Warm Period (CWP). The MCA period (~1000-1100 CE) thus appears marked by increase sedimentation rate supported by higher terrigenous input linked to erosive events particularly increases in precipitation. During the LIA, particularly from ~1450 CE to 1600 CE, there is a great variation towards a decrease of terrigenous input, which is related to a decrease on sedimentation rate and increase Mg-calcite precipitation, suggesting less precipitation and high evaporation respectively during dry climate conditions. The MCA-LIA transition (~1200-1400 CE) is characterized by variations between terrigenous input, Mg-calcite formation and organic matter deposition, which indicate succession of dry and humid conditions. The CWP (1800-2000 CE) shows a progressive increase on sedimentation rate and decrease of grey level, which indicate more organic matter sedimentation as consequence of anthropogenic activities in the surrounding basin of the lake. High-resolution grey level analysis, which reflects principally variations in terrigenous input, carbonate mineral formation and organic matter deposition, shows that the AMO, NAO, PDO and ENSO are the principal modes affecting the hydro-climatic changes in Haiti during the last millennium. In addition, temporal correlation of other Caribbean paleoclimate records with our geochemical and mineralogical data, suggests that trends observed in Lake Azuei were controlled by regional climate, likely associated with shifts in the position of the ITCZ.

## Keywords

Climate change, hydroclimate variation, lake sediment core, geochemistry, Lake Azuei, Haiti

## 1. Introduction

The climate of the Caribbean region is subject to the influences of synoptic features of both tropical Atlantic and Pacific basins. Reconstructions of Caribbean climate during the last millennia offer a basis for understanding these influences, and better predicting future global climate. Some studies (Mann et al., 2009; Tierney et al., 2015) have shown that climate modes, particularly the Atlantic Multidecadal Oscillation (AMO) and North Atlantic Oscillation (NAO), the Pacific Decadal Oscillation (PDO) and El Niño-Southern Oscillation (ENSO), have influenced the hydro-climate changes during the last millennium. At the multidecadal timescale various studies (Mann et al. 2009, Knudsen et al. 2011, Apaestegui, et al., 2014) have shown that the tropical climate variability is driven by the interplay between AMO and PDO. In addition to these climate modes, the NAO affects rainfall patterns in the Caribbean through its influence on the strength and position of the North Atlantic Subtropical High (NAH) (Wang, 2007; Cook and Vizy, 2010) and consequently the Caribbean Low Level Jet (CLLJ) (Burn and Palmer, 2014). Mean annual precipitation in the northeastern Caribbean has also been shown to be synchronous with variations in the NAO, at least since 1914 (Malmgren et al., 1998). Furthermore, the amount of rainfall and their variability are also strongly modulated by changes in the Pacific climate mode including ENSO phenomenon (Chen et al. 1997; Giannini, Kushinir and Cane 2000;
Taylor, Enfield and Chen 2002; Ashby, Taylor and Chen 2005; Gamble, Parnell and Curtis, 2008). Superimposed on those climate modes, which dominate the interannual variations observed over the last decades, Black et al., (2004) has shown that solar variability plays a role in influencing the hydrologic balance of the circum-Caribbean region.

In inter-tropical regions, variations in the hydrological cycle have more consequences than variations in temperature on physical ecosystems and systems such as lakes (Goosse and Klein, 2021) which are particularly sensitive to changes in hydro-climatic conditions. These impacts therefore leave important signals in the paleoclimatic records that allow us to reconstruct indices characterizing wet or dry conditions. The lacustrine sediments preserve several markers (organic, inorganic) which provide valuable information about the history of the surrounding basin's lake, its current state and its environment and consequently climate changes. The inorganic sedimentation process is therefore influenced by hydrological factors as erosion which can be linked to changes in precipitation and human activities (agriculture, industrial wastewater, and mining activity) and mineral formation under different physico-chemical conditions. Mineralogical elements composition and concentrations in sediments can vary depending on natural abundance, intensity of precipitation and physico-chemical lacustrine water conditions, morphology of lake surrounding basin and land use practices. Indeed, inorganic elements (Al, Fe, Ti, Zr, K) and calcites can be used as indicators of detrital and lake water temperature respectively

Curtis and Hodell (1993) and Higuera-Gundy et al. (1999), using pollen and isotopic compositions of a sediment core from Lake Miragoâne in southwest Haiti, documented climatic and environmental changes in Haiti during the last 10,500 years, and in particular, changes in the precipitation regime. The results of geochemical evaluation of sediment of Lake Azuei indicated also there were changes in the precipitation regime during the last century (Eisen-Cuadra et al., 2013). However, climate modes haven't been proposed to elucidate these changes. In addition, to date, no detailed study has been done on climate variability during the past millennium in Haiti. Therefore, more temporal and spatial data are needed to constrain Haiti climate change.

To date, few studies have addressed climate variability in the northern Caribbean, (except for the few references from the team of Dave Hodell team: Curtis et al., 1993; Hodell et al., 1994; Higuera-Gundy et al., 1999; Curtis et al., 2001). Instead, most of the focus has been on the southern Caribbean (Lin et al., 1997; Haug et al., 2001; Tedesco and Thunell, 2003; Peterson and Haug, 2006; Schneider et al., 2014) and eastern Central America (Leyden et al., 1994; Brenner et al., 2003; Haug et al., 2003; Hodell et al., 2005; Appendini et al., 2019; Andrade-Velázquez et al., 2021).

Here, we aim to reconstruct the climatic variability in Haiti during the last millennium and discuss how climate mechanisms and modes such as AMO, NAO, PDO and ENSO may have influenced this variability. To that purpose, we carefully analyzed an 84 cm-long core collected from Lake Azuei. Analytical techniques applied include inorganic compositional analysis,
mineralogical analysis, and organic carbon analysis which was carried out on discrete samples
collected every 2 cm down the core. Indeed, inorganic analysis can inform on variations in
terrigenous input to the lake and, by proxy, on variations in surface runoff and riverine inflow.
Mineralogical compositional analysis, such as the measurements of Ca-calcite anomalies versus
Mg-calcite anomalies, are used to determine past variations in water temperatures and are thus
used as proxies for lake evaporation. Lastly, our analysis includes continuous measurements of
grey levels down the core, which provides a higher resolution of sedimentological variability
than discrete samples. Indeed, continuous measurements of grey levels reveal the presence of
small bands and laminae structures whose periodicity may then be compared to that of climatic
modes

Study site

The sediment core LA17BCO2 was collected in January 2017 from Lake Azuei, also known as “Étang Saumâtre” (Fig. 1). This Lake, which is the largest lake in Haiti and the second largest lake in Hispaniola, is located in the Cul-de-Sac watershed, around 29 kilometers east of Port-au-Prince. Its area has experienced a remarkable increase since the end of the 20th century.

Lake Azuei is 22 km long, from northwest to southeast; its maximum width is 12 km and it
measures 30 m at its deepest (James et al., 2019). It is located in one of the driest regions of the
country (Moron et al., 2015) due to the Cordillera Central rain shadow effect. The lake is
endorheic, which means that its level is extremely sensitive to variations in precipitation. It is
located in an alluvial plain (Cul-de-Sac) bordered by mainly carbonate mountain. It lies across
the Enriquillo-Plantain Garden Fault, part of a system of faults that mark the complex boundary
between the North American and Caribbean plates (Mann et al., 1995).
<figure><img src="image_57.png" /><figcaption>Fig. 1: (a) Spatial correlation between instrumental AMO and Sea Surface Temperature (SST) from ERA5-OP5DEG from 1950 to 2020. (b) Bathymetric chart compiled from depth soundings collected between 2013 and 2017 (Cormier et al., 2018). Contour interval is 1 m. Yellow line indicates the Haitian-Dominican border</figcaption></figure>

**2. Materials and method**

**2.1. Lake sediment Coring**

Coring system used was provided by the NSF National Facility “LacCore” at the University of
Minnesota-Minneapolis. The core LA17BCO2, 84 cm length, was collected at 19.8 m of water
depth using the Bolivia corer which is a piston rod corer. Its GPS coordinates are 18 ° 30.0931'
N, 71 ° 54.0302' W. The core sub-sampling was carried out at the Graduate School of
Oceanography, United States. The samples were taken every two centimeters, except in some
level where samples had already been taken for radio-isotope dating. In total, 32 samples were
taken from the core for the geochemical and mineralogical analysis.

**2.2. Dating**

Ten ¹⁴C measurements by AMS were made on 3 samples consisting of gastropod shells, 1 wood sample, and 6 bulk sedimentary organic carbon samples. Dating of gastropod shells and wood was performed in the U.S.A at the Beta Analytical Laboratory, Miami, Florida, and at the NOSAMS facility in Woods Hole, Massachusetts. Dating of bulk organic matter sediment was carried out at the LMC14 laboratory, Saclay, Paris, France. To date the upper part of the core more precisely, activities of ²¹⁰Pbxs (unsupported Pb) were carried out at the University of Rhode Island every centimeter over the upper 10 centimeters. Sedimentation rates were estimated by applying the constant initial concentration (CIC) model of ²¹⁰Pb. Because atmospheric radiocarbon production has varied over geologic time, radiocarbon ages have been calibrated to provide dates in years CE. Thus, calibrated ages (2 sigma) in “approximate calendar” years were obtained from Stuiver et al. (1998) by means of the calibration program CALIB 8.2 software (Stuiver and Reimer, 2022).

**2.3. Lithology, grey level and wavelet analyses**

Physical characteristics such as sediment color, bands and laminae structures, were determined both at the macroscopic and microscopic scales. Grey levels were measured using Image software on a high resolution photo of the core taken at the University of Rhode Island. The image software, ImageJ, is a Java-based image processing program developed at the National Institutes of Health and the Laboratory for Optical and Computational Instrumentation (LOCI, University of Wisconsin). The grey level was set from 0 to 255. Larger numbers imply brighter colors (Cortijo et al., 1995).

