Submitted:
12 August 2025
Posted:
13 August 2025
You are already at the latest version
Abstract
Keywords:
1. Introduction
2. Materials and Methods
2.1. Stratospheric 7Be Production, Deposition and Measurement in Casaccia Research Center
2.2. Datasets and Data Analysis

2.3. De-Trending Methods
2.4. Advanced Measures of Statistical Dependence
2.4.1. Correlation Metrics
- Pearson’s correlation coefficient r - the metric measures the strength and direction of a linear relationship between two variables. It is defined as:where denotes the covariance between X and Y, and and are the standard deviations of X and Y, respectively. The covariance is given by:where and are the sample means of X and Y respectively. The coefficient r ranges from (perfect negative linear relationship) to (perfect positive linear relationship), with indicating no linear association.
- Spearman’s rank correlation coefficient - the metric measures the strength and direction of a monotonic relationship by computing the Pearson correlation between the ranked values of the variables:where denotes the covariance and the standard deviation of the ranked variables. In this context, ranking transforms the original vector of values into a vector of ranks, where each rank indicates the position of a value in the ordered dataset. The coefficient ranges from (perfect decreasing monotonic relationship) to (perfect increasing monotonic relationship), with indicating no monotonic association. Spearman’s is particularly effective in detecting relationships that are nonlinear but still consistently increasing or decreasing.
- Kendall’s rank correlation coefficient - the metric is based on counting the number of concordant and discordant pairs among all possible pairs of observations:where is the number of concordant pairs and is the number of discordant pairs, with n representing the sample size. Two observations and are considered concordant if the ranks of both variables increase or decrease together (i.e., and , or and ). They are discordant if one variable increases while the other decreases (e.g., but ). The coefficient also ranges from (complete inversion of ranks) to (perfect agreement in rank order), with corresponding to no association.
2.4.2. Dependence Metrics
-
Distance correlation - this metric measures the statistical dependence between two variables or vectors, capturing both linear and nonlinear relationships. Unlike Pearson’s correlation, distance correlation is equal to zero if and only if the variables are statistically independent, making it a true test of independence. Mathematically, distance correlation is defined as:where denotes the distance covariance between X and Y. The distance covariance quantifies how much the pairwise distances between observations in X are associated with the pairwise distances in Y. To compute it, the first step is to calculate the pairwise Euclidean distance matrices:These matrices are then transformed through a centering process, where the row means () and column means () are subtracted to the initial value and the grand mean () is added back, yielding the doubly centered matrices:and similarly for . The squared distance covariance is computed as:By normalizing the distance covariance with the distance variances of X and Y, the distance correlation coefficient , defined in eq. 8, is obtained. The coefficient ranges from 0 (independence) to 1 (perfect dependence) and can detect complex relationships that are not necessarily linear or monotonic. This makes distance correlation a valuable tool for exploring dependencies in environmental and geophysical data.
- Mutual information I - the metric quantifies the amount of information shared between two variables and is rooted in information theory. It is defined as:where is the joint probability distribution and , are the marginal distributions of X and Y, respectively. The index is always non-negative and equals zero if and only if X and Y are independent. Unlike correlation coefficients, mutual information has no fixed upper bound, and its magnitude depends on the entropy of the individual variables.
- Maximal Information Coefficient MIC - the metric allows to capture complex and potentially nonlinear relationships between time series. This method belongs to the family of maximal information-based nonparametric exploration (MINE) statistics and is designed to detect a wide range of association types, regardless of their functional form or strength. Conceptually, MIC measures how well one variable can be used to predict another by exploring how data points distribute over different grid partitions of the scatter plot. The algorithm divides the plane defined by variables X and Y into multiple grids of varying resolutions (up to a maximum resolution determined by the sample size). For each grid, it computes the mutual information—a measure quantifying how much knowing one variable reduces uncertainty about the other. The MIC is then defined as the highest normalized mutual information observed across all tested grids, formally expressed as:where denotes the maximum mutual information achievable with a grid of cells, and limits the maximum grid resolution based on the sample size n. This normalization ensures that MIC scores remain comparable across different grid sizes. A key advantage of MIC is its capacity to identify not only linear and monotonic relationships but also more complex patterns—such as periodic, exponential, or piecewise associations that traditional measures like Pearson or Spearman correlations might fail to detect. MIC values range between 0 and 1, where values close to 1 indicate strong dependence (irrespective of shape), and values near 0 suggest little or no association.
