TY - JOUR A1 - Nelson, Daniel B. A1 - Knohl, Alexander A1 - Sachse, Dirk A1 - Schefulss, Enno A1 - Kahmen, Ansgar T1 - Sources and abundances of leaf waxes in aerosols in central Europe JF - Geochimica et cosmochimica acta : journal of the Geochemical Society and the Meteoritical Society N2 - Atmospheric transport is an understudied mechanism for leaf wax hydrogen isotope applications that contributes to mobilizing and depositing these compounds on the surface of the Earth. While previous efforts have identified the importance of atmospheric leaf wax deposition in remote marine locations, the processes are not well constrained on land in temperate latitudes where lakes are common and sedimentary leaf wax hydrogen isotope values are an attractive tool for understanding past precipitation changes. This work presents results from a field study that was conducted in 2010 and 2011 at Hainich National Park, Germany in order to evaluate the quantity and sources of leaf waxes in the atmosphere. Aerosols were sampled at approximately weekly intervals inside the forest canopy, and n-alkane distributions and hydrogen isotope values were compared with those from major tree species surrounding the sampling site. Despite sampling in what was expected to be a major production center, the distribution and hydrogen isotope values of atmospheric n-alkanes bore little resemblance to those of the local vegetation. Comparison with local meteorological data and to 10-day and 36-h back air mass trajectories indicated shifting effects of winds and temperature, and that mesoscale transport processes were more important than longrange mechanisms. Back trajectories also highlighted source effects, with easterly winds coinciding with relatively lower leaf wax hydrogen isotope values from more continental regions. These results suggest that leaf wax aerosols average over spatial scales that exceed typical surface catchment areas for small lake systems, even in forested areas, yet that the area over which these compounds are derived is still relatively regional. Depositional fluxes were also estimated in order to assess the potential importance of atmospheric transport to sedimentary archives. Although difficult to constrain, these estimates suggest that atmospheric deposition may be non-negligible for lake systems in cases where inputs from rivers or surface runoff are limited. Together, these observations provide new insights on how leaf waxes from different sources are integrated during aeolian transport and the spatial scales over which these processes occur. KW - Hydrogen isotopes KW - Leaf wax KW - Aerosols KW - n-Alkanes KW - Biomarkers KW - Lakes KW - Sediments Y1 - 2016 U6 - https://doi.org/10.1016/j.gca.2016.11.018 SN - 0016-7037 SN - 1872-9533 VL - 198 SP - 299 EP - 314 PB - Elsevier CY - Oxford ER - TY - JOUR A1 - Rach, Oliver A1 - Kahmen, Ansgar A1 - Brauer, Achim A1 - Sachse, Dirk T1 - A dual-biomarker approach for quantification of changes in relative humidity from sedimentary lipid D/H ratios JF - Climate of the past : an interactive open access journal of the European Geosciences Union N2 - Past climatic change can be reconstructed from sedimentary archives by a number of proxies. However, few methods exist to directly estimate hydrological changes and even fewer result in quantitative data, impeding our understanding of the timing, magnitude and mechanisms of hydrological changes. Here we present a novel approach based on delta H-2 values of sedimentary lipid biomarkers in combination with plant physiological modeling to extract quantitative information on past changes in relative humidity. Our initial application to an annually laminated lacustrine sediment sequence from western Europe deposited during the Younger Dryas cold period revealed relative humidity changes of up to 15% over sub-centennial timescales, leading to major ecosystem changes, in agreement with palynological data from the region. We show that by combining organic geochemical methods and mechanistic plant physiological models on well characterized lacustrine archives it is possible to extract quantitative ecohydrological parameters from sedimentary lipid biomarker delta H-2 data. Y1 - 2017 U6 - https://doi.org/10.5194/cp-13-741-2017 SN - 1814-9324 SN - 1814-9332 VL - 13 SP - 741 EP - 757 PB - Copernicus CY - Göttingen ER - TY - JOUR A1 - Sachse, Dirk A1 - Dawson, Todd E. A1 - Kahmen, Ansgar T1 - Seasonal variation of leaf wax n-alkane production and delta H-2 values from the evergreen oak tree, Quercus agrifolia JF - Isotopes in environmental and health studies N2 - In order to understand the timing of leaf wax synthesis in higher plants, we analysed the