Global and Planetary Change 224 (2023) 104102 Contents lists available at ScienceDirect Global and Planetary Change journal homepage: www.elsevier.com/locate/gloplacha Solar forcing for nutricline depth variability inferred by coccoliths in the pre-industrial northwestern Mediterranean Alessandro Incarbona a, b, *, Sergio Bonomo c, Isabel Cacho d, Fabrizio Lirer e, c, Giulia Margaritelli f, Delia Pecoraro a, Patrizia Ziveri g, h a Università Degli Studi di Palermo, Dipartimento di Scienze della Terra e del Mare, Via Archirafi 22, 90134 Palermo, Italy b National Biodiversity Future Center (NBFC), Piazza Marina 61, Palermo 90133, Italy c Istituto di Geologia Ambientale e Geoingegneria (CNR-IGAG), Area Della Ricerca di Roma 1- Strada Provinciale 35d, Montelibretti 9-00010, RM, Italy d GRC Geociències Marines, Dept. de Dinàmica de la Terra i de l’Oceà, Facultat de Ciències de la Terra, Universitat de Barcelona, Barcelona 08028, Spain e Sapienza Università di Roma, Dipartimento di Scienze della Terra, Piazzale A. Moro 5, Roma 00185, Italy f Istituto di Ricerca per la Protezione Idrogeologica (IRPI), CNR, Via Madonna Alta 126, Perugia 06128, Italy g Universitat Autònoma de Barcelona (UAB), Institute of Environmental Science and Technology (ICTA), Edifici Z, Carrer de les Columnes, Campus de la UAB, 08193 Bellaterra (Cerdanyola del Vallès), Barcelona, Spain h Catalan Institution for Research and Advanced Studies (ICREA), 08010 Barcelona, Spain A R T I C L E I N F O A B S T R A C T Editor: Dr. Fabienne Marret-Davies The oceanic system has been rapidly changing under human-induced climate change that is taking place at unprecedented rates. The paleoclimate archive of the last two millennia is often adopted to discern the ongoing anthropogenic global warming from the pre-industrial natural climate variability. The Mediterranean Sea is an especially critical system, being particularly affected by climate change. A common group of marine unicellular planktonic calcifiers, coccolithophores, are forming calcite plates, coccoliths. When reaching the sediments, they have been employed as a proxy in many paleoenvironmental reconstructions and are increasingly used in the last centuries. Recent studies indicate a subtle response to historical climate changes, except for primary productivity switches during the Little Ice Age and, most importantly, across the Industrial age. In this work, we use coccolith decadal-scale resolution data from core HER-MC-MR3.3, recovered in the Balearic Sea, exploring their variability over the pre-industrial age, from 700 BCE to 1740 CE. Results are compared to planktonic foraminifera stable isotopes, planktonic foraminiferal assemblages, alkenone-derived SSTs and foraminiferal Mg/Ca-derived SSTs, previously acquired in the same sediment core. Abundance varia­ tions in coccolith assemblages, expressed as Shannon-Wiener diversity H-index changes or as trends and fluc­ tuations in ecological groups are associated with historical climate changes, among others the Medieval Climatic Anomaly and the Little Ice Age, indicating repeated modifications in surface water conditions, in response to hydrological and atmospheric changing patterns. A tight relationship between deep nutricline and upper water column stratified conditions, derived from high abundance of Florisphaera profunda, and high solar irradiation levels is established. The solar activity fingerprint in the F. profunda distribution pattern is further assessed by spectral analysis, with the emergence of significant periodicities observed in solar activity proxies, among others the well-known de Vries-Suess cycle. Finally, we notice small but statistically significant abundance fluctuations in holococcoliths (solution susceptible coccolith forms) that may be tied to their enhanced preservation during increased rainfall in western Europe. This implies the advection of westerlies and long-lasting blocking events that may have promoted deep-water formation and seafloor ventilation during this time. The comparison with sedimentological proxies of bottom current strength shows some inconsistencies but still defines variable and intermittent deep-water formation rates in the Gulf of Lions over the pre-industrial period. * Corresponding author at: Università Degli Studi di Palermo, Dipartimento di Scienze della Terra e del Mare, Via Archirafi 22, 90134 Palermo, Italy. E-mail address: alessandro.incarbona@unipa.it (A. Incarbona). https://doi.org/10.1016/j.gloplacha.2023.104102 Received 7 November 2022; Received in revised form 4 March 2023; Accepted 24 March 2023 Available online 29 March 2023 0921-8181/© 2023 Elsevier B.V. All rights reserved. A. Incarbona et al. Global and Planetary Change 224 (2023) 104102 1. Introduction foraminiferal stable isotopes and sediment grain size parameters (Cis­ neros et al., 2016, 2019; Margaritelli et al., 2018). We show that sig­ Greenhouse gases emission from human activity since the second nificant abundance variations and/or trends in coccolith assemblages industrial revolution (1857 Common Era – CE) led to monthly average are associated with historical climate changes, indicating repeated CO2 and CH4 atmospheric levels of respectively ~420 ppm and ~ 1900 modifications in surface water conditions, in response to hydrological ppb (https://gml.noaa.gov/ccgg/trends/; https://www.esrl.noaa.gov/g and atmospheric changing patterns. md/ccgg/trends_ch4/), whose values are much higher than the highest ones recorded in the Antarctica ice cores over the last 800 kiloyears and 2. Material and methods the last nine glacial/interglacial cycles (Loulergue et al., 2008; Lüthi et al., 2008; Siegenthaler