Isomer Excitation Research Articles

Laser-based approach to measure small nuclear cross sections in plasma

We demonstrate an approach successfully measuring very small nuclear isomeric excitation cross sections (on the order of 10 to 100 picobarns) via laser-cluster interaction. The interaction between an intense laser pulse and Kr atomic clusters generates a high-temperature and high-density plasma ball in which nuclear excitations are facilitated by inelastic electron scattering. The electron temperature reaches several hundred keV (corresponding to 10[Formula: see text] K), similar to a stellar environment. The very small nuclear excitation cross sections are extremely challenging to measure otherwise, for example using traditional accelerator-based approaches. Our method opens a broad avenue of measuring small nuclear cross sections and holds promise for advancing understanding of nuclear transition mechanisms and exploring pathways in the evolutionary dynamics of elements within stellar environments.

Controlling 229Th isomeric state population in a VUV transparent crystal

The radioisotope thorium-229 (229Th) is renowned for its extraordinarily low-energy, long-lived nuclear first-excited state. This isomeric state can be excited by vacuum ultraviolet (VUV) lasers and 229Th has been proposed as a reference transition for ultra-precise nuclear clocks. To assess the feasibility and performance of the nuclear clock concept, time-controlled excitation and depopulation of the 229Th isomer are imperative. Here we report the population of the 229Th isomeric state through resonant X-ray pumping and detection of the radiative decay in a VUV transparent 229Th-doped CaF2 crystal. The decay half-life is measured to 447(25) s, with a transition wavelength of 148.18(42) nm and a radiative decay fraction consistent with unity. Furthermore, we report a new “X-ray quenching” effect which allows to de-populate the isomer on demand and effectively reduce the half-life. Such controlled quenching can be used to significantly speed up the interrogation cycle in future nuclear clock schemes.

Isomeric Excitation Energy for ^{99}In^{m} from Mass Spectrometry Reveals Constant Trend Next to Doubly Magic ^{100}Sn.

The excitation energy of the 1/2^{-} isomer in ^{99}In at N=50 is measured to be 671(37)keV and the mass uncertainty of the 9/2^{+} ground state is significantly reduced using the ISOLTRAP mass spectrometer at ISOLDE/CERN. The measurements exploit a major improvement in the resolution of the multireflection time-of-flight mass spectrometer. The results reveal an intriguing constancy of the 1/2^{-} isomer excitation energies in neutron-deficient indium that persists down to the N=50 shell closure, even when all neutrons are removed from the valence shell. This trend is used to test large-scale shell model, abinitio, and density functional theory calculations. The models have difficulties describing both the isomer excitation energies and ground-state electromagnetic moments along the indium chain.

Theory of isomeric excitation of 229Th via electronic processes

A unified theoretical framework is presented for the isomeric excitation of the 229Th nucleus via electronic processes. These processes include nuclear excitation by electron transition (NEET), nuclear excitation by electron capture (NEEC), and nuclear excitation by inelastic electron scattering (NEIES). Detailed calculation results on the excitation rate and the excitation cross section are presented.

Excitation and probing of low-energy nuclear states at high-energy storage rings

$^{229}\mathrm{Th}$ with a low-lying nuclear isomeric state is an essential candidate for a nuclear clock as well as many other applications. Laser excitation of the isomeric state has been a long-standing goal. With relativistic $^{229}\mathrm{Th}$ ions in storage rings, high-power lasers with wavelengths in the visible range or longer can be used to achieve high excitation rates of $^{229}\mathrm{Th}$ isomers. This can be realized through direct resonant excitation or excitation via an intermediate nuclear or electronic state, facilitated by the tunability of both the laser-beam and ion-bunch parameters. Unique opportunities are offered by highly charged $^{229}\mathrm{Th}$ ions due to the nuclear-state mixing. The significantly reduced isomeric-state lifetime corresponds to a much higher excitation rate for direct resonant excitation. Importantly, we propose electric dipole transitions changing both the electronic and nuclear states that are opened by the nuclear hyperfine mixing. We suggest using them for efficient isomer excitation in Li-like $^{229}\mathrm{Th}$ ions, via stimulated Raman adiabatic passage or single-laser excitation. We also propose schemes for probing the isomers, utilizing nuclear radiative decay or laser spectroscopy on electronic transitions, through which the isomeric-state energy can be determined with an orders-of-magnitude higher precision than the current value. The schemes proposed here for $^{229}\mathrm{Th}$ could also be adapted to low-energy nuclear states in other nuclei, such as $^{229}\mathrm{Pa}$.