Wavelet analysis is used to study the frequency composition and to visualize variability of some periodicities (Torrence and Compo, 1998). It was applied in our study to the high-resolution grey level measurements to extract the dominant frequencies embedded in the fine-scale sediment layers.

**2.4. Inorganic compositional analyses.**

Major and trace (Ca, Al, Fe, K, Ti, Zr) element concentrations were analyzed by ICP-MS (Agilent 7500 cx) at IRD, LOCEAN, Bondy, after acid digestion following the methodology used by Valdés et al. (2014) : 1) samples weighing 20 to 25 mg into savilex vessel were treated with a combination of nitric acid (HNO₃) and hydrofluoric acid (HF), followed by heating at 150
°C for 48h; 2) HF and perchloric acid (HClO₄) solution was added and digested at 150°C for 24 h ; 3) HNO₃ attack was done twice at 150 °C to evaporate all acid from the samples; 4) the resulting material was brought to 35 mL with HNO₃. The analytical procedure was controlled by the routine replicate analysis, target material, and MESS-3 certified reference material. The analytical validation data showed accuracy with a relative error that did not exceed 5 %.

**2.5. Mineralogical analyses.**

The mineralogical composition was determined by X-ray diffraction (XRD) at IRD, LOCEAN, Bondy, using a PANalytical X'Pert powder diffractometer with Ni-filtered CuKα at 40kV and 40mA, equipped with a PIXcel detector. Samples, previously ground with an agate mortar were prepared as randomly oriented powder mounts and scanned from 2 to 70° (2θ) with a step size of 0.0131 °2θ. Mineral identification was performed using the High score 3.0 software (PANalytical®) and two databases: ICSD (Inorganic Crystal Structure Database) and COD (Crystallography Open Database) (Grazulis et al., 2009).

Estimation of the contribution of the main detected minerals was achieved by using the integrated peak area of the most intense diffraction peak of calcite (d₁₀₄, 3.03 Å), Mg-calcite (d₁₀₄, at 2.99 Å), aragonite (d₁₁₁, 3.40 Å), quartz (d₁₀₁, 3.34 Å) and clays (represented by a common diffraction peak at 4.50 Å). The relative contribution of each mineral, expressed as a percentage of the sum of all the measured peak areas, does not represent a mass percentage but allow following the variability of the mineralogical composition along the core.

**2.6.Organic carbon analyses.**

Organic carbon content (Corg) was measured with an elemental analyzer Flash 2000HT from Thermo Fischer Scientific coupled to a thermal conductivity detector (TCD) at LOCEAN, Bondy, France. Each sample was weighted in a precision balance and placed in tin capsules. Prior to the analyses, carbonates were removed with hydrochloric acid 10% (Nava-Fernández et al., 2022).

**3. Results**

**3.1.Chronology and sedimentation rate**

The ¹⁴C measurements and ²¹⁰Pb dating are represented in Table 1 and Table 2, respectively.
<table><caption>Table 1. Sediment Depth-Age Relations using dating <sup>14</sup>C for LA17BCO2</caption><thead><tr><th>Laboratory</th><th>Depth (cm)</th><th>Sample (material)</th><th>Age <sup>14</sup>C (BP)</th><th>Calibration</th><th>Reservoir corrected <sup>14</sup>C age BP</th><th>Calibrated Age 2σ (CE)</th></tr></thead><tbody><tr><td>NOSAMS-USA</td><td>6-7</td><td>AMS <sup>14</sup>C gastropod</td><td>2680 +/- 25</td><td>IntCal20</td><td>48 +/- 25</td><td>1902</td></tr><tr><td>LMC14-France</td><td>10-11</td><td>Sediment</td><td>2465 +/- 25</td><td>IntCal20</td><td>115 +/- 25</td><td>1870</td></tr><tr><td>LMC14-France</td><td>16-17</td><td>Sediment</td><td>2595 +/- 35</td><td>IntCal20</td><td>245 +/- 30</td><td>1715</td></tr><tr><td>LMC14-France</td><td>28-29</td><td>Sediment</td><td>2730 +/- 30</td><td>IntCal20</td><td>490 +/- 30</td><td>1430</td></tr><tr><td>Beta-Analytic-USA</td><td>42-43</td><td>AMS 14C wood</td><td>990 +/- 30</td><td>IntCal20</td><td>990 +/- 30</td><td>1130</td></tr><tr><td>Beta-Analytic-USA</td><td>42-43</td><td>AMS 14C gastropod</td><td>3230 +/- 30</td><td>IntCal20</td><td>990 +/- 30</td><td>1120</td></tr><tr><td>LMC14-France</td><td>56-57</td><td>Sediment</td><td>2860 +/- 30</td><td>IntCal20</td><td>620 +/- 30</td><td>1310</td></tr><tr><td>Beta-Analytic-USA</td><td>63-64</td><td>AMS 14C gastropod</td><td>2970 +/- 30</td><td>IntCal20</td><td>730 +/- 30</td><td>1280</td></tr><tr><td>LMC14-France</td><td>68-69</td><td>Sediment</td><td>3275 +/- 30</td><td>IntCal20</td><td>1035 +/- 30</td><td>750</td></tr><tr><td>LMC14-France</td><td>81-82</td><td>Sediment</td><td>3110 +/- 30</td><td>IntCal20</td><td>870 +/- 30</td><td>1200</td></tr></tbody></table>

Lake Azuei is a hard-water lake varying in hardness between 525-2260 mg/l of CaCO$_3$ (Matthes, 1988). Consequently the radiocarbon dates of shells and bulk sedimentary organic carbon are subjected to errors resulting from the dilution of <sup>14</sup>C by “old” carbon (i.e. <sup>14</sup>C-free) which is derived from the dissolution of calcareous bedrock; this is called "hard - water - lake error (HWLE)". Taking into account the dates of <sup>210</sup>Pb and the gastropods for the 6-7 cm interval and those of wood and gastropods for the 42-43 cm interval, three corrections of hard water effect can be estimated. In the upper part (6-7 cm), a HWLE of 2630 yrs BP was removed from the <sup>14</sup>C date. From 10 to 17 cm, a HWLE of ~2350 yrs BP was removed from the <sup>14</sup>C dates, assuming a constant sedimentation rate between 6 cm and 42 cm. Below 28 cm, they are subtracted from 2240 yrs BP based on the dating of the wood sample.

<table><caption>Table 2. <sup>210</sup>Pb measurements performed on the upper core. Regression through these measurements indicates a sedimentation rate of 0.134 cm/yr</caption><thead><tr><th>Depth (cm)</th><th><sup>210</sup>Pbxs (dpm/g)</th><th>ln (<sup>210</sup>Pb<sub>xs</sub>)</th><th>rate sedimentation (cm/yr)</th></tr></thead><tbody><tr><td>0-1</td><td>2.717</td><td>1</td><td>0.134</td></tr><tr><td>1-2</td><td>1.791</td><td>0.583</td><td>0.134</td></tr><tr><td>2-3</td><td>1.482</td><td>0.393</td><td>0.134</td></tr><tr><td>3-4</td><td>0.987</td><td>-0.013</td><td>0.134</td></tr><tr><td>4-5</td><td>0.884</td><td>-0.124</td><td>0.134</td></tr><tr><td>5-6</td><td>0.698</td><td>-0.359</td><td>0.134</td></tr><tr><td>6-7</td><td>0.694</td><td>-0.365</td><td>0.134</td></tr></tbody></table>

<sup>210</sup>Pb and radiocarbon dates were combined to form a Bayesian age-depth model using the rBacon package within *R* (Blaauw and Christen 2011). Mean ages were extracted from the model
and used for the representation and interpretation of the proxy data. Observing the graphical representation of the age-depth used to establish the chronology (Fig. 2a).

<figure><img src="image_58.png" /></figure>

Fig. 2: (a) Bayesian age-depth model for core LA17BCO2 generated using rBacon for R, displaying ¹⁴C dates corrected for HWLE. The jagged blue error bars display the ¹⁴C age probability distribution for each sample; the dotted red line follows the mean ages. In detail at the top from left to right; number of iterations, sedimentation rate and memory, this is interpreted as the dependence of the accumulation rate between neighboring depths. (b) Sedimentation rate (cm/yr) calculated from age-depth model. Average sedimentation rate in sediment core determined with the age-depth model (Fig. 2b), was 0.128 ± 0.079 cm/yr. The higher values are observed between: 84 to 76 cm (1000 to 1150 CE), 68 to 41 cm (1100-1250 CE) and 10 to 0 cm (1900-2000 CE). From 38 to 10 cm (1300 to 1900 CE) we observed a trend to decrease of sedimentation rate.

## 3.2. Lithology and grey level

Based on the visual characteristics of the sediments, different stratigraphic levels could be identified for LA17BCO2 (Fig. 3, core image). The different levels were characterized either by the clay facies or by frequent alternation of organic matter within clayey to homogeneous silty levels or by less frequent alternation of organic matter and a more silty level. The upper levels have a much darker color, therefore much richer in organic matter. The macrofauna is mainly composed of gastropods. In the middle of the core there is a particularly high concentration of gastropods. Microscopic observation of some samples indicates that the sediment facies contain fine grains of authigenic limestone. Amorphous and fluorescent organic matter is also present. Some plant debris were observed.

The observed grey level values varied between 32 (darker) and 240 (brighter). The grey level data exhibit high variations in different level of the core (Fig. 3). Brighter colors were found in
the lower part of the core than in the upper part. Highest values are recorded for two intervals, between 80 to 72 cm, and 60 to 48 cm. From 42 to 36 cm grey level show high fluctuations between low and high grey level values. Finally, a tendency towards a decrease of grey level values was observed from 28 cm and reaches the minimum between 12 cm and the top of the cores.

