, ±0.0062, ±0.0064, and ±0.00006 for 208 Pb/ 204 Pb,207 Pb/ 204 Pb,206 Pb/ 204 Pb and 207 Pb/ 206 Pb, respectively. Blanks were typically below 250 pg so that blank contributions to the Pb analyses can be neglected. Repeated processing and analysis of MAG-1 (n = 16) gave a mean value ±2 standard deviations of 38.811 ± 0.011, 15.658 ± 0.003, and 18.863 ± 0.002 for 208 Pb/ 204 Pb, 207 Pb/ 204 Pb, and 206 Pb/ 204 Pb, respectively. These Pb isotope values agree well with those previously reported for MAG-1 (Nath et al., 2009).
For the determination of clay mineral assemblages the separated claysize fraction (<2 µm) was suspended in an ultrasonic bath and placed on 0.2 µm filters by applying a vacuum below the filters. The XRD runs were performed following glycol-dehydration for 24 h. The analyses were conducted using a Phillips X-Ray diffractometer (PW series) with CoKα radiation and a Ni filter under a voltage of 40 kV and an intensity of 35 mA. The relative amount of each clay mineral was estimated according to the position of the (001) series of the basal reflections on the XRD diagrams that is, smectite (001) at 17 Å, illite (001) at 10 Å, kaolinite (001), and chlorite (002) at 7 Å. Kaolinite and chlorite were discriminated according to the relative proportions deduced from the ratios of the 3.57 Å and 3.54 Å peak areas. One sample was measured several times (n = 5) and the reproducibility of the semi-quantitative clay mineral analysis was ±2% (1σ). Although the leaching steps to isolate silicates are not always performed prior to clay mineral analysis similar clay mineral results have been obtained in the region without leaching (see supplementary discussion) and only the relative changes in clay minerals should be interpreted.

Results
The Sr, Nd, and Pb isotope compositions measured on the clay-size fraction are provided in Data Set S1 and are displayed in Figures 2-4 Compared to the different source lithologies these ranges are remarkably narrow. Although exhibiting different absolute values and a smaller range, the data from the Ninety East Ridge clays record similar trends to those observed in clays and bulk sediments from the Bengal fan ( Figure 3). The results of the clay mineral analyses are listed in Data Set S1 and displayed in Figure 5. Illite, chlorite, smectite and kaolinite are present in all analyzed samples. Illite and chlorite contents vary from 3% to 27% (average ∼12%) and 0%-19% (average ∼6%), respectively. Smectite is the dominant clay mineral ranging from 39% to 69% (average ∼56%). The abundance of kaolinite varies from 11% to 46% (average 26%).
ALI ET AL.   . Error bars represent the external 2σ reproducibility of the data based on the repeated measurement of the MAG-1 marine sediment reference material.

Provenance of Bay of Bengal Clays
Analyzing the radiogenic isotope composition of the clay size (<2 microns) fraction minimizes transport-related grain size effects ( Figure 2;  that influence the composition of the detrital sediments at the Ninety East Ridge . Considering the wide range of ages and types of rocks surrounding the BoB (Figure 1), the variations in isotope composition of the clays are small ( Figure 2) suggesting that the mixture of sources of detrital clays to the Ninety East Ridge has remained remarkably constant over the past 27 Myrs ( Figure 2). The Himalayas themselves are composed of mostly the same sequence of rocks (TSS and HHC) so would provide mixtures of sediment with similar isotopic compositions. This is consistent with active Himalayan erosion for the last 38 Myrs  and confirms and extends results from the Bengal Fan suggesting a constant Himalayan source of material for the last ∼16 Myrs Galy et al., 2010).
