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Let us estimate the γ activity of isomeric nuclei excited according to the given scheme. Let the density of the
$ ^{229} $ Th nuclei in the target sample at depth x be$ n_{\rm{gr}}(x,t) $ , and the density of the resulting$ ^{229m} $ Th isomers be$ n_{\rm{is}}(x,t) $ . The equations describing the system are as follows:$ \begin{aligned}[b] {\rm d}n_{\rm{is}}(x,t)/{\rm d}t=&\sigma \varphi n_{\rm{gr}}(x,t) - (\lambda_{\rm{tot}}(x)+\tilde{\sigma} \varphi) n_{\rm{is}}(x,t),\\ {\rm d}n_{\rm{gr}}(x,t)/{\rm d}t=&-\sigma \varphi n_{\rm{gr}}(x,t) + (\lambda_{\rm{tot}}(x)+\tilde{\sigma} \varphi) n_{\rm{is}}(x,t), \end{aligned} $
(1) where σ is the isomer excitation cross section for inelastic electron scattering in the process of
$ ^{229} $ Th$ (e,e') $ $ ^{229m} $ Th,$ \tilde{\sigma} $ is the cross section of the reverse process (calculated from the principle of detailed balance and coincides in order of magnitude with σ [10]),$ \varphi=j/S $ is the electron flux density through a target with area S when passing the current j, and$ \lambda_{\rm{tot}}(x) $ is the total decay constant or isomeric state width (with using the unit system$ \hbar=c=1 $ ) in the sample at depth x. The expressions in Eq. (1) are solved with initial conditions$ n_{\rm{is}}(x,0)=0 $ and$ n_{\rm{gr}}(x,0)=n_{\rm{gr}}(x) $ . It should also be noted that the electron flux density of a given energy φ is practically independent of x due to the small thickness of the dielectric layer.Let us simplify Eq. (1). 1) We neglect the decrease in the density of the
$ ^{229} $ Th nuclei in the ground state with time, that is, let$ n_{\rm{gr}}(x,t)=n_{\rm{gr}}(x) $ . 2) We discard the term$ -\tilde{\sigma} \varphi n_{\rm{is}}(x,t) $ , which describes the inverse process$ ^{229m} $ Th$ (e,e') $ $ ^{229} $ Th of nuclei deexcitation during inelastic electron scattering. These simplifications are to be made as the condition$ \sigma \varphi \tau \ll 1 $ is met for the considered current density of the order of 1 A cm$ ^{-2} $ (in this case,$ 1/(\sigma \varphi) \gtrsim 10^6 $ s) and the expected lifetime of the isomeric state$ \tau(x) = 1/\lambda_{\rm{tot}}(x) \simeq 10^2 $ –$ 10^3 $ s (see below). On the one hand, this condition implies that the main decay channel for$ ^{229m} $ Th is the spontaneous decay of the isomeric level, and not the transition to the ground state upon inelastic electron scattering. On the other hand, the density of the excited$ ^{229m} $ Th nuclei at depth x increases according to the characteristic law$ n_{\rm{is}}(x,t)=n_{\rm{gr}}(x) \frac{\sigma \varphi}{\lambda_{\rm{tot}}(x)} \left(1-{\rm e}^{-\lambda_{\rm{tot}}(x)t} \right), $
(2) where
$ \sigma \varphi/ \lambda_{\rm{tot}}(x) $ is the relative equilibrium concentration of isomeric nuclei at depth x at times$ t\gg \tau $ . In order of magnitude,$ \sigma \varphi/ \lambda_{\rm{tot}}(x)\simeq 10^{-4} $ , and density$ n_{\rm{gr}}(x) $ does not change much with time.Now let us return to the question of the value
$ \tau(x) $ . For this, we first estimate the characteristic radiative width of the isomeric state$ \Gamma_{\gamma} $ in vacuum$ \Gamma_{\gamma}=10\omega_{\gamma}^3\mu_N^2 B_{\rm{W.u.}}(M1, {\rm{is}}\rightarrow {\rm{gr}}), $
where
$ \mu_N $ is the nuclear magneton, and$ M1 $ is the multipolarity of isomeric transition.In order to calculate
$ \Gamma_{\gamma} $ , it is necessary to know the reduced probability of nuclear transition in Weiskopf units$ B_{\rm{W.u.}}(M1, {\rm{is}}\rightarrow {\rm{gr}}) $ . In Ref. [58], the value$ B_{\rm{W.u.}}(M1, {\rm{is}}\rightarrow {\rm{gr}}) = 0.03 $ was obtained based on experimental data [59–62] for the$ M1 $ transitions between the rotation bands$ K^{\pi}[Nn_z\Lambda] = 3/2^+[631] $ and$ 5/2^+[633] $ in the$ ^{229} $ Th nucleus and the Alaga rules [58, 63]. Here,$ K^{\pi}[Nn_z\Lambda] $ are the asymptotic quantum numbers for nuclear levels in the Nilsson model [64]). The other value,$ B_{\rm{W.u.}}(M1, {\rm{is}} \rightarrow {\rm{gr}}) = 0.006-0.008 $ , was obtained in Ref. [65]. It was the result of a computer calculation made in compliance with modern nuclear models. These two values for$ B_{\rm{W.u.}}(M1, {\rm{is}}\rightarrow {\rm{gr}}) $ give the time interval$ T_{1/2}=\ln(2)/\Gamma_{\gamma}= $ 20–100 min for the radiative decay of the isomer in thorium ions in vacuum at the nuclear transition energy$ \omega_{\gamma}=E_{\rm{is}}=8.2 $ eV.The probability of decay of the