### 3.3. Variation of the mineralogical composition

<figure><img src="image_59.png" /></figure>

Fig. 3 Core picture; lithological profile, grey level variation, and distribution of the mineral content expressed as a peak area percentage of the core LA17BCO2 are plotted against depth.

The mineralogical composition of the different samples is homogeneous. The most prominent mineral phase throughout the core consists of carbonates: Calcite ($CaCO_3$, called here $Ca-calcite$), Mg-calcite ($Mg_xCa_{1-x}CO_3$) and aragonite ($CaCO_3$). The peak area percentages of $Ca-calcite$, Mg-calcite, aragonite, quartz and clays are shown in Fig. 3. $Ca-calcite$, quartz and clays have the same behaviour and are strongly positively correlated (Fig. 3, Table 3). By contrast, Mg-calcite has an exact opposite behaviour as quartz, clays and $Ca-calcite$. For aragonite, there is almost no variation in its proportions in the different levels except a slight increase in the 36 cm.
3.4. Variation of the geochemical composition

<figure><img src="image_60.png" /><figcaption>Fig. 4 The temporal variations of the geochemical composition (core LA17BCO2) of Lake Azuei.</figcaption></figure>

The most abundant major element in the lake sediments is Ca, in agreement with the high calcite (Ca-calcite and Mg-calcite) content (Fig. 3). Following in order of abundance are Al, Fe, K, Ti and Zr. Indeed, the average percentages of the elements analyzed: Ca, Al, Fe, K, Ti, Zr, are, respectively, 32.48 ± 5.06 %, 1.21 ± 0.31%, 1.05 ± 0.22 %, 0.23 ± 0.04 %, 0.12 ± 0.03 %, and 0.0016 ± 0.00004 %; with a maximum value at 43 cm and a minimum values at 36 cm. Variations in concentrations Al, Fe, K, Ti and Zr are correlated as confirmed by the coefficient of Pearson (Fig. 4, Table 3). The greatest amplitude of the variation in the concentrations of elements is observed between 46 and 22 cm. Ca concentrations vary in opposition to Al, Fe, K, Ti and Zr concentrations in the upper half of the core: From 48 to 10 cm, where Ca concentrations increase, there is decrease in Al, Fe, K, Ti and Zr concentrations.
The organic carbon content, C<sub>org</sub>, varies in a narrow range from 0.6 % to 4.9 % (average of 2.5 ± 1.22 %). It is highly variable and trend to increase in the topmost sediments. C<sub>org</sub> varies in an opposite trend to Ca (Fig. 4).

## 4. Discussion and interpretation

The results are discussed and interpreted according to three major periods that have marked the climate during the last millennium: Medieval Climate Anomaly (MCA, 1000-1100 CE), the Little Ice Age (LIA, 1450-1800 CE) and the Current Warm Period (CWP, from 1850 CE to present) (Bird et al., 2011).

### 4.1. Terrigenous input (Detrital input)

A Pearson correlation analysis (Table 3) confirms a positive correlation between the terrigenous fractions (Al, Fe, Ti, K, and Zr), and their negative correlation with Ca. Indeed, Al, Fe, Ti, K and Zr correlate well with each other indicating that all those elements are from the same source area. They also show similar variations (Fig. 4), suggesting that the variation of water balance components (surface runoff, riverine inflow) through the watershed affect the input of these elements into the lake. K, Ti and Zr are significantly correlated to Al and Fe confirming their common and crustal origin. In addition, Al, Fe, Ti, K, and Zr are strongly correlated with the Ca-calcite content (Fig. 5, Table 3) and the detrital minerals (clays and quartz) (Table 3), suggesting their common origin, and negatively correlated with the Mg-calcite content. Lower Mg-calcite contents correspond to higher proportion of the other minerals (Fig. 3).

<table><caption>Table 3. Pearson's correlation coefficient matrix between metals and mineral compositions</caption><thead><tr><th>Variables</th><th>Al</th><th>Ti</th><th>Fe</th><th>Zr</th><th>K</th><th>Clays</th><th>Quartz</th><th>Ca-Calcite</th><th>Mg-Calcite</th><th>Ca</th></tr></thead><tbody><tr><td>Al</td><td>1</td><td></td><td></td><td></td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>Ti</td><td>0.957</td><td>1</td><td></td><td></td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>Fe</td><td>0.965</td><td>0.973</td><td>1</td><td></td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>Zr</td><td>0.959</td><td>0.975</td><td>0.955</td><td>1</td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>K</td><td>0.844</td><td>0.938</td><td>0.930</td><td>0.875</td><td>1</td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>Clays</td><td>0.716</td><td>0.728</td><td>0.760</td><td>0.710</td><td>0.762</td><td>1</td><td></td><td></td><td></td><td></td></tr><tr><td>Quartz</td><td>0.843</td><td>0.722</td><td>0.792</td><td>0.759</td><td>0.559</td><td>0.625</td><td>1</td><td></td><td></td><td></td></tr><tr><td>Ca-Calcite</td><td>0.871</td><td>0.771</td><td>0.780</td><td>0.824</td><td>0.559</td><td>0.606</td><td>0.876</td><td>1</td><td></td><td></td></tr><tr><td>Mg-Calcite</td><td>-0.670</td><td>-0.623</td><td>-0.596</td><td>-0.702</td><td>-0.443</td><td>-0.451</td><td>-0.631</td><td>-0.748</td><td>1</td><td></td></tr><tr><td>Ca</td><td>-0.258</td><td>-0.241</td><td>-0.231</td><td>-0.237</td><td>-0.179</td><td>-0.396</td><td>-0.403</td><td>-0.445</td><td>0.315</td><td>1</td></tr></tbody></table>

One of the first parameters that can strongly influence the concentrations of elements independently of the redox conditions or the productivity of the environment at the time of deposition is terrigenous input. Indeed, parts of the elements of most sediment are of detrital origin (Tribovillard et al., 2006). The impact of detritus on the concentrations of the studied
elements would be verified if their concentrations were correlated to that of aluminum (Calvert and Pedersen, 1993; Hild and Brumsack, 1998; Böning et al., 2004; Tribovillard et al., 2006), as is indeed the case for our measurements (Table 3). These elements are therefore mainly of detrital origin and can be used to interpret the depositional conditions. Al, Fe, Ti, K and Zr variations in the Lake Azuei are not diagenetically controlled, and can be interpreted to reflect changes in terrigenous inputs and the pedogenic processes occurring in the surrounding basin. The variations of Al, Fe, Ti, K and Zr content in the sediment will thus be interpreted as a proxy of soil erosion, with low concentrations indicating less transport and, conversely, high concentrations indicating more transport to the lake. Indeed, the MCA period (1000-1100 CE) is characterized by positive anomalies of terrigenous input (Fig. 5), related to detrital input in the lake. The MCA-LIA transition (1200-1400 CE) is characterized by variations between positive and negative anomalies of terrigenous input. However, the LIA (1400-1800 CE) period is characterized by negative anomalies of terrigenous input (Fig. 5), related to less detrital input in the lake. Additionally, some periods characterized by positive (negative) anomalies for the sum of Al, Fe and Ti, display negative (positive) anomalies of Ca (Fig. 5). The negative anomalies of Ca may be the result of increased dilution by terrigenous particles derived from erosion (Baumann et al., 1993). On the other hand, the positive anomalies of Ca are linked to precipitations of calcium carbonates when there is a decrease in terrigenous elements (negative anomalies of sum Al, Fe, and Ti).

## 4.2. Calcite formation.

Several studies have explained the formation and sedimentation processes of calcium carbonate in lakes (Müller et al., 1972; Müller and Wagner 1978; Last, 1982; Effler and Johnson, 1987; Last and De Deckker, 1990; Queralt et al., 1997; Elfil and Roques, 2001; Gal et al., 2002; Morse et al., 2007; Dean, 2009; Solotchina and Solotchin, 2014; Tompa et al., 2014). Various calcium carbonate minerals may occur in the aquatic environment either as primary carbonates or as the results of diagenetic processes in the sediments. Lake water temperature and its concentration in Mg/Ca ratio are the two main factors that determine the composition and crystallographic variety of precipitated calcium carbonate: Ca-calcite, aragonite, Mg-calcite (Müller et al., 1972; Kelts and Hsii, 1978; Morse et al., 2007; Dean, 2009). Temperature not only affects biogenic factors but also the solubility of CO₂ in water (Schwoerbel, 1999). Also, through temperature-dependent evaporation the total volume of water influencing the ion concentration within the lake is modified. Calcite is the most stable crystalline variety of calcium carbonate at ambient temperature and pressure, with aragonite being stable at high pressure (Cölfen, 2003; Nan et al., 2007). Last (1982) showed that the incorporation of significantly higher amounts of Mg in the calcite lattice to form Mg-calcite is associated with increased water temperature. In addition, the little different atomic radius of the Ca²⁺ and Mg²⁺ cations, the identical crystalline structure of their carbonate (rhombohedral), their charges and their similar electronegativities are all factors favorable to the formation of Mg-calcite instead of calcite (Ca-calcite) with an increase in water temperature (Müller et al., 1972; Last and De Deckker, 1990; Queralt et al., 1997; Morse et al.,
2007). The opposite variations of Ca-calcite and Mg-calcite in the Lake Azuei sediments (Fig. 5) can be used to interpret changes in water temperature, and thus used as a proxy of water lake evaporation. During the LIA period (1400-1800 CE), we observed positive anomalies for the Mg-calcite and negative anomalies for the Ca-calcite, indicating that the lake water was warmer than during the MCA period (1000-1100 CE), which is characterized by negative and positive anomalies for Mg-calcite and Ca-calcite, respectively. The MCA-LIA transition (1200-1400 CE) is characterized by variations between negative and positive anomalies of Mg-calcite.