However, the Ninety East Ridge clays are clearly not exclusively Himalayan in origin as they are characterized by more radiogenic Nd and less radiogenic Sr and Pb isotope signatures than Himalayan rocks and most Bengal Fan sediments (Figures 2 and 4). Direct comparison of our clay fraction isotope signatures to river sediment data from the literature is potentially complicated by grain size dependent mineral sorting given that very few of these analyses were performed on clay size separates. The few measurements of the clay size fraction of Brahmaputra sediments indicates clays have slightly more radiogenic Nd compositions compared to bulk river bed sediments (Singh & France-Lanord, 2002) between 0.2 and 0.9 eNd units more radiogenic and with 87 Sr/ 86 Sr values 0.002 to 0.02 more unradiogenic. Similar differences between clay size and bulk sediment Sr and Nd isotopes have been found in the turbidite sediments of Himalayan origin delivered by the Indus to the Arabian Sea . Comparison of clay isotope compositions with bulk detrital measurements from similarly aged sediments at the same core location suggests the grain size influence ranges between 2.3 and 2.4 epsilon units for Nd and between 0.0001 and 0.008 for 87 Sr/ 86 Sr ratios ( Figure S1). Considering these differences the main sources of clays at the Ninety East Ridge over the ALI ET AL.  past 27 Myrs have been the Brahmaputra and the Irrawaddy/Indo-Burma Ranges (IBR) (Figure 2). Bengal Fan silicates generally plot in the High Himalayan Crystalline (HHC) field but samples from hemi-pelagic fan sediments plot close to the Ninety East Ridge bulk detrital silicates and the clay size fraction (Galy et al., 2010) clearly indicating that the radiogenic isotope signatures of the Ninety East Ridge clays reflect the finegrained sediment supplied to the basin (Figure 2).
The eastern Brahmaputra tributaries and the IBR (via Arakan coast and Irrawaddy rivers) are the most likely sources of the radiogenic Nd isotope signature of the Ninety East Ridge clays given that contributions from other highly radiogenic sources such as the Deccan Traps or Sumatra are unlikely as discussed below. Compared to Sr and Nd there are few Pb isotope data in the literature for the region but Pb isotopes are more sensitive to crustal processes (Hemming & McLennan, 2001) and some data for the suspended sediments from the Ganges, Brahmaputra, and Lower Meghna rivers are available ( Figure 4). The Pb isotope compositions of the clays plot at the lower end of the Himalayan river sediments and show a close similarity to those of the Brahmaputra supporting our Sr and Nd isotope results (Figure 4).
Although a wide range of Sr, Nd and Pb isotope values have been reported for the Deccan basalts (Data Set S4) this is mostly the result of lithospheric contributions in the magmas of the early lava flows (e.g., Lightfoot et al., 1990). The younger and more voluminous flows all have highly radiogenic εNd (unradiogenic 87 Sr/ 86 Sr) and distinctly unradiogenic Pb isotope signatures (Figure 4), precluding a significant Deccan contribution to the Ninety East Ridge clays, as suggested previously for distal fan clays (France-Lanord et al., 1993). The distribution of Deccan basalt-derived clays from Indian peninsular rivers is likely to restricted to the Indian margin by the monsoon-induced Indian coastal current (Kumar et al., 2006). In addition, the sediment load of the peninsular Indian rivers draining the Deccan basalt areas (246 Mt/year compiled load of Krishna, Godavari and Mahanadi) (Milliman & Syvitski, 1992) are simply swamped by the big rivers (G-B and I combined supply 1320 Mt/year) (Milliman & Syvitski, 1992;Robinson et al., 2009). Such a vast amount of suspended sediment also means that the potential influence of finegrained mineral dust in this region is small with identified continental dust sources either being the Ganges plain with Himalayan provenance (Tripathi et al., 2013) (Thar dessert Figure 2) or air masses from SE Asia with low mineral dust loadings (e.g., Srinivas & Sarin, 2013).
