An extensive screening campaign has preceded the selection and procurement of all materials used in the construction of CUORE (for details on material assay techniques commonly adopted in this field see [44]). The focus was on the most ubiquitous natural contaminants \(^{232}\)Th and \(^{238}\)U (with their respective progenies), and on a few cosmogenically activated contaminants: \(^{60}\)Co, \(^{110}\)Ag and \(^{110\mathrm{m}}\)Ag [45]. All these isotopes emit, in their decay chains, particles that have enough energy to mimic a \(0\nu \beta \beta \) decay. Even if the mentioned isotopes do not include all the natural or comogenic radionuclei, all other isotopes are expected to yield minor, if not negligible, contributions in the ROI.
The selection of all the CUORE components comprised the certification of the material activity, both for bulk and surface contaminations. Surface contamination can occur during the processes of machining and cleaning, or during exposure to contaminated air. In addition, the effect of breaks in the secular equilibrium of a radioactive chain can be quite relevant for surface contaminations, as it is the case for \(^{210}\)Pb in the \(^{238}\)U chain. Indeed, \(^{222}\)Rn emanation from any material containing \(^{238}\)U impurities produces excess concentrations of \(^{210}\)Pb (the only long-lived isotope in the \(^{222}\)Rn progenies) in the air and dust that, in turn, can contaminate exposed components.
The techniques adopted in the various phases of material screening include \(\gamma \) spectroscopy with heavily-shielded high purity germanium (HPGe) diodes, to investigate bulk contaminations, and \(\alpha \) spectroscopy with large-area low-background silicon surface barrier (SiSB) diodes, to screen for surface contaminations. Additionaly, inductively coupled plasma mass spectrometry (ICPMS) and neutron activation analysis (NAA), both particularly suitable for small samples, were also used. Alpha and gamma spectroscopy and ICPMS analysis were performed at LNGS [46, 47], Milano-Bicocca [48], Baradello Laboratory [49] and Lawrence Berkeley National Laboratory (LBNL) [50]. Neutron activation analysis was carried out in collaboration with the Laboratory of Applied Nuclear Energy (LENA) in Pavia, Italy [51, 52].
All materials constituting the CUORE experimental setup, as well as those in contact with the detector components during the production and cleaning phases, have thus been carefully selected according to their bulk contamination levels. Then, for materials in the far region (see Table 2), careful cleaning and storage with standard techniques are enough to ensure that surface contributions are negligible. This was routinely confirmed with SiSB detectors. On the other hand, in the near region the radiopurity requirement for material surfaces can be as strict as a few nBq/cm\(^2\). In fact, in elements sufficiently close to the bolometers \(\alpha \) and \(\beta \) particles can also mimic a \(0\nu \beta \beta \) event. For these particles the detection efficiency is much higher (since the absorption probability is nearly 1), and even contaminants with a small activity can produce a relevant background rate in this case. In critical cases when the required sensitivity was not achievable with SiSB detectors, NAA and ICPMS have been exploited to certify material surface contamination.
Finally, in the few cases where all the above techniques failed in reaching the required sensitivity, bulk and/or surface contamination levels were determined through particle spectroscopy with TeO\(_2\) detectors [9, 37, 53]. These measurements were carried out underground at LNGS using arrays of CUORE-like TeO\(_2\) bolometers. One of the most remarkable results obtained in this case is the evaluation of the radioactive sources contaminating the CUORE-0 detector with an unprecedented precision, as will be discussed later.
In the next sections the evaluation of contaminant activities in all the materials used for the CUORE construction will be presented. The evaluation of bulk contaminants will be discussed first, followed by surface ones. The CUORE-0 results, both for bulk and surface contaminations, will instead be discussed in two dedicated sections.
Cosmogenic activation
Cosmogenic activation is a well-known mechanism for the production of radioactive nuclei in the bulk of materials, mainly through spallation processes. At sea level, cosmic rays are comprised of charged pions, protons, electrons, neutrons, and muons, with relative flux intensities of roughly 1:13:340:480:1420 [54]. Neutrons are clearly the dominant source of cosmogenic activation above ground. At the CUORE experimental site at LNGS, the cosmic ray flux is decreased to an almost negligible level (only muons survive the rock overburden), and hence cosmogenic activation is drastically reduced. Therefore, in this paper we analyze only activation of materials before their underground storage.