<figure><img src="image_61.png" /><figcaption>Fig.5 Temporal variations in grey level intensity, terrigenous input (% Al + % Fe + % Ti), Ca-calcite, Mg-calcite, Ca and $C_{org}$ in sediment core LA17BCO2. The time scale along the vertical axis is derived from the age-depth model displayed in Fig. 2a.</figcaption></figure>

### 4.3. Grey level correlation with proxies

The grey level reflects the combination of all materials (organic as well as inorganic) present in the core sediment. Thus, its variation depends on the variations of these materials according to their sedimentation conditions. Indeed, the grey level intensities exhibit a somewhat similar variability to that of the terrigenous elements and calcite formation (Fig. 5). The lighter (darker) colors coincide with more (less) terrigenous input. The agreement between grey level and
inorganic input is supported by a negative correlation between grey level and $C_{org}$ (r = -0.6, Fig. 6), suggesting that their variations may be controlled by the same environmental parameters.

<figure><img src="image_62.png" /><figcaption>Fig. 6 Correlation between grey level and organic carbon from 1000 to 1870 CE</figcaption></figure>

**4.4. Hydroclimate interpretation and comparison with other regional records**

In order to gain insights into the dynamical link between the climate and the dominant modes of variability, we applied wavelet analysis (Fig. 7j). This analysis reveals interannual, decadal and multi-decadal spectral wavelets which could be associated with ENSO, PDO and AMO, respectively. In addition a spectral analysis of average wavelet power of our record indicate an oscillation with periods in ~ 20, ~ 64, ~128 years which could be related to PDO, AMO and some multi-decadal variability respectively (Fig. 8).

Trend toward negative anomalies for both terrigenous inputs (Fig. 7a) and grey levels (Fig. 7b) and positive anomalies for Mg-calcite/Ca-calcite ratio (Fig. 7c) in sediment of Lake Azuei from 1000 to 1800 CE suggests a progressive decrease in precipitation in Haiti over this period. Indeed, proxy indicators suggest trends to dry conditions. Results from other studies in the circum-Caribbean region contain also evidence for this trend. The oxygen isotope and Sr/Ca records from Lake Miragoâne (Haiti) reveal a trend towards higher salinity conditions during the last millennium, which is linked to an increase in the E/P ratio and therefore to dry conditions (Curtis et Hodell, 1993). The sediment titanium composition from the Cariaco Basin (Venezuela) (Haug et al., 2001, Fig. 7d) show also a trend to more negative anomalies, related to a decrease in precipitation patterns. The higher-resolution G. ruber $\delta^{18}$O record spanning the last 2000 years from the Cariaco Basin show a trend toward more positive values that reflect a decrease SSTs and an increase SSSs over the Caribbean and tropical North Atlantic (Black et al. 2004, Fig. 7e).
Indeed, the δ¹⁸O value of foraminiferal calcite is a function of temperature and salinity, whereby an increase in δ¹⁸O is associated with a decrease of SST and an increase of SSS, and vice versa. These studies thus indicate a decreasing precipitation over the circum-Caribbean that may be associated with a southward migration of the ITCZ during this period. Indeed, Lechleitner et al. (2017) have shown a trend to more southerly mean annual position of ITCZ from 1000 to 1800 CE. Thus, in Haiti the precipitations at secular scale are also controlled by the migration of the ITCZ. The overall correlation between the terrigenous inputs in Lake Azuei, the G. ruber δ¹⁸O record (Black et al. 2004) and the sediment titanium composition from the Cariaco Basin (Haug et al., 2001) show that the Caribbean region observed a common climate pattern over the past millennium.

The MCA period appears marked by positive anomalies for terrigenous input linked to positive anomalies for grey level (Fig. 7a, 7b), which have been confirmed by increase in sedimentation rate (Fig. 2b). This tendency was likely related to the pattern of rainfall and runoff from the surrounding watershed and suggests an environment characterized by wet conditions. The negative Mg-calcite/Ca-calcite ratio anomaly recorded during this period (Fig. 7c), indicates a low Mg-calcite concentration in sediment which related to a low evaporation of the lake water. This is consistent with other proxy records from the northern tropical Americas, including the Yucatan (Hodell et al., 2005), the Gulf of Mexico (Richey et al., 2007), lowland Venezuela (Curtis et al., 1999), and the Cariaco Basin (Haug et al., 2001; Black et al., 2004), and the Las Lagunas (Castilla, Felipe, Clara, Salvador) in Dominican Republic (Lane et al., 2009). The Las Lagunas sediment records provide evidence of a relatively wet MCA in the eastern Caribbean (Lane et al., 2009). Black et al. (2004) document a negative shift in mean isotopic values of G. ruber (foraminifera) occurred between ~ 1000 and 1100 CE in Cariaco Basin (Fig. 7e). This negative shift suggests that the Caribbean and tropical North Atlantic were warmer during the MCA. During the early MCA a positive anomaly of Ti also occurs in the Cariaco basin (Haugh et al., 2001; Fig. 7d), which is indicative of increased sediment transport by runoff during periods of increased precipitations, characterizing wet conditions. The latter are related to more northerly mean position of ITCZ during this period (Lechleitner et al., 2017). Grey level and wavelet power analysis of the sediment core from Lake Azuei during the MCA period show multidecadal variations, suggesting that multidecadal mode of climate variability, such as AMO, may indeed affect the hydro-climatic conditions in Haiti. Multi-decadal mode variability was observed also in the South American regions during MCA (Viulle et al., 2012, Apaestegui et al., 2014). In addition, the MCA period coincides with positive anomalies of AMO, NAO and PDO (Mann et al., 2009, Fig. 7f, 7g, 7i); which reflects a warm sea surface temperature and is related to wets conditions.

The MCA-LIA transition (~1200-1400 CE) corresponds to high climate variability conditions, related to alternations between wet and dry conditions, underlined by the high fluctuations between terrigenous input which correlated with a large variation in the sedimentation rate, Mg Calcite precipitation and organic carbon deposition. The wavelets power analysis of grey level
during this period highlights interannual variability, which probably corresponds to Niño-3, conditions (Fig. 7g). Even if we note a chronological phase shift of 50 years between our record and Niño-3 index estimated by Mann et al. 2009, which could be due to the errors of extrapolations of our age models during this period, we think that dry conditions during the MCA-LIA transition have been largely influenced by El Niño.

During the LIA, from ~1450 to ~1800 CE, unlike MCA, more negative anomalies of terrigenous input are recorded (Fig. 7b). This reduced transport of terrigenous elements to the lake is related to a decrease in sedimentation rate (Fig. 2b), suggesting a decrease in rainfall patterns. On the other hand, we observed more positive anomalies for Mg-calcite/Ca-calcite ratio during this period (Fig. 7c). Thus, there is formation of Mg-calcite which is a consequence of evaporation related to dry conditions. Other studies have reported evidence of dry conditions in the region during the LIA (Haug et al., 2001; Hodell et al., 2005; Peterson and Haug; 2006, Lane et al., 2009, 2011). The Lagunas Castilla and Salvador records provide further evidence that the LIA may have been, on average, one of the most arid periods in the circum-Caribbean in the last 2000 years (Lane et al., 2009). In the Cariaco basin (Haug et al., 2001), drier conditions are suggested for the LIA by decreased Ti content in core linked to decreased detritus from local rivers (Fig. 7d). The coincident increase in aridity in the geographically distinct locales of the Yucatan Peninsula (Hodell et al., 2005), Panama (Linsley et al., 1994), northern South America (Haug et al., 2001; Peterson and Haug, 2006), Puerto Rico (Nyberg et al., 2001), along the southern slope of the Cordillera Central of the Dominican Republic (Lane et al., 2009; 2011) and Lake Azuei in Haiti (this study) provides evidence that the ITCZ in the Caribbean was located at a more southerly mean annual position during the LIA. The hydroclimate records discussed by Lechleitner et al. (2017) confirmed also a southward ITCZ shift broadly synchronous with the LIA period. LIA dry conditions are consistent to multidecadal mode highlighted by wavelet analysis of grey level, which corresponds to negative phase of AMO and PDO index (Mann et al., 2009, Fig. 7f, 7h) and trend to more negative NAO index than MCA period (Trouet et al., 2009, Fig. 7g). Thus, these negative phases reflect a cold sea surface temperature and are related to dry conditions.