Another proximal and therefore potential source is the Sunda arc (Figure 1), but material from this source is unlikely to reach the Ninety East Ridge given the prevailing SW or NE winds and ocean currents in the Andaman Sea. A wide range of isotopic values have been reported for Sumatran volcanic rocks as some of the most recent lavas bear a signature of crustal contamination and inclusion of subducted sediments (e.g., Gertisser et al., 2003). However, compared to the age of our sediment record these volcanic rocks are young (Quaternary) and Miocene and older Sumatran formations (and also some Quaternary/Pliocene volcanics) exhibit more radiogenic εNd (unradiogenic 87 Sr/ 86 Sr) and distinctive Pb isotopes (Figure 4), making a significant supply of material from Sumatra unlikely. Furthermore, over the course of the last 30 Myrs, the NER has moved closer and closer to Sumatra (Hall, 2012) (Clift et al., 2008) from the South China Sea as a record of East Asian Monsoon development, (e) Nd and Pb isotope composition of ODP Site 758 clays (g) mineral flux record (Hovan & Rea, 1992) of ODP Site 758 recalculated using updated linear sedimentation rates from the new age model (see supporting information), and sedimentation rates from the Bengal fan DSDP Site 218 and IODP Site U1451 (France-Lanord et al., 2016;Galy et al., 2010) and at the bottom a summary of the regional tectonic events (Allen & Armstrong, 2012). 1, High Himalayan Uplift, Main Central Thrust (MCT); 2, Onset of normal Fault, South Tibet; 3, Surface Uplift East Tibet; 4, Initial thrusting on Main Boundary Trust; 5, Fast exhumation at Himalayan syntaxes, Outward growth of NE Tibet. The ages of literature data plotted have been updated to the more recent GTS12 time scale (Gradstein et al., 2012). surrounding Sumatra have been repeatedly exposed and flooded (Zahirovic et al., 2016), either presenting easily erodible material or trapping sediment. Such changes should have strongly affected any possible sediment supply from Sumatra are not consistent with the remarkably invariable radiogenic isotope composition of Ninety East Ridge clays over the last 27 Myrs. Instead, like the sedimentary rocks of the Andaman Islands and the Nicobar fan (Awasthi & Ray, 2020;Chen et al., 2020;McNeill et al., 2017), the source of detrital sediments to the Ninety East Ridge has been dominated by sources from the north where SAM rainfall and exhumation are most intense.

Clay Mineralogy
Secondary clays formed during silicate weathering dominate the clay mineral assemblage (Data Set S1) with smectite ranging from 39% to 69% (average ∼56%) while the abundance of kaolinite varies from 11% to 46% (average 26%). Illite (average ∼12%) and chlorite (average ∼6%) are primary minerals derived by physical erosion of the Himalayan formations (France-Lanord et al., 1993). Analyses of Brahmaputra suspended sediments have revealed that the <2 μm fraction only represents 0.5%-3% and is composed of illite, vermiculite and chlorite, but no detectable kaolinite or smectite (Singh & France-Lanord, 2002). Near the confluence with the Ganga, and in delta sediments, secondary clays are found (Heroy et al., 2003). This strongly suggests that the secondary clay minerals formed by silicate weathering occurring in the floodplain (France-Lanord et al., 1993) where smectite can preferentially form in poorly drained soils (Alizai et al., 2012;Thiry, 2000). The primary clay minerals have been eroded, transported and possibly stored in the floodplain, while the secondary clays formed in floodplain soils, before being eroded and transported to the Ninety East Ridge. The timescales of these processes are poorly constrained (Thiry, 2000), but changes in Holocene clay mineralogy on the floodplain seem to be climatically controlled (Heroy et al., 2003) and recent work on the Ganga river suggests minimal floodplain storage (Lupker et al., 2011). In view of the million-year resolution record presented here, any potential time lag should be negligible.
A smectite content >39% could indicate a strong contribution from volcanic rocks like the Deccan trap basalts but clays from the Indus floodplain also have relatively high-smectite contents without substantial amounts of volcanic rocks in the basin (Alizai et al., 2012). The isotopic data and the considerations above argue against a major Deccan trap contribution as established for the smectite rich clay layers from the distal Bengal Fan based on major and trace elements (Fagel et al., 1994) and stable isotope compositions (France-Lanord et al., 1993). Some instances of authigenic smectite have been reported in biogenic opal rich sediments from the central Indian Ocean with acid leaches of clay sized sediments having an isotope composition similar to Indian Ocean seawater (Fagel et al., 1997). A significant seawater contribution to the Ninety East Ridge clays can be ruled out given that the 87 Sr/ 86 Sr measured on the strongly pre-leached clays (carefully removing authigenic phases except for possibly some barite) of this study is always higher than that of contemporary and Miocene seawater (McArthur et al., 2001) and neither the clay 87 Sr/ 86 Sr, nor the offset between clay and contemporaneous seawater 87 Sr/ 86 Sr, correlates with the smectite content ( Figure S2). Although some reverse weathering likely occurs on the shelf (Michalopoulos & AIIer, 1995), the Sr incorporated (and by inference the Nd and Pb as well given that seawater Sr concentrations are much higher) into these clays is sourced from the river sediments and not seawater. Furthermore, the smectite content is