variability in leaf wax n-alkane concentration, composition (expressed as average chain length (ACL)), and delta H-2(wax) values as well as plant source water delta H-2 values (xylem and leaf water) in the evergreen tree Quercus agrifolia over a period of 9 months, beginning with leaf flush. We identified three distinct periods of leaf development with the first month following leaf flush being characterized by de novo synthesis and possibly removal of n-alkanes. During the following 3 months, n-alkane concentrations increased sevenfold and delta H-2(wax) and ACL values increased, suggesting this period was the major leaf wax n-alkane formation period. During the remaining 4 months of the experiment, stable values suggest cessation of leaf wax n-alkane formation. We find that n-alkane synthesis in Q. agrifolia takes place over 4 months, substantially longer than that observed for deciduous trees. KW - leaf wax KW - oak tree KW - hydrogen-2 KW - isotope ecology KW - n-alkanes Y1 - 2015 U6 - https://doi.org/10.1080/10256016.2015.1011636 SN - 1025-6016 SN - 1477-2639 VL - 51 IS - 1 SP - 124 EP - 142 PB - Routledge, Taylor & Francis Group CY - Abingdon ER - TY - JOUR A1 - Crausbay, Shelley A1 - Genderjahn, Steffi A1 - Hotchkiss, Sara A1 - Sachse, Dirk A1 - Kahmen, Ansgar A1 - Arndt, Stefan K. T1 - Vegetation dynamics at the upper reaches of a tropical montane forest are driven by disturbance over the past 7300 years JF - Arctic, antarctic, and alpine research : an interdisciplinary journal N2 - We assessed tropical montane cloud forest (TMCF) sensitivity to natural disturbance by drought, fire, and dieback with a 7300-year-long paleorecord. We analyzed pollen assemblages, charcoal accumulation rates, and higher plant biomarker compounds (average chain length [ACL] of n-alkanes) in sediments from Wai 'anapanapa, a small lake near the upper forest limit and the mean trade wind inversion ('IWI) in Hawai`i. The paleorecord of ACL suggests increased drought frequency and a lower awl elevation from 2555-1323 cal yr B.P. and 606-334 cal yr B.P. Charcoal began to accumulate and a novel fire regime was initiated ca. 880 cal yr B.P., followed by a decreased fire return interval at ca. 550 cal yr B.P. Diebacks occurred at 2931, 2161, 1162, and 306 cal yr B.P., and two of these were independent of drought or fire. Pollen assemblages indicate that on average species composition changed only 2.8% per decade. These dynamics, though slight, were significantly associated with disturbance. The direction of species composition change varied with disturbance type. Drought was associated with significantly more vines and lianas; fire was associated with an increase in the tree fern Sadleria and indicators of open, disturbed landscapes at the expense of epiphytic ferns; whereas stand-scale dieback was associated with an increase in the tree fern Cibotium. Though this cloud forest was dynamic in response to past disturbance, it has recovered, suggesting a resilient TMCF with no evidence of state change in vegetation type (e.g., grassland or shrubland). Y1 - 2014 U6 - https://doi.org/10.1657/1938-4246-46.4.787 SN - 1523-0430 SN - 1938-4246 VL - 46 IS - 4 SP - 787 EP - 799 PB - Institute of Arctic and Alpine Research, University of Colorado CY - Boulder ER - TY - JOUR A1 - Kahmen, Ansgar A1 - Sachse, Dirk A1 - Arndt, Stefan K. A1 - Tu, Kevin P. A1 - Farrington, Heraldo A1 - Vitousek, Peter M. A1 - Dawson, Todd E. T1 - Cellulose delta O-18 is an index of leaf-to-air vapor pressure difference (VPD) in tropical plants JF - Proceedings of the National Academy of Sciences of the United States of America N2 - Cellulose in plants contains oxygen that derives in most cases from precipitation. Because the stable oxygen isotope composition, delta O-18, of precipitation is associated with environmental conditions, cellulose delta O-18 should be as well. However, plant physiological models using delta O-18 suggest that cellulose delta O-18 is influenced by a complex mix of both climatic and physiological drivers. This influence complicates the interpretation of cellulose delta O-18 values in a paleo-context. Here, we combined empirical data analyses with mechanistic model simulations to i) quantify the impacts that the primary climatic drivers humidity (e(a)) and air temperature (T-air) have on cellulose delta O-18 values in different tropical ecosystems and ii) determine which environmental signal is dominating cellulose delta O-18 values. Our results revealed that e(a) and T-air equally influence cellulose delta O-18 values and that distinguishing which of these factors dominates the delta O-18 values of cellulose cannot be accomplished in the absence