et al., 2005). The global temperature (0.8- 2.1. Material 1.2 ◦ C) and sea-level (20 cm) rise took place at unprecedented rates and are thought to be especially harmful in the Mediterranean Sea, an The MR3.3 27-cm long multicore was recovered in the deep-water important climate change hotspot region (Lionello et al., 2006; MedECC, Minorca sediment drift (40◦ 29′ N; 3◦ 37′ E) at 2117 m water depth 2021). (Fig. 1). The sediment consists of brown nannofossil and foraminifera A two thousand years (2 k) time window is often paralleled to discern silty clay and includes pteropods rich-layers, gastropods fragments and the human-induced climate change from the natural climatic variability dark layers. A light bioturbation is often visible (Cisneros et al., 2016). and trend. The pre-industrial worldwide Sea Surface Temperature (SST) was gently declining, likely due to sunspot minimum activity and 2.2. Coccoliths explosive volcanism (McGregor et al., 2015). Different climatic phases in the Middle-Late Holocene (e.g. Little Ice Age, Medieval Climatic Coccolith analysis was carried every 0.5-1 cm, for a total of 42 Anomaly, Roman period) have been identified by historical documen­ samples, which were analysed with a polarized microscope at ~1000× tation and paleoclimatic proxies and their influence on ancient civili­ magnification. Rippled smear slides were prepared following standard zation rise and fall is well-established (e.g. Büntgen et al., 2016; Drake, procedures (Bown and Young, 1998) on the <63 μm sediment residue. 2012; Hodell et al., 2001; Margaritelli et al., 2020a). Their better un­ 1000 specimens were identified following the taxonomic concepts of derstanding, in terms of impact of climatic forcing on terrestrial and Young et al. (2003) and Jordan et al. (2004). Taxa were grouped in marine paleoenvironments, mechanisms and processes in place, is still a ‘placoliths’, ‘miscellaneous group’, ‘upper photic zone (UPZ) group’, basic requisite to manage natural hazards related to the ongoing climate ‘lower photic zone (LPZ) group’ and ‘holococcoliths’ (Di Stefano and change. Over the last 2700 years of the studied record, we identify five Incarbona, 2004; Incarbona et al., 2010b). Placoliths include Emiliania climatic periods, whose duration follows Büntgen et al. (2016), Mar­ huxleyi, small Gephyrocapsa, Gephyrocapsa muellerae, and Gephyrocapsa garitelli et al. (2018) and Neukom et al. (2019): Talaiotic period (TP) oceanica. The miscellaneous group includes Helicosphaera spp., Coccoli­ base of the record – 0 CE (correspond to the Bronze Age in Margaritelli thus pelagicus, Syracosphaera histrica, Pontosphaera spp., Calcidiscus lep­ et al., 2018); Roman warm period (RP) 0-400 CE; Dark Age (400-800 toporus, Coronosphaera spp., Braarudosphaera bigelowii, Oolithotus fragilis, CE), which includes a short Late Antique Little Ice Age between 540 and Syracosphaera pulchra, Umbilicosphaera sibogae, Ceratolithus spp., Cal­ 660 CE (Büntgen et al., 2016); Medieval Climate Anomaly (MCA) 800- ciosolenia spp., and specimens of all the other species. UPZ group in­ 1250 CE; Little Ice Age (LIA) 1250-1850 CE. cludes Umbellosphaera spp., Rhabdosphaera spp. and Discosphaera Coccolithophores are golden-brown unicellular planktonic algae, tubifera. LPZ group includes F. profound and a negligible number of with calcite plates, the so-called coccoliths, that are dispersed on the Gladiolithus flabellatus specimens. Holococcoliths include all the cocco­ seafloor after their sinking. Living coccolithophores play a key role in liths produced during the haploid life-cycle stage (Incarbona et al., today’s ocean in regulating carbonate chemistry and CO2 atmospheric 2019a). levels (Ziveri et al., 2023). Coccoliths are employed in a large set of The N ratio is used to reconstruct the nutricline dynamics and is paleoenvironmental and paleoceanographic reconstructions (Baumann calculated following Flores et al. (2000): small placoliths / (small pla­ et al., 2005) and in the Mediterranean Sea show a ready response to coliths + F. profunda), where small placoliths are E. huxleyi, small abrupt climate changes, such as Dansgaard-Oeschger events or Holocene Gephyrocapsa and G. muellerae. High values in the N ratio indicate a rapid climatic changes, mainly in terms of primary productivity vari­ shallow nutricline, while low values in the N ratio indicate a deep ability and vertical water column dynamics (Ausín et al., 2015; Bazzi­ nutricline. calupo et al., 2018, 2020; Cascella et al., 2021; Colmenero-Hidalgo The Shannon-Wiener diversity H-index was assessed by: et al., 2004; Di Stefano et al., 2015; Flores et al., 1997; Incarbona et al., ∑ 2008, 2013, 2019a; Triantaphyllou, 2014; Triantaphyllou et al., 2009a). H= − [(pi )* log(pi ) ] More subtle seems to be the response to historical climate changes, generally lacking any sign of significant abundance variation or where pi = n/N and where n is the number of coccoliths of a given expressed like just general trends (Bonomo et al., 2016; Cascella et al., species and N is the total number of coccoliths of the assemblage. 