also high in Pleistocene turbidite sediments from sea level low stands in the northern BoB (Joussain et al., 2016) suggesting the smectite rich clays were eroded from the shelf sediments from the eastern BoB. Although smectite can be preferentially scavenged during flocculation in the estuary as inferred for the Indus (Li et al., 2019) if it escapes to or is formed on the shelf it can preferentially remain in suspension compared to other clay minerals (Chamley, 1989). Transport processes clearly influence the clay mineralogy of Bengal Fan surface sediments  but such fine material will remain in suspension until flocculated or incorporated into larger particles (Milligan & Hill, 1998). The deposition of fine clays on the Ninety East Ridge is linked to productivity and the sinking of biogenic particles as the seasonal variability of the lithogenic flux to sediment traps in the southern BoB follows the carbonate and opal fluxes peaking during the summer monsoon months (Unger et al., 2003). Such a deposition process is unlikely to selectively influence the clay size mineralogy. Although the Himalayas and river mouths were further away in the early Miocene (Hall, 2012;Najman et al., 2008) the detrital mineral flux to the site was elevated compared to more distal sites in the Indian Ocean with similar sedimentation rates (Hovan & Rea, 1992) demonstrating the persistence of enhanced continental weathering inputs to the BoB. A final consideration is the occurrence of ash layers that could weather to smectite in the sediments. We were careful not to sample any ash layers and the occurrence of ash layers does not start until the middle Miocene and increases into the Pleistocene (Pierce et al., 1989), opposite to the pattern of decreasing smectite abundance observed in the middle Miocene core section. Therefore, we are confident that our clay mineral assemblages represent weathering processes in the big river basins, albeit passed through the filter of transport to the Ninety East Ridge.

SAM Induced Silicate Weathering
The radiogenic isotope signatures suggest that silicate weathering in the Brahmaputra and IBR regions supplied the vast majority of the clays to the Ninety East Ridge over the past 27 Myrs (Figure 2). Today these are the locations of the highest monsoon rainfall over South Asia (Figure 1b). We do not interpret any subtle changes in the mixture of sources given that these would be ambiguous in view of the range in source rock compositions (Figures 2-4). However, there is a clear shift in both Sr and Pb isotope compositions around 8 Ma which is not clearly mirrored by the Nd isotope signatures suggesting incongruent weathering effects as opposed to source changes (Frank et al., 2002). For example the preferential weathering of biotite under cooler climates would result in clay minerals with higher 87 Sr/ 86 Sr  and radiogenic Pb isotopes are also preferentially released from the first minerals weathering chemically (Harlavan et al., 2009). However, these changes in Sr and Pb isotopes are subtle (Figures 2-4) and the apparently stable spatial distribution of silicate weathering during the major tectonic reorganizations of the Miocene (e.g., Allen & Armstrong, 2012) argues for SAM precipitation as the primary control on regional erosion and weathering, although precipitation is closely related to relief in the region today (Damodararao et al., 2016). We can constrain the rock types and ages being weathered but the location of the weathering may have changed over time. The processes of erosion and silicate weathering can be separated in both time and space, for example, the IBR consist of sediments produced by the erosion of the Himalayas (Licht et al., 2013) that are weathered under a wet tropical climate. Sedimentary rocks with IBR composition have contributed a large portion of the clays produced by silicate weathering and transported to the Ninety East Ridge over the last 27 Myrs but the location of the weathering may have changed as the formations were eroded, deposited and uplifted to form the IBR (Najman et al., 2020). Although the Lesser Himalayan (LH) lithologies have been exposed to erosion since approximately 16 Myrs ago (Colleps et al., 2018) the isotopic constraints indicate the LH contribution to the Ninety East Ridge clays must be very small. The products of Himalayan erosion deposited on land (Siwaliks) and on the Bengal fan also do not exhibit a significant contribution from these formations with highly unradiogenic Nd isotope signatures (Galy et al., 2010;Galy & France-Lanord, 2001). In the western Himalaya the delivery of LH material to the Indus fan occurred only in the Pliocene, later than in the foreland basin records . Although the LH rocks currently contribute a large proportion of the dissolved Sr content of the Ganga river during the monsoon months (Bickle et al., 2005), the minimal LH signals in the regional weathering products of the last few million years suggests that the radiogenic Sr isotope composition of seawater was a more reliable recorder of continental silicate weathering than often considered (e.g., Colleps et al., 2018). Ultimately the provenance of clay minerals documented here may differ from silicates eroded and transported by turbidity currents to form the Bengal and Nicobar fans (e.g., Chen et al., 2020;Najman et al., 2019). While the fan deposits record the sources of eroded material, the clays are dominated by secondary minerals formed in the weathering environment and changes in the formations being eroded may not be synchronous with changes in chemical silicate weathering.