of additional environmental information. However, the individual impacts of e(a) and T-air on the delta O-18 values of cellulose can be integrated into a single index of plant-experienced atmospheric vapor demand: the leaf-to-air vapor pressure difference (VPD). We found a robust relationship between VPD and cellulose delta O-18 values in both empirical and modeled data in all ecosystems that we investigated. Our analysis revealed therefore that delta O-18 values in plant cellulose can be used as a proxy for VPD in tropical ecosystems. As VPD is an essential variable that determines the biogeochemical dynamics of ecosystems, our study has applications in ecological-, climate-, or forensic-sciences. KW - stable isotopes KW - plant-water relations KW - paleoecology KW - climate change KW - Hawaii Y1 - 2011 U6 - https://doi.org/10.1073/pnas.1018906108 SN - 0027-8424 VL - 108 IS - 5 SP - 1981 EP - 1986 PB - National Acad. of Sciences CY - Washington ER - TY - JOUR A1 - Kahmen, Ansgar A1 - Dawson, Todd E. A1 - Vieth, Andrea A1 - Sachse, Dirk T1 - Leaf wax n-alkane delta D values are determined early in the ontogeny of Populus trichocarpa leaves when grown under controlled environmental conditions JF - Plant, cell & environment : cell physiology, whole-plant physiology, community physiology N2 - The stable hydrogen isotope ratios (delta D) of leaf wax n-alkanes record valuable information on plant and ecosystem water relations. It remains, however, unknown if leaf wax n-alkane delta D values record only environmental variation during the brief period of time of leaf growth or if leaf wax n-alkane delta D values are affected by environmental variability throughout the entire lifespan of a leaf. To resolve these uncertainties, we irrigated Populus trichocarpa trees with a pulse of deuterium-enriched water and used compound-specific stable hydrogen isotope analyses to test if the applied tracer could be recovered from leaf wax n-alkanes of leaves that were at different stages of their development during the tracer application. Our experiment revealed that only leaf wax n-alkanes from leaves that had developed during the time of the tracer application were affected, while leaves that were already fully matured at the time of the tracer application were not. We conclude from our study that under controlled environmental conditions, leaf wax n-alkanes are synthesized only early in the ontogeny of a leaf. Our experiment has implications for the interpretation of leaf wax n-alkane delta D values in an environmental context, as it suggests that these compounds record only a brief period of the environmental variability that a leaf experiences throughout its life. KW - cuticle KW - plant water relations KW - stable isotopes Y1 - 2011 U6 - https://doi.org/10.1111/j.1365-3040.2011.02360.x SN - 0140-7791 VL - 34 IS - 10 SP - 1639 EP - 1651 PB - Wiley-Blackwell CY - Hoboken ER - TY - JOUR A1 - Garcin, Yannick A1 - Schwab, Valerie F. A1 - Gleixner, Gerd A1 - Kahmen, Ansgar A1 - Todou, Gilbert A1 - Sene, Olivier A1 - Onana, Jean-Michel A1 - Achoundong, Gaston A1 - Sachse, Dirk T1 - Hydrogen isotope ratios of lacustrine sedimentary n-alkanes as proxies of tropical African hydrology insights from a calibration transect across Cameroon JF - Geochimica et cosmochimica acta : journal of the Geochemical Society and the Meteoritical Society N2 - Hydrogen isotope values (delta D) of sedimentary aquatic and terrestrial lipid biomarkers, originating from algae, bacteria, and leaf wax, have been used to record isotopic properties of ancient source water (i.e., precipitation and/or lake water) in several mid-and high-latitude lacustrine environments. In the tropics, however, where both processes associated with isotope fractionation in the hydrologic system and vegetation strongly differ from those at higher latitudes, calibration studies for this proxy are not yet available. To close this gap of knowledge, we sampled surface sediments from 11 lakes in Cameroon to identify those hydro-climatological processes and physiological factors that determine the hydrogen isotopic composition of aquatic and terrestrial lipid biomarkers. Here we present a robust framework for the application of compound-specific hydrogen isotopes in tropical Africa. Our results show that the delta D values of the aquatic lipid biomarker n-C(17) alkane were not correlated with the delta D values of lake water. Carbon isotope measurements indicate that the n-C(17) alkane was derived from multiple source organisms that used different hydrogen pools for biosynthesis. We demonstrate that the delta D values of the n-C(29) alkane were correlated with the delta D values of surface