Introduction
Stars are responsible for creating elements heavier than helium. The first generation of stars, also called Population III (Pop III) stars or primordial stars, were formed from primordial matter (mainly H and He) left behind by the Big Bang. These first stars play a special role in seeding the universe with the first metals and in creating suitable conditions for future generations of stars.
The first stars were predominantly very massive and spent the majority of their lives quiescently fusing hydrogen into helium in their cores through catalytic carbon-nitrogen-oxygen (CNO) cycles, where carbon was produced in the previous triple alpha process or the sequential alpha capture mechanism [1-4]. As a catalytic reaction, the net CNO mass fraction remains constant unless a breakout reaction sequence causes a leak toward the NeNa mass region or the temperature and density are high enough to forge new carbon by the triple alpha (3α) process, as is the case for primordial massive stars. A leak via the 19F(p, γ)20Ne reaction causes an irreversible flow from the CNO to the NeNa region because none of the (p, α) feedback processes via Ne isotopes are energetically possible [5]. For materials that leak through fluorine, protons capture and decay along the stability valley, leading to the production of a double magic nucleus 40Ca [6-8]. The leakage depends on the thermonuclear rate ratio of the break-out 19F(p,γ)20Ne reaction and the competing back-processing 19F(p, α)16O reaction.
Previously, the (p, γ) reaction was assumed to be extremely weak compared with the competing (p, α) reaction, and models predicted that most of the 19F produced by the CNO cycle would be recycled back into 16O without significant changes in chemical abundance [9]. This assumption was made by simply extrapolating the high-energy cross-section data of 19F(p, γ)20Ne down to the region of astrophysical interest, which can introduce large uncertainties, as shown in the present work, due to the absence of low-energy resonances [10]. In contrast, the (p, α) rate was determined with more reliable experimental data because of its larger cross-section [11-13]. It was pointed out that if this ratio was approximately 10 times larger than the currently adopted value, the observed Ca abundance at the oldest star, SMSS0313-6708, could be reproduced by the stellar models [7].
Despite the importance of the 19F(p, γ)20Ne reaction, experimental data within the Gamow window (Ec.m. = 76–146 keV) of Pop III stars’ hydrogen-burning temperatures (∼0.1 GK) is notably lacking due to the extremely low cross section of the 19F(p, γ)20Ne reaction at low energy. Previous experimental studies focused mainly on the energy range of Ec.m. > 300 keV, where the absolute cross section is higher [10, 14-20]. Even in this high-energy region, experimental data remain scarce, primarily because of the intricate challenges posed by the strong 6130 keV γ-ray background originating from the 19F(p,αγ)16O reaction.
Some early measurements used low-resolution and relatively small-volume NaI(TI) detectors to measure the > 11 MeV γ rays emitted from the primary transition to the first excited state of 20Ne(see Fig. 1)[14-17]. However, the energy resolution was insufficient to separate the primary transition γ rays from the 12.26 MeV pileup peak of the 19F(p,αγ)16O reaction; thus, large uncertainties may still exist. Here, the 12.26-MeV pileup peak originated from the 6130-keV γ rays (i.e., ‘γ2’ in Fig. 1) produced by the 19F(p, αγ)16O reaction, whose cross-section is ∼1000 times larger than that of the (p, γ) channel of present interest. When two 6130-keV γ rays are detected simultaneously within a single time window, a pileup peak around 12.26 MeV is produced. Subsequent advancements, such as the use of high-resolution Ge(Li) detectors, have provided improved measurement results, such as those by Subotic et al. [18] and Clifford [19]. However, detection limitations and uncertainties persist owing to low efficiency and restricted energy ranges. In Subotic et al., 24 cm3 and 36 cm3 Ge(Li) detectors and a 7.6 cm × 7.6 cm NaI(Tl) crystal were used to measure the excitation functions and angular distribution. It should be noted that the angular distribution was only measured for the resonance Ep = 1091 keV. Because of its low detection efficiency, this measurement was limited to the on-resonance region of Ep = 340–935 keV, which is much higher than the Ec.m. = 76–146 keV Gamow window of Pop III stars in the hydrogen-burning stage. Clifford’s measurement is similar to that of Subotic et al., but is limited to an even higher energy range of Ec.m. = 470–670 keV.