$ ^{229m} $ Th isomer in the sample in Fig. 1 is influenced by two factors — the refractive index of the medium [45, 53] and the presence of interfaces between the media (the Purcell effect) [37]. The probability of magnetic dipole ($ M1 $ ) γ radiation of$ ^{229m} $ Th in a medium with a refractive index n increases by$ n^3 $ times compared to the probability of radiation in vacuum [45,53]. The Purcell factor,$ f_P(x) $ , that is the ratio of the probability of emission in a medium with boundaries to the probability of emission in an infinite medium, affects the decay of$ ^{229m} $ Th more intricately. Figure 2 shows the Purcell factors for the$ M1 $ γ transition with the energy of 8.2 eV for the system shown in Fig. 1. The calculation was made within the framework of the approach developed and described in detail in Ref. [66] (we provide a graphical representation of the result, since the analytic expressions for$ f_P(x) $ for four media are highly complex). Pd and Au were taken as examples of the deposited metal contact. Their characteristics, namely,$ n=1.3 $ and$ \kappa=0.9 $ for Pd and$ n=1.3 $ and$ \kappa=1.5 $ for Au at the energy of 8.2 eV, are given in Ref. [67]. The thickness of the Pd or Au layers is estimated to be equal to 10 nm. It is limited by the requirement of contact transparency for VUV photons. The fraction of the incident power, propagated through the material with thickness d, is given by exp(-$ d/l_0 $ ), where$ l_0=\lambda_{\rm{is}}\kappa/(4\pi) $ and$ \lambda_{\rm{is}} \approx 150 $ nm. Using the values of κ for Pd and Au from Ref. [67] given earlier, we find that, in a metal layer of thickness 10 nm, the VUV photon flux is attenuated by a factor of approximately 3 for Pd and 2 for Au.Figure 2. (color online) The radiative,
$ f_P^{\rm{r}}(x) $ , nonradiative,$ f_P^{\rm{nr}}(x) $ , and total,$ f_P^{\rm{tot}}(x)= f_P^{\rm{r}}(x)+f_P^{\rm{nr}}(x) $ components of the Purcell factors for the$ M1 $ (8.2 eV) γ transition in the scheme in Fig. 1 with$ h=15 $ nm for thickness of the large band gap dielectric and 10 nm metal layer thickness. The thickness of the substrate in calculations is assumed to be infinite. Solid lines — the Si/$ ^{229} $ Th:SiO$ _2 $ /Pd sample and dashed lines — the Au/$ ^{229} $ Th:MgF$ _2 $ /Au sample.At the SiO
$ _2 $ /Metal interface, there are surface states whose levels are located inside the SiO$ _2 $ band gap. The presence of these levels can lead to an increase in the probability of the isomeric decay of$ ^{229m} $ Th through the internal conversion or electron bridge for the thorium atoms located within 2–3 monolayers from the interface. Additional losses in the photo output can be avoided by lowering the concentration of thorium atoms in the near-surface layer so that the doping profile reaches a maximum at a depth of approximately 1 nm (of the order of 3 coordination radii). In the case of a uniform distribution of$ ^{229} $ Th, this problem will affect 10–15% of the nuclei, reducing the optical output by the same amount.Figure 2 shows the probability of radiative decay determined by
$ f_P^{\rm{r}}(x) $ to decrease due to the interfaces Pd/SiO$ _2 $ ($ x=0 $ ) — SiO$ _2 $ /Si ($ x=h $ ) and Au/MgF$ _2 $ ($ x=0 $ ) — MgF$ _2 $ /Au ($ x=h $ ). However, the total decay probability increases significantly due to the factor$ f_P^{\rm{nr}}(x) $ . It characterizes the nonradiative decay of$ ^{229m} $ Th, which arises from the imaginary part of the dielectric constants of Si, Pd, and Au [66]. As for the silicon oxide, the imaginary part of the dielectric constants of SiO$ _2 $ lies in the range of 0.02–0.03 at the energy of 8.2 eV [68, 69]. Thus, κ is very small for SiO$ _2 $ , and it can be neglected in calculations. For MgF$ _2 $ $ \kappa \approx 3\times10^{-7} $ at 8.2 eV [68].With respect to these factors, it is possible to derive the formula for the total γ activity caused by an electric current in the entire sample