Observation of the radiative decay of the 229Th nuclear clock isomer.

The radionuclide thorium-229 features an isomer with an exceptionally low excitation energy that enables direct laser manipulation of nuclear states. It constitutes one of the leading candidates for use in next-generation optical clocks1-3. This nuclear clock will be a unique tool for precise tests of fundamental physics4-9. Whereas indirect experimental evidence for the existence of such an extraordinary nuclear state is substantially older10, the proof of existence has been delivered only recently by observing the isomer's electron conversion decay11. The isomer's excitation energy, nuclear spin and electromagnetic moments, the electron conversion lifetime and a refined energy of the isomer have been measured12-16. In spite of recent progress, the isomer's radiative decay, a key ingredient for the development of a nuclear clock, remained unobserved. Here, we report the detection of the radiative decay of this low-energy isomer in thorium-229 (229mTh). By performing vacuum-ultraviolet spectroscopy of 229mTh incorporated into large-bandgap CaF2 and MgF2 crystals at the ISOLDE facility at CERN, photons of 8.338(24) eV are measured, in agreement with recent measurements14-16 and the uncertainty is decreased by a factor of seven. The half-life of 229mTh embedded in MgF2 is determined to be 670(102) s. The observation of the radiative decay in a large-bandgap crystal has important consequences for the design of a future nuclear clock and the improved uncertainty of the energy eases the search for direct laser excitation of the atomic nucleus.

Isomeric Excitation of ^{229}Th in Laser-Heated Clusters.

We consider theoretically isomeric excitation of ^{229}Th in a laser-heated cluster. A ^{229}Th cluster is first radiated by an intense femtosecond laser pulse, causing ionization of the constituting atoms. The cluster will then survive for a time on the order of 1ps, during which the electrons collide with the nuclei repeatedly and excite them to the isomeric state. Two mechanisms are responsible for the isomeric excitation: nuclear excitation by electron capture (NEEC) and nuclear excitation by inelastic electron scattering (NEIES). By changing the laser intensity, one can tune between NEEC and NEIES continuously. This laser-heated-cluster scheme not only provides a highly efficient means for isomeric excitation, but also provides an approach for the confirmation of the NEEC process, which has been predicted for over forty years without conclusive experimental verifications.

Quasiclassical theory of Th229m excitation by laser pulses via electron bridges

In the quasiclassical approximation it is studied excitation of the 8.2 eV isomer $^{229m}\mathrm{Th}$ in the electron bridges (EB), initiated by a laser pulse. While the nucleus and atomic electron are treated quantum mechanically, the laser pulse is described by a time-dependent wave packet, formed by classic electromagnetic waves. Two types of the EB are taken into consideration: via the continuous electron spectrum and via discrete atomic levels. In calculations of the excitation probability of $^{229m}\mathrm{Th}$ by a laser pulse I employ the generalized formalism of Floquet functions, which allows one to solve the time-dependent Schr\"odinger equation by the methods of stationary scattering theory. The task is solved for weak lasers as well as for the conventional lasers of arbitrary intensity. In the first case the results well correlate with those obtained previously when treating the laser pulse as a bunch of uncorrelated photons. If conventional lasers generate EB through an atomic level, its population suffers Rabi oscillations. Therefore application of the $\ensuremath{\pi}$ pulses may strongly enhance the effect of the isomer excitation. For the same EB the excitation probability of the isomer as a function of the laser carrier frequency is shown to have two peaks associated with two resonant levels.

Skyrme–Hartree–Fock–Bogoliubov mass models on a 3D mesh: II. Time-reversal symmetry breaking

Models based on nuclear energy density functionals can provide access to a multitude of observables for thousands of nuclei in a single framework with microscopic foundations. Such models can rival the accuracy of more phenomenological approaches, but doing so requires adjusting parameters to thousands of nuclear masses. To keep such large-scale fits feasible, several symmetry restrictions are typically imposed on the nuclear configurations. One such example is time-reversal invariance, which is generally enforced via the Equal Filling Approximation (EFA). Here we lift this assumption, enabling us to access the spin and current densities in the ground states of odd-mass and odd-odd nuclei, which contribute to the total energy of such nuclei through so-called ‘time-odd’ terms. We present here the Skyrme-based BSkG2 model whose parameters were adjusted to essentially all known nuclear masses without relying on the EFA, refining our earlier work [G. Scamps et al., EPJA 57, 333 (2021)]. Moving beyond ground state properties, we also incorporated information on the fission barriers of actinide nuclei in the parameter adjustment. The resulting model achieves a root-mean-square (rms) deviation of (i) 0.678 MeV on 2457 known masses, (ii) 0.027 fm on 884 measured charge radii, (iii) 0.44 MeV and 0.47 MeV, respectively, on 45 reference values for primary and secondary fission barriers of actinide nuclei, and (iv) 0.49 MeV on 28 fission isomer excitation energies. We limit ourselves here to a description of the model and the study the impact of lifting the EFA on ground state properties such as binding energies, deformation and pairing, deferring a detailed discussion of fission to a forthcoming paper.