The study lacks indirect data on the last five decades. Then, we didn't have data for inorganic analysis related to the CWP and new studies need to be done with more evidence. However, there was a trend to increase of sedimentation rate (Fig. 2b). In addition, the lithology profile shows the sediments linked to this period consists of dark brownish clay with a large amount of OM (Fig. 4). This could be due to the input of sediments and organic matter into the lake during rainy periods.
<figure><img src="image_63.png" /></figure>

Fig. 7 Comparison of grey scale analysis of the sediment core and sum % Al, Fe, and Ti composition and Mg-calcite/Ca-calcite ratio (this study, (a), (b), (c)) with sediment titanium composite on representing continental runoff through time (Haug et al., 2001, (d)), and G. ruber δ¹⁸O that reflect sea surface temperature (SST) and Intertropical Convergence Zone (ITCZ) precipitation-related salinity variations over the Caribbean and tropical North Atlantic (Black et al., 2004, (e)), AMO index representing sea surface temperature (SST) anomalies (°C) averaged over the North Atlantic ocean (Mann et al., 2009, (f)), Niño-3 temperature anomaly representing SST anomalies in the eastern Pacific ocean (Mann et al., 2009, (g)), NAO index (Trouillet et al., 2009, (h)), PDO temperature anomaly representing SST anomalies in the eastern Pacific ocean (Mann et al., 2009, (i)) and wavelet power spectrum: The smooth white line marks the cone of influence; results below that line are unreliable. The color bar indicates the range of wavelet
power in the wavelet power spectrum, with hotter colors corresponding to the maximum peaks in
wavelet power (j)

<figure><img src="image_64.png" /><figcaption>Fig. 8 Spectral analyses of the average wavelet power spectrum of the Fig. 7i</figcaption></figure>

**5. Conclusions**

We use a combination of geochemical and mineralogical data supported by statistical analysis
from a core taken in Lake Azuei, to reconstruct hydro-climatic variations in Haiti during the last
millennium. The terrigenous elements in the sediments of the lake display a long-term trend
toward decreasing content, particularly from 1000 to 1600 CE. These opposites' trends suggest
progressively drier conditions in Haiti over this period related to a southward shift of the ITCZ.
Therefore the MCA period was characterized by more wet conditions in contrast to the LIA
period. The MCA-LIA transition was characterized by more unstable conditions, with alternating
wet and dry conditions. The CWP is characterized by an increase of sedimentation rate, which is
linked to the input of more material into the lake by erosion processes in the lake's catchment as
consequence of anthropogenic activities. This study demonstrates also that links exist between
precipitations in Haiti and mean changes in the Atlantic and Pacific Oceans through AMO,
NAO, PDO and ENSO. In addition temporal correlation of other Caribbean paleoclimate records
with our geochemical and mineralogical data, suggests that trends observed in Lake Azuei were
controlled by regional climate, likely associated with shifts in the position of the ITCZ. This
record provide new detailed information on hydroclimate variations in Haiti during the last
millennium and exhibits trends that are similar to regional patterns identified in other proxy
records from the Caribbean and northern tropical Americas. Future studies should focus on other
records with higher resolution to better understand interannual and decadal variability.
**Competing interests:** The contact author has declared that neither they nor their co-authors have any competing interests.

**Acknowledgements**

We gratefully acknowledge the co-authors for their critical discussions and valuable comments. The acquisition of the cores and their initial analysis was funded through U.S. National Science Foundation grants EAR-1624583 and EAR-1624556. These initial activities involved significant contributions from C.W. Heil, C.K. Hearn, and A.N. Murray. We are especially grateful to our colleagues at the State University of Haiti, D. Boisson, K. Guerrier, and R. Momplaisir for all their help with field logistics and also Eric Calais for supporting this work. The navigation skills and resourcefulness of J. Roy from Pegasus Diving & Services were also key to the success of the coring operations. The participation of Francisco Briceño-Zuluaga in this study is the result of the academic exercise as professor at the Nueva Granada Military University. Francisco Briceño-Zuluaga was also supported by CHARISMA Project (JE0ECCHARI, JEAI-IRD). This research was supported by the “Agence Universitaire de la Francophonie (AUF)” and by the “Projets structurants de formation au Sud” de l’IRD (PSF-CLIMACTS). Geochemical and mineralogical analyses were performed on the ALYSES facility (IRD-SU) that was supported by grants from Région Ile de-France. We would like to think also LMC14 laboratories for the support in ¹⁴C dating.

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## Article 2 soumis à PPP

# Tracing environmental and climatic change in Haiti through sedimentary organic matter processes in Lake Azuei over the last millennium

David Noncent<fnref n="1" />,<fnref n="2" />, Abdelfettah Sifeddine<fnref n="1" />,<fnref n="2" />,<fnref n="3" />, Evens Emmanuel<fnref n="1" />,<fnref n="2" />, Marie-Helene Cormier<fnref n="4" />, Francisco J. Briceño-Zuluaga<fnref n="5" />, Jorge Valdés<fnref n="6" />, Mercedes Mendez-Millan<fnref n="2" />,<fnref n="3" />, Bruno Turcq<fnref n="2" />,<fnref n="3" />, Juan Pablo Bernal<fnref n="8" />, John W. King<fnref n="4" />, Irina Djouraev<fnref n="3" />, Fethiye Cetin<fnref n="3" />, Heather Sloan<fnref n="8" />

## Abstract

The focus of this study is to use sedimentary organic processes to reconstruct the past environment of Lake Azuei over the last millennium. Bulk and isotopic organic matter (OM), stratigraphic markers, and a well-chronological model based on 11 ¹⁴C ages and 6 ²¹⁰Pb analyses are used to support this reconstruction. TOC and TN contents reveal that the sediments of Lake Azuei are more or less poor in organic matter. The δ¹³C and C/N results suggest a mix of algae and C₃ plant material dominates OM in lake sediment. It appears that denitrification is connected to physical and chemical conditions, such as temperature and/or the availability of nitrate and organic matter. Distributed according to the MCA -subdivided into MCA1 (A.D.1000-1050) and MCA2 (A.D.1050-1100)-, LIA (A.D. 1400-1800), MCA-LIA (A.D. 1150-1400) and CWP (A.D.1800-2000) periods, three types of sedimentary processes have been highlighted observing the δ¹³C vs C/N analysis cross diagram. During the MCA1 and LIA periods, a decrease in TOC and TN, as well as a decrease in plankton-derived OM, was observed. This was accompanied by an increase in δ¹⁵N, which suggests more denitrification due to suboxic conditions, likely caused by an increase in lake water temperature and dry conditions. A second sedimentary process, including the MCA2 and CWP periods, is characterized by the increase of TOC and TN values,

<footnote n="1">¹ERC2, Université Quisqueya, 218 Ave Jean-Paul II, 6110 Port-au-Prince, Haïti</footnote>

<footnote n="2">²International Joint Research Laboratory CARIBACT. IRD-France and UEH-Haïti</footnote>

<footnote n="3">³IRD, CNRS, SU, MNHN, IPSL, LOCEAN, 32 Av. Henri Varagnat, 93143 Bondy, France</footnote>

<footnote n="4">⁴Graduate School of Oceanography, University of Rhode Island, Narragansett, RI 02882, USA</footnote>

<footnote n="5">⁵Faculty of Basic and Applied Sciences, New Granada Military University (UMNG), Bogotá (Colombia)</footnote>

<footnote n="6">⁶Laboratorio de Sedimentología y Paleoambientes, Instituto de Ciencias Naturales A. v. Humboldt, Facultad de Ciencias del Mar y de Recursos Biológicos, Universidad de Antofagasta, Antofagasta, Chile</footnote>

<footnote n="7">⁷Universidad Nacional Autónoma de México, Centro de Geociencias, Campus Juriquilla, 76001 Querétaro, QRO, México</footnote>

<footnote n="8">⁸Department of Earth, Environmental, and Geospatial Sciences, Lehman College-City University of New York, Bronx, NY 10468, USA</footnote>
and decrease of δ¹³C and δ¹⁵N values. This process is chiefly attributable to more organic material input which is derived from C₃ terrestrial vegetation growing around the lake. A decrease in δ¹⁵N indicates a decrease in denitrification, which further suggests the increased input of organic matter. The sedimentation process during these periods occurred when there was more transport related to wet conditions. The third sedimentary process, related to MCA-LIA transition period, is characterized by many variations of proxies (COT, δ¹³C and δ¹⁵N). The organic matter deposited during this period appears to be a mixture of material originating from both autochthonous phytoplankton and allochthonous C₃ plant. There was climate instability during this period, with alternations between wet and dry conditions, thus variations in the lake level.

# 1. Introduction

The input and production of Sedimentary Organic Matter (SOM) in lake systems are regulated by seasonal and long-term climatic changes (Brenner et al., 1999; Meyers and Teranes, 2002; Sifeddine et al., 2004, Fan et al., 2017). Indeed, SOM in lake sediment contains information that allows us to reconstruct past environmental conditions, evaluate histories of climate change, and assess the impacts of humans on local ecosystems (Meyers and Teranes, 2002, Sifeddine et al., 2004). The deposition and preservation of SOM in lake environments are controlled by several parameters including its origin, productivity, redox conditions of water column and sediments, and sedimentation rates (Hebting et al., 2006). These parameters can be highlighted by organic proxies such as total nitrogen, carbon content, and isotopic compositions (δ¹³C and δ¹⁵N). Temporal changes in fluxes or cycles of organic matter in aquatic systems can often be indicated by these proxies (Schelske and Hodell, 1991; Gu et al., 2006; Zhuo et al., 2021). Between these, the Total Organic Carbon (TOC) and Total Nitrogen (TN) concentrations are fundamental for describing the origin and abundance of sedimentary organic matter.

The concentration of TOC is a measure of the amount of non-mineralized SOM present in sedimentation, which is determined by the initial biomass production and the extent of its subsequent degradation. The TN can demonstrate the sources and processes of degradation and recycling of SOM, as well as the processes involved (Meyers and Teranes, 2002). Processes of decomposition of the sedimented algal biomass can affect the biogeochemical cycles of N, which are present in the sediments. Shi et al. (2022) found that wind-induced algal migration in the overlying water manipulated the temporal and spatial patterns of denitrification N-loss in sediments. C/N ratio analysis of the same material helps to define the source of the organic matter (Silliman et al., 1996). Lower organisms such as algae, phytoplankton, and zooplankton are characterized by high protein content, hence low C/N ratios, while terrestrial plants, which are the main source of terrestrial organic matter, are characterized by low protein content, hence high C/N ratios. Algae typically have atomic C/N ratios between 4 and 10, whereas vascular land plants have C/N ratios > 20 (Meyer et al., 1999). C/N ratios are used as a powerful complement
to their isotope values in evaluating the relative proportions of autochthonous and allochthonous OM.

