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13 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Atom-at-a-Time Radioactive Molecule Identification: Looking toward Studies of Superheavy Elements

The chemical behavior of superheavy elements (SHEs, Z > 103) remains poorly understood. Their chemical properties are expected to deviate from established trends, challenging the predictive power of the periodic table. To investigate these elements experimentally, they must first be synthesized through nuclear reactions and then quickly subjected to chemical studies before they decay. Given the low production rates of these reactions and the need for measurements on an atom-at-a-time basis, innovative techniques are needed. Here, to address these challenges, a novel gas-phase chemistry method has been developed at Lawrence Berkeley National Laboratory, utilizing the Berkeley Gas-filled Separator and FIONA. This technique enables the production, identification, and study of molecular species formed by SHEs. As a proof of concept, we present measurements on the formation and identification of 151,152 HoO + molecules, demonstrating the capability to study the production of radioactive molecules under controlled conditions and directly identify them via their mass-to-charge ratio. These measurements validate the effectiveness of this technique for low-statistics SHE studies, highlighting the potential of this approach to ignite the next generation of experimental SHE chemistry research, offering a path to re-evaluate SHE placement on the periodic table.

Chemistry↗
DOE OSTI2026

Comparing the fluorination of Pb+ and Po+: insights into p-block relativistic effects for superheavy elements

It is expected that the chemical properties of the heaviest of the superheavy elements (SHEs, = 113 – 118) do not align with what is suggested by their current positions on the periodic table. Specifically, the onset of significant relativistic effects, including increased spin–orbit splitting of the p-orbitals may lead to enhanced stability of low-oxidation states. Notably, it is predicted that flerovium ( = 114) may exhibit pseudo-noble gas behavior from a electron configuration that acts as an ‘inert pair’. Even though it is expected that the – splitting becomes pronounced toward the end of the p-block’s sixth row, there is currently limited experimental evidence to confirm its extent or impact. Here, the production of gas-phase lead ( = 82) and polonium ( = 84) fluoride cations (PbF and PoF ) were compared to elucidate differences in accessible oxidation states. The PoF and PbF species were produced and identified with the FIONA spectrometer at the Lawrence Berkeley National Laboratory 88-Inch Cylctron Facility. Polonium showed notably different fluorination chemistry than lead, producing PoF and PoF as primary products compared to lead’s PbF and PbF . The distribution of PoF products observed offer insights as to the role of spin–orbit splitting for polonium. Similar studies of superheavy elements would elucidate the accessibility of their low-oxidation states as well as to inform chemical predictions for eighth-row elements not yet discovered.

Pore, Jennifer L [Nuclear Science Division, Lawren↗
DOE OSTI2025

Direct identification of Ac and No molecules with an atom-at-a-time technique

The periodic table provides an intuitive framework for understanding chemical properties. However, its traditional patterns may break down for the heaviest elements occupying the bottom of the chart. Here, the large nuclei of actinides (Z > 88) and superheavy elements (Z ≥ 104) give rise to relativistic effects that are expected to substantially alter their chemical behaviours, potentially indicating that we have reached the end of a predictive periodic table. Relativistic effects have already been cited for the unusual chemistry of the actinides compared with those of their lanthanide counterparts. Unfortunately, it is difficult to understand the full impact of relativistic effects, as research on the later actinides and superheavy elements is scarce. Beyond fermium (Z = 100), elements need to be produced and studied one atom at a time, using accelerated ion beams and state-of-the-art experimental approaches. So far, no experiments have been capable of directly identifying produced molecular species. Here ions of actinium (Ac, Z = 89) and nobelium (No, Z = 102) were synthesized through nuclear reactions at the 88-Inch Cyclotron facility at Lawrence Berkeley National Laboratory and then exposed to trace amounts of H 2 O and N 2 . The produced molecular species were directly identified by measuring their mass-to-charge ratios using FIONA (For the Identification Of Nuclide A). These results mark the first, to our knowledge, direct identification of heavy-element molecular species using an atom-at-a-time technique and highlight the importance of such identifications in future superheavy-element chemistry experiments to deepen understanding of their chemical properties.

