The frequency distribution taking data from to shows a significant periodicity at around 0. To further confirm the correlation between the solar cycle and tritium of precipitation, cross-correlation analyses and wavelet transform analyses were performed. Spline average and bomb peak corrected time series of tritium concentration of precipitation from fourteen stations were applied for cross-correlation analysis. These cross-correlation calculations further corroborate the positive correlation between neutron count rate and tritium time series at most of the locations Supplementary Fig.
Cross-correlation coefficients are weaker in the case of spline-averaged tritium time series without bomb correction , which can be explained by the attenuating contribution of artificial tritium from nuclear weapon experiments. Wavelet transform analyses exploit the spectral power of frequency and cross-correlation patterns in time. Continuous wavelet calculations also show a month period in all cases Fig.
The Spectrum and Charge Composition of the Primary Cosmic Radiation
This is in a good agreement with the well known seasonality of tritium concentration of precipitation 26 — This year period is obviously seen in the neutron count rate time series, while for Kaitoke and Cuxhaven the year period is weaker but still significant. Wavelet coherence analysis based on neutron and tritium data for Kaitoke and Cuxhaven provides stronger evidence for an year periodicity. In Fig. The period is also determined to be about 11 years. Wavelet analysis. Wavelet coherence analyses for Cuxhaven and Kaitoke between tritium concentration of precipitation and neutron count rate of Oulu for Cuxhaven and Hermanus for Kaitoke.
The shading indicates areas outside the cone of influence. Arrows indicate phase angle in the all case of time series are in phase when the arrows point to the right. These mathematical analyses provide the first evidence for the existence of years periodicity of tritium and its correlation with secondary neutron flux for the period studied. Moreover, it is also important to consider other factors which might influence the magnitude of the temporal and spatial variation of the global tritium in the water cycle: 1.
We believe that artificial tritium emissions due to either weapon tests or nuclear facilities do not account for the pattern which we have shown to be synchronous with the solar cycle. Our previous study has demonstrated that an emission of 3. In fact, Kaitoke is known to be free of these sources. Even precipitation at coastal locations at the North Sea, like Cuxhaven, are not significantly affected by local or regional contamination sources The Cuxhaven precipitation is slightly affected by the moisture evaporated from North Sea, which is contaminated by artificial tritium from the Le Hague reprocessing plant However, this local contamination is not co-varying with the solar cycle, rather this gives a constant tritium offset to the meteoric precipitation at the coastal region of northern France, Belgium, The Netherlands and Germany.
However, natural processes might contribute to the tritium variation which have similar signature to an year periodicity. Since tritium concentration depends on the geographical location of the precipitation as well as the moisture source, one has to consider whether long-term changes in the distribution of air mass sources may be linked to solar cycles. We can show that the distribution of moisture source carrying the tritium are independent of the solar magnetic variations, and these sources did not change in the last 25 years See Supplementary.
To evaluate how solar cycles might affect the origin of the moisture sources, hour backward trajectories have been calculated for our four locations Supplementary Information For each year, the trajectories have been selected based on their source region and a frequency value has been calculated for all moisture source areas. Supplementary Fig. For the European stations, five different source regions, while for Wellington three source regions could be defined. No long-term changes are present in the plots Supplementary Fig.
Hence it suggests that changes in the prevailing moisture source distribution have not influenced the visible long-term fluctuation of tritium concentration in precipitation. Consequently, shifts in the main moisture sources can be excluded as a main process driving tritium variability in precipitation. Although it is very hard to assess the influence of these processes on the tritium concentrations in precipitation, we have made an attempt to evaluate positive feedback controlling the tritium content of precipitation.
In order to further explore the natural variation of tritium in the precipitation and its relationship with other cosmogenic isotopes, the signal resulting from the nuclear weapon tests has been subtracted from the observed tritium concentration in Kaitoke and Cuxhaven. Similar behaviour can be seen for 10 Be. Therefore, it is expected that the magnitude of the yr cycle in 10 Be is greater than that in NM data. As for tritium variation, the magnitude is also higher than that of NM time series. Temporal variations of neutron count rate Oulu, Finland , tritium concentrations of precipitation and 7 Be concentrations of atmospheric air.
The values are expressed as a relative deviation compared to the long term averages. Note that the Kaitoke and Cuxhaven time series have been corrected for the contribution of the bomb peak. However, the response of tritium variation in precipitation to the solar cycle also can help us understand what processes play a role in the water cycle from the tritium formation in the troposphere and stratosphere down to the surface 47 , Tritium is an important environmental tracer for understanding the global water cycle, and the tritium variation in precipitation that we found has implication for the use of cosmogenic tritium for dating young groundwater, e.
Nevertheless, further analysis needs to be performed over the next decades, in order to reveal the behaviour of tritium in precipitation related to solar effects. To study the correlation between solar cycle and tritium in precipitation, further precipitation as well as arctic or glacier ice cores, as an archive of precipitation accumulated before the nuclear era should also be investigated in the near future 49 , In this latter case very sensitive analytical capabilities with a precision of 0. In case of water, 1 TU equals to 0. Cuxhaven and Debrecen precipitation samples have been analysed using the 3 He ingrowth method 33 , This approach is based on the mass spectrometric measurement of the accumulation of 3 He, the daughter product of tritium, from the decay of tritium.
When analysing the Debrecen samples, a special isotope dilution technique was applied, where an ultrapure 4 He spike was added to the sample in order to eliminate systematic errors 36 , The uncertainty of the 3 He ingrowth method is about 0.
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It was decided to collect each individual precipitation in a month. The quantity corresponding to the collecting interval was recorded, and stored at low temperatures and at the end of the month both the individual precipitation for tritium concentration determination and the weighted mean of monthly precipitation were prepared, and they were measured in the same conditions.
The tritium concentrations average of individual precipitation was calculated for current month and it was compared with the tritium concentration determined in the monthly composite precipitation. The reported values are the same taking into account the measurement uncertainty for both evaluations. This double-check allowed the use of recorded results even for results near the limit of detection. Due to the use of electrolytic enrichment of the water, the Kaitoke samples 1—5 TU have a better uncertainty of 0. Samples for 3 H were vacuum distilled and enriched by electrolysis prior to being analysed by liquid scintillation spectrometry using Quantulus ultra-low-level counters at GNS, New Zealand.
Following the improvements from Morgenstern and Taylor the sensitivity is now further increased to a lower detection limit of 0. For two time series x and y, the cross-correlation value at lag time m is:. The summations and the mean values are only taken over the parts where the sequences overlap for a given time lag. The equation shows that for positive lags, x is compared with a y that has been delayed by m samples.
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A high correlation value at positive lags thus means that features in y are leading, while x lags behind. For negative lags, features in x are leading. Cross-correlation significance has been calculated by the Ebisuzaki method The spline smoothing was done using Past 3. In the second step, we calculated the bomb-peak corrected BPC time series as the subtraction of the tritium time series and the exponential function.
The parameters of this exponential function have been determined with an optimisation algorithm. The application of wavelet transformation has became widespread in the non-linear time series analysis. This method was applied in our time series. In addition, the Mexican Hat provides better detection and localization of patch and gap events over the Morlet function. Peaks and troughs in the scalogram of WAC relatively extreme values of the wavelet coefficient from Mexican hat can be directly linked to events and site conditions.
In contrast, the Morlet offers improved scale detection and localization over the Mexican Hat.
We thank A. All authors reviewed the manuscript. Publisher's note: Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Kosmische Strahlung II / Cosmic Rays II
Supplementary information accompanies this paper at National Center for Biotechnology Information , U. Sci Rep. Published online Aug Timothy Jull 1, 8.
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Scherrer The effects of galactic cosmic rays, modulated by solar terrestrial magnetic fields, on the climate Russian Journal of Earth Sciences, Volume 6, Number 5, October — V. Teilen: E-Mail Drucken Facebook.
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