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Later, Couture et al. [10] from the University of Notre Dame developed a Q-value gating technique for measurement optimization with NaI and HPGe detectors. The NaI array was used to detect the high-energy primary transition to the 1.634-MeV first excited state of 20Ne, and the HPGe detector was used to detect the deexcited 1.634-MeV γ-rays(see Fig. 1). A sum energy gate of ≥ 10 MeV was applied to filter out most of the 6–7 MeV γ-rays from the concurrent (p, αγ) reactions. It is important to note that this technique is only sensitive to 1.634-MeV first excited state transitions; therefore, no direct transitions to the ground state of 20Ne were measured. The 19F(p, γ1)20Ne reaction was measured to be as low as Ec.m. ≈ 220 keV, but only the upper limits were given below Ec.m. ≈ 300 keV, which is still very far from the Ec.m. = 76–148 keV Gamow window of primordial stars.
The latest measurement by Williams et al. [20] was performed using the inverse kinematics technique at TRIUMF. This work focused on the Ec.m. = 323 keV resonance. A coincidence measurement of 20Ne recoils and scattered γ-rays was used to suppress the high-intensity γ-ray background of the 19F(p, αγ)16O reaction. The resonance branching ratio was determined for the first time in this study. The resonance strength was newly determined as
deBoer et al. [21] summarized all the available experimental data of the 19F + p system and performed a comprehensive R-matrix analysis to obtain newly evaluated 19F(p, γ)20Ne and 19F(p, α)16O rates. Their (p, γ)/(p, α) rate ratio was approximately four times lower than that of a previous NACRE estimation [11]. This smaller ratio reduces the mass fractions of Z > 9 elements in the hydrogen-burning process of massive Pop III stars and intensifies the Ca production problem [21]. Furthermore, the estimated uncertainty of the 19F(p, γ)20Ne rate below 0.1 GK was as large as two orders of magnitude due to the lack of experimental data below 300 keV. This highlights the need for measuring the 19F(p, γ)20Ne reaction at low energies. In the present experiment, this break-out reaction was directly measured in the energy region Ec.m. = 186–332keV, which is the lowest energy region achieved to date. The brief results have been published elsewhere [22]. Here, we report the full experimental results, including the detailed γ-ray spectra and branching ratios, the contribution of the previously expected 212.7 keV resonance, and plans for future work.
Experiment
The China Jinping Underground Laboratory (CJPL) [23] is located in the traffic tunnel of a hydropower station under Jinping Mountain, with a vertical marble rock overburden of approximately 2400 m. The CJPL is currently the deepest operational underground laboratory for particle and nuclear physics experiments worldwide. The cosmic-ray-induced background measured at the CJPL [24] was approximately two orders of magnitude lower than that of LUNA (1400-m-thick dolomite rocks) in Italy [25]. Therefore, Jinping Underground laboratory for Nuclear Astrophysics (JUNA) [26] has been increasingly promoted owing to its unique extra-low-background environment [27]. At JUNA, we successfully conducted a 19F(p, αγ)16O direct measurement campaign [28, 13] as a day-one experiment [29-34].