2019; Vallefuoco et al., 2012), though primary productivity changes have been inferred during the Little Ice Age (Incarbona et al., 2010a) 2.3. Chronology and, most importantly, for the first time, across the Industrial age (Pallacks et al., 2021). The shortage of robust evidence of coccolitho­ The MR3.3 core chronology follows Cisneros et al. (2016). Summa­ phore changes contrasts with more evident variability found in plank­ rizing, the age model was assessed by 6 AMS Δ14C dates and two eco- tonic foraminiferal assemblages (Incarbona et al., 2019b; Lirer et al., biostratigraphic horizons in a Bayesian deposition model by the Bacon 2014; Margaritelli et al., 2016, 2018; Margaritelli et al., 2020b; Pallacks software with the statistical package R. A tuning between Mg/Ca SST et al., 2021; Vallefuoco et al., 2012). However, this difference may be variations and Mn peaks was carried out with the companion HER-MC- tied to the lower number of coccolith studies and to less sensitive MR3.1 and 3.2 cores, where 210Pb and 137Cs activity profiles were also oceanographic settings. acquired. Any readjustment from the tuning was within the 95% con­ Here we explore the variability of pre-industrial (from 700 BCE to fidence level of the Bayesian age model. The average sedimentation rate 1740 CE) coccolith assemblages in sediments of core HER-MC-MR3.3 is 11.0 cm/kyr, the average coccolith analysis resolution is 62 years from (thereafter MR3.3) recovered in the Balearic Sea. Previous data ac­ the base of the core up to sample 15-16 cm (where the sampling pace quired on the MR3.3 core deal with alkenone-derived and Mg/Ca SST, was every 1 cm) and 36 years from sample 14.5-15 cm to the top of the planktonic foraminiferal assemblages, multi-species planktonic core (where the sampling pace was every 0.5 cm). 2 A. Incarbona et al. Global and Planetary Change 224 (2023) 104102 Fig. 1. Bathymetric map of the western Mediterra­ nean Sea (Ocean Data View software), location map of MR-3.3 core (blue circle) and oceanographic fea­ tures modified from Millot (1999), Pinardi and Masetti (2000) and Seyfried et al. (2019). Black ar­ rows show the MAW path: AC, Algerian Current; LG, Lions Gyre, deep-water formation site; LPCC, Liguro- Provenço-Catalan Current. Black dotted arrows show meso-scale eddies from AC instability. White circles, location of: 1, Nmin 1 and 2 cores (Cisneros et al., 2019); 2, Mallorca speleothems (Cisneros et al., 2021); 3, Cava de Asiul speleothems (Smith et al., 2016). White and yellow stars respectively show stations of the coccolithophore surveys VICOMED I and II. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.) 2.4. Spectral analysis Grelaud et al., 2012; Incarbona et al., 2019a; Incarbona et al., 2022; Negri et al., 1999; Triantaphyllou et al., 2009b). The analysis of non-stationary (frequency changes with time) and UPZ are so-called ‘K-strategist’ taxa. They are specialized to exploit a non-linear signals was performed by applying the Ensemble Empirical minimum uptake of nutrients in surface water when a deep summer Mode Decomposition algorithm (EEMD) by Wu and Huang (2009). thermochline takes place (Bazzicalupo et al., 2020; Di Stefano and The EEMD is adaptive noise-assisted data analysis method, that im­ Incarbona, 2004; Incarbona et al., 2013; Young, 1994). Miscellaneous proves the ordinary Empirical Mode Decomposition (EMD) by Huang taxa reflect the lack of distinctive ecological preference, with a possible et al. (1998). This decomposition provides a powerful method to weak K-strategy (Incarbona et al., 2010b; Young, 1994). Holococcoliths investigate the different processes behind a given time series data and prefer dwelling in warm, oligotrophic surface water, like UPZ taxa separates short time-scale events from a general trend. This technique (D’Amario et al., 2017; Kleijne, 1991; Knappertsbusch, 1993; Oviedo relies upon the assumption that any complicated signal can be decom­ et al., 2015). Preservation of holococcoliths improves when dense water posed into a finite and often small number of components called renewal ensures vigorous ventilation/oxygenation of the seafloor and “Intrinsic Mode Functions” (IMFs) (Huang et al., 1998). Each IMF rep­ gets worse in sapropel layers (Crudeli et al., 2006; Incarbona et al., resents an embedded characteristic simple oscillation on a separated 2019a; Incarbona et al., 2022; Incarbona and Di Stefano, 2019). timescale. The IMF components were analysed with “REDFIT” and Cross-wavelet transform (XWT). All data were detrended prior to anal­ 4. Study area ysis. All analyses were carried out with R (version 4.1.3) using Rlibeemd (Luukko et al., 2016), dplR (Bunn, 2010), and WaveletComp (Roesch The Mediterranean anti-estuarine circulation pattern is forced by its and Schmidbauer, 2014) packages. negative hydrological balance (Robinson and Golnaraghi, 1994). Sur­ face water enters the Gibraltar Strait (Modified Atlantic Water - MAW) 3. Coccolithophore ecology and surveys and occupies the first 100-200 m of the water column. MAW flows along the North African coast and reaches the Sicily Strait (Millot, 1999), Placoliths are ‘r-strategist’ taxa, rapidly exploit nutrients in the where it is split (Robinson et al., 1999) into the Tyrrhenian Sea, along photic zone, (Young, 1994). In the Mediterranean Sea, placoliths bloom the northern coast of Sicily and the Italian Peninsula (Millot, 1999) in winter, after nutrient fertilization from deeper water layers, when the (Fig. 1). The flows of MAW west and east of Corsica join and form the water column is mixed (Di Stefano et al., 2011; Keuter et al., 2022; Liguro-Provenço-Catalan Current, also called Northern Current, which is Knappertsbusch, 1993; Triantaphyllou et al., 2004; Ziveri et al., 2000; extended at least as far as the Channel of Ibiza (Millot, 1999). An intense Rutten et al., 2000). thermal front is found between the Gulf of Lions, where relatively cool Florisphaera profunda is a deep photic zone species, whose high Northwesterlies blow, and the Balearic Sea that is far less windy (Millot, relative abundance is linked to the occurrence of a deep nutricline 1999). Part of the Liguro-Provenço-Catalan Current continues south­ (McIntyre and