Pore, Jennifer L. [Lawrence Berkeley National Labo↗
DOE OSTI2024

Impact of tensor forces on quasifission product yield distributions

Quantum shell effects are crucial for the stability and structure of atomic nuclei and play a key role in the discovery of superheavy elements. Furthermore, during nuclear collisions, the dynamical evolution of these shell effects disrupts the equilibration process necessary for forming a compound nucleus, leading to the breakup of the initial composite as a result of quasifission. As such, quasifission reactions hinder the formation of a superheavy element.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Decay spectroscopy of an isomeric state in 251 Md

Superheavy elements ( Z ≥ 104) owe their existence to quantum shell effects which stabilize them against fission. Experimental studies of their structure are challenging, and only recently has direct information begun to emerge. Meanwhile, the comparative ease of producing the transfermium nuclei offers an alternative approach. These nuclei are well-deformed ( β 2 ≈ 0.28) owing to the existence of deformed gaps in the single particle spectrum near Z = 100 and N = 152. Because of this, the proton orbitals near the Fermi surface in this region are expected to originate from the spherical sub shells which define the shell gaps near Z = 114. In this sense, the transfermium nuclei act as a testing ground for theoretical models used to describe the superheavy region. Deformed odd-mass nuclei are of particular interest since they can provide direct insight into the single particle structure.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Enhanced sensitivity for electron affinity measurements of rare elements

The electron affinity (EA), the energy released when a neutral atom binds an additional electron, is a fundamental property of atoms that is governed by electron-electron correlations and is strongly related to an element’s chemical reactivity. However, conventional techniques for EA determination lack the experimental sensitivity to probe very scarce samples. As a result, the EA for the heaviest elements of the periodic table is entirely uncharted. Here, we present a novel technique to determine EAs through Laser Photodetachment Threshold Spectroscopy, performed in an electrostatic ion beam trap to increase the samples’ exposure to laser photons and, thus, improve the experimental signal sensitivity by three orders of magnitude. Moreover, the additional exposure time allows the use of lower-power continuous-wave narrow-band lasers that reduce uncertainties associated with broadening effects induced by the laser bandwidth. By applying this technique, we measure the EA of 35 Cl to be 3.612720(44) eV, achieving state-of-the-art precision while employing five orders of magnitude fewer anions. The demonstrated sensitivity paves the way for systematic EA measurements across isotopic chains - including isotope shifts and hyperfine splittings - and ultimately for the first direct determination of electron affinities in superheavy elements.

Maier, F. M. [Univ. of Greifswald (Germany); Europ↗
DOE OSTI2025

Effect of competition of spherical and deformed shells in quasifission of superheavy nuclei

Quasifission and fusion-fission represent the two most likely reaction outcomes to occur postcapture in collisions leading to superheavy nuclei. As such, understanding these mechanisms and how they relate to one another is key to understanding the intricate dynamics that drive the formation (or dissociation) of the nascent compound nuclei formed in fusion reactions. This understanding directly translates to a more informed picture of suitable reaction partners and can provide vital information for experimental efforts to study the physics and chemistry of superheavy elements. In this work we report results from time-dependent simulations of 48 Ca + 238 U and 50 Ti + 236 Th reactions at incident energies just above the Coulomb barrier with a focus on the quasifission process that prevent the formation of a fully equilibrated 286 Cn compound nucleus. We study these reactions systematically and consider a wide range of initial configurations to extract a robust estimate of primary fragment yields for the quasifission process. Multiple preferred exit channels are observed, with both spherical and deformed shell effects in the heavy and light fragments driving contributions to the production yields depending on the initial configuration of the system. Orientation effects of the deformed actinide targets are found to be a primary driver of which exit channels are populated. Here, the impact of moving away from a doubly magic projectile is explored with implications towards the reactions considered for current and future superheavy searches.

Gumbel, Richard [Michigan State University, East L↗
DOE OSTI2025

Spinor-based coupled cluster thermochemistry: RgF and CnF 0/+ as compared to AuF and HgF 0/+

A relativistic coupled cluster approach that includes spin-orbit variationally in the eXact 2-component (X2C) approximation with the inclusion of the Gaunt interaction (X2Cg) was used to probe the thermochemistry and ground state spectroscopic constants of RgF, CnF, and CnF + . Utilizing large sequences of correlation consistent basis sets at the X2Cg-CCSD(T) level of theory, this work reports 0 K bond dissociation energies (BDEs) of AuF, RgF, HgF 0/+ , and CnF 0/+ , as well as ionization energies of Au, Rg, Hg, Cn, HgF, and CnF.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Two-loop MHV form factors from the periodic Wilson loop

We discuss how to compute maximal-helicity-violating (MHV) form factors for the chiral part of the stress-tensor supermultiplet from periodic light-like polygon Wilson loops in planar $\mathcal{N}$ = 4 super Yang-Mills theory beyond the one-loop level. We show that the periodicity imposes path ordering on points on different edges, which explains the appearance of square roots coming from non-planar Feynman diagrams. Taking such diagrams into account, we provide the integrand of the two-loop n-particle MHV form factor, compute all diagrams, prove the cancellation of divergences and finally compute the two-loop 5-particle and 6-particle form factors as examples.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Paths to superheavy nuclei