This 19F(p, γ)20Ne experiment was also conducted on the high-current 400-kV JUNA accelerator [35] at CJPL. A detailed diagram of the JUNA platform and the experimental setup is shown in Fig. 2. A proton beam from the accelerator was collimated by two apertures (ϕ15 mm upstream and ϕ12 mm downstream) and then impinged on a water-cooled target with a spot size of approximately 10 mm in diameter. For low-energy measurements away from the Ec.m. = 323.9 keV resonance, where the cross section was low and a high-intensity beam was used (I≈ 1 mA), the beam was undulated periodically over the target surface to reduce target damage. However, because of the limited space, a beam raster was not installed in the first-stage JUNA experiments. Alternatively, the beam was scanned by periodically changing the magnetic field of the beam deflector installed approximately 3 m upstream of the target. Accordingly, the intense beam was spread over a rectangular area of approximately 40 mm × 40 mm. For the energy region close to the 323.9-keV resonance, the beam current was reduced to 1–10 μA to reduce the pile-up of those strong 6130-keV γ rays from the 19F(p, αγ2)16O channel (see Fig. 1), and a beam-scanning system was not used. An inline Cu shroud cooled to the LN2 temperature was extended close to the target to minimize carbon build-up on the target surface. There was no sign of carbon buildup upon visual inspection of any of the targets during the experiment. Together with the target, the Cu shroud constituted a Faraday cup for beam charge integration. A negative voltage of 300 V was applied to the shroud to suppress the secondary electrons from the target. The beam-current error was estimated to be 1%, mainly because of Faraday cup leakage (typically < 10 nA) [36, 37]. Two strong and durable implanted 19F targets developed in recent years were used in this study. The targets were fabricated by implanting 40 keV 19F ions into 3-mm-thick high-purity Fe backing and then sputtering approximately 50-nm-thick Cr foils to further prevent fluorine material loss (see Refs. [38, 39]. The target characteristics were monitored by scanning the yield of the Ec.m. = 323.9 keV resonance attributed to the (p, α γ) channel (see Refs. [13, 22, 39] for details). The 19F target used for the 19F(p, γ) measurement was similar to that used in Ref. [36]. The target characterization is shown in Fig. 5 in Ref. [36]. In the present experiment, the target endured only 40 ℃ bombardment and could therefore be considered stable.
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A 4π BGO detector array specially designed for the JUNA project [26], which has already been used and characterized in previous studies [13, 22, 31, 30]), was used for γ-ray detection. The BGO array was composed of eight identical segments with a length of 250 mm and radial thickness of 63 mm, each covering a 45 ° azimuthal angle. For the 1634-keV γ-rays of interest, the coincidence efficiency was ≈14%, with an ≈10% energy resolution achieved via alcohol cooling of the BGO crystals (≈5 ℃). To suppress the natural γ-ray background emitted from the rocks and induced by the neutron capture reactions on the material around the detector (e.g., support structures and rocks), the BGO array was shielded with 5-mm copper, 100-mm lead, and 1-mm cadmium. A constant nitrogen gas flow was injected into the BGO array to eliminate radioactive radon gas and avoid vapor buildup on the cold BGO crystals. A detailed description of this BGO array can be found in Ref. [40].
The spectrum of the sum of the energies of all eight BGO segments (hereafter referred to as ‘sum’ spectrum) and the spectrum of the energy measured by each single segment (called ‘single’ spectrum) were obtained. Figure 3 shows seven typical γ-ray energy spectra obtained at beam energies of Ep = 210–362 keV. As in our previous work [13, 22], Ep denotes the proton beam energy before the Cr protective layer of the implanted fluorine target. The background peaks at 1460.8 keV (from 40K) and 2614.5 keV (from 208Tl), along with the 6130-keV peak from the 19F(p, αγ2)16O (i.e., the α2 channel) reaction, were used for energy calibration. Due to the high efficiency of the BGO array, only full energy peaks were observed in the ‘sum’ spectrum, and the single and double escape contributions are almost negligible. In addition, we observed γ-rays induced by the 12C, 13C, and 11B impurities from the target materials and beam apertures (see the lower panel in Fig. 3).