In CUORE, the most abundant materials are TeO\(_2\), copper, and lead. Among these, only Te and Cu isotopes exhibit large enough cross sections for radioisotope production via cosmogenic activation. In order to contribute to the ROI, cosmogenic nuclei must have a transition energy greater than \(Q_{\beta \beta }\), a sizable production cross section, and a relatively long half-life (compared to the time scale of the experiment). Based on the neutron flux at sea-level [55, 56], the exposure time of copper and TeO\(_2\) to cosmic rays, and the measured or calculated neutron spallation cross sections [45, 57,58,59,60,61,62,63,64,65], two isotopes fulfill these criteria: \(^{60}\)Co and \(^{110\mathrm{m}}\)Ag.
\(^{60}\)Co (\(\tau _{1/2} = 5.27\) years, Q = 2.82 MeV) is produced both in copper and tellurium. It \(\beta \)-decays with the simultaneous emission of two \(\gamma \) rays (1.17 MeV and 1.33 MeV). To mimic the energy of a \(0\nu \beta \beta \) event, both the \(\gamma \) rays and the electron must deposit their energy in the same crystal, requiring \(^{60}\)Co to be either in the TeO\(_2\) crystals or in the copper parts close to the bolometers (CuNOSV).
\(^{110\mathrm{m}}\)Ag (\(\tau _{1/2} = 250\) days) is produced in tellurium. It can either \(\beta \)-decay to the stable isotope \(^{110}\)Cd (B.R. = \(98.7\,\%\), Q = 3.01 MeV), or it can make an isomeric transition to \(^{110}\)Ag (B.R. = \(1.3\%\), Q = 0.118 MeV), which then further \(\beta \)-decays to \(^{110}\)Cd (B.R. = \(99.7\,\%\) and Q = 2.89 MeV). \(^{110}\)Ag has a short half-life (\(\tau _{1/2} = 24.6\) s) and will therefore be in secular equilibrium with \(^{110\mathrm{m}}\)Ag during the expected 5 years of CUORE data-taking. Both \(^{110\mathrm{m}}\)Ag and \(^{110}\)Ag emit numerous photons in their decays. The decay of either isotope can mimic a \(0\nu \beta \beta \) event when the total energy deposited in a single crystal by the photons and electrons is within the ROI.
To minimize the activation levels of TeO\(_2\) and copper (both NOSV and OFE), their exposure to cosmic rays was reduced as much as possible. Approximately 3 months elapsed from crystal growth to underground storage at LNGS for the TeO\(_2\) crystals, followed by an average cooling time of 4 years before use. 4 months elapsed from casting of the raw materials to underground storage for all the machined and cleaned CuNOSV components. Requirements were less stringent for OFE copper since this is used in the far region. The activation levels of TeO\(_2\) crystals at the start of CUORE have been estimated based on the results of neutron and proton activation measurements published in [65] and [45]. Estimation of activation levels for CuNOSV follows [66] and incorporates the CUORE-0results. The estimates of the activation levels are given as conservative upper limits, evaluated approximately one year prior to the beginning of CUORE data taking. These are:
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\(<20\) nBq/kg of \(^{110\mathrm{m}}\)Ag + \(^{110}\)Ag (in secular equilibrium with each other) in the \(TeO_2\) [65];
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\(<1\) nBq/kg of \(^{60}\)Co in the \(TeO_2\) [65]. This level of contamination is far below both the HPGe sensitivity and the sensitivity achieved in CUORE-0 (30 \(\upmu \)Bq/kg [42]);
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\(< 35~\upmu \)Bq/kg of \(^{60}\)Co in the CuNOSV. This limit is in good agreement with the HPGe measurements performed on a few CuNOSV samples (\(<25~\upmu \)Bq/kg) and also with the \(^{60}\)Co activity resulting from the same copperFootnote 4 in CUORE-0.