Having confirmed the stable source provenance of clay minerals at the Ninety East Ridge with their radiogenic isotope signals, the clay mineralogy provides additional information on the weathering regime and climate of the source region (France-Lanord et al., 1993). Kaolinite forms under hot and humid tropical weathering with strong hydrolysis (e.g., Chamley, 1989) and the kaolinite percentage in Ninety East Ridge clays has decreased only modestly as global climate cooled (Figure 5b). This indicates that tropical weathering persisted in the watersheds with the strongest monsoon rainfall today and was even more prevalent in the late Oligocene and early Miocene. Smectite abundance was variable but has remained high throughout the last 27 Myrs. Data from an experimental catchment in the monsoon dominated Western Ghats found smectite dissolution/precipitation to be the main control of the chemical weathering flux of dissolved Si (Violette et al., 2010). Smectite is not stable in a climate with high precipitation (>900 mm/yr) but instead forms under semi-arid conditions (900-500 mm/yr). Under the current climate in the Western Ghats smectite dissolves and kaolinite precipitates. Therefore, the higher kaolinite abundances during the late Oligocene and Miocene strongly suggests that more regions received rainfall >900 mm/yr.

Middle Miocene Increase in Physical Weathering
The most prominent change in the clay minerals delivered to the Ninety East Ridge was the pronounced increase in the primary minerals illite and chlorite around 13.9 Ma (Figure 5f) accompanying a major global cooling step (Figure 5a). This was also coincident with the start of the major increase in detrital mineral flux to the site (Figure 5g) but the change in illite content experienced a much sharper transition while chlorite abundance increased gradually (Figure 5f). The marked increase in detrital mineral flux to ODP Site 758 was originally interpreted to represent the start of monsoon induced erosion and weathering but may also have resulted from the progradation of the Bengal Fan reaching a point where suspensions originating from turbidity flows were able to reach the top of the Ninety East Ridge. There were coeval increases in sedimentation at the nearby drill sites on the Bengal Fan (Figure 5g) while the Nicobar fan on the other side of the Ninety East Ridge only started accumulating rapidly after 9.5 Ma (McNeill et al., 2017). Industry wells on the western Bengal Fan suggest that sedimentation rates were high throughout the Miocene (Krishna et al., 2016) suggesting a major shift in the location of sediment deposition during the Miocene is unlikely. If these few long drill holes are representative, this suggests that the mid Miocene increase in the supply of detrital minerals to the Ninety East Ridge represents a general increase in supply to the BoB region.
