Thermal demagnetization of the three-axis composite IRM and thermomagnetic analysis indicated that the magnetic minerals contained in the ash samples were predominantly titanomagnetite including both, Ti-rich and Ti-poor titanomagnetite. The Ti content of Ti-rich titanomagnetite varies depending on the time of collection; however, a Tc of approximately 300°C was generally observed throughout the entire period, indicating that Ti-rich titanomagnetite of this composition is the main magnetic mineral.
The hysteresis parameters Mrs/Ms and Bc were determined from hysteresis loop measurements, where Mrs/Ms is the ratio of saturation remanent magnetization to saturation magnetization and Bc is the coercive force. These values showed a good correlation (Fig. 1c), and each changed with the time of sample collection. Generally, the larger the values of Mrs/Ms and Bc, the higher the single-domain (SD) volume fractions; meaning that the size distribution of magnetic grains becomes finer (Dunlop, 2002). The Mrs/Ms values in Fig. 1c indicate that the volcanic ash, which erupted in 2019–2020, contained magnetic minerals with particle sizes varying from multi-domain (MD) grain to SD grain sizes. Figure 2 shows a FORC diagram of some of the volcanic ash samples collected between September 2019 and January 2020 in chronological order. The results for October 14 and November 6, 2019, show the predominance of stable SD grains with high coercivity compared to those of the other periods. More detailed coercivity changes can be observed in the result of the thermal demagnetization of the three-axis composite IRM (Fig. 3). Measurements on the sample from September 14, 2019, showed a predominance of low-coercivity components below 100 mT, and a minor component above 300 mT could be identified. In contrast, the sample from October 14, 2019, showed a predominance of moderate coercivity components in the 100–300 mT range, and components with coercivity > 300 mT were confirmed. These variations were also observed in samples from January to February 2020. In addition, this behavior of Bc can be observed for both Ti-rich and Ti-poor titanomagnetite.
The results of the thermomagnetic analysis are shown in Fig. 4. Titanomagnetite (Fe3 − xTixO4) with a Tc of 300°C has a composition of approximately x = 0.4 based on the formula of Hunt et al. (1995). Depending on the timing of the eruption, some of these compositions appeared simultaneously with lower or higher Tc values. Titanomagnetite with titanium-rich compositions and Tc < 200°C (x approximately equal to 0.6) can be seen from mid-October to early November 2019, late December 2019, and late January to late February 2020. Ti-poor titanomagnetite showed a Tc phase of approximately 500°C, which was identified in a sample taken just before the cessation of the eruption in June 2020. Moreover, this sample does not contain any Tc of approximately 300°C and is systematically included in the other samples; the magnetic minerals of this sample are completely different from those of the other samples.
Temporal Changes Of Rock Magnetic Properties
We discuss how chronologically ordered changes in rock magnetic properties are related to eruptive activity. The remarkable behavior of the magnetic properties of volcanic ash was confirmed as follows: Hysteresis loop parameters of Mrs/Ms and Bc that show particularly significant variation increased during the periods from mid-October to early November 2019, late January to mid-February, and early June 2020. Hc is the coercivity of magnetic minerals, and its increase indicates that the stability of the magnetic minerals is enhanced. As Mrs/Ms and Bc increase, the magnetic mineral becomes closer to the SD grain, which is a more stable magnetic property.
The periods of high values in Mrs/Ms and Bc were mid-October to early November 2019, late January to mid-February, and early June 2020. The values of Mrs/Ms and Bc were larger during this period, indicating that the contribution of the SD particles increased significantly. The temporal change in the FORC diagram (Fig. 2) shows an increase in coercivity and the contribution of non-interacting SD grains from September to October 2019, which is consistent with the behavior of Mrs/Ms and Bc. The predominance of the 100–300 mT component in the IRM-TD measurement also coincided with the period when the component above 300 mT could be confirmed (Fig. 3). The increase in the SD volume fraction was probably due to the increased supply of SD titanomagnetite. However, the value of Ms per unit weight did not correlate with the variation indicated by the Mrs/Ms and Bc parameters. Because the value of Ms per unit weight is a parameter indicating the total amount of magnetic minerals, it can be considered that the total amount of magnetic minerals did not change but the MD-like magnetic minerals changed to SD grains with changes in temporal volcanic activity. The results of the September 4, 2019, FORC diagram show the typical MD grain character (Roberts et al., 2018), where the distribution of Bu values on the low-coercivity side is broadened. This feature is common to periods when magnetic minerals with low coercivity dominate. Because MD grains are known to have a larger grain size and lower coercivity than SD grains, it is estimated that the volume fraction of MD grains is high during periods when low coercivity magnetic materials predominate. Particularly, during a series of eruption activities, magnetic particles in volcanic ash, which are composed of MD + SD grains, possibly temporarily increase the volume fraction of SD grains.
The results of the rock magnetic measurements indicate that magnetic minerals in volcanic ash have periods of increased SD and Ti-rich titanomagnetite grains, which have slightly lower Tc than those of the other periods (Fig. 4). This period of dominance of SD grains was named the “fine titanomagnetite period (FTP)” and its relationship to volcanic phenomena is discussed below.
Comparison With Volcanic Phenomena
The first crater of Nakadake volcano, Aso, magmatic activity started on July 26, 2019, and the eruptions continued until June 15, 2020, with multiple pauses. During the active period, a large amount of ash fall, an increase in volcanic gases, and volcanic glow events over the crater were observed (Miyabuchi et al., 2021). Contrasting various observational data with the rock magnetic results of this study suggests that the results are related to volcanic glow observations according to the Japan Meteorological Agency (JMA). Volcanic glow events were frequently observed from late July to early August 2019, early October to mid-November and late December 2019, and late January to late February 2020. The FTP coincides well with the observed volcanic glow period (JMA, 2021, Fig. 5). As mentioned in the previous section, FTP is the time when the SD particles increase and titanomagnetite with a high titanium content is identified. The conditions under which the magnetic minerals change are discussed. The value of Ms per unit weight does not correlate clearly with changes in the values of Mrs/Ms or Bc, and it can be considered that the variation in Mrs/Ms and Bc is not due to the supply of total magnetic minerals in the magma. Since MD particles have a larger particle size than SD particles, it is thought that the time required for crystal growth from crystallization to cooling is longer than that for SD particles. This implies that physical and/or thermal changes inside the conduit are altered during the eruption process, and that the magnetic minerals reflect these changes. Moreover, the coincidence of the increase in SD volume fraction and the timing of the observation of volcanic glow also support the idea that FTP is capturing the phenomena inside the conduit. Mujin and Nakamura (2014) noted changes in particle size as the magma rose; they found that when the magma head was located deep inside the crater, relatively large particles were crystallized due to depressurization and a calm temperature gradient, but as the magma head rose, finer particles were newly formed owing to the effects of degassing, rapid cooling, and oxidation. Their assertions support the results of this study, and it will be important to examine the correspondence with the results obtained from physical observations in the future. This indicates that the rock magnetic properties of volcanic ash can contribute to the elucidation of the eruption process.