water (i.e., river water and groundwater), which, on large spatial scales, reflect the isotopic composition of mean annual precipitation. Such a relationship has been observed at higher latitudes, supporting the robustness of the leaf-wax lipid delta D proxy on a hemispheric spatial scale. In contrast, the delta D values of the n-C(31) alkane did not show such a relationship but instead were correlated with the evaporative lake water delta D values. This result suggests distinct water sources for both leaf-wax lipids, most likely originating from two different groups of plants. These new findings have important implications for the interpretation of long-chain n-alkane delta D records from ancient lake sediments. In particular, a robust interpretation of palaeohydrological data requires knowledge of the vegetation in the catchment area as different plants may utilise different water sources. Our results also suggest that the combination of carbon and hydrogen isotopes does help to differentiate between the metabolic pathway and/or growth form of organisms and therefore, the source of hydrogen used during lipid biosynthesis. Y1 - 2012 U6 - https://doi.org/10.1016/j.gca.2011.11.039 SN - 0016-7037 VL - 79 IS - 4 SP - 106 EP - 126 PB - Elsevier CY - Oxford ER - TY - JOUR A1 - Kahmen, Ansgar A1 - Schefuss, Enno A1 - Sachse, Dirk T1 - Leaf water deuterium enrichment shapes leaf wax n-alkane delta D values of angiosperm plants I experimental evidence and mechanistic insights JF - Geochimica et cosmochimica acta : journal of the Geochemical Society and the Meteoritical Society N2 - Leaf wax n-alkanes of terrestrial plants are long-chain hydrocarbons that can persist in sedimentary records over geologic timescales. Since meteoric water is the primary source of hydrogen used in leaf wax synthesis, the hydrogen isotope composition (delta D value) of these biomarkers contains information on hydrological processes. Consequently, leaf wax n-alkane delta D values have been advocated as powerful tools for paleohydrological research. The exact kind of hydrological information that is recorded in leaf wax n-alkanes remains, however, unclear because critical processes that determine their delta D values have not yet been resolved. In particular the effects of evaporative deuterium (D)-enrichment of leaf water on the delta D values of leaf wax n-alkanes have not yet been directly assessed and quantified. Here we present the results of a study where we experimentally tested if and by what magnitude evaporative D-enrichment of leaf water affects the delta D of leaf wax n-alkanes in angiosperm C3 and C4 plants. Our study revealed that n-alkane delta D values of all plants that we investigated were affected by evaporative D-enrichment of leaf water. For dicotyledonous plants we found that the full extent of leaf water evaporative D-enrichment is recorded in leaf wax n-alkane delta D values. For monocotyledonous plants we found that between 18% and 68% of the D-enrichment in leaf water was recorded in the delta D values of their n-alkanes. We hypothesize that the different magnitudes by which evaporative D-enrichment of leaf water affects the delta D values of leaf wax n-alkanes in monocotyledonous and dicotyledonous plants is the result of differences in leaf growth and development between these plant groups. Our finding that the evaporative D-enrichment of leaf water affects the delta D values of leaf wax n-alkanes in monocotyledonous and dicotyledonous plants albeit at different magnitudes - has important implications for the interpretation of leaf wax n-alkane delta D values from paleohydrological records. In addition, our finding opens the door to employ delta D values of leaf wax n-alkanes as new ecohydrological proxies for evapotranspiration that can be applied in contemporary plant and ecosystem research. Y1 - 2013 U6 - https://doi.org/10.1016/j.gca.2012.09.003 SN - 0016-7037 VL - 111 SP - 39 EP - 49 PB - Elsevier CY - Oxford ER - TY - JOUR A1 - Hoffmann, Bernd A1 - Kahmen, Ansgar A1 - Cernusak, Lucas A. A1 - Arndt, Stefan K. A1 - Sachse, Dirk T1 - Abundance and distribution of leaf wax n-alkanes in leaves of Acacia and Eucalyptus trees along a strong humidity gradient in northern Australia JF - Organic geochemistry : the international journal for rapid publication of current research in organic geochemistry and biochemistry N2 - Environmental parameters such as rainfall, temperature and relative humidity can affect the composition of higher plant leaf wax. The abundance and distribution of leaf wax biomarkers, such as long chain n-alkanes, in sedimentary archives have therefore been proposed as proxies reflecting climate