The concentrations of δ¹⁵N and δ¹³C in the SOM deposited in sediments reflect the changes in the relative abundance of nitrogen and carbon sources, as well as the biogeochemical processes that affect these two essential nutrients in lake water (Schelske and Hodell, 1991; Douglas et al., 2022). The difference in δ¹³C between terrestrial higher plants (-27 ‰) and phytoplankton (-17 to -24 ‰ with an average of -21 ‰) has been used to differentiate between lacustrine and terrestrial sources of SOM (Gearing, 1988). On the other hand, δ¹⁵N can be easily distinguished from typical lacustrine planktonic δ¹⁵N values, which range from 5 to 15 ‰ with an average of 8 ‰, and terrestrial SOM, which ranges from -10 to 10 ‰ averaging 2 ‰ (Meyers et al., 1998). Because phytoplankton discriminates against ¹³CO₂, and ¹⁵NO₃⁻; during uptake, the C and N isotopic composition of OM exported from the photic zone preferentially removes ¹²C and ¹⁴N from the dissolved inorganic carbon (DIC) and nitrogen (DIN) pools in epilimnetic waters, respectively. As supplies of CO₂ or NO₃⁻ become depleted and isotopically heavier in surface waters, phytoplankton discriminates less against ¹³C and ¹⁵N, and sinking organic matter becomes progressively enriched in ¹³C and ¹⁵N.

The δ¹⁵N organic matter in lake sediments can be affected by alterations in phytoplankton assemblages, the introduction of heterotrophs, and the existence of nitrogen fixers (Brenner et al., 1999; Talbot and Laerdal, 2000). An increase in the abundance of nitrogen-fixing cyanobacteria, which directly fix atmospheric N₂, would decrease δ¹⁵N values in deposited organic matter (Fogel and Cifuentes, 1993; Zhan et al., 2014). In contrast, the addition of heterotrophic organic matter will increase the δ¹⁵N of organic matter because δ¹⁵N increases by 3-4‰ with each trophic transfer (Minagawa and Wada, 1984; Peterson and Fry, 1987; Teranes and Bernasconi, 2000). Therefore, the δ¹³C and δ¹⁵N composition of SOM has been used to monitor past alterations in productivity and its association with environmental modifications in both lacustrine and marine ecosystems (Hollander et al. 1992; Schelske and Hodell 1991; Altabet and Francois 1994; Woszczyk et al., 2021).

Research on the climatology and environment of the Lake Azuei region, the second largest lake in Hispaniola, has been limited to a few articles. Previous studies have examined the fluctuations in its level over the past few decades, using historical documents, CHIRP seismic data, satellite imagery, and regional meteorological data (Wright et al., 2015; Hotz, 2019; Comarazamy et al., 2014; Moknatian and Piasecki, 2021). The environmental history of Lake Azuei has been studied over the past century using sediment cores (Eisen-Cuadra, 2013). In order to gain a better understanding of the evolution of the environment of Lake Azuei, this study analyzed organic markers in a sediment core from the lake for the past thousand years. This is the first time that environmental changes in Lake Azuei have been studied over such a long period. In this sense, the aim of this study is to identify processes that control the sedimentation of organic matter and
consequently to reconstruct past environmental conditions of Lake Azuei and their associated climatic conditions.

## Site study

Lake Azuei is located in the lowland Cul-de-Sac Plain, western Haiti (18°35'51" N, 72°0'53" W, Fig. 1). It is 22 km long, from northwest to southeast; its maximum width is 12 km and it measures 30 m at its deepest (James et al., 2019). The lake is endorheic, which means that its level is extremely sensitive to variations in precipitation. It is surrounded by meadows and cacti. Lake Azuei is located in one of the driest regions of the country (Moron et al., 2015) due to the Cordillera Central rain shadow effect. The area climate is characterized by two rainy seasons (long and short), alternating with two dry seasons. The rainy seasons occur in the spring (April-June) and autumn (September-November), and dry seasons occur in summer and winter (Perrissol and Lescoulier, 2011). The average annual rainfall in the area varies between 663 and 814 mm at lower altitudes, while the higher areas are subject to much greater rainfall rates, with average annual precipitation between 1230 mm to 2590 mm (Perrissol and Lescoulier, 2011).

The land surrounding Lake Azuei has been heavily modified by human activity. Agricultural land-use and changes in land-cover due to deforestation dominate the west and east regions of the lake basin, which impact the watershed of Lake Azuei. The mountains surrounding are actively exploited for building materials used in the construction of houses and other infrastructure (Hadden and Minson, 2010). These changes have been reflected in temporal variations of TOC, TN, and TP combined with temporal variations of $\delta^{13}C_{TOC}$ and $\delta^{15}N_{TN}$ in the region over the past 74-108 years. Indeed, a gradual increase in Total Phosphorous (TP) (0.2-0.3µmol yr$^{-1}$) deposition since 1960, a decrease in the TOC/TN (-0.026 yr$^{-1}$) since 1903, depletion in $\delta^{13}C_{TOC}$ (-0.6 to -1.6‰) since 1990, and enrichment in $\delta^{15}N_{TN}$ (0.5 to 2.7‰) since 1990, results from land-use changes (i.e., agricultural development) that increase nutrient loading due to human and animal waste inputs (Eisen-Cuadra, 2013).
<figure><img src="image_65.png" /></figure>

Figure 1. Bathymetric chart compiled from depth soundings collected between 2013 and 2017 (Cormier et al., 2018). Contour interval is 1 m. Yellow line indicates the Haitian-Dominican border. Sampling site is also indicated in red.

**2. Materials and method**

**2.1. Sediment core characteristics**

LA17BCO2, a sediment core, was recovered at a depth of ~20 m in the southern part of the lake using the Bolivia core corer, a piston rod corer. This 84 cm long core was observed to have good banding both macroscopically and microscopically, as well as other physical characteristics such as color and laminae structures. The ¹⁴C dating of gastropod shells, wood, and bulk organic matter from the sediment core was conducted using a mass accelerator spectrometer. To gain a more precise date for the upper part of the core, activities of ²¹⁰Pbxs (unsupported Pb) were measured every centimeter over the top 10 centimeters. More details of chronological model are described in Noncent et al. (2023).

**2.2. Organic elemental carbon and nitrogen analysis.**

Organic carbon (Corg) and total nitrogen was measured with an elemental analyzer Flash 2000HT from Thermo Fischer Scientific coupled to a thermal conductivity detector (TCD) at LOCEAN, Bondy, France. Each sample was weighted in a precision balance and placed in tin capsules. Prior to the analyses organic carbon, carbonates were removed with hydrochloric acid 10%.
Since the carbon analyzes were performed on decarbonated samples unlike nitrogen, the percentage of total organic carbon is determined by the following equation:

$$TOC (\%) = (m_d/m_r) * \%C_d$$

Where m_d is the mass of the decarbonated sample, m_r mass of the raw sample and %C_d is the percentage of carbon determined by IRMS in the decarbonated sample.

The TOC and TN values were used to calculate the C/N ratio. Molar ratios were then determined using atomic weights:

$$C/N = (\%C / 12.01) / (\%N / 14.002)$$

C/N values reflect the ratio of aquatic organic matter to terrestrial organic matter (Meyers and Lallier-Vergas, 1998).

## 2.3. Organic isotopic carbon and nitrogen analysis

Before the organic isotopic carbon analysis, the samples were decarbonated to remove the different forms of carbonates present by releasing carbon dioxide with hydrochloric acid 10 %. Ten to thirty mg of the sample was placed into ultra-clean tin capsules. To obtain the most precise analysis possible, ultra-pure standards of known isotopic composition (EMAP2, Sorghum, HOS) were used to calibrate the measurements. All samples were combusted in an elemental analyzer and the released CO₂ was transmitted to an isotope ratio mass spectrometer (IRMS) at LOCEAN, Bondy, France. The isotopic composition of samples is reported in conventional δ-notation, in per mil (‰) relative to Vienna Pee Dee Belemnite standards (VPDB) for carbon and atmospheric N₂ (AIR) for nitrogen, respectively:

$$\delta^{13}C (\delta^{15}N)_{sample} (‰) = [(R_{sample} - R_{standard}) / R_{standard}] * 1000$$

where R is ¹³C/¹²C or ¹⁵N/¹⁴N ratio of the sample and the standard, respectively.

# 3. Results

## 3.1. Lithology

Based on the visual characteristics of the sediments, different stratigraphic levels could be identified for LA17BCO2 (Fig. 3, core image). The different levels were characterized either by the clay facies or by frequent alternation of organic matter within clayey to homogeneous silty
levels or by less frequent alternation of organic matter and a more silty level. The upper levels have a much darker color, therefore much richer in organic matter (Noncent et al., 2023).

## 3.2. Chronology

The chronology was presented and detailed by Noncent et al. (2023). $^{210}$Pb and radiocarbon dates were combined to form a Bayesian age-depth model using the rBacon package within R (Blaauw and Christen 2019). Mean ages were extracted from the model (Fig. 2, Noncent et al., 2023) and used to represent and interpret the proxy data.

<figure><img src="image_66.png" /></figure>

Fig. 2: (a) Bayesian age-depth model for core LA17BCO2 generated using rBacon for R, displaying $^{14}$C dates corrected for HWLE. The jagged blue error bars display the $^{14}$C age probability distribution for each sample; the dotted red line follows the mean ages. In detail at the top from left to right; number of iterations, sedimentation rate and memory, this is interpreted as the dependence of the accumulation rate between neighboring depths. (b) Sedimentation rate (cm/yr) calculated from age-depth model. Average sedimentation rate in sediment core determined with the age-depth model (Fig. 2b), was 0.128 ± 0.079 cm/yr. The higher values are observed between: 84 to 76 cm (1000 to 1150 CE), 68 to 41 cm (1100-1250 CE) and 10 to 0 cm (1900-2000 CE). From 38 to 10 cm (1300 to 1900 CE) we observed a trend to decrease of sedimentation rate. (Noncent et al., 2023)

## 3.3. C and N elemental and isotopic composition of Organic fraction

The range and the average of used SOM proxies are represented in Table 1.