$ \begin{equation*} Q_{\gamma}(t)=\sigma \varphi S \int_0^h{} {\rm d}x\, n_{\rm{gr}}(x) \frac{f_P^{\rm{r}}(x)}{f_P^{\rm{tot}}(x)} \left(1- {\rm e}^{-\lambda_{\rm{tot}}(x) t}\right) , \label{eq:Q_gamma(t)} \end{equation*} $
where
$ \lambda_{\rm{tot}}(x)=n^3 f_P^{\rm{tot}}(x) \Gamma_{\gamma} $ .Figure 3 shows the graphs of induced activity.
$ Q_{\gamma} $ for the sample from Fig. 1 is seen to behave much more differently than the γ activity of an equivalent target of$ ^{229} $ Th$ ^{+,++...} $ ions in vacuum or in an infinite medium of SiO$ _2 $ or MgF$ _2 $ . Both the emissivity and the observed effective half-life of the entire set of isomeric nuclei change significantly.Figure 3. (color online) The γ-activity of the sample per 1 A of electric current and per 1 ng of
$ ^{229} $ Th as a function of the irradiation time. 1 — the$ ^{229} $ Th$ ^{+,++...} $ ion target in vacuum, 2 (2') — the same target in the infinite medium of SiO$ _2 $ (MgF$ _2 $ ), 3 (3') — the$ ^{229} $ Th target in the Si/Th:SiO$ _2 $ /Pd (Au/Th:MgF$ _2 $ /Au) sample in Fig. 1 with a uniform distribution of nuclei in depth$ n_{\rm{gr}}(x)={\rm{Const}}=N_{\rm{gr}}/(hS) $ ($ N_{\rm{gr}} $ is the total number of$ ^{229} $ Th nuclei implanted in a dielectric layer), 4 (4') — all the$ ^{229} $ Th nuclei located in a thin layer inside SiO$ _2 $ (MgF$ _2 $ ) at a depth of$ x\approx 6 $ nm, where the functions$ f_P^{\rm{nr}}(x) $ have a minimum value (this is a type of upper limit for the γ-activity for the sample in Fig. 1).As can be seen from Fig. 3, gamma activity in the sample upon reaching equilibrium at times
$ t\approx{} T_{1/2}/2 $ is approximately$ 10^5 $ photons/s per 1 A of electric current and 1 ng of$ ^{229} $ Th.$ ^{229} $ Th is an α emitter with$ T_{1/2} = 7880 $ yr. Alpha particles, decelerated in SiO$ _2 $ (MgF$ _2 $ ), produce a background radiation. Alpha activity of 1 ng of$ ^{229} $ Th is 7 Bk. The mean free path of α particles with the energy 4–5 MeV in SiO$ _2 $ (MgF$ _2 $ ) is approximately 20 μm. With a dielectric layer thickness of 15 nm, only$ 10^{-3} $ α particles lose energy in the dielectric and contribute to the background (alpha particles in the Si (Au) substrate and metal contacts do not produce an optical background). Assuming that the ionization potential is 10 eV, and that all energy of the alpha particles is converted into photons, we get a background of approximately$ 10^3 $ photons per second, per 1 ng of$ ^{229} $ Th purified from daughter nuclides. This means that we can secure two orders of magnitude for current, until the signal falls to the background level.Let us compare this estimate with the background from
$ ^{233} $ U. To have the same number of the 8.2 eV γ quanta as from 1 ng of$ ^{229} $ Th, the α activity of$ ^{233} $ U should be at the level of$ 10^5\times $ 50 (taking into account the 2% isomer population). This requires approximately 140 mg$ ^{233} $ U. In this case, the host crystal will have a volume of at least$ 10^{-1} $ cm$ ^3 $ . Alpha particles will be completely decelerated in such a crystal and leave all their energy in it. Thus, other things being equal, the background for$ ^{233} $ U exceeds the estimate obtained for 1 ng$ ^{229} $ Th by 8 orders of magnitude. This underlies the advantage of using the proposed scheme with thorium.Another source of the background radiation could be the electron flux through the carrier substrate. In this case, the radiation in the vacuum ultraviolet range comes from the processes of exciton recombination. In experiments specifically carried out in 2021, it has been found that, in the Si substrate and SiO
$ _2 $ matrix, the emerging background in the wavelength region around 150 nm is very small and only slightly exceeds the intrinsic noise of the detector [70].The emission line from the isomeric decay of