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Results
The 19F(p, γ)20Ne reaction is mainly dominated by decay through the first excited state (i.e., (p, γ1)) and the ground state (i.e., (p, γ0)) transitions [10, 20]. Therefore, a coincidence gating technique [22, 31, 30] was developed to analyze the data. By gating the ∼13000-keV peak in the ‘sum’ spectrum (see Fig. 3), which corresponds to the total reaction energy (i.e., Q-value plus incident energy), the 1634-keV peak can be clearly seen in the ‘single’ spectrum. As opposed to the ‘sum’ peak, which represents the total reaction energy, this gated ‘single’ spectrum reflects more individual transitions due to the smaller azimuthal angles (45 °) covered by each BGO segment. The count of this 1634-keV peak was analyzed and used to calculate the 19F(p, γ1)20Ne contribution [22]. The gate ranges were adjusted for each energy point to minimize fitting errors. Moreover, the gated ‘single’ spectrum is very sensitive to the decay routines. By reproducing this gated spectrum using the Geant4 simulation [41], the relevant γ-transition branching ratios and coincidence efficiency were determined for each energy point. Besides, it is possible for the 1634-keV γ-ray to enter a single BGO crystal simultaneously with other cascade γ rays, which is known as the “summing effect.” This results in the presence of a sum of two energies on the ‘single’ spectrum, which affects the true counts of the 1634-keV γ-ray. For the ‘single’ spectrum with Ep = 250 keV, the summing effect accounted for approximately 16%. This effect is considered in Geant4 when calculating the absolute efficiency. The ∼13000-keV peak in the ‘sum’ spectrum includes the contributions from both the (p, γ0) and (p, γ1) branches. The (p, γ0) branch yields were determined by subtracting the (p, γ1) contribution determined above from the sum of the ∼13000-keV peak, that is, (p, γtot), after correcting for the respective energy-dependent efficiency values. The experimental data for the (p, γ0) and (p, γ1) yields are reported in Ref. [22]. Figure 4 shows the yield ratios of (p, γ0) and (p, γtot) obtained in the energy region of Ep = 280–360 keV. Here, the error bars indicate statistical significance. In general, this ratio is constant at ≈26.5%, as indicated by the solid line in Fig. 4. In other words, the (p, γ1) branch dominated the entire energy region measured in this study, whereas the (p, γ0) branch contributed only ≈26.5% over the energy region shown in the figure. The total ≈5.2% error band shown, including systematic and statistical errors, was calculated using Eq. 1. The systematic error comes mainly from the respective 11.5% and 4.7% relative errors of the (p, γ1) and (p, γ0) channels, which stems mainly from the detection efficiency uncertainty simulated by Geant4, which in turn results mainly from the uncertainty of the adopted branching ratio. The average statistical error of the eight data points shown in the figure is adopted as the statistical error (i.e., ≈3.97%). The coincidence efficiency was obtained through Geant4 simulations, which were verified using two standard 60Co and 137Cs sources. The uncertainty of the γ-ray energy difference in the Geant4 simulations between the radioactive sources and the (p, γ1) reaction is far less than the branching ratio uncertainty. In addition, it should be noted that the (p, γ0) contribution cannot be determined reliably for the two energy points at Ep=210 and 220 keV because of serious 11B contamination and the statistics; here, we roughly estimate its contribution at ∼26%, which is consistent with the trend shown for the non-resonant-energy region (see Fig. 4). Furthermore, no noticeable (p, γ0) contribution was observed over the newly observed resonance.
