Physicists have obtained the first detailed picture of the internal structure of radium monofluoride (RaF) thanks to the molecule’s own electrons, which penetrated the nucleus of the molecule and interacted with its protons and neutrons. This behaviour is known as the Bohr-Weisskopf effect, and study co-leader Shane Wilkins says that this marks the first time it has been observed in a molecule. The measurements themselves, he adds, are an important step towards testing for nuclear symmetry violation, which might explain why our universe contains much more matter than antimatter.

RaF contains the radioactive isotope ²²⁵Ra, which is not easy to make, let alone measure. Producing it requires a large accelerator facility at high temperature and high velocity, and it is only available in tiny quantities (less than a nanogram in total) for short periods (it has a nuclear half-life of around 15 days).

“This imposes significant challenges compared to the study of stable molecules, as we need extremely selective and sensitive techniques in order to elucidate the structure of molecules containing ²²⁵Ra,” says Wilkins, who performed the measurements as a member of Ronald Fernando Garcia Ruiz’s research group at the Massachusetts Institute of Technology (MIT), US.

The team chose RaF despite these difficulties because theory predicts that it is particularly sensitive to small nuclear effects that break the symmetries of nature. “This is because, unlike most atomic nuclei, the radium atom’s nucleus is octupole deformed, which basically means it has a pear shape,” explains the study’s other co-leader, Silviu-Marian Udrescu.

Electrons inside the nucleus

In their study, which is detailed in Science, the MIT team and colleagues at CERN, the University of Manchester, UK and KU Leuven in the Netherlands focused on RaF’s hyperfine structure. This structure arises from interactions between nuclear and electron spins, and studