Geophysical Journal (1989) 96, 519-528 Palaeomagnetism of stalagmites (speleothems) in SVV Japan Hayao Morinaga Division of Environmental Science, The Graduate School of Science and Technology, Kobe University, Nada, Kobe 657,Japan Hiroo Inokuchi and Katsumi Yaskawa Faculty of Science, Kobe University, Nada, Kobe 657,Japan Accepted 1988 September 19.Received 1988 September 19; in original form 1987 November 16 SUMMARY A palaeomagnetic study has been carried out on three stalagmites from two limestone caves in SW Japan. Remanent magnetizations of the stalagmite samples are weak, but stable enough to record the geomagnetic field. The results indicate an internal consistency between several time-equivalent samples drilled from the same stalagmite. A tentative correlation is suggested between palaeomagnetic data from two stalagmites collected from the same cave, and data from two different limestone caves. Combined curves of declination and inclination variations are constructed on the basis of this tentative correlation between the alternatingfield cleaned results from the three stalagmites. These variation curves can also be tentatively correlated with those deduced from archaeomagnetic studies in SW Japan. In consequence, the curves are believed to represent records of past geomagnetic secular variation. The tentative age of the oldest end of this secular variation curve can be estimated at about 15 OOO yr BP, based on the correlation with the archaeomagnetic results. A possible long period of westerly declination and steep inclination is recognized in the older part of the variation curve. Key words: limestone cave, palaeomagnetism, remanent magnetization, secular variation, stalagmite 1 INTRODUCTION Palaeomagnetic investigations of lake, shallow marine and cave sediments have been widely used to explore fine-scale features of the past geomagnetic field, and to establish a magnetic time-scale for the late Pleistocene to Recent (e.g. Hyodo & Yaskawa 1980, 1986a, b; Creer & Tucholka 1983; Creer, Tucholka & Barton 1983; Noel & St Pierre 1984; Noel 1986a, b). Unconsolidated sediments sometimes may provide nearcontinuous records of geomagnetic and climatic changes owing to their near-continuous deposition. They do, however, acquire remanent magnetizations after deposition, known as post-depositional remanent magnetization, PDRM (Irving 1957; Irving & Major 1963; Kent 1973), and, depending on the nature of the sediment, may possess magnetic records resulting from a convolution of the geomagnetic field and a moment fixing function (Hyodo 1984). Therefore, the magnetic recording process for sediments may be subjected to amplitude attenuation and phase lag. Using a deconvolution method (Hyodo 1984), a virtual geomagnetic secular variation record can be derived from the magnetization records. This method, however, can be utilized only for homogeneous sediments. Natural sediments commonly have variously disturbed magnetic records due to depositional and post-depositional factors, variable secondary overprinting and sampling disturbance (e.g. Verosub 1977; Rosenbaum & Larson 1983). On the other hand, as pottery and bricks from pottery kilns and ancient fireplaces commonly carry a stable thermoremanent magnetization, more detailed aspects of the geomagnetic field direction and intensity may be deduced from their magnetizations (archaeomagnetism) . The disadvantage of archaeomagnetism is that it is able to give only discontinuous records (‘spot readings’) of the geomagnetic field, and it may fail to reveal fine-scale behaviour. However, by using a combination of both archaeomagnetism and palaeomagnetism of sediments and other materials which can continuously record the geomagnetic field, it may be possible to establish a synthesized secular variation curve which expresses more completely the true behaviour of the field. With this aim in mind, we have studied the palaeomagnetism of speleothems (limestone cave formations) to see if they can provide a reliable palaeosecular variation record. Stalagmites, which are one type of speleothem, may carry a stable remanent magnetization due to the presence of fine grained magnetite (Morinaga, Inokuchi & Yaskawa 1986). Owing to their continuous growth these formations may play 520 H.Morinaga, H . Inokuchi and K . Yaskawa an important role as recorders of the past geomagnetic field. Stalagmites are deposited in limestone caves -through a chemical precipitation from dripping ground water, making mound-like, tall cylindrical or conical shapes. The growth of stalagmites, which takes place as calcium carbonate films are successively deposited on their surface, is believed commonly to be slower than that of unconsolidated lake sediments. As stalagmite samples are able to be easily divided into disc specimens with a thickness of a few millimetres, slowness of growth does not become a serious problem in their sampling for palaeomagnetic investigations. In addition, the process of magnetization in a calcium carbonate film deposited on to a stalagmite surface seems to be simultaneous with its crystallization, differing from that for unconsolidated sediments (Morinaga et al. 1989). Latham et al. (1979) showed that the natural remanent magnetizations (NRMs) of several speleothems were stable and were apparently unaffected by surface conditions such as roughness, dripping rates and crystal growth. Possible secular variations in the geomagnetic field direction for the last several thousands of years were detected through the investigations of stalagmites and flowstones in a number of regions (Latham et al. 1982; Latham, Schwarcz & Ford 1986, 1987). Palaeomagnetic investigations of speleothems have also been camed out in Japan with the aim of producing a more detailed secular variation curve. These investigations utilized two separate procedures. The first involved repeated magnetization measurements after successive chipping of small amounts of carbonate material from a block sample under analysis (Inokuchi, Morinaga & Yaskawa 1981). The subtraction vector of the latter from the former measured values represents the remanence of the chipped materials from the block sample. The second procedure involved magnetization measurements of thin disc subsamples sliced from long cylindrical samples (the 'microsampling' method of Morinaga et al. 1985, 1986). The disc subsamples were 2.5cm in diameter and about 1.5mm thick. In principle both procedures provide the opportunity for recording geomagnetic field behaviour with a high time resolution. The results of the second procedure indicated that the surface subsamples, which were being dripped on at the time of sampling, have much the same remanent direction as that of the present geomagnetic field in the sampling region. A geomagnetic secular variation curve for west Japan over the last 4000yr was obtained through this procedure. This curve corresponded to other curves obtained from archaeomagnetic measurements (Hirooka 1971, 1983) and palaeomagnetic investigations of shallow marine and lake sediments (Hyodo & Yaskawa 1980; Yamazaki, Joshima & Saito 1985) in Japan. The purpose of the present paper is to demonstrate the from the reliability of NRM recorded in stalagmites, combined results of our recent stalagmite palaeomagnetic investigations, and previously published ones (Morinaga et uf. 1985, 1986). Although there is no independent dating control on the investigated samples, we also present a provisional secular variation curve for the geomagnetic field in west Japan, which is derived from tentative correlations of the results from the three stalagmites with archaeomagnetic results. 2 SAMPLES Two stalagmites were sampled from Komori-Ana cave (34"13'N, 131"19'E) in Akiyoshi Plateau, Yamaguchi Prefecture, West Japan. Caves distributed in Akiyoshi Plateau are divided into six of the development level categories. Komori-Ana cave is situated on the lowest development level and is characterized by a horizontal cavity. The formation age of this cave is believed to be late Pleistocene to Recent (Fujii, personal communication 1988). This cave seems to be still active because of the presence of water flow. Palaeomagnetic, palaeoclimatic and other investigations have already been performed for one of the stalagmites, KM1 (Morinaga et al. 1985, 1986). Nine vertical (time-equivalent) samples were drilled out from the mound-like stalagmite body (Fig. 1, left). The samples were cylindrical in form, of 2.5 cm diameter, and about 18 cm in length. All samples were orientated in situ using a mount and a magnetic compass. The orientation is considered accurate to within f5" in inclination and declination. The other stalagmite (KM2) had a conical shape, with a diameter less than 20cm and a height of 25cm. Six parallel (time-equivalent) samples were drilled horizontally from the outer portion of this stalagmite (Fig. 1, centre). Each sample was of 2.5 cm diameter and 4-5 cm in length. The growth layers of parallel samples drilled from two stalagmites had similar patterns, so that for each stalagmite, simultaneous growth layers could be identified in respective samples from their characteristic patterns. A third stalagmite (RYU) was sampled in Ryuga-Do cave (33"36'N, 133'45'E) in Kochi Prefecture, SW Japan. This cave is regarded as having a similar age o r being rather older than Komori-Ana cave, and also seems to be active at present because of the presence of water flow. The stalagmite had a columnar shape, about lOcm in diameter and 86 cm in height. Seventeen successive (time-serial) core samples, 2.5 cm in diameter and 5 cm in length, were taken from the vertical centre part of this stalagmite (Fig. 1, right). All three of these stalagmites were growing up till their collection, since their tops were being dripped on at the time of sampling. All samples except those from stalagmite KM1 were wrapped in polyvinyl chloride film and set using plaster of paris. Setting in plaster of pans prevented the samples from breaking or crumbling, while the use of polyvinyl chloride film protected them from possible contamination by the plaster. Then they were fixed on a non-magnetic mount by non-magnetic glue and were cut by a diamond blade into thin disc subsamples of 1.5-2.5 mm thick. The samples from KM1 were fixed and cut using a similar process without the wrapping and the setting. The total numbers of disc subsamples taken from the three stalagmites KM1, KM2 and R W are 311, 68 and 309, respectively. 3 MAGNETIC MEASUREMENTS AND RESULTS Magnetic measurements were carried out using a cryogenic magnetometer whose sensitivity is lo-" Am2 emu). demagnetization was ProPessive alternating field (*) performed on all disc subsamples in order to examine the Palaeomagnetism of stalagmites 521 RYU '@ 1.5-2.5 0.4mm ItI- . .. . .. . . ... SUBSAMPLES KMI E f E 0 \o Qo .7 *.. E E E E 0 0 0 t I. L n cw N I__ 200 mm -4 F3gnre 1. Schematic views of the three stalagmites, KM1, KM2 and RYU, showing their growth layer patterns and positions of subsamples taken for magnetic measurements. magnetic stability and to define the characteristic component of their magnetization. The NRM intensities of disc subsamples before AF demagnetization were in the range 10-5-10-7 Am2 kg-' (emu g-'). The intensities of samples from the KM2 and RYU stalagmites were generally weaker than those from the KM1 stalagmite, by one order. All the subsamples had very stable components and only weak low coercivity components, which could be removed at AF levels up to about 10 mT (Fig. 2). Median destructive fields fell in the range 10 to 15 mT for almost all the subsamples. Optimum demagnetizing fields for definition of the stable characteristic magnetization differed for each subsample and ranged from around 6 to 12mT. Possible primary components for most subsamples were very stable, and their directions changed only slightly during demagnetizing up to 40 mT. The results of the magnetization determinations obtained from the three stalagmites are shown in Figs 3 and 4 for declination and inclination, respectively. In the case of the parallel samples taken from the two stalagmites KM1 and KM2, correlation with respect to positions of disc specimens taken from each cylindrical sample was determined by observation and comparison of the pattern of the growth layers. The positions of all subsamples were then adjusted to distance from the surface of a 'master' sample selected for each stalagmite by stretching and compressing the records. In Figs 3(a) and 4(a), the direction (declination and inclination) data are plotted against distance from the top of the R W stalagmite. In Figs 3(b), (c), 4(b) and (c), they are plotted against distance from the surface of the master sample for stalagmites KM1 and KM2. Sequential five-point moving average curves are also shown in these figures. The results for the RYU stalagmite reveal anomalously westerly declination and steep inclination below 60 cm. However, the 522 H . Morinaga, H . Inokuchi and K . Yaskawa -- - KM 1 15-75 -- KM2 3-04 NRM I N T . - ~ =029x10 Am/Kg A - N SI 0. -- RYU 111 -- NRM INT -6 =O 21x10 Am /Kg NRM INT = 2 4x10-6 Am/Kg 2 S-c - Horizontal ; 0 Vertical Figore 2. Typical orthogonal vector component diagrams for progressive AF demagnetization of stalagmite subsamples. Numbers adjacent to open circles denote peak demagnetizing AF in mT. Figure 3. AF-cleaned declinations for the three stalagmites plotted against distance from the top or the surface of the stalagmite (dots and squares). Sequential five-point moving vector averages are also shown (lines). Palaeomagnetism of stalagmites . (b) KM2 'O*] 70' 523 4 ( c ) KMI .: . - .. . . .. * c . F3gure 4. AF-cleaned inclinations for the three stalagmites plotted against distance from the top or the surface (dots and squares). Sequential five-point moving vector avenges are also shown (lines). remanences of subsamples near the base show similar NRM intensities and stabilities to other subsamples during progressive AF demagnetization. 4 DISCUSSIONS A N D CONCLUSIONS 4.1 Consistency of results from parallel samples from two stalagmites The results from six parallel samples taken from stalagmite KM2 are shown individually in Fig. 5 as a function of distance from the surface of the master sample. Curves of declination, inclination and NRM intensity variation for each parallel sample are, for the most part, consistent with each other, showing good internal consistency within one stalagmite. However, there is some scatter in inclination curves at the top and in declination curves at the bottom. These inconsistencies may be attributed mainly to the misfitting of the distance relative to the 'master sample' near to both ends. Also, because the top and bottom subsamples are irregularly shaped (not perfect discs), measurement errors may exist in these subsamples. The generally high level of internal consistency indicates that the remanent magnetizations may be attributed to an identical source for this stalagmite. The precisions of sequential five-point moving average directions calculated using all KM2 specimens range from k = 41.6 (a,,= 12.0") to k = 1015.0 (a9,= 2.4'). An average value of the precisions is k = 263.1 (a9s = 5.5"). The internal consistency of data for stalagmite KM1 is similar to that for KM2 (Morinaga et al. 1986). The precisions range from k = 28.2 (a,5= 14.7') to k = 1913.0 (agS = 1.7') and the average value is k = 217.5 (a,,= 6.6') for the KM1 stalagmite. 4.2 Tentative correlation of results from the three stalagmites Sequential five-point moving average curves of direction (declination and inclination) obtained from the two Komori-Ana stalagmites, KM1 and KM2, are shown in Fig. 6(a) and (b), respectively. The curves can be tentatively correlated with each other on the basis of their amplitudes and variations, showing a possible consistency between two stalagmites in the same limestone cave. The comparison between the data for these two stalagmites was made through direct eye observation so as not to bring about great discrepancies in the growth rates of the two stalagmites. The declination of stalagmite KM2 is relative, because this stalagmite was not orientated owing to its having been already broken at the sampling time. The declination curve for stalagmite KM2, thus, is shifted by a constant value, so as to fit that of stalagmite KM1. Considering the close proximity of these two stalagmites. 524 H . Morinaga, H . Inokuchi and K . Yaskawa c KM2 STALAGMITE 20 -26 O I I NRM INTENSITY (AmVKg) 0 1 2 3 4 (cml Figure 5. Consistency between the palaeomagnetic results for six parallel samples from stalagmite KM2. This shows generally high internal consistency within the stalagmite. the degree of correlation between their magnetization records is surprisingly poor. Factors contributing to this may include differences of subsample numbers and ratios of signal to noise between the two stalagmites. The variation curves of direction (declination and inclination) obtained from the R W and KM1 stalagmites are shown in Fig. 7(a) and (b), respectively. The curves are drawn with sequential five-point moving averages as a function of distance from the top or from the surface. These curves can be tentatively correlated with each other, showing a possible regional consistency between two different limestone caves. This comparison was also made through direct eye observation, so as not to bring about great discrepancies in the growth rate of the two stalagmites. This tentative correlation suggests that the remanent magnetizations in the two stalagmites probably reflect the same magnetization source, most likely the past geomagnetic field. Based on the tentative correlations of the results from the three investigated stalagmites, provisional geomagnetic secular variation curves for SW Japan can be constructed (Fig. 8) as a function of distance from the top of the RYU stalagmite. The curves of the declination and the inclination were drawn with average values every 2mm down to a distance of about 12cm from the top and with sequential five-point moving averages in the rest of the range because of the limited amount of directional data. 4.3 Tentative correlation between the results of this study and those of arrhaeomagnetic studies in SW Japan Figure 8 shows variation curves of the past geomagnetic field direction (declination and inclination, respectively) in SW Japan obtained from (i) palaeomagnetic results for the three stalagmites described in the present study and (ii) archaeomagnetic results (Hirooka 1971, 1983). The curves for the latter results are based on average values for 50yr intervals. The curves, especially the inclination curve, show a reasonably good degree of correlation. The small inconsistencies between the declination curves may be attributed, at least in part, to the misfitting of relative distances for the results from the stalagmites. The relatively good correlation suggests that the remanent magnetization of the stalagmites does reflect the past geomagnetic field and that, under favourable circumstances, stalagmites may be excellent recorders of the geomagnetic field. It is concluded that the curves obtained from the palaeomagnetism of the three stalagmites most probably do represent geomagnetic secular variation records, although the absolute ages of these stalagmites have not yet been determined independ- Palaeomagnetism of stalagmites 525 DECLINATION 0' -20' I I KM2 -10' 70° 50' FQwe 6. Tentative correlation between the palaeomagnetic results for two stalagmites (KM1 and KM2) from the same limestone cave (Komori-Ana cave). 526 H . Morinaga, H . Znokuchi and K . Yaskawa DECLI NATION I IN C L I NAT I ON Figure 7. Tentative correlation between palaeomagnetic results for two stalagmites from different limestone caves, (i) Ryuga-Do cave and (ii) Komori-Ana cave. This shows a possible regional consistency between the data from different limestone caves. ently. The extrapolated age of the oldest end of the curves is about 15000yr BP, based on correlation with the archaeomagnetic results, although this estimate is highly tentative. 4.4 Characteristic featores of the provisional secular variation curves of the geomagnetic field direction A long interval of westerly declination is recognized in the older half (below 60cm in stalagmite R W ) of the provisional secular variation curve (Fig. 8, upper). The maximum deflection is about 9OW. Inclination values during this period are steeper (6@ 80') than expected from the geocentric axial dipole (Fig. 8, lower). Such a westerly declination and steep inclination period before 6600yr BP - has already been reported from palaeomagnetic studies of unconsolidated sediments from the inland sea in Japan (Muroi & Yaskawa 1977; Hyodo & Yaskawa 1986b). The geomagnetic field behaviour during this period may be explained by an abnormally large standing component of the non-dipole field in the vicinity of East Asia, such as the Mongolian positive anomaly at present (Yukutake & Tachinaka 1969). It may possibly be related to proposed short-period geomagnetic excursions during a similar period (Morner & Lanser 1974, 1975; Noel & Tarling 1975; Morner 1977; Morinaga, Morinaga & Yaskawa 1987), although the existence of this excursion has been questioned (e.g. Thompson & Berglund 1976; Jacobs 1984). Further investigations of the characteristic features of the geomagnetic secular variation records of stalagmites are required and are now in progress by ourselves. Palaeomagnetism of stalagmites 527 I NCIL I NAT I ON 50' 30' c . I . . . Figure 8. Tentative correlation between (i) provisional secular variation curves obtained from the three stalagmites described in the present study and (ii) archaeomagnetic secular variation curves (from Hirooka 1971, 1983). 4.5 Further diecussions and hture works on stalagmites Stalagmites may be very useful in establishing the palaeosecular variation curve in the direction as mentioned above. The palaeomagnetism of stalagmites is a promising technique which may compensate for the inevitable problems and potential defects in archaeomagnetic studies and palaeomagnetic studies of unconsolidated sediments. Synchroneity between crystallization and magnetization acquisition of a calcium carbonate film deposited on a stalagmite surface has been investigated through laboratory experiments making synthetic stalagmites using sodium 528 H . Morinaga, H . Inokuchi and K . Yaskawa thiosulfate (Morinaga et al. 1989). The present results indicate that t h e magnetization acquisition occurs at much the same time as crystallization an d also that the remanent directions are parallel to the ambient direct field. The remanent magnetization is believed to be acquired through chemical fixation of the magnetic particles along the ambient direct field and among t h e crystals. Since stalagmites are predominantly composed of calcium carbonate, they may be useful in estimating palaeotemperature fluctuations. This, and synchroneity of the crystallization and magnetization acquisition suggests potential for exploring relationships between the geomagnetic field and the air temperature in the past using stalagmites (Morinaga et af. 1985). ACKNOWLEDGMENTS We thank Dr M. Ikeya, Faculty of Science, Osaka University, Dr T. Miki, Technical College, Yamaguchi University, and D r T. 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