Molfino, 1996; Molfino and McIntyre, 1990). In low- and ward from the Channel of Ibiza, but with less energy and tends to enter middle-latitude open ocean regions, the abundance of F. profunda is a the Alboran Sea where it encounters the energetic flow of recent MAW proxy for primary productivity (Beaufort et al., 1997, 2001; Hernández- (Millot, 1999) (Fig. 1). Almeida et al., 2019). Levantine Intermediate Water (LIW) formation occurs in the eastern In the Mediterranean Sea, except for a limited area in the central part Mediterranean in winter, due to surface cooling on salt-enriched water of the basin, there is no apparent relationship between F. profunda masses (Malanotte-Rizzoli et al., 2014; Malanotte-Rizzoli and Hecht, abundance and satellite-observed primary productivity values 1988) and is established at 200-600 m depth. LIW crosses the Sicily (Hernández-Almeida et al., 2019; Incarbona et al., 2008). However, Channel and flows into the Tyrrhenian Sea (Lermusiaux and Robinson, F. profunda has been generally used to decipher water column stratifi­ 2001; Millot, 1999). LIW maintains almost unaltered values of temper­ cation and development of a deep nutricline due to monsoon-fuelled ature and salinity (14.0-14.5 ◦ C and about 38.5 ‰) from the Ligurian Sea freshwater discharge in the eastern Mediterranean (Castradori, 1993; and the Gulf of Lions to the Balearic and Alboran Seas (Millot, 1999) and 3 A. Incarbona et al. Global and Planetary Change 224 (2023) 104102 is the main source of Mediterranean Outflow Water which passes an important result, given that abundance changes in individual species through the Gibraltar Strait. Deep water formation takes place in the do not cross the treshold of 95% confidence level. Miscellaneous group Gulf of Lions (Western Mediterranean Deep Water - WMDW) and in the and holococcoliths share the same abundance variation pattern (Fig. 3), Adriatic and Aegean Seas (Eastern Mediterranean Deep Water), where but the R2 = 0.27 is not significant. The UPZ group do not show any permanent cyclonic gyres are established. In the Gulf of Lions, Mistral significant abundance fluctuation, even though its abundance since the winds produce surface water cooling and evaporation in winter, leading latest MCA is on average higher than before (Fig. 5). The only correla­ to water column convection, mixing up with LIW and sinking to the tion index value significant, except that already mentioned between seafloor (Malanotte-Rizzoli et al., 2014; Pinardi and Masetti, 2000; placoliths and F. profunda, is the R2 = 0.42 between the Miscellaneous Rohling et al., 2015). Dense shelf water cascading in winter and early group and F. profunda (Fig. 6), that show opposite patterns and fluctu­ spring is a further mechanism that may contribute to the sink of water to ations somewhere in the record (Fig. 5). the seafloor (Canals et al., 2006). WMDW production from convection is The Shannon Wiener index shows abrupt and repeated values thought to be the most relevant process for deep water renewal and may changes between 2.0 and 3.2, with higher frequency modifications since occur while dense shelf water cascading is weak (Durrieu de Madron the Dark ages (Fig. 2). High diversity peaks since the MCA are due to et al., 2017). increased percentage abundances of F. profunda and miscellaneous The transition between the subtropical high-pressure belt over North group taxa (Figs. 2-3). Africa and westerlies over central and western Europe control seasonal atmospheric variations in the Mediterranean/European region. The 6. Discussion displacement of this transition leads to high-pressure established in summer and penetration of northern storm tracks in winter (Rohling 6.1. Solar activity and nutricline depth variations et al., 2015). The Mediterranean region is mainly influenced by the North Atlantic Oscillation (NAO). During positive NAO-index phases, Placoliths and F. profunda are anticorrelated throughout the MR3.3 westerlies blow over the western parts of northern Europe, while dry core record (Fig. 3-4) and their relative abundance fluctuations indicate conditions are experienced in southern Europe and northern Africa and nutricline depth variations within the photic zone (Bazzicalupo et al., vice versa during negative NAO-index phases (Comas-Bru and McDer­ 2018, 2020; Colmenero-Hidalgo et al., 2004; Di Stefano et al., 2015; mott, 2014). However, a very limited impact on modern WMDW pro­ Flores et al., 2000; Incarbona et al., 2008, 2013; Incarbona et al., 2010a, duction is observed by NAO variability, especially in comparison with 2010b; Incarbona et al., 2022). The shallow nutricline associated to a the East Atlantic pattern, whose North-South pressure dipole is centred higher number of placolith and vice versa a deep nutricline for a higher between Greenland and Scandinavia (Josey et al., 2011; Rutten et al., number of F. profunda specimens is summarized by the N-ratio (Fig. 5A). 2000). The comparison with the Total Solar Irradiance (TSI) (Steinhilber et al., 2009) clearly address a tight relationship, with a deep nutricline asso­ 5. Results ciated with high TSI and a shallow nutricline associated to solar activity minima (Fig. 5B). The solar forcing may have acted directly on the water Coccoliths in MR3.3 core are always abundant, well preserved and column dynamics, favoring the summer thermocline deepening during diversified. The distribution patterns of selected taxa are shown in phases of high irradiance and thus establishing a deep photic zone Figs. 2 and briefly commented below. Emiliania huxleyi < 4 μm is the stratification that fosters F. profunda cells proliferation (Hernández- dominant species (71.9-80.2%, 75.6% on average) and shows a general Almeida et al., 2019; Incarbona et al., 2008; Incarbona et al., 2010b). increasing abundance trend to the top of the record (Fig. 2). Emiliania The comparison with G. ruber δ18O values in the MR3.3 core (Margar­ huxleyi > 4 μm abundance is between 0.0 and 2.2% and increases during itelli et al., 2018), suggests the occurrence of warmer/fresher summer the LIA (Fig. 2). Florisphaera profunda is the second most abundant surface water (Rohling et al., 2004) associated with a deep nutricline species, (7.0-18.8%, 11.3% on average), and shows several statistically over the studied record (Fig. 5C). The TSI forcing may also have acted significant variations, with minima centered on the end of the TP, on the indirectly on the Balearic Sea water column dynamics, promoting the end of the Dark Age, in part of MCA and of LIA (Fig. 2). Among occurrence of severe winter conditions in Europe and in the Mediter­ gephyrocapsids, small Gephyrocapsa (1.8-8.8%) shows a decreasing ranean Sea during solar minima, by the long-lasting advection of cold air abundance trend since the Dark Age, G. oceanica (0.0-0.9%) is always from the Arctic or blocking events in the eastern Atlantic (Brugnara rare and its distribution pattern is rather scattered since the MCA et al., 2013; Lockwood et al., 2010; Sirocko et al., 2012). Strong (Fig. 2). Holoccoliths (0.1-2.3%, 1.1% on average) show several abrupt northerly wind events may in turn have caused the southward abundance fluctuations throughout the record, that despite the low displacement of the North Balearic Front and the subsequent SST cooling magnitude are often significant at a 95 % confidence level (Fig. 2). and erosion of the water column stratification, as recently observed in All the other coccolith taxa exhibit abundance values <2% (Cocco­ oceanographic surveys and numerical modelling (Seyfried et al., 2019). lith raw data are available in Supplementary Data Table 1). Umbellos­ The advection of northern cold air masses in the northwestern phaera spp. and Rhabdosphaera spp. do not show significant abundance Mediterranean Sea and the southward displacement of the North fluctuations. Discosphaera tubifera is absent during Dark Age and the Balearic Front associated with a shallow nutricline in the Balearic Sea early MCA. Calcidiscus leptoporus, S. pulchra, S. histrica, Coronosphaera during Roman, Oort, Wolf, Spörer and Maunder TSI minima is supported spp., Helicosphaera carteri, Helicosphaera pavimentum, U. sibogae and by lower foraminiferal Mg/Ca-derived SST in MR-3.3 core, that ac­ Calciosolenia spp. are generally more abundant in the upper part of the cording to G. bulloides ecology in the Balearic Sea should primarily record and during the cold TP, Dark Age and LIA. reflect spring SST (Cisneros et al., 2016; Rigual-Hernández et al., 2012), The most significant result from grouping coccolith taxa is the and cold episodes in the Mediterranean SST stack (Marriner et al., 2022) continuous opposite pattern (both abundance fluctuations and trend) (Fig. 5D-E). between placoliths and F. profunda (LPZ group) (Fig. 3), whose R2 = The solar activity fingerprint in the F. profunda’s MR-3.3 record is 0.66 (Fig. 4). Significant R indices, evaluated by student t-tests (p < clearly visible by the power spectrum, with significant periodicities at 0.005) among different coccolith groups are summarized in Table 1 and 231, 317 and 613 years and by comparison with TSI in the IMF5 shown in Fig. 4. Though six group relationships passed the student t-test component (Fig. 6A-B). The 231-years periodicity (over the CI 99%) is (Table 1), scatter plots in Fig. 4 show the little significance for most of referred to the well-known de Vries-Suess cycle and it has been already them, in terms of correlation Index (R2) values. The miscellaneous group found in the F. profunda record of the central Mediterranean Sea over the exhibits at least one significant abundance fluctuation, centred around whole Holocene and over the last four centuries (Incarbona et al., 2008; the Dark and a distinctive positive trend since the MCA (Fig. 3). This is Incarbona et al., 2010b). The 317- and 613-years periodicity match with 4 A. Incarbona et al. Global and Planetary Change 224 (2023) 104102 Fig. 2. Downcore variations of selected coccolith taxa (%) and coccolith diversity index (Shannon-Wiener H-Index) in core MR-3.3, plotted versus age expressed in years CE. Black horizontal bars show the error associated to countings for a 95% confidence level. Thick black lines represent the 3-pt running average. Grey and white boxes show preindustrial changes in climate and society, drawn following Büntgen et al. (2016), Margaritelli et al. (2018) and Neukom et al. (2019). TP: Talaiotic Period; RP: Roman Period; Dark Age; LA LIA: Late Antique Little Ice Age; MCA: Medieval Climate Anomaly; LIA: Little Ice Age. 5 A. Incarbona et al. Global and Planetary Change 224 (2023) 104102 Table 1 foraminiferal data in core MR-3.3 would respectively confirm a sus­ results from the T-student test for coccolith groups. In red, R values. In Blue, p tained nutricline shallowing and productivity increase in the pre- values. In bold, statistically significant results (p < 0.005). industrial central-western Mediterranean (Incarbona et al., 2010b, Placoliths UPZ Miscellaneous LPZ Holococcoliths 2019b; Margaritelli et al., 2018; Pallacks et al., 2021). Placoliths 1.00 0.01 0.01 0.66 0.11 UPZ 0.01 1.00 0.31 0.25 0.20 6.2. Holococcolith preservation and deep-water production Miscellaneous 0.01 0.31 1.00 0.42 0.27 LPZ 0.66 0.25 0.42 1.00 0.06 Holococcoliths (coccoliths