<table><caption>Table 1. Range and average of different proxies</caption><thead><tr><td>Proxies</td><td>Range (min-max)</td><td>Average +/- Std. dev.</td></tr></thead></table>
<table><tr><td>TOC (%)</td><td>0.58 - 4.89</td><td>2.5 +/- 1.22</td></tr><tr><td>TN (%)</td><td>0.06 - 0.40</td><td>0.22 +/- 0.10</td></tr><tr><td>δ<sup>13</sup>C (‰)</td><td>-26.83 - -23.09</td><td>-24.71 +/- 0.67</td></tr><tr><td>δ<sup>15</sup>N (‰)</td><td>3.83 - 10.07</td><td>6.68 +/- 1.71</td></tr><tr><td>C/N</td><td>8.07 - 20.05</td><td>12.98 +/- 1.8</td></tr></table>

The content of TOC and TN (Fig. 3) showed similar values over time and varied in a narrow range from 0.6 % to 4.9 % (average of 2.5 ± 1.22 %) and from 0.06 % to 0.40 % (average of 0.22 ± 0.09 %), respectively. Their contents are highly variable with increases and decreases in different depths. TOC is strongly correlated with TN (r = 0.97), suggesting a common origin. The stable isotope δ¹³C (Fig. 3) varied between -26.83 ‰ to -23.09 ‰ (average of -24.71 ± 0.67 ‰). The lowest value of δ¹³C (-26.83 ‰) is observed at 41 cm where a rapid decline is recorded; and the largest value (-23.09 ‰) at 28 cm. Values of δ¹³C tend to increase between 64 cm-44cm and to decrease between 76-64 cm and 20-10 cm. Overall, δ¹³C varies inversely with Corg and TN. The δ¹⁵N values varied from 3.88 ‰ to 10.07 ‰ (average of 6.68 ± 1.7 ‰), showing an opposite trend to TN and TOC. There is a concomitant variation between δ¹⁵N and δ¹³C except from 64 to 46 cm. The lowest values of δ¹⁵N (δ¹⁵N < 5 ‰) are observed at 66 cm and at 41 cm; on the other hand, the enrichment value (δ¹⁵N > 7 ‰) is observed at 73 cm. The C/N ratio varied from 8 to 20.05 (average of 13 ± 1.8). From 31 to 10 cm, C/N ratio shows low variability. On the other hand, from 64 to 31 cm, a greater variability is observed. The C/N ratio values are exhibited elevated in cores sections that have high percentages of organic carbon and nitrogen.

<figure><img src="image_67.png" /></figure>
# 4. Interpretation and discussion

## 4.1. Origin and sedimentary process of organic matter in Lake Azuei

The concentrations of TOC and TN in lake Azuei's sediments range from 0.6% to 4.9% and 0.06% to 0.40%, respectively, indicating that the sediments are relatively low in SOM. The C/N values (8 to 20; average of 13 ± 1.8) and δ13C values (-26.83 ‰ to -23.09; average of -24.71 ± 0.67 ‰) of SOM in the sediments of Lake Azuei suggest that the organic matter present there is derived from both aquatic and terrestrial sources (Meyers et al., 1999); particularly from algae of the lake and C₃ plant around the lake environment, respectively (Fig. 4a). C/N values between 10 and 20 typically indicate a mix of aquatic and terrestrial organic matter (Talbot and Lærdal 2000, Li et al., 2009, Wang et al., 2013). However, this result should be taken with caution. Variability in these ranges may result from differing relative contributions from terrestrial biomass and floating planktonic material, as well as from variations in other chemical parameters of the lacustrine environment. Possible anthropic sources existing in the study area such as urban waste and nitrogen fertilizers could be influencing the composition of SOM in the lake. Indeed, changes in precipitation and anthropogenic activities in the watershed related to agriculture, sewage runoff, and deforestation will likely result in changes in terrestrial organic matter input. Deforestation and enhanced storm intensities are expected to increase surface runoff and accelerate erosion (Eisen-Guadra, 2013). This enhances the input of allochthonous material to the lake such as soil nutrients, organic matter, and inorganic matter-ultimately changing the composition of the lake sediment.

Exceptionally, in the middle section of the core (at ~ 41 cm, Fig. 3,) there was a considerable contribution of OM with an increase in both TOC (4%) and then C/N ratio (20) and a decrease in δ¹³C (-26.83‰). High C/N and TOC values indicate terrestrial organic matter was transported into the lake. SOM from peripheral terrigenous materials, particularly from C3 plants, suggests a more humid environment and increased precipitation during this period.

In Lake Azuei δ¹³C is not correlated with TOC (Table S1), thus it could be a proxy of source more than productivity (Hollander and McKenzie, 1991; Hollander et al., 1992; Hodell and Schelske, 1998; Brenner et al., 1999; Albuquerque et al., 2014). This may be related to the process of diagenesis during their burial. It has been suggested that post-burial diagenesis of SOM can change the bulk and isotopic composition of C and N isotopes and thereby obscure potential signals of paleoproductivity (Herczeg, 1988).
We observed an opposite trend between δ¹⁵N and TOC; i.e increase (decrease) in δ¹⁵N related to a decrease (increase) in TOC (Fig. 3). This could be related to denitrification in the sediment instead of the water column. Lake sediments present an ideal environment for denitrification. They are a concentration site for organic matter from the water column, which upon decomposition releases NH₄⁺. The NH₄⁺ is then available for nitrification and subsequent denitrification (Blackburn and Henriksen, 1983). In addition, NO₃⁻ from the overlying water can diffuse into the sediments (Andersen et al., 1984), especially in relatively eutrophic systems where NO₃⁻ concentrations in the water are high. These characteristics, in combination with the close juxtaposition of aerobic and anaerobic sites within a few mm of the sediment-water interface, lead to high denitrification activity in aquatic sediments (Seitzinger, 1990). Eadie et al. (1995) suggested that most of the historic increase in δ¹⁵N may be due to denitrification. During denitrification in suboxic environments, NO₃⁻ is converted to N₂, with a strong fractionation leaving the dissolved NO₃⁻ enriched in δ¹⁵N. The decomposition of organic matter likely releases labile carbon substrates and consumes oxygen, creating favorable conditions for denitrification in sediments. A number of environmental factors have been shown to influence denitrification in freshwater sediment including oxygen, NO₃⁻ and organic matter concentrations, pH, temperature, and compounds from anthropogenic sources (Seitzinger, 1990). Many of these factors are interrelated, resulting in complex spatial and temporal patterns of denitrification. Bacterial activity is probably stimulated by an increase in water temperature (Messer and Brezonik, 1983; van Luijn et al., 1999) and is disproportionately high in warm littoral zones (den Heyer and Kalff, 1998). Both nitrate and organic matter supply can be rate limiting for denitrifiers (Seitzinger, 1990). Shi et al. (2022) showed that decay of algal biomass generated organic carbon and created anoxia, favoring denitrification, while excessive algal biomass could deplete oxygen and inhibit nitrification, causing nitrate limitation for denitrification. Sediment redox potential has also been shown to affect denitrification rates, with higher rates in more reduced sediments (van Kessel, 1977). In the sediments of Lake Azuei, based on variations of TN, TOC, and δ¹⁵N, denitrification appears to be related to physical and chemical conditions such as temperature and/or nitrate and organic matter supply. Indeed, δ¹⁵N is opposite to both TN and TOC (Table S1) which characterize the abundance of organic matter in sediments.
<figure><img src="image_68.png" /><figcaption>Figure 4. (a) δ¹³C values and C/N ratios of organic matter indicate sources of OM in Lake Azuei sediments, the ranges of δ¹³C and C/N values for potential OM sources are from Meyers and Lallier-Vergès, (1999) (b) the δ¹³C values and C/N ratios of the different periods (MCA1, MCA2, LIA, MCA-LIA and CWP) are represented and grouped inside the circles.</figcaption></figure>

Distributed according to the MCA -subdivided into MCA1 (1000-1050 CE) and MCA2 (1050-1100 CE)-, LIA (1400-1700 CE), MCA-LIA (1150-1400 CE) and CWP (A.D.1700-2000 CE) periods (Fig. 3), three types of sedimentary processes have been highlighted observing the δ¹³C vs. C/N plot (Fig. 4b).
A first sedimentary process, concerned by the MCA1 and LIA periods, is characterized by a decrease in TOC and TN (Fig. 3) reveal that the sediments are poor in organic matter. The C/N vs. δ¹³C plot (Fig. 4b) shows a general distribution of points lying close to the planktonic organic matter signal. The δ¹³C trend is generally constant during these periods suggesting relatively stable levels of exchange between lake OM and CO₂ (aq) supply from the catchment. In addition, the δ¹⁵N trend to increase suggests more process of denitrification. More denitrification can also relate to a suboxic condition. The latter could result in the water column stratification linked to an increase in the temperature of the lake water column. Indeed, this may be due to a simultaneous decrease in the oxygen supply by advection (a stronger thermal stratification) and an increase in oxygen consumption by microbial denitrified.

A second sedimentary process, including the MCA2 and CWP periods, is characterized by the increase of TOC and TN values, and a decrease of δ¹³C and δ¹⁵N values. This process is chiefly attributable to organic material derived from C₃ terrestrial vegetation growing around the lake during these periods (Fig. 4b). The decrease in δ¹⁵N is related to a decrease in denitrification due to more organic matter input.