3. Results
3.1. Correlation on the Raw Data
3.2. De-Trending Methods Results
- Running Average: A window length of 70 months was chosen to effectively suppress high-frequency atmospheric oscillations, including the annual cycle ( 12 months), the quasi-biennial oscillation ( 2.2 years), and other meteorological variations such as ENSO ( 7 years), while preserving lower-frequency components linked to solar activity, particularly the 11-year solar cycle. This window was identified as an optimal compromise, ensuring that the extracted trend predominantly reflects variability of cosmic origin with minimal contamination from terrestrial atmospheric dynamics.
- Fourier Series: The trend component of the 7Be time series was reconstructed using the first five Fourier harmonics, aiming to isolate variability on multi-annual to decadal timescales. This spectral resolution was selected to capture the dominant long-term modulation associated with the 11-year solar cycle, while effectively filtering out higher-frequency fluctuations driven by meteorological and seasonal processes. The resulting low-frequency component defines the primary large-scale variability inherent in the 7Be record.
- STL Decomposition: The STL method was applied with a seasonal period of 36 months to suppress intra-annual and inter-annual fluctuations driven by meteorological processes and stratosphere-troposphere dynamics. This configuration isolates the low-frequency trend component of the 7Be time series, preserving variability potentially linked to solar-cycle modulation, while reducing the influence of shorter-term atmospheric oscillations.
3.3. Correlation and Dependence Metrics Results
4. Discussion
5. Conclusions
Author Contributions
Funding
Data Availability Statement
Acknowledgments
Conflicts of Interest
Abbreviations
| GCR | Galactic Cosmic Rays |
| SEP | Solar Energetic Particles |
| ENSO | El Niño–Southern Oscillation |
| QBO | Quasi-Biennial Oscillation |
| STL | Seasonal-Trend decomposition using Loess |
| MIC | Maximal Information Coefficient |
| MI | Mutual Information |
References
- Libby, W. F. Atmospheric Helium Three and Radiocarbon from Cosmic Radiation. Phys. Rev. 1946, 69, 671. [CrossRef]
- Arnold, J. R.; Al-Salih, H. A. Beryllium-7 produced by cosmic rays. Science 1955, 121, 451. [CrossRef]
- Young, J. A.; Silker, W. B. Aerosol deposition velocities on the Pacific and Atlantic Oceans calculated from 7Be measurements. Earth Planet. Sci. Lett. 1980, 50, 92–104. [CrossRef]
- Sanak, J.; Lambert, G.; Ardouin, B. Measurement of stratosphere-to-troposphere exchange in Antarctica by using short-lived cosmonuclides. Tellus B 1985, 37, 109–115. Available online. [CrossRef]
- Mohan, M. P.; D’Souza, R. S.; Nayak, S. R.; Kamath, S. S.; Shetty, T.; Kumara, K. S.; Mayya, Y. S.; Karunakara, N. Influence of rainfall on atmospheric deposition fluxes of 7Be and 210Pb in Mangaluru (Mangalore) at the Southwest Coast of India. Atmos. Environ. 2019, 202, 281–295. Available online: https://www.elsevier.com/locate/atmosenv.
- Liu, H.; Considine, D.B.; Horowitz, L.W.; Crawford, J.H.; Rodriguez, J.M.; Strahan, S.E.; Damon, M.R.; Steenrod, S.D.; Xu, X.; Kouatchou, J.; Carouge, C.; Yantosca, R.M. Using beryllium-7 to assess cross-tropopause transport in global models. Atmos. Chem. Phys. 2016, 16, 4641–4659. Available online. [CrossRef]
- Liu, J.; Starovoitova, V. N.; Wells, D. P. Long-term variations in the surface air 7Be concentration and climatic changes. J. Environ. Radioact. 2013, 116, 42–47. Available online: https://www.elsevier.com/locate/jenvrad. [CrossRef]
- Batrakov, G. F.; Kremenchutsky, D. A.; Kholoptsev, A. V. El Nino / Southern Oscillation and beryllium-7 concentration in the atmospheric boundary layer. Eur. Res. 2013, 45, [pages unknown].