The secondary (Smectite + Kaolinite) over primary (Illite + Chlorite) clay mineral ratio is a measure of chemical versus physical weathering ( Figure 6) and is of particular interest in the BoB given that the amount of organic carbon buried in the Bengal Fan is more than 3 times greater in smectite-kaolinite dominated sediments compared to illite-chlorite sediments (France-Lanord & Derry, 1997). After the increase in primary clay mineral supply in the middle Miocene, the changes in primary clay mineral abundance on the Ninety East Ridge exhibit a similarity to the East Asian Monsoon record from the South China Sea (Clift et al., 2008) suggesting that the peaks in physical erosion were related to a generally strong monsoon across Asia ( Figure 5). Although the result of different transport pathways, a similar shift to a more primary clay mineral dominated assemblage (also without major source changes) was also observed during the Miocene in the South China Sea (Wan et al., 2007) and Sea of Japan (Shen et al., 2017;Figure 6), suggesting that this is a regional signal and likely of global importance. Although we observe a strong increase in physical erosion with global cooling across the Asian monsoon region, secondary clay minerals formed by silicate weathering still dominate and silicate weathering persisted in the same regions with the highest monsoon rainfall as today over the last 27 Myrs. This persistence may point to a tectonically driven control where rainfall follows orography and exhumation drives more uplift (e.g., Thiede et al., 2004) (Holbourn et al., 2018) represents ice volume and deep sea temperature highlighting the global climate changes of the last 16 Myrs. The age model for Site U1443 and therefore the samples from Hole ODP Site 758 used here have been directly tied to these high resolution records of middle Miocene climate change (Lübbers et al., 2019). Periods of global cooling, after (Zachos et al., 2008) are marked with blue bars, and the Middle Miocene Climatic Optimum is marked with a red bar. (c and d) Clay mineralogy of ODP Site 758 S + K/I + Ch (Smectite + Kaolinite)/ (Illite + Chlorite) compared with ODP Sites 717 & 718 (Bouquillon et al., 1990) (e) Seawater Li isotope records from planktic foraminifera replicated in different ocean basins as a tracer of global silicate weathering intensity (Hathorne & James, 2006;Misra & Froelich, 2012) (f) Clay mineral records of ODP Site 1146 in the South China Sea (Wan et al., 2007) and IODP Site U1430 from the Japan Sea (Shen et al., 2017) (g) Global seawater Sr isotope record compiled by McArthur et al. (2001).

SAM Intensity, Silicate Weathering Regime and Global Climate
The clay mineral data indicate that weathering was more intense under warmer and wetter Miocene climates and decreased slightly as global climate cooled, but what are the implications for the monsoon intensity in the past? This question is difficult to answer as monsoon intensity can be defined based on the amount of precipitation, the seasonality of precipitation, or wind speed and direction. The monsoon today is a seasonal phenomenon with the monsoon climate being characterized by a relatively dry climate for two thirds of the year. Many lines of evidence interpreted as the start of the SAM occurred around either the mid-Miocene global cooling (e.g., Betzler et al., 2016) or the late Miocene global cooling (e.g., Quade et al., 1989), but other records point to a decrease in weathering or precipitation during the late Miocene in the SAM and EAM regions (Clift et al., 2008;Holbourn et al., 2018;Steinke et al., 2010). One way to reconcile these seemingly disparate views is that these changes represent the development of the dry season between monsoon rains and the NE winter monsoon, like inferred for the late Miocene in east Asia (Holbourn et al., 2018). In the SAM domain it appears that the emergence of the dry season accompanied middle Miocene global cooling while the late Miocene saw increases in secondary clays and clay abundance on the Ninety East Ridge and secondary clays in the distal Bengal fan (Figures 5 and 6), implying increased silicate weathering. However, the records of vegetation change recorded in the Siwalik deposits across the Himalayas suggest the aridification was more pronounced in the west compared to the eastern range supplying the material to the Bay of Bengal (Vögeli et al., 2017). The Miocene increase in primary clay mineral supply was also associated with various regional tectonic events such as the proposed breakoff of the Indian plate slab (Webb et al., 2017;Figure 5) and was accompanied by an exponential increase in the deposition of terrigenous material at the Ninety East Ridge (Figure 5e), causing a clear change in the color of the sediments ( Figure S3) and, importantly, an increase in clay content ( Figure 6). As all these changes were accompanied by only subtle changes in the mixture of sources being weathered they point to a shift in the weathering regime in the SAM region. A shift in the weathering regime during the mid and late Miocene cooling resulting from increased aridity and changes in the large scale atmospheric circulation in the SAM domain can reconcile much of the contrasting evidence for SAM initiation (cf. Betzler et al., 2016;Clift et al., 2008;Quade et al., 1989) but such a shift would also have wider implications for atmospheric CO 2 and global climate.