produced by different species during the Holococcoliths 0.11 0.20 0.27 0.06 1.00 haploid. phase of the life cycle) behave as unique ecological category, with a ~350-years and with 500-700 periodicities found in solar activity distinct preference for warm and oligotrophic surface waters (D’Amario proxies over the Holocene in Antarctica ice cores (Soon et al., 2014). The et al., 2017). In the Mediterranean sedimentary record, holococcolith cross-wavelet analysis between F. profunda percentage values and the abundance is tightly controlled by preservation, which is enhanced by TSI shows that the 500-700 years signal is present throughout the last seafloor ventilation (Crudeli et al., 2006; Di Stefano et al., 2015; 2700 years and that higher frequency signals emerge since the Dark Age Incarbona et al., 2019a; Incarbona and Di Stefano, 2019). In core MR- (Fig. 6C). The match between F. profunda abundance changes in the 3.3, most of the holococcoliths belong to the species Calyptrosphaera Balearic Sea and TSI values provides further evidence that solar vari­ oblonga, as for Holocene sapropel S1 studies (Crudeli et al., 2006; Di ability is a main climatic forcing for water column and phytoplankton Stefano et al., 2015; Incarbona et al., 2019a; Incarbona et al., 2022; dynamics during the preindustrial age. Incarbona and Di Stefano, 2019), suggesting the prevalent action of A recent climate simulation suggested that, during insolation seafloor selective preservation in shaping their distribution. Thus, hol­ minima, an atmospheric pattern like the East Atlantic/Western Russian ococcoliths would indicate different episodes of increased seafloor developed over the Mediterranean region, which favors continental cold ventilation during the end of TP and of Dark Age, and across part of the winds to penetrate the Aegean Sea and blocks their influence in the Gulf MCA and of LIA, rather than changes in paleoecological conditions of Lions (Cortina-Guerra et al., 2021). This atmospheric pattern, and the (Fig. 7A). subsequent SST gradient between the two Mediterranean subbasins, The recent (last few millennia) history of the Mediterranean deep- would explain the slight delay of N-ratio peaks, with respect to Roman, water formation, either in the western or eastern Mediterranean Sea, Oort, Wolf, and Spörer TSI minima (Fig. 5A-B), that the cross-correlation is still unclear. Organic geochemical proxies point to enhanced Aegean analysis estimates in a 50-60-year lag (Fig. 6D). Sea deep-water formation during MCA and the earliest LIA (Fig. 7B) Coccolithophore geographic distribution is mainly influenced by (Gogou et al., 2016), possibly linked to recurrent Eastern Mediterranean hydrology (surface and subsurface currents, fronts) and water column Transient-like episodes, during which water exchange in the Sicily dynamics, rather than solely SST. However, E. huxleyi > 4 μm specimens Channel was enhanced (Incarbona et al., 2016). In the western Medi­ seem to be a tracer of cold surface water masses in the Atlantic Ocean terranean, the non-cohesive silt fraction (UP10) records, whose oscil­ and Mediterranean Sea sediments of the latest Pleistocene (Colmenero- lations follow the deep-water circulation strength, have been recently Hidalgo et al., 2004; Flores et al., 2010). The amount of large E. huxleyi acquired for the here studied location (Fig. 7C) (Cisneros et al., 2019). specimens in the Mediterranean during the Holocene is largely negli­ In the studied record, holococcolith enhanced preservation is in line gible (Colmenero-Hidalgo et al., 2004; Di Stefano et al., 2015), as in the with δ18O negative values of the Cueva de Asiul speleothem (Fig. 7D), pre-industrial Balearic Sea, where values are <2.5 % (Fig. 5F). Though which marks increased rainfall in North Spain (Smith et al., 2016). In the low abundance variability, E. huxleyi > 4 μm shows a distinctive their original work, Smith et al. (2016) interpreted δ18O negative values peak within the Dark Age (coinciding with the Roman TSI minimum) as a result of Atlantic wet air masses advection into the western Medi­ and values significantly above the average in the LIA (coinciding with terranean, like today’s NAO negative phases. However, the δ18O Cueva Wolf, Spörer and Maunder TSI minima), suggesting its high sensitivity to de Asiul speleothem variability seems to be different from current NAO slight SST changes, whose magnitude is <2 ◦ C (Fig. 5). reconstructions (Faust et al., 2016; Olsen et al., 2012; Trouet et al., Percentage values of the deep photic zone F. profunda in sediment 2009), for instance during the MCA (Fig. 7F). In any case, independently cores are used for quantitative primary paleoproductivity reconstruction from the NAO pattern, it is evident that enhanced holococcolith pres­ at low- and middle-latitude, after calibration by satellite-derived pro­ ervation match with increased North Spain rainfall during the middle ductivity estimates (Hernández-Almeida et al., 2019). In the Mediter­ MCA and LIA and even during TP and Dark Ages (Fig. 7). A closer spe­ ranean Sea, the relationship between F. profunda relative abundance and leothem record from Mallorca Island (Fig. 7E) (Cisneros et al., 2021) primary productivity estimates is questioned (Hernández-Almeida et al., provides further evidence that holococcolith enhanced preservation 2019). Living coccolithophore data from six and five stations in the area occurred when speleothem δ18O negative values suggest enhanced (around Balearic Islands and in the Gulf of Lions) were respectively rainfall in this part of the Mediterranean Sea. In this speleothem com­ recovered by the Vicomed I (September-October) and II (February- posite record, a hiatus exists for the MCA and early LIA, but the late LIA March) expeditions (white and yellow stars in Fig. 1) (Knappertsbusch, wet phase (~ 1700 CE), coincides with the last holococcolith abundance 1993). A relevant amount of F. profunda cells is found just in two stations peak (Fig. 7). during the summer-autumn cruise, and unexpectedly, in a station in Increased North Spain and Mallorca rainfall implies the advection of winter (Knappertsbusch, 1993). A consistent distribution of F. profunda strong and prolonged westerlies, possibly by long-lasting blocking cells compared to hydrological parameters (e.g. SST, thermocline depth) events that modifies their blow and thus impacting western Europe is not evident for both Vicomed I and II. Maybe, this is due to the too (Margaritelli et al., 2020b). Blockings and prolonged westerlies action short interval of the investigation that obscure coccolithophore may be among the main triggers for deep-water formation (Cacho et al., blooming episodes, detected by long-series investigation, such as trap 2000; Moreno et al., 2005), promoting seafloor ventilation and hol­ sediments (Auliaherliaty et al., 2009; Hernández-Almeida et al., 2011; ococcolith preservation. Abundance peaks of planktonic foraminifera Ziveri et al., 2000). However, at least the linear trend of nutricline Globorotalia truncatulinoides during MCA and LIA suggest the occurrence shallowing before the Second Industrial Revolution (~ 1850 CE) is of a winter deep mixed layer in the Balearic Sea (Margaritelli et al., consistent with the same trend in planktonic foraminifera proxies for 2018; Margaritelli et al., 2020) and support the strengthened atmo­ surface water productivity (Fig. 5G) and deep chlorophyll maximum spheric circulation. (Fig. 5H) (Margaritelli et al., 2018). Thus, coccolith and planktonic Holococcolith preservation is also in good match with the lightest G. bulloides δ18O seawater values in the same MR-3.3 core (Fig. 7G). 6 A. Incarbona et al. Global and Planetary Change 224 (2023) 104102 Fig. 3. Downcore variations of coccolith groups (%) in core MR-3.3, plotted versus age expressed in years CE. Black horizontal bars show the error associated to countings for a 95% confidence level. Thick black lines represent the 3-pt running average. Grey and white boxes show preindustrial changes in climate and society, drawn following Büntgen et al. (2016), Margaritelli et al. (2018) and Neukom et al. (2019). TP: Talaiotic Period; RP: Roman Period; Dark Age; LA LIA: Late Antique Little Ice Age; MCA: Medieval Climate Anomaly; LIA: Little Ice Age. 7 A. Incarbona et al. Global and Planetary Change 224 (2023) 104102 Fig. 4. scatter plots of coccolith groups (%) in core MR-3.3, whose correlation is significant adopting results from the T-student test (see Table 1). Florisphaera profunda equals LPZ group. The black line shows the linear fit. The equation of the linear fit, R2 correlation index and number of samples are also reported. 8 A. Incarbona et al. Global and Planetary Change 224 (2023) 104102 (caption on next page) 9 A. Incarbona et al. Global and Planetary Change 224 (2023) 104102 Fig. 5. Downcore variations of selected coccolith taxa (%) in core MR-3.3, plotted versus age expressed in years CE, in comparison with climatic and oceanographic proxies. A: coccolith N-Ratio in core MR-3.3 (this study), as a proxy of the nutricline depth. The thick black line shows the linear trend. B: Total Solar Irradiation (W/ m2) (Steinhilber et al., 2009). The thick red curve represents the 3-pt running average. The red filling shows values lower than -0.2 of solar minima. C: Globigerinoides ruber δ18O (‰) in core MR-3.3 (Margaritelli et al., 2018). D: Globigerina bulloides Mg/Ca SST (◦ C) in core MR-3.3 (Cisneros et al., 2016). E: Mediterranean SST (◦ C) stack (Marriner et al., 2022). The thick green curve represents the 15-pt running average. F: Emiliania huxleyi (%) in core MR-3.3 (this study). Note the reverse axis. The brown filling shows values higher than 1.0%. G: the sum of Turborotalita quinqueloba and Globigerinita glutinata (%) in core MR-3.3 (Margaritelli et al., 2018), as a proxy of surface water productivity. The thick grey curve represents the 3-pt running average. The thick grey line shows the linear trend. H: the sum of Neo­ globoquadrina incompta and Neogloboquadrina dutertrei (%) in core MR-3.3 (Margaritelli et al., 2018), as a proxy of deep chlorophyll maximum. The thick purple curve represents the 3-pt running average. The thick purple line shows the linear trend. Grey and white boxes show preindustrial changes in climate and society, drawn following Büntgen et al. (2016), Margaritelli et al. (2018) and Neukom et al. (2019). TP: Talaiotic Period; RP: Roman Period; Dark Age; LA LIA: Late Antique Little Ice Age; MCA: Medieval Climate Anomaly; LIA: Little Ice Age. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.) Fig. 6. Spectral analysis of Florisphaera profunda data in core MR-3.3 and comparison with TSI. A: Bias-corrected power spectrum of unevenly sampled F. profunda abundance. Red and green lines respectively refer to 99 and 95% confidence level. Significant periodicities are indicated. B: Cross-wavelet analysis between F. profunda percentage values in core MR-3.3 and TSI (Steinhilber et al., 2009) throughout the last 2700 years of the record (years in CE). C: IMF5 of F. profunda percentage values in core MR-3.3 and TSI (Steinhilber et al., 2009) throughout the last 2700 years of the record (years in CE). Grey and white boxes show prein­ dustrial changes in climate and society, drawn following Büntgen et al. (2016), Margaritelli et al. (2018) and Neukom et al. (2019). TP: Talaiotic Period; RP: Roman Period; Dark Age; LA LIA: Late Antique Little Ice Age; MCA: Medieval Climate Anomaly; LIA: Little Ice Age. D: Cross-correlation analysis between F. profunda percentage values in core MR-3.3 and TSI (Steinhilber et al., 2009) throughout the last 2700 years of the record. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.) There at least two possible explanations for this relationship, linked to speleothems (Figs. 7D-E); 2) the arrival of meso-scale eddies associated prolonged wind action, enhanced deepwater formation in the Gulf of to the Algerian Current, characterized by lower salinity from not or little Lions and the southward shift of the North Balearic Front: 1) the arrival modified (poorly vertically mixed) Atlantic surface water (Barral et al., in the Minorca Rise area of Rhone River freshwater plumes (Barral et al., 2021). 2021), that would be in agreement with enhanced rainfall from Spain The holococcolith distribution pattern is instead apparently quite 10 A. Incarbona et al. Global and Planetary Change 224 (2023) 104102 (caption on next page) 11 A. Incarbona et al. Global and Planetary Change 224 (2023) 104102 Fig. 7. Downcore variations of holococcoliths (%) in core MR-3.3, plotted versus age expressed in years CE, in comparison with climatic and oceanographic proxies. A: holococcoliths in core MR-3.3 (this study), as a proxy of seafloor ventilation. Note the reverse axis. The black filling shows values higher than 1.5%. B: C26OH (%) Index Aegean Sea (Gogou et al., 2016). The grey filling shows values lower than 30.0%. C: non-cohesive silt fraction (UP10) percentage values from NMin1 (red curve) and NMin2 (blue curve) Balearic Sea cores (Fig. 1) (Cisneros et al., 2019). Red (> 42.5%) and blue (37.5%) fillings refer to numerical sills that would determine deepwater formation events. D: δ18O (‰) from Cueva de Asiul speleothems, North Spain (Fig. 1) (Smith et al., 2016). The brown filling shows values lower than 0.0‰. The black dashed refers to detrended data. E: δ18O Mallorca speleothem composite record (Fig. 1) (Cisneros et al., 2021). The green filling shows values lower than 0.0‰. F: NAO reconstructions (Trouet et al., 2009, blue line; Olsen et al., 2012, orange line; Faust et al., 2016, light green line). The three curves represent a 5-pt running average. G: Globigerina bulloides δ18Oseawater in core MR-3.3 (Cisneros et al., 2016). The purple curve represents a 3-pt running average. Grey and white boxes show preindustrial changes in climate and society, drawn following Büntgen et al. (2016), Margaritelli et al. (2018) and Neukom et al. (2019). TP: Talaiotic Period; RP: Roman Period; Dark Age; LA LIA: Late Antique Little Ice Age; MCA: Medieval Climate Anomaly; LIA: Little Ice Age. (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.) different from the UP10 record from Nmin1 and Nmin2 cores (Fig. 7C) proxies that make them sensitive to chemical and physical changes (Cisneros et al., 2019). The UP10 data were interpreted as a proxy for respectively. In any case, both proxy records suggest the intermittent deep convection in the Gulf of Lions, and thus they provide an appar­ activity of deep-water formation in the Gulf of Lions over the pre- ently conflicting view with the here presented results. However, looking industrial period. at numerical sills in the UP10 records that would determine deepwater Supplementary data to this article can be found online at https://doi. formation events (> 37.5% in Nmin1 and > 42.5% in Nmin2 cores, see org/10.1016/j.gloplacha.2023.104102. red and blue fillings in Fig. 7C curves), the strongest discrepancy may be restricted to the RP. Nevertheless, the holococcoliths and UP10 proxies have a very different nature and thus respond to different environmental Declaration of Competing Interest variables related to WMDW formation in the Gulf of Lions. On one side, holococcoliths should be rather tied to seafloor ventilation conditions The authors declare that they have no known competing financial (oxygen content and seawater carbonate chemistry, see Incarbona et al., interests or personal relationships that could have appeared to influence 2019a; Incarbona et al., 2022) while UP10 should reflect bottom current the work reported in this paper. strength (physical features like speed, see Cisneros et al., 2019). Such chemical and physical variables could not always have an equal Data availability response in front to different WMDW formation mechanisms (i.e. pref­ erentially record deep water convection versus dense shelf water Data will be available on Pangaea cascading). In any case, the combination of the two micropaleontolog­ ical and sedimentological proxies suggests the intermittent operation of Acknowledgments the Gulf of Lions over the pre-industrial period which needs to be further explored with a wider range of proxies and records. The cores HER-MC-MR3.1A/3.3 has been collected aboard of R/V Hespérides. AI acknowledges the support received from the NBFC, 7. Conclusion funded by the Italian Ministry of University and Research, PNRR, Mis­ sione 4 Componente 2, ‘Dalla ricerca all’impresa’, Investimento 1.4, In the Balearic Sea, northwestern Mediterranean Sea, significant project CN00000033. This research has been financially supported by abundance variations in coccolith assemblages were associated with ERC-Consolidator TIMED project (REP-683237). This research is historical/cultural periods: Talaiotic period, base of the record – 0 CE; contributing to the BIOCAL project (PID2020-113526RB). 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