A third process sedimentary, related to MC-LIA transition period, is characterized by many variations of proxies. The organic matter deposited during this period appears to be a mixture of material originating from both phytoplankton and C₃ plant (Fig. 4b). For example, the abrupt increase of TOC, TN, and C/N values at 1250 CE is prominent in this stage. δ¹³C displays one peak depleted fall in this time. The increased C/N ratio, coinciding with the increased content of TOC confirms that the allochthonous organic debris and the soil organic matter are major sources of OM in this period. This contribution of OM would come from peripheral organic materials, particularly from C₃ plants. The lowering of δ¹³C values may be thought of as due to a decrease in the supply of molecular CO₂ caused by more flushing and a relative increase in floating planktonic material. Around 1320 CE we observed an abrupt decrease in TOC and TN. C/N ratios also drop below 10 indicating an almost exclusively autochthonous phytoplankton source of organic matter.

## 4.2. Climate Variability

A principal component analysis was run on the core proxies using data of inorganic composition (Al, Fe, Ti, Noncent et al., 2023) and organic composition (COT, δ¹⁵N, δ¹³C, C/N). More than 75% of variance is explained by two principal components (Fig. 5). Here, we present only the first component (PC1, which explains 25% of the variability of the data), which is correlated negatively with sum Al, Fe and Ti, TOC and positively with δ¹⁵N and δ¹³C (Fig. 5). The PC1 temporal variability (Fig. 6d) is compared with the sum Al, Fe and Ti (Fig. 5b; Noncent et al., 2023), Mg-calcite (Fig. 6c; Noncent et al., 2023) and Ti (Fig. 6a°; Haug et al., 2001,). The PC1 variability shows agreement with the Mg-calcite variation, contrary terrigenous inputs variations.
<figure><img src="image_69.png" /><figcaption>Figure 5. Principal component analysis of sum (Al, Fe, Ti; Noncent et al., 2023), TOC and δ¹⁵N and δ¹³C</figcaption></figure>

During MCA1 (1000-1050 CE) and LIA(1400-1800 CE), Fig. 6d showed positive values of PC1, indicating a decrease in TOC values, which was related to a decrease in OM input. This decrease in OM input was further confirmed by an increase in δ¹⁵N values, indicating more denitrification. All characteristics of this process sedimentary elaborated by the parameters above can be evidenced by dry conditions which could be related to an increase in evaporation (E) and a decrease in precipitation (P), thus a decrease in the lake level. These dry conditions experienced in the environment of Lake Azuei during this process agree with Noncent et al. (2023) where less transport of terrigenous elements to the lake are presented and related to a decrease in sedimentation rate, suggesting a decrease in rainfall patterns. During this period, lake hydrology and chemistry were controlled by decreased precipitation. Indeed, more negative anomalies of terrigenous input are recorded, suggesting a decrease in rainfall patterns (Fig. 6c). On the other hand, we observed more positive anomalies for Mg-calcite during this period (Fig. 6b). This suggests increase in the formation of Mg-calcite which is a consequence of evaporation related to dry conditions. This dry period has been demonstrated by other studies in the region (Haug et al., 2001; Hodell et al., 2005; Peterson and Haug, 2006; Lane et al., 2009). This behavior during LIA is supported by paleolimnological records from the Caribbean slope of the Cordillera Central, Dominican Republic (Lane et al., 2009) and from Aguada X'caamal, Mexico which also indicate increased aridity and decreased lake levels (Hodell et al., 2005).

During the MCA2 (1050-1100 CE) the values of PC1 indicating an increase of TOC values which related to more terrigenous input. During these periods δ¹³C values trend to decrease which characterizes OM coming from terrestrial sources, particularly C₃ plants. Thus, the process sedimentation during this period occurred when there was more transport which was confirmed by more terrigenous elements input in (Noncent et al., 2023). Following the detrital
proxies (sum Al+Fe+Ti) the MCA2 period appears marked by positive anomalies for terrigenous input (Fig. 6c). It is likely that this trend was caused by the pattern of rainfall and runoff from the surrounding watershed, indicating a wet environment. The negative Mg-calcite anomaly recorded during this period (Fig. 6b), indicates a low Mg-calcite concentration in sediment which is related to low evaporation of the lake water. However, regional Cariaco record (Venezuela) indicates a decrease in Ti content (Haug et al., 2001, Fig. 6a) related to a wet condition from about 1050 to 1200 CE.

During the MCA-LIA transition, there was a variation of negative and positive PC1 values. This transition period corresponds to more variability climate conditions, with alternations between wet and dry conditions (Noncent et al., 2023), thus variations in the lake level.

For the CWP (1800-2000 CE) period, an increase in TOC and TN values could be attributed to an increase in nutrients. Indeed, a decrease of δ¹³C signatures while TOC and TN increase is commonly found in lakes that are heavily influenced by human and livestock waste inputs (Hodell and Schelske, 1998; Michener and Lajtha, 2008; Eisen-Cuadra, 2013). δ¹³C signatures are expected to be enriched as nutrient loading increases, but human and animal wastewater and other terrestrial organic matter can deplete the δ¹³C signature (Burnett and Schaeffer, 1980; Gearing et al., 1991). Indeed, in the 18th century, large sugar refineries developed in Haiti, which required groupings of land by ten hectares (Cauna, 2013). The land-use/land-cover change has greatly contributed to the increasing rate of runoff in the area and therefore the carry-over effects of sediment during the CWP. Thus, terrestrial OM might be effectively transported to Lake Azuei through land surface runoff.
<figure><img src="image_70.png" /></figure>

Figure 6. Variations of PC1, sum Al, Fe, Ti (Noncent et al., 2023) Indicating greater or lesser input of detrital material, Mg-calcite ((Noncent et al., 2023), like witness of temperature variability and Ti content (Haug et al., 2001) like proxy of regional precipitation,

**Conclusion**

In this study, we produced a record of paleoenvironmental since 1000 years based on organic matter analysis using a sediment core from Lake Azuei, Haiti. The core was dated from A.D. 1000 to A.D. 2000 based on accelerator mass spectrometry (AMS) ¹⁴C and ²¹⁰Pb dating. TOC and TN concentrations reveal that the sediments of Lake Azuei are more or less poor in organic matter. The δ¹³C and C/N results suggest a mix of algae and C₃ plant material dominates OM in lake sediment. The opposite trend between δ¹⁵N and TOC is related to denitrification in the sediment instead of the water column. This denitrification appears to be related to physical and chemical conditions such as temperature and/or nitrate and organic matter supply. Three types of sedimentary processes were observed based on the δ¹³C values and C/N ratios of the different periods (MCA1 (A.D.1000-1050), MCA2 (A.D.1050-1100), LIA (A.D. 1400-1700), MCA-LIA (A.D. 1150-1400) and CWP (A.D.1700-2000)). A first sedimentary process, concerned by the MCA1 and LIA periods, is characterized by lees organic matter input which is plankton origin. During these periods there were more denitrification related to a suboxic condition that could be related to increase temperature of lake water and linked to dry conditions. A second sedimentary process, including the MCA2 and CWP periods, is characterized by more OM input which is chiefly attributable to organic material derived from C₃ terrestrial vegetation growing around the
lake during these periods linked to a decrease in denitrification. These periods are related to wet conditions. A third process sedimentary, related to MCA-LIA transition period, is characterized by many variations of proxies. The organic matter deposited during this period appears to be a mixture of material originating from both autochthonous phytoplankton and allochthonous C3 plant. There was climate instability during this period, with alternations between wet and dry conditions, thus variations in the lake level.

In this study, the environmental changes recorded at Lake Azuei are studied for a longer period contrary to previous studies. The results indicate relatively minor shifts in the lake's environment, particularly in the paleo-vegetation, during the last millennium excepted after A.D. 1700, despite strong evidence from paleo-climate reconstructions in the region of significant shifts in regional precipitation over the course of the last millennium. This study contributes to better understand the evolution of lake's environment for different periods.

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Supplementary Material

<table><thead><tr><th></th><th>TOC(%)</th><th>TN (%)</th><th>C/N</th><th>d13C (‰)</th><th>d15N (‰)</th></tr></thead><tbody><tr><td>TOC(%)</td><td></td><td>1</td><td>0,9663261</td><td>0,5461053</td><td>-0,448515</td><td>-0,7602503</td></tr><tr><td>TN (%)</td><td>0,9663261</td><td></td><td>1</td><td>0,3213693</td><td>-0,3304876</td><td>-0,6917136</td></tr><tr><td>C/N</td><td>0,5461053</td><td>0,3213693</td><td></td><td>1</td><td>-0,6045665</td><td>-0,5493331</td></tr><tr><td>d13C (‰)</td><td>-0,448515</td><td>-0,3304876</td><td>-0,6045665</td><td></td><td>1</td><td>0,4522006</td></tr><tr><td>d15N (‰)</td><td>-0,7602503</td><td>-0,6917136</td><td>-0,5493331</td><td>0,4522006</td><td></td><td>1</td></tr></tbody></table>

p-values:

<table><caption>Table 1S. Correlations between indicators of SOM, with its respective *p*-values.</caption><thead><tr><th></th><th>TOC(%)</th><th>TN (%)</th><th>C/N</th><th>d13C (‰)</th><th>d15N (‰)</th></tr></thead><tbody><tr><td>TOC(%)</td><td></td><td>0.0000</td><td>0.0015</td><td>0.0114</td><td>0.0000</td></tr><tr><td>TN (%)</td><td>0.0000</td><td></td><td>0.0779</td><td>0.0694</td><td>0.0000</td></tr><tr><td>C/N</td><td>0.0015</td><td>0.0779</td><td></td><td>0.0003</td><td>0.0014</td></tr><tr><td>d13C (‰)</td><td>0.0114</td><td>0.0694</td><td>0.0003</td><td></td><td>0.0106</td></tr><tr><td>d15N (‰)</td><td>0.0000</td><td>0.0000</td><td>0.0014</td><td>0.0106</td><td></td></tr></tbody></table>
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