- Papastefanou, C.; Ioannidou, A.; Stoulos, S.; Manolopoulou, M. Atmospheric deposition of cosmogenic 7Be and 137Cs from fallout of the Chernobyl accident. Sci. Total Environ. 1995, 170, 151–156. [CrossRef]
- Todorovic, D.; Popovic, D.; Djuric, G. Concentration measurements of 7Be and 137Cs in ground level air in the Belgrade city area. Environ. Int. 1999, 25, 59–66. https://doi.org/10.1016/S0160-4120(98)00099-3.
- Phillips, G. W.; King, S. E.; August, R. A.; Ritter, J. C.; Cutchin, J. H.; Haskins, P. S.; McKisson, J. E.; Ely, D. W.; Weisenberger, A. G.; Piercey, R. B.; Dyble, T. Discovery of Be-7 Accretion in Low Earth Orbit. In Proceedings of the 14th Annual AAS Guidance and Control Conference, Keystone, Colorado, USA, February 1991; DTIC Report AD-A236 614. Available online: https://apps.dtic.mil/sti/pdfs/ADA236614.pdf.
- Wilson, J. K.; Rees, M. H.; Allen, L. V. Beryllium-7 concentrations in the mesosphere-lower thermosphere measured by high-altitude balloon flights. J. Geophys. Res. Atmos. 1993, 98, 20479–20484. Available online: https://doi.org/10.1029/93JD02253.
- Mewaldt, R. A.; Stone, E. C.; Tylka, A. J. Enhanced beryllium-7 concentrations in the upper atmosphere following solar proton events. Geophys. Res. Lett. 2001, 28, 2585–2588. Available online. [CrossRef]
- Chen, D. L.; Zell, S. E.; Paulikas, G. A. Observations of cosmogenic beryllium-7 in the mesosphere and lower thermosphere. J. Atmos. Solar-Terr. Phys. 1993, 55, 707–714. Available online: https://doi.org/10.1016/0021-9169(93)90003-8.
- Golubenko, K.; Rozanov, E.; Kovaltsov, G.; Leppänen, A.-P.; Sukhodolov, T.; Usoskin, I. Chemistry-climate model SOCOL-AERv2-BEv1 with the cosmogenic Beryllium-7 isotope cycle. Geosci. Model Dev. Discuss. 2021. Available online. [CrossRef]
- Nelson, G. A. Space Radiation and Human Exposures, A Primer. Radiat. Res. 2016, 185, 349–358. Available online. [CrossRef]
- Rizzo, A.; Borra, E. M.; Ciciani, L.; Di Fino, L.; Romoli, G.; Santi Amantini, G.; Sperandio, L.; Vilardi, I.; Narici, L. Foundations of radiological protection in space: the integrated multidisciplinary approach for next manned missions in deep space. Eur. Phys. J. Plus 2023, 138, Article 1001. Available online. [CrossRef]
- Papastefanou, C.; Ioannidou, A. Beryllium-7 and solar activity. Appl. Radiat. Isot. 2004, 61, 1493–1495. Available online. [CrossRef]
- Rajacic, M. M.; Todorovic, D. J.; Krneta Nikolic, J. D.; Puzovic, J. M. The impact of the Solar magnetic field on 7Be activity concentration in aerosols. Appl. Radiat. Isot. 2017, 125, 27–29. Available online. [CrossRef]
- Aldahan, A.; Hedfors, J.; Possnert, G.; Kulan, A.; Berggren, A.-M.; Söderström, C. Atmospheric impact on beryllium isotopes as solar activity proxy. Geophys. Res. Lett. 2008, 35, L21812. Available online. [CrossRef]
- Kremenchutskii, D. A.; Konovalov, S. K. Beryllium-7 and its variability in the near-surface atmosphere of Crimea, the Black Sea region. Atmos. Pollut. Res. 2022, 13, 101406. Available online. [CrossRef]
- Brattich, E.; Liu, H.; Tositti, L.; Considine, D. B.; Crawford, J. H. Processes controlling the seasonal variations in 210Pb and 7Be at the Mt. Cimone WMO-GAW global station, Italy: a model analysis. Atmos. Chem. Phys. 2017, 17, 1061–1080. Available online. [CrossRef]