$ ^{229m} $ Th is planned to be registered using the same setup that was used to measure the background. The setup device is as follows. A converging short-focus lens made of a material transparent in the VUV range (MgF$ _2 $ ) is placed in front of the sample. A focused beam of light falls on the slit of a diffraction spectrometer. The spectrometer is made according to the Paschen-Runge optical scheme, in which the entrance slit of the spectrometer and the spherical diffraction grating are located on the Rowland circle, and the radiation from the entrance slit falls almost normal to the diffraction grating. This scheme has the following advantages: 1 - only one reflection is used, which makes it possible to minimize the loss of incoming radiation; 2 - it is possible to change the grating tilt to capture the desired part of the spectrum, which allows us to measure spectra in a wide range.The background spectrum and the
$ ^{229m} $ Th radiation wavelength are determined from the diffraction pattern using a charged-coupled device (CCD) matrix cooled to a temperature of -20$ ^{\circ} $ C under vacuum conditions no worse than$ 10^{-8} $ Torr. With the CCD matrix, we can accumulate the signal simultaneously (without scanning) over all channels of the selected region of the spectrum, which in turn allows for measuring the emission spectrum with a high decay rate over time. The maximum luminosity of the spectrometer reaches$ 10^4 $ (i.e., one photon is registered out of every$ 10^4 $ photons arriving at the spectrometer input).The experiment can be carried out in two modes. (1) Registration and measurement of the spectrum occur directly during the passage of electric current through the sample. (2) Registration occurs after the electron current is turned off and after the completion of the relaxation of electron-hole pairs and other transient processes — the background sources. In both modes of operation, to take into account the background correctly, it is necessary to carry out measurements on samples without
$ ^{229} $ Th. Such a scheme allows us to separate photons originating during the decay of the$ ^{229m} $ Th isomer from the contributions of all other possible electronic transitions in the Th shell. The background accumulation time is required to correspond to the useful signal accumulation time (see Fig. 3), i.e., approximately$ 10^3 $ s. The described sequential consideration of the signal from samples with$ ^{229} $ Th and$ ^{232} $ Th will single out the desired emission line of the$ ^{229m} $ Th isomer.Consider the size of the sample in Fig. 1 in terms of the allowable concentration of the thorium atoms. Let us take SiO
$ _2 $ as an example, since we have all necessary data for it. According to the results of Ref. [71], where thorium ions are implanted into SiO$ _2 $ , thorium is oxidized to the ThO$ _2 $ form. The ThO$ _2 $ band gap is approximately 6.5 eV. Therefore, the appearance of the ThO$ _2 $ impurity in SiO$ _2 $ leads to a decrease in the band gap of the sample as a whole. It was theoretically and experimentally established in Ref. [71] that, up to a thorium concentration of 20%, the band gap in such SiO$ _2 $ +ThO$ _2 $ dielectrics exceeds 8.5 eV. Thus, in a dielectric matrix of the size 1 cm$ ^2\times $ 15 nm, approximately 10 ng of$ ^{229} $ Th can be placed (note that, in the theoretical work of a group from the Vienna University of Technology, it has been found that the band gap of thorium-doped MgF$ _2 $ decreases with the concentration of thorium [56].)As a result, we obtain the following estimate: at a moderate current of 1 A, detector quantum efficiency
$ \gtrsim 10^{-1} $ , and photon collection angle$ \approx 2\pi $ , the γ radiation detector registers approximately$ 10^4 $ –$ 10^5 $ counts/s from such a matrix, which is sufficient for the effect to be reliably detected above the background level.
Proposal for a nuclear light source
- Received Date: 2022-10-08
- Available Online: 2023-02-15
Abstract: This study considers a principal possibility of creating a nuclear light source of the vacuum ultra violet (VUV) range based on the