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In this experiment [22], a key resonance was discovered at Ec.m. = 225.2 keV in the (p, γ) channel for the first time. This corresponds to the Ex = 13.069 MeV (3-) excited state in 20Ne, which has already been observed in the (p, αγ) channel [12, 39, 13, 36]. Its strength is determined by integrating its yield curve AY [42]:
G.S. | 1.634 MeV | 4.248 MeV | 4.967 MeV | |
---|---|---|---|---|
225.2 | - | 62% | 35% | 3% |
323.9 | 34% | 45% | - | 21% |
For the 323.9-keV (p, γ) resonance, only five energy points were measured owing to the limited beam time (see Fig. 1a in Ref. [22]), which is insufficient for obtaining a perfect yield curve. Instead, the (p, γ) strength was determined by directly comparing the corresponding (p, γ1) and (p, γ0) yields with the (p, αγ2) yields using Eq. 2. For the 323.9-keV resonance, three reaction channels–(p, γ0), (p, γ1), and (p, αγ2)–were measured at five energy points near the resonance. Therefore, the resonance strength ratio of these three channels is equal to the ratio of their γ-ray yields to the corrected detection efficiency. The (p, αγ) strength was previously determined as
Regarding the previously expected Ec.m. = 212.7 keV (corresponding to the Ex = 13.056 MeV (2-) excited state) resonance, which was always thought to dominate the (p, γ) reaction rate at low temperature below ∼0.26 GK, the estimates placed the upper limits on its strength at 1.3 [11], 0.93 [10] and 0.83 μeV [21]. The contribution of this resonance was investigated by assuming different strengths relative to those of the 225.2-keV resonance, as shown in Fig. 5. Four strengths, 0%, 1%, 5%, and 10%, relative to that of
For the non-resonant-energy region, the product of the number of 19F atoms and the absolute efficiency of the BGO detector was determined via the (p, αγ) yield over the Ec.m. = 323.9 keV resonance [36, 22]. Using this method, the astrophysical S-factors of the 19F(p, γ)20Ne reaction were calculated using this product and the γ-ray yields, as shown in Fig. 1b in Ref. [22]. The systematic uncertainty of the S-factors includes: (i) a 5% uncertainty estimated for the Geant4 simulation by assuming a 0.5-keV uncertainty in the reconstructed Ec.m. energy; (ii) a 3.9% uncertainty of the 323-keV resonance strength (from the normalization); and (iii) a 5%–-10% uncertainty of the 1634-keV γ-ray coincidence efficiency. From this, we conservatively estimate an overall systematic uncertainty of ∼12%.
R-matrix analysis
A multi-level, multi-channel R-matrix analysis of the 20Ne system near the proton separation energy [21] using the AZURE2 code [43] was used to reproduce the experimental data (see Fig. 7). Because of off-resonance data scarcity, owing to the limited beam time and the rather high-level density, which may not be fully known, there is some ambiguity regarding the underlying reaction components that produce a fairly constant S-factor at the lowest energies. For example, as shown in Fig. 7, the trend of the experimental data can be reproduced using the high-energy tail of either a very-low-energy resonance or a subthreshold resonance. Furthermore, the level density in this energy region is sufficiently high such that there are several subthreshold state candidates, any of which, or a combination thereof, can equally reproduce the observed energy dependence. Moreover, the total threshold resonance width has large uncertainties [12, 21]. If the width is near its upper limit, a high-energy tail can significantly enhance the low-energy S-factor.
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Under the above assumptions, Bayesian uncertainty analysis (see Extended Data Fig. 4 in Ref. [22]) was performed using the Python package BRICK [44]. BRICK acts as a mediator, allowing communication between the Python MCMC sampler emcee [45] and the C++ R-matrix code AZURE2. This analysis was used to estimate the uncertainty of the low-energy S-factor.
The phenomenological R-matrix is not a predictive theory. Instead, it relies on a presupposed knowledge of the level structure. When this information is incomplete, it translates into large uncertainties that must be estimated based on the theoretical limits of the resonance parameters. While not indicated in Fig. 7, additional resonance contributions are possible given the high density of 20Ne at these energies [46]. These resonances could be broad, corresponding to those observed in 16O(α,α)16O data [47, 48], but could also be narrow, such as the one reported here at 225.2 keV. If so, further enhancement of the S-factor would be possible; accordingly, further low-energy studies are highly encouraged.
Reaction Rate
The astrophysical S-factors obtained by the R-matrix fitting were used to calculate the thermonuclear 19F(p, γ)20Ne reaction rate (see Fig. 2 in Ref. [22]), which is not repeated here. As discussed in the Introduction, the ratio of the 19F(p, γ)20Ne and 19F(p, αγ)16O reaction rates influences Ca production in Population III stars. Figure 6 shows the corresponding rate ratios and associated uncertainties.
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The mean value (solid line) and upper and lower limits (boundary of the colored band) were calculated using the adopted/adopted, highlow, and low/high combinations of the corresponding (p, γ) and (p, α) rates. At the hydrogen-burning temperature ∼0.14 GK of first stars of interest, the (p, γ)/(p, α) ratio (mean value) is 8.7×10-4, which is approximately 6.4 and 18.3 times larger than the NACRE [11] and deBoer et al. [21] estimations, respectively.