The relative reduction in secondary clay mineral formation across the Asian monsoon region would imply a decrease in the silicate weathering in the region supplying most sediments to the ocean today (Milliman & Syvitski, 1992). Although clastic sedimentation around Asia decreased from around 12 Ma to a low at 10 Ma, overall the flux was elevated since the Oligocene (Clift, 2006). Meanwhile, the Ninety East Ridge detrital mineral flux and accumulation rates on the nearby Bengal Fan increased following the global cooling ( Figure 5) possibly compensating for temporary reductions elsewhere in Asia at this time (Clift, 2006). Incorporating the new results from the uniquely long and continuous record for the region obtained from the Ninety East Ridge, it seems that the total supply of sediments from Asia, and the silicate weathering of Asia may have increased during the Miocene with the potential to reduce atmospheric CO 2 concentrations. This scenario is supported by the increase in the marine Sr isotope composition (Raymo & Ruddiman, 1992) although a break in slope around the point of middle Miocene cooling ( Figure 6) suggests a decrease in the supply of continental Sr. However, as the global seawater Sr isotope composition is particularly sensitive to contributions from carbonates associated with metamorphic rocks in the Lesser Himalayas (Oliver et al., 2003;Bickle et al., 2005) the research has shifted to new silicate weathering proxies such as lithium (Hathorne & James, 2006;Misra & Froelich, 2012) and beryllium isotopes (e.g., Dixon & von Blanckenburg, 2012). Using these proxies to constrain silicate weathering in a model of the geological carbon cycle suggests that to maintain the reduction in atmospheric CO 2 reconstructed for the Cenozoic while silicate weathering fluxes were constant within a few percent, the temperature (pCO 2 ) dependence of silicate weathering (the silicate weathering feedback) varied significantly (Caves Rugenstein et al., 2019). This hypothesized shift in the weathering regime agrees well with the observed regional changes in clay minerals and a general decrease in weathering intensity since the mid Miocene. This change is opposite to that expected from the modern system, where more secondary clays formed by silicate weathering cause river and seawater Li isotope ratios to increase (e.g., Bagard et al., 2015), as the particularly intense weathering of the middle Miocene dissolved secondary clays, thereby releasing the initially sequestered 6 Li (Caves Rugenstein et al., 2019). The increase of the weatherability of Miocene regolith is consistent with the relative increase in the supply of physical weathering products but the increased supply of detrital clays (Figure 6), including secondary clays, is apparently at odds with the constant silicate weathering flux inferred from meteoric Be isotopes. A constant silicate weathering flux is also hard to reconcile with variable carbonate accumulation in the Atlantic, Pacific and Indian Ocean basins during the Miocene (e.g., Lübbers et al., 2019) and other factors related to global cooling and increased aridity such as the expansion of grasslands with thick soils (Retallack, 2001). The global sea level drop associated with Miocene global cooling may have limited the supply of alkalinity from silicate weathering reaching the oceans with more being trapped in soil carbonates. Additionally, the increase in clay supply to the Bay of Bengal and secondary clays reaching the distal Bengal fan (Figures 6d and 6g) would have increased the potential for organic carbon burial thereby potentially reducing atmospheric CO 2 (France-Lanord & Derry, 1997). Deciphering the complex interactions of monsoon climate, silicate weathering, erosion and tectonics in detail will require higher resolution records across key tectonic and climatic events. However, the data presented here strongly argue for a global shift in silicate weathering regime during the Miocene with reduced weathering intensity linked to global cooling and possibly the development of the dry winter monsoon season in Asia.

Conclusions
Radiogenic Sr-Nd-Pb isotope compositions of the clay-size fraction of sediments from the Bay of Bengal indicate that the clays originated from a relatively stable mixture of sources. This indicates that the spatial pattern of regional weathering, which today is strongest where monsoon rains are highest, has persisted over the last 27 Myrs. A pronounced increase in primary clay mineral abundance occurred around 13.9 Myrs ago and indicates a relative increase in physical weathering intensity around this time. This change in weathering regime was accompanied by an increased delivery of terrigenous material and clays to the core site. In combination with data obtained from cores from the east and west, a general increase in the delivery of terrigenous material to the Bay of Bengal and a regional shift in weathering regime is inferred. The timing of this shift was coincident with middle Miocene global cooling and regional tectonic reorganizations but higher resolution records will be required to distinguish between the causes. However, the emergence of the dry winter monsoon season during the Miocene would explain the regional shift in weathering regime and reconcile much of the contrasting evidence for SAM initiation at this time.

Data Availability Statement
The data presented in this study are included in the supplementary information and all new data are freely available on the PANGAEA data repository (https://doi.pangaea.de/10.1594/PANGAEA.927027).