- Kulan, A.; Aldahan, A.; Possnert, G.; Vintersved, I. Distribution of 7Be in surface air of Europe. Atmos. Environ. 2006, 40, 3855–3868. Available online. [CrossRef]
- Baldwin, M. P.; Gray, L. J.; Dunkerton, T. J.; Hamilton, K.; Haynes, P. H.; Randel, W. J.; Holton, J. R.; Alexander, M. J.; Hirota, I.; Horinouchi, T.; Jones, D. B. A.; Kinnersley, J. S.; Marquardt, C.; Sato, K.; Takahashi, M. The quasi-biennial oscillation. Rev. Geophys. 2001, 39, 179–229. Available online. [CrossRef]
- Casselman, J. W.; Lübbecke, J. F.; Bayr, T.; Huo, W.; Wahl, S.; Domeisen, D. I. V. The teleconnection of extreme El Niño–Southern Oscillation (ENSO) events to the tropical North Atlantic in coupled climate models. Weather Clim. Dyn. 2023, 4, 471–487. Available online. [CrossRef]
- Yu, N.; Chen, G.; Ray, J.; Chen, W.; Chao, N. Semi-decadal and decadal signals in atmospheric excitation of length-of-day. Earth Space Sci. 2019, 6, 1205–1216. Available online. [CrossRef]
- Lal, D.; Peters, B. Cosmic Ray Produced Radioactivity on the Earth. In Kosmische Strahlung II / Cosmic Rays II; Sitte, K., Ed.; Springer: Berlin, Heidelberg, 1967; Vol. 9, pp. 1–50.
- Talpos, S.; Cuculeanu, V. A Study of the Vertical Diffusion of 7Be in the Atmosphere. J. Environ. Radioact. 1997, 36, 93–106. [CrossRef]
- Sitte, K.; Stierwalt, D. L.; Kofsky, I. L. Development of Air Showers in the Atmosphere. Phys. Rev. 1954, 94, 988–993. Available online: https://link.aps.org/doi/10.1103/PhysRev.94.988. [CrossRef]
- Papastefanou, C.; Ioannidou, A. Beryllium-7 Aerosols in Ambient Air. Environ. Int. 1996, 22, S125–S130.
- Zheng, M.; Liu, H.; Adolphi, F.; Muscheler, R.; Lu, Z.; Wu, M.; Prisle, N. L. Simulations of 7Be and 10Be with the GEOS-Chem global model v14.0.2 using state-of-the-art production rates. Geosci. Model Dev. 2023, 16, 7037–7057. Available online. [CrossRef]
- Zhang, F.; Wang, J.; Baskaran, M.; Zhong, Q.; Wang, Y.; Paatero, J.; Du, J. A global dataset of atmospheric 7Be and 210Pb measurements: annual air concentration and depositional flux. Earth Syst. Sci. Data 2021, 13, 2963–2994. Available online. [CrossRef]
- Yoshimori, M. Beryllium 7 radionuclide as a tracer of vertical air mass transport in the troposphere. Adv. Space Res. 2005, 36, 828–832. Available online: https://www.sciencedirect.com/science/article/abs/pii/S0273117705004356.
- Koch, D. M.; Jacob, D. J.; Graustein, W. C. Vertical transport of tropospheric aerosols as indicated by 7Be and 210Pb in a chemical tracer model. J. Geophys. Res. Atmos. 1996, 101, 18651–18666. Available online. [CrossRef]
- Długosz-Lisiecka, M.; Bem, H. Seasonal fluctuation of activity size distribution of 7Be, 210Pb, and 210Po radionuclides in urban aerosols. J. Aerosol Sci. 2020, 144, 105544. Available online. [CrossRef]
- NMDB Event Search Tool (NEST). Available online: https://www.nmdb.eu/nest/ (accessed on 25 October 2024).
- WDC-SILSO. Royal Observatory of Belgium, Brussels. Available online: https://www.sidc.be/SILSO/datafiles (accessed on 25 October 2024).