Table 3 Values and 90% C.L. (95% C.L. for HPGe measurements) upper limits on \(^{232}\)Th and \(^{238}\)U bulk contaminations of detector and cryostat materials (the various components are described in Section 2), as obtained in the material screening campaign. Activities are expressed in Bq/kg (1 Bq/kg = 246 \(\times \) 10\(^{-9}\) g/g for \(^{232}\)Th and 81 \(\times \) 10\(^{-9}\) g/g for \(^{238}\)U). The quoted uncertainties are statistical. In the last column, the measurement technique is indicated, as described in the text. We only include the results shown in bold in the background budget evaluation, as discussed in Sect. 6
Table 4 90% C.L. upper limits on surface contamination of various CUORE detector components, as obtained in the material screening campaign. To infer the surface contamination from the measured data, different contamination depths were considered (column 1): the limits reported in the table are the ones corresponding to the contamination depth that gives the highest background contribution, as explained in the text. In the last column, the measurement technique is indicated
\(^{238}\)U and \(^{232}\)Th bulk contamination
Table 3 shows the \(^{238}\)U and \(^{232}\)Th bulk activities of the different CUORE materials as obtained in the radioactive assay campaign. The detection efficiency in each measurement is determined using a GEANT4-based Monte Carlo simulation that reproduces the detector geometry and distribution of contaminants in the sample. For each isotope we report the result (or upper limit) of the most sensitive method employed, even if more than one technique may have been used for the same material (i.e. \(^{232}\)Th and \(^{238}\)U results may come from different assay techniques for the same material).
In the case of the bulk contamination of CuNOSV, we report in Table 3 the limits obtained with direct measurements and in Table 5 the limits obtained in the CUORE-0 analysis (the latter are discussed in the next section). As discussed in Sect. 6, the results obtained with the CUORE-0 detector are used for the CUORE background budget evaluation.
The bulk contamination of the NTDs here refers to the impurity concentration certified by the manufacturer for undoped wafers. The doping is done in a nuclear reactor producing a large number of short-lived radioactive isotopes. The hypothesis that long-lived isotopes potentially dangerous for a \(0\nu \beta \beta \) bolometric experiment could also be produced during reactor exposure was investigated in [67] and rejected. After the doping process, an ohmic contact is created on the Ge surface. This operation could cause contamination of the thermistor, that is analyzed as a surface contribution. It is anyway worth noting that signals originating from nuclear decays occurring in the thermistor volume are deformed in their shape, and can therefore be efficiently rejected by the standard pulse shape cuts applied by the analysis process.
\(^{238}\)U, \(^{232}\)Th and \(^{210}\)Pb surface contamination
In Table 4, we report the most sensitive upper limits obtained for the surface activities of the materials used in the near region.
As it was done for the bulk contamination, a Monte Carlo simulation was used to determine, in each measurement, the detection efficiency of the surface contamination. While for bulk contamination the free parameter is only the bulk activity of the sample (always considered to be uniformly distributed in its volume), in the case of surface contamination the impurity distribution is described according to Eq. 1 using two parameters. In all the measurements discussed in this section, experimental data are not enough to measure both \(\lambda \) and \(\rho _0\). Therefore we proceed by evaluating, for each \(\lambda \), the contaminant density \(\rho _0\) compatible with the experimental data. The integral of \(\rho \) over the contaminated volume, divided by the surface of the sample yields the impurity concentration measured in Bq/cm\(^2\). After having evaluated the surface impurity concentration for a wide range of depths (\(\lambda \)), we chose the one producing the highest background contribution, and quoted this limit in Table 4. The minimum depth considered in this analysis is 0.001 \(\upmu \)m for \(TeO_2\) and 0.1 \(\upmu \)m for any other material. Indeed, these are the most shallow distributions whose effects can be experimentally identified. The maximum depth is \(\sim \)10 \(\upmu \)m for \(TeO_2\) and CuNOSV (the range of 5 MeV \(\alpha \) particles in these materials is \(\sim \)10 \(\upmu \)m and \(\sim \)15 \(\upmu \)m, respectively), and 30 \(\upmu \)m for PTFE (where the range of 5 MeV \(\alpha \) particles is \(\sim \)23 \(\upmu \)m). Larger depths are almost indistinguishable from bulk contaminations.
While NTDs and PEN were measured through \(\alpha \) spectroscopy with SiSB diodes, in the case of the heaters the small size of the sample required a more sensitive technique. The \(\alpha \) spectrometer used in this case was an array of two 5 \(\times \) 5 \(\times \) 5 cm\(^3\) TeO\(_2\) bolometers operated in the cryogenic facility of Hall C at LNGS. A matrix of heaters, 5 \(\times \) 5 cm\(^2\) in total area, was oriented towards the crystals and the \(\alpha \) induced background was analyzed with the technique illustrated in [5]. In the case of \(^{238}\)U and \(^{232}\)Th impurities in PTFE, the best upper limits are obtained with the NAA technique (analyzing the results as if all measured contaminants were contained in a surface layer). Giving information only on the progenitor, such technique is insensitive to \(^{210}\)Pb contamination. A bolometric detector array (TTT, for Three Tower Test) was used to compare different copper surface treatments and to analyze the CuNOSV contamination level. The TTT detector [39] consisted of three small towers, each with 12 TeO\(_2\) detectors and enclosed inside its own copper box. The limits reported in Table 4 are those obtained with the TECM cleaning, wich showed the lowest background level and was therefore chosen as the baseline cleaning protocol for all the CuNOSV pieces of the CUORE detector.