change. However, a robust palaeoclimatic interpretation requires a thorough understanding of how environmental changes affect leaf wax n-alkane distributions in living plants. We have analysed the concentration and chain length distribution of leaf wax n-alkanes in Acacia and Eucalyptus species along a 1500 km climatic gradient in northern Australia that ranges from subtropical to arid. We show that aridity affected the concentration and distribution of n-alkanes for plants in both genera. For both Acacia and Eucalyptus n-alkane concentration increased by a factor of ten to the dry centre of Australia, reflecting the purpose of the wax in preventing water loss from the leaf. Furthermore, Acacian-alkanes decreased in average chain length (ACL) towards the arid centre of Australia, whereas Eucalyptus ACL increased under arid conditions. Our observations demonstrate that n-alkane concentration and distribution in leaf wax are sensitive to hydroclimatic conditions. These parameters could therefore potentially be employed in palaeorecords to estimate past environmental change. However, our finding of a distinct response of n-alkane ACL values to hydrological changes in different taxa also implies that the often assumed increase in ACL under drier conditions is not a robust feature for all plant species and genera and as such additional information about the prevalent vegetation are required when ACL values are used as a palaeoclimate proxy. Y1 - 2013 U6 - https://doi.org/10.1016/j.orggeochem.2013.07.003 SN - 0146-6380 VL - 62 IS - 9 SP - 62 EP - 67 PB - Elsevier CY - Oxford ER - TY - JOUR A1 - Sachse, Dirk A1 - Kahmen, Ansgar A1 - Gleixner, Gerd T1 - Significant seasonal variation in the hydrogen isotopic composition of leaf-wax lipids for two deciduous tree ecosystems (Fagus sylvativa and Acer pseudoplatanus) N2 - Compound specific hydrogen isotope ratios (delta D) of long chain sedimentary n-alkanes, which mostly originate from the leaf waxes of higher terrestrial plants, are increasingly employed as paleoclimate proxies. While soil water is the ultimate hydrogen source for these lipids and the isotopic fractionation during biosynthesis of lipids is thought to remain constant, environmental parameters and plant physiological processes can alter the apparent hydrogen isotopic fractionation between leaf-wax lipids and a plant's source water. However, the magnitude and timing of these effects and their influence on the isotopic composition of lipids from higher terrestrial plants are still not well understood. Therefore we investigated the seasonal variability of leaf-wax n-alkane delta D values for two different temperate deciduous forest ecosystems that are dominated by two different tree species, Beech (Fagus sylvatica) and Maple (Acer pseudoplatanus). We found significant seasonal variations for both tree species in n-alkane delta D values of up to 40%. on timescales as short as one week. Also, the isotopic difference between different n-alkanes from the same plant species did vary significantly and reached up to 50 parts per thousand at the same time when overall n-alkane concentrations were lowest. Since delta D values of soil water at 5 and 10 cm depth, which we assume represent the delta D value of the major water source for the investigated beech trees, were enriched in autumn compared to the spring by 30 parts per thousand, whereas n-alkane delta D values increased only by 10 parts per thousand, we observed variations in the apparent fractionation between beech leaf derived n-alkanes and soil water of up to 20 parts per thousand on a seasonal scale. This observed change in the apparent fractionation was likely caused by differences in leaf water isotopic enrichment. Based on mechanistic leaf water models we conclude that changes in the isotopic difference between water vapor and soil water were the most likely reason for the observed changes in the apparent fractionation between n- alkanes and soil water. The large variability of n-alkane concentrations and delta D values over time implies a continuous de nova synthesis of these compounds over the growing season with turnover times possibly as short as weeks. The signal to reach the soil therefore represents an integrated record of the last weeks before leaf senescence. This holds true also for the sedimentary record of small catchment lakes in humid, temperate climates, where wind transport of leaf-wax lipids is negligible compared to transfer through soil and the massive input of leaves directly into the lake in autumn. Y1 - 2009 UR - http://www.sciencedirect.com/science/journal/01466380 U6 - https://doi.org/10.1016/j.orggeochem.2009.02.008 SN - 0146-6380 ER -