- von Storch, H.; Zwiers, F. W. Statistical Analysis in Climate Research; Cambridge University Press: Cambridge, UK, 1999.
- Wilks, D. S. Statistical Methods in the Atmospheric Sciences, 3rd ed.; Academic Press: San Diego, USA, 2011.
- Cleveland, R. B.; Cleveland, W. S.; McRae, J. E.; Terpenning, I. STL: A Seasonal-Trend Decomposition Procedure Based on Loess. J. Off. Stat. 1990, 6, 3–73.
- Bloomfield, P. Fourier Analysis of Time Series: An Introduction; John Wiley & Sons: Hoboken, NJ, USA, 2004.
- Spearman, C. The Proof and Measurement of Association Between Two Things. Am. J. Psychol. 1904, 15, 72–101.
- Kendall, M. G. A New Measure of Rank Correlation. Biometrika 1938, 30, 81–93. [CrossRef]
- Conover, W. J. Practical Nonparametric Statistics, 3rd ed.; John Wiley & Sons: New York, USA, 1999.
- Kendall, M.; Gibbons, J. D. Rank Correlation Methods, 5th ed.; Edward Arnold: London, UK, 1990.
- Székely, G.J.; Rizzo, M.L.; Bakirov, N.K. Measuring and testing dependence by correlation of distances. Ann. Stat. 2007, 35, 2769–2794. Available online. [CrossRef]
- Szekely, G. J.; Rizzo, M. L. Brownian distance covariance. Ann. Appl. Statist. 2009, 3, 1236–1265. Available online. [CrossRef]
- Kraskov, A.; Stögbauer, H.; Grassberger, P. Estimating mutual information. Phys. Rev. E 2004, 69, 066138. Available online. [CrossRef]
- Reshef, D.N.; Reshef, Y.A.; Finucane, H.K.; Grossman, S.R.; McVean, G.; Turnbaugh, P.J.; Lander, E.S.; Mitzenmacher, M.; Sabeti, P.C. Detecting novel associations in large data sets. Science 2011, 334, 1518–1524. Available online. [CrossRef]




| Pair | r | p-value (r) | p-value () | p-value () | MI | MIC | |||
| Be-7 vs Neutron Counts | 0.23 | 0.31 | 0.21 | 0.29 | 0.34 | 0.22 | |||
| Be-7 vs Sunspot Number | -0.16 | -0.27 | -0.19 | 0.24 | 0.35 | 0.21 | |||
| Neutron Counts vs Sunspot | -0.87 | -0.88 | -0.69 | 0.86 | 0.91 | 0.70 |
| Method | Period [years] |
Lower Bound [years] |
Upper Bound [years] |
Systematic Range [years] |
|---|---|---|---|---|
| Running Avg | 10.92 | 9.96 | 10.92 | 0.96 |
| Fourier | 9.79 | 9.80 | 11.42 | 1.62 |
| STL | 10.54 | 10.46 | 10.79 | 0.33 |
| Pair | Method | r | p-value(r) | p-value() | p-value() | MI | MIC | |||
| Be-7 vs Neutron | fourier | 0.54 | 0.62 | 0.43 | 0.59 | 0.79 | 0.51 | |||
| running | 0.65 | 0.75 | 0.55 | 0.69 | 0.93 | 0.60 | ||||
| stl | 0.52 | 0.61 | 0.46 | 0.60 | 0.93 | 0.58 | ||||
| Be-7 vs Sunspot | fourier | -0.38 | -0.47 | -0.31 | 0.43 | 0.70 | 0.33 | |||
| running | -0.48 | -0.58 | -0.40 | 0.51 | 0.68 | 0.39 | ||||
| stl | -0.39 | -0.48 | -0.35 | 0.46 | 0.72 | 0.39 | ||||
| Neutron vs Sunspot | raw | -0.87 | -0.88 | -0.69 | 0.86 | 0.91 | 0.70 |
Disclaimer/Publisher’s Note: The statements, opinions and data contained in all publications are solely those of the individual author(s) and contributor(s) and not of MDPI and/or the editor(s). MDPI and/or the editor(s) disclaim responsibility for any injury to people or property resulting from any ideas, methods, instructions or products referred to in the content. |
© 2025 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/).