This significantly enhanced new ratio leads to a much stronger break-out from the CNO cycles to the heavier mass region, as far as the doubly magic isotope 40Ca. Here, the typical temperature of these oldest stars is approximately four times warmer than that of modern massive stars, and may thus be considered as a “warm" CNO cycle (see the Supplemental Materials in Ref. [22]). Therefore, the observed Ca abundance in the oldest star known to date, SMSS0313-6708, can be reproduced using this new ratio (see Fig. 3 in Ref. [22]). Furthermore, 19F(p, γ)20Ne is the only reaction that can remove the catalytic material from the cycle at low temperatures, causing an irreversible flow from the CNO to the NeNa region, because back-processing via 22Ne(p, α)19F is not energetically possible. Thus, this break-out permanently removed the catalytic material from the CNO cycles and significantly changed the energy-production rate and stellar lifetime for hydrogen burning [5, 22].
Summary
This paper reports the full experimental results for the astrophysical important 19F(p, γ)20Ne reaction. The measurement directly reached the lowest energy region of Ec.m. ≈ 186–332 keV, relying on the extra-low background deep underground environment, as well as the extensive proton beam from the JUNA facility. A gating technique was developed to determine the 19F(p, γ)20Ne yield. The astrophysical S-factors were obtained from an R-matrix analysis along with MCMC Bayesian uncertainty estimation. A new resonance at Ec.m. = 225.2 keV was observed, and its resonance strength was precisely determined to be
Figure 7 shows the present 19F(p, γ1)20Ne astrophysical S-factors (upper panel) and cross-sections (lower panel), along with the three most probable R-matrix fitted curves [22]. The Gamow window shown for this break-out reaction is located at Ec.m. ≈ (112±36) keV for the Pop III stars, typical temperature of ≈0.1 GK. Because of the limited beam time, the present two lowest data (within the red circle) still have ∼30% statistical error, and the predicted S-factor uncertainty by the R-matrix fits is as large as a factor of approximately 1.8 at the Gamow peak. Therefore, it is necessary to measure this reaction directly down to the Gamow window. Thus, a reaction rate around 0.1 GK of astrophysical importance and the properties of the Ec.m. = 11 keV near-threshold resonance can be constrained more strictly based on solid experimental ground.
It is expected that the cross section will exhibit an exponential decline with decreasing beam energy; for example, the cross section will decrease to 10-14 ∼ 10-11 b within the Gamow window; therefore, the 11B contamination in the implanted 19F target, with a much larger (p, γ) cross section, will become the main obstacle. Recently, we built a new target-making device on an electromagnetic isotope separator [49], in which a 180 ° analyzing magnet and an LN2 cold trap were applied to reduce contamination during implantation. Moreover, to reduce boron contamination in the Fe backing, a high-purity Fe coating is now magnetron-sputtered onto the original Fe backing, and such an additional coating can effectively reduce boron contamination. Preliminary results show that 11B contamination in new targets can be reduced by more than a factor of 10 [50].
In a future JUNA experiment, we will use the newly developed implanted targets and the new 4π BGO array to extend the 19F(p, γ)20Ne measurements directly to the Gamow window. Additional experimental data over the 212.7-keV resonance will be acquired to accurately characterize its strength. These precise experimental data will be very helpful for understanding the nucleosynthesis and evolution of first stars in our early Universe, as the observation of first stars is one of the key mission targets of the James Webb Space Telescope (JWST) [51]. Furthermore, as shown in Fig. 6, the present (p, γ)/(p, α) rate ratio is approximately 200 times larger than the NACRE estimation at temperatures of approximately 0.01 GK. This strikingly enhanced break-out may have important astrophysical implications, and the impact of our reported rate on novae, X-ray bursts, asymptotic giant branch (AGB) stars, and other stellar sites is still the subject of future research.
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