This document summarizes the discussions and outcomes of the Facility for Rare Isotope Beams (FRIB) Theory Alliance topical program ‘The path to Superheavy Isotopes’ held in June 2024 at FRIB. Its content is non-exhaustive, reflecting topics chosen and discussed by the participants. The program aimed to assess the current status of theory in superheavy nuclei (SHN) research and identify necessary theoretical developments to guide experimental programs and determine fruitful production mechanisms. This report details the intersection of SHN research with other fields, provides an overview of production mechanisms and theoretical models, discusses future needs in theory and experiment, explores other potential avenues for SHN synthesis, and highlights the importance of building a strong theory community in this area.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2026

Investigation of the 244 Pu ⁢( 48 Ca,𝑥⁢𝑛) 292−𝑥 Fl reaction with the LBNL SHREC detector: Investigation of decay chains of isotopes of flerovium (𝑍=114)

The 244 Pu ⁢( 48 Ca,𝑥⁢𝑛)⁢ 292−𝑥 Fl reaction was investigated at Lawrence Berkeley National Laboratory’s 88 Inch Cyclotron using the Berkeley Gas-filled Separator (BGS), the newly installed Superheavy Recoil detector, along with an upgraded digital electronics and data acquisition system. Seven decay chains were observed starting with an evaporation residue, followed by a single 𝛼 decay and a spontaneous fission. The decay characteristics of these seven decay chains led to an assignment to 288 Fl , the product of the 4⁢𝑛 reaction channel. Two additional chains were (tentatively) assigned to the decay of the 3⁢𝑛 exit channel, 289 Fl . Cross sections for the 4⁢𝑛 and 3⁢𝑛 exit channels were 𝜎 prod =6.7⁢($^{36}_{25}$) pb and 𝜎 prod =1.6⁢($^{22}_{11}$) pb, respectively. Another decay chain, tentatively assigned to the 5⁢𝑛 exit channel through the 48 Ca + 244 Pu reaction or the 3⁢𝑛 exit channel of the 48 Ca + 242 Pu reaction, was also detected. Detailed information regarding the observed decay chains and their nuclear structure aspects is discussed, along with the performance of the BGS and the new detection system.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Weak decays in superheavy nuclei

Superheavy nuclei represent the extreme atoms and nuclides known at the limit of mass and charge. The observed superheavy nuclei are all proton-rich; they decay primarily by emitting 𝛼 particles and by fission with a possible small electron capture (EC) branch. Here, due to the huge atomic numbers and associated relativistic effects, EC decays of superheavy systems are expected to differ from what is known in lighter nuclei. In this letter, using the quantified relativistic nuclear density functional theory and the quasiparticle random-phase approximation with the interaction optimized to experimental EC/𝛽 ± -decay half-lives, and Gamow-Teller resonance energies, we study the EC/𝛽 ± -decays in 𝑍=101–118 nuclei. Both allowed (1 + ) and first-forbidden (0 − ,1 − and 2 − ) transitions are considered. We show that the first-forbidden 1 − transitions dominate the decay rates in almost all studied nuclei. For proton-rich nuclei, EC dominates over 𝛽 + decay. Based on calculations with two relativistic energy density functionals, we identify 45 candidate nuclei in which a competition between weak decays and 𝛼 decay and spontaneous fission is expected.

A ≥ 220↗
DOE OSTI2025

Electron capture of superheavy nuclei with realistic lepton wave functions

The superheavy nuclei push the periodic table of the elements and the chart of the nuclides to their limits, providing a unique laboratory for studies of the electron-nucleus interactions. The most important weak decay mode in known superheavy nuclei is electron capture (EC). In the standard calculations of EC, the lepton wave functions are usually considered in the lowest-order approximation. In this work, we investigate the sensitivity of EC rates on the choice of the electron wave functions by (i) assuming the single-particle approximation for the electron wave functions, and (ii) carrying out Dirac-Hartree-Fock (DHF) calculations. The nuclear response is generated based on the state-of-the-art quasiparticle random phase approximation employing relativistic nuclear energy density functional theory. Here, we show that using the improved lepton wave functions reduces the EC rates up to 40% in the superheavy nucleus oganesson (𝑍=118). Interestingly, because of screening effects, the difference between the EC rates obtained with the DHF and single-particle calculations is fairly small.

Atomic orbital↗