Nuclear excitation cross section of Th229 via inelastic electron scattering

Nuclear excitation cross section of $^{229}\mathrm{Th}$ from the ground state to the low-lying isomeric state via inelastic electron scattering is calculated, on the level of Dirac distorted wave Born approximation. With electron energies below 100 eV, inelastic scattering is very efficient in the isomeric excitation, yielding excitation cross sections on the order of ${10}^{\ensuremath{-}27}$ to ${10}^{\ensuremath{-}26}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{2}$. Systematic analyses are presented on elements affecting the excitation cross section, including the ion-core potential, the relativistic effect, the knowledge of the reduced nuclear transition probabilities, etc.

Nuclear excitation of Th229 induced by laser-driven electron recollision

Previously we proposed a new approach of exciting the $^{229}\mathrm{Th}$ nucleus using laser-driven electron recollision [Wang, Zhou, Liu, and Wang, Phys. Rev. Lett. 127, 052501 (2021)]. The current article is aimed at elaborating the method by explaining further theoretical details and presenting extended new results. The method has also been improved by adopting the electronic excitation cross sections calculated recently by Tkalya [Tkalya, Phys. Rev. Lett. 124, 242501 (2020)]. The new cross sections are obtained from Dirac distorted-wave calculations instead of from Dirac plane-wave calculations as we used previously. The distorted-wave cross sections are shown to be 5 to 6 orders of magnitude higher than the plane-wave results. With the excitation cross sections updated, the probability of isomeric excitation of $^{229}\mathrm{Th}$ from electron recollision is calculated to be on the order of ${10}^{\ensuremath{-}12}$ per nucleus per (femtosecond) laser pulse. The dependency of the excitation probability on various laser parameters is calculated and discussed, including the laser intensity, the laser wavelength, and the laser pulse duration.

β - and γ -spectroscopy study of Pd119 and Ag119

Neutron-rich $^{119}\mathrm{Pd}$ nuclei were produced in fission of natural uranium, induced by 25-MeV protons. Fission fragments swiftly extracted with the Ion Guide Isotope Separation On-Line method were mass separated using a dipole magnet and a Penning trap, providing mono-isotopic samples of $^{119}\mathrm{Pd}$. Their ${\ensuremath{\beta}}^{\ensuremath{-}}$ decay was measured with $\ensuremath{\gamma}\ensuremath{\gamma}$- and $\ensuremath{\beta}\ensuremath{\gamma}$-spectroscopy methods using low-energy germanium detectors and a thin plastic scintillator. Two distinct nuclear-level structures were observed in $^{119}\mathrm{Ag}$, based on the $1/{2}^{\ensuremath{-}}$ and $7/{2}^{+}$ isomers reported previously. The ${\ensuremath{\beta}}^{\ensuremath{-}}$-decay work was complemented by a prompt-$\ensuremath{\gamma}$ study of levels in $^{119}\mathrm{Ag}$ populated in spontaneous fission of $^{252}\mathrm{Cf}$, performed using the Gammasphere array of germanium detectors. Contrary to previous suggestions, our data show that the $1/{2}^{\ensuremath{-}}$ isomer is located below the $7/{2}^{+}$ isomer and is proposed as a new ground state of $^{119}\mathrm{Ag}$ with the $7/{2}^{+}$ isomer excitation energy determined to be 33.4 keV. Our data indicate that there are two $\ensuremath{\beta}$ unstable isomers in $^{119}\mathrm{Pd}$, a proposed ground state of $^{119}\mathrm{Pd}$ with tentative spin $1/{2}^{+}$ or $3/{2}^{+}$ and a half-life of 0.88 s and the other one about 350 keV above, having spin ($11/{2}^{\ensuremath{-}}$) and a half-life of 0.85 s. The higher-energy isomer probably decays to the $1/{2}^{+}$ or $3/{2}^{+}$ ground state via a $\ensuremath{\gamma}$ cascade comprising 18.7-219.8-$\mathrm{X}$-keV transitions. The unobserved isomeric transition with energy $X\ensuremath{\approx}100$ keV probably has an $E3$ multipolarity. Its hindrance factor is significantly lower than for analogous $E3$ isomeric transitions in lighter Pd isotopes, suggesting an oblate deformation of levels in $^{119}\mathrm{Pd}$. Oblate configurations in $^{119}\mathrm{Ag}$ are discussed also.

Exciting the Isomeric ^{229}Th Nuclear State via Laser-Driven Electron Recollision.

We propose a new approach to excite the isomeric ^{229}Th nuclear state, which has attracted much attention recently as a potential "nuclear clock." Our approach is based on a laser-driven electron recollision process, the core process of strong-field atomic physics. Bringing together knowledge of recollision physics and of the related nuclear physics, we calculate the isomeric excitation probability. This new approach does not require precise knowledge of the energy of the isomeric state. The excitation is well timed which may be exploited to control the coherence of the isomeric state. Experimental realization is within reach using tabletop laser systems.

Mass measurements of neutron-rich indium isotopes for r -process studies

A new series of neutron-rich indium mass measurements is reported from the TITAN multiple-reflection time-of-flight mass spectrometer (MR-TOF-MS). These mass measurements cover In125−134 (N=76–85) and include ground states as well as isomeric states. The masses of nuclei in this region are known to be of great importance for accurately modeling r-process nucleosynthesis, and the significance of the reported neutron-rich indium masses is discussed in this context. Results are compared with earlier experimental data where available as well as theoretical mass models. The measurements reported here include the first mass measurements of In133,134, as well as the first direct mass measurement of In132. The masses of In125−131 ground states and several isomers were previously measured to higher precision by Penning trap mass spectrometry, which also resolved some low-lying isomers that could not be resolved in this work. The earlier Penning trap measurements serve as excellent cross-checks for the MR-TOF-MS measurements, and in some cases the MR-TOF-MS measurements improve the literature uncertainties of higher-lying isomer masses and excitation energies. A new isomeric state for In128, recently reported for the first time by the JYFLTRAP group, is also confirmed by the TITAN MR-TOF-MS, with a measured excitation energy of 1813(17) keV.Received 24 November 2020Accepted 8 February 2021DOI:https://doi.org/10.1103/PhysRevC.103.025811©2021 American Physical SocietyPhysics Subject Headings (PhySH)Research AreasBinding energy & massesNuclear astrophysicsr processProperties90 ≤ A ≤ 149TechniquesSpectrometers & spectroscopic techniquesNuclear Physics

The photochemical isomerization 2-furylidenetetralone

A DFT study on the photochemical isomerization of furylidenetetralone derivatives is reported. The excitation of the trans isomer of the starting material can give the cis one, converts the S1 into the corresponding triplet state, or can be converted directly into the transposed product. The excitation of the cis isomer of the starting material can give the same triplet state observed with the trans isomer; however it cannot be converted into the transposed product because the energy of the transition state is too high. Finally, compounds with the structure HetCHCHCOPh can give a sensitized dimerization reaction, never observed in this case. The calculations showed that, while with compounds such HetCHCHCOAr the biradical intermediate of the dimerization reaction was obtained in very fast exothermic reaction, in the case of the furylidenetetralone derivative, the formation of the dimeric biradical intermediate is highly endothermic and, than, less probable.

Masses of ground and isomeric states of In101 and configuration-dependent shell evolution in odd- A indium isotopes

We report first precision mass measurements of the $1/2^-$ isomeric and $9/2^+$ ground states of $^{101}$In. The determined isomeric excitation energy continues a smooth trend of odd-$A$ indium isotopes up to the immediate vicinity of $N=50$ magic number. This trend can be confirmed by dedicated shell model calculations only if the neutron configuration mixing is considered. We find that the single particle energies are different for different states of the same isotope. The presented configuration-dependent shell evolution, type II shell evolution, in odd-$A$ nuclei is discussed for the first time. Our results will facilitate future studies of single-particle neutron states.

A novel method for the measurement of half-lives and decay branching ratios of exotic nuclei

.A novel method for simultaneous measurement of masses, Q-values, isomer excitation energies, half-lives and decay branching ratios of exotic nuclei has been demonstrated. The method includes first use of a stopping cell as an ion trap, combining storage of mother and daughter nuclides for variable durations in a cryogenic stopping cell (CSC), and afterwards the identification and counting of them by a multiple-reflection time-of-flight mass spectrometer (MR-TOF-MS). We utilized our method to record the decay and growth of the 216Po and 212Pb isotopes (alpha decay) and of the 119m2Sb isomer (t_{1/2} = 850pm 90 ms) and 119gSb isotope (isomer transition), obtaining half-lives consistent with literature values. The amount of non-nuclear-decay losses in the CSC up to sim 10 s is negligible, which exhibits its extraordinary cleanliness. For 119Sb isotopes, we present the first direct measurements of the mass of its ground state, and the excitation energy and decay branching ratios of its second isomeric state (119m2Sb). This resolves discrepancies in previous excitation energy data, and is the first direct evidence that the 119m2Sb isomer decays dominantly via gamma emission. These results pave the way for the measurement of branching ratios of exotic nuclei.

Nuclear isomer excitation in Th229 atoms by superintense laser fields

Excitation of the isomeric nuclear state 229m Th in the process of thorium atom irradiation by two-color femtosecond pulse of Ti: Sa laser at the fundamental wavelength and second harmonic is analyzed. It is shown that the rate of isomeric state excitation can be enhanced significantly with respect to other nucleus excitation processes in laser plasma or by an external coherent source at the resonance wavelength. This enhancement is due to the process of nonlinear laser nuclear excitation based on the following. First, the atomic current associated with the motion of valence electrons in strong field is a nonlinear function of the field amplitude. Secondly, the energy of photons at frequency of the Ti:Sa laser fifth harmonic coincides with the energy of the 229m Th state. Yield of this harmonic is much higher if the two-color (1st and 2nd harmonics of the fundamental) is used. Thirdly, the intensity of the field produced by valence electrons at atomic nucleus reaches the near-atomic value, which exceeds significantly the field strength associated with any other mechanism of laser plasma emission.

Collective effects in Th229 -doped crystals

Vacuum-ultraviolet-transparent crystals have been proposed as host lattice for the coherent driving of the unusually low-lying isomer excitation in $^{229}$Th for metrology and quantum optics applications. Here the possible collective effects occurring for the coherent pulse propagation in the crystal system are investigated theoretically. We consider the effect of possible doping sites, quantization axis orientation and pulse configurations on the scattered light intensity and signatures of nuclear excitation. Our results show that for narrow-pulse driving, the rather complicated quadrupole splitting of the level scheme is significantly simplified. Furthermore, we investigate complex driving schemes with a combination of pulsed fields and investigate the occurring interference process. Our theoretical results support experimental attempts for first direct driving of the nuclear transition with coherent light.

Primed for Efficient Motion: Ultrafast Excited State Dynamics and Optical Manipulation of a Four Stage Rotary Molecular Motor.

All isomers of a four stage rotary molecular motor, dimethyl-tetrahydro-bi(cyclopenta[α]napthal-enylidene), are studied with ultrafast transient absorption spectroscopy. Single and two pulse excitations (pump and delayed repump with a different wavelength) are used to optically probe the excited state dynamics. These measurements demonstrate that this motor is not only designed for unidirectional isomerization, but is also "primed" for efficient rotary motion. The yield for photoisomerization from the stable P-cis isomer to the metastable M-trans isomer is 85% ± 10%, while the yield for the undesired back reaction is ca. 0.08 (+0.02, -0.05). The yield for photoisomerization from stable P-trans to the metastable M-cis isomer is ca. 85% ± 3% and the yield for the back reaction is 15% ± 3%. Excitation of P-trans in the lowest singlet state results in formation of a dark state on a 3.6 ps time scale and formation of the M-cis isomer on a ca. 12 ps time scale. Excitation of P-cis in the lowest singlet state results in formation of a dark state on ca. 13 ps time scale and formation of the M-trans isomer on a 71 ps time scale. Excitation of either isomer at 269 nm, higher in the excited state manifold, accesses additional excited state pathways, but does not change the ultimate product formation. This result suggests that pulse sequences accessing higher excited states may provide a tool to manipulate the molecular motor. Pulse sequences using a 269 nm pump pulse and a 404 nm repump pulse are able to increase the yield of the P-cis to M-trans reaction but only decrease the yield of the P-trans to M-cis reaction. These pulse sequences are unable to access reaction pathways that bypass the helix inversion step, although other wavelengths and time delays might yet provide optical control of the entire reaction cycle. We propose intermediates and candidate conical intersections between all four isomers.