Contamination from CUORE-0 analysis
In [42], the sources contributing to the CUORE-0 event rate were reconstructed by fitting a number of Monte Carlo simulations to the measured spectra. The fit was performed with a Bayesian approach which allows to exploit any previous knowledge on material contamination by defining priors on source activities. For many sources, a sensitivity on contaminant concentration better than that achieved with standard techniques was obtained, along with a more efficient disentanglement of contamination species and a detailed study of secular equilibrium violations in radioactive chains.
Tables 5 and 6 summarize the results obtained for the impurity concentrations in materials that belong to the same production batches of CUORE, i.e. the TeO\(_2\) crystals and the NOSV copper (that in CUORE-0 analysis was taken as representative of the whole detector holder structure – see later). For the bulk contamination levels, the sensitivity improvements obtained by the CUORE-0 analysis are minor (compare the limits reported for \(TeO_2\) in Tables 3 and 5 or those reported for CuNOSV in Table 3 and for Holder in Table 5). On the contrary, for surface contaminations the improvements are significant: the CUORE-0 analysis allowed to derive a model for the impurity density profiles meanwhile achieving a high sensitivity in the determination of their activity. Moreover, since the procedure adopted in CUORE-0 background reconstruction was to simultaneously fit all the simulated spectra to the measured one, it was possible to find the best evaluation for each contaminant concentration as well as the correlation factor among different sources (see Fig. 3).
Table 5 Values and 90% C.L. upper limits on bulk contaminations in the TeO\(_2\) crystals and the Holder based on the background model of CUORE-0 [42]. Contaminants are identified as follows: when the progenitor is indicated all the chain is assumed in secular equilibrium, in all other cases single isotopes or sub-chains of \(^{232}\)Th and \(^{238}\)U are considered. Each contaminant is assigned a unique index for future reference
Table 6 90% C.L. upper limits and values for surface contamination of the TeO\(_2\) crystals and the Holder based on the background model of CUORE-0 [42]. Contaminants are identified as follows: when the progenitor is indicated all the chain is assumed in secular equilibrium, in all other cases single isotopes or sub-chains of \(^{232}\)Th and \(^{238}\)U are considered. Each contaminant is assigned a unique index for future reference
A separate discussion applies to the small parts used to build the CUORE-0 detector – i.e. NTD thermistors, PEN cables, Si heaters, Au bonding wires, glue and PTFE supports – also belonging to the same production batch of CUORE. In fact, in CUORE-0 analysis these small mass/surface components exhibit spectra that are completely degenerate with those of the NOSV copper detector structure; therefore only the latter was considered in the model under the name of Holder (see Tables 5, 6), chosen to underline that the resulting activities also include the small parts contribution. This contribution is expected to be negligible in the CUORE-0 background, as confirmed by Fig. 4. In these plots the experimental rate of the different planes of the CUORE-0 detector in the energy region between 2.7 and 3.9 MeV (i.e. the interval dominated by degraded \(\alpha \) contributions from surface contaminants) is compared to the rate expected from a \(^{210}\)Pb contamination in the NOSV copper detector structure or in the PTFE supports (chosen as representative of all the small parts, because of their bigger mass/surface) – similar plots are obtained for \(^{232}\)Th and \(^{238}\)U contaminants. The degeneracy between these two sources can be broken by examining the detector plane dependence of the counting rate. This is illustrated in Fig. 4. The detectors in the upper and lower planes of the CUORE-0 tower (1 + 13 floors in Fig. 4) face a larger copper surface of the 10 mK shield, while seeing a slightly smaller surface of PTFE and other small parts compared to the middle floors of CUORE-0. The CUORE-0 data shown in Fig. 4 suggest that the contribution to the overall background in the 2.7–3.9 MeV region from PTFE supports is compatible with zero. The resulting PTFE supports surface contaminations are reported in Table 7 (to be compared to the corresponding ones in Table 4).
Table 7 90% C.L. upper limits for surface contamination of the PTFE supports based on the background model of CUORE-0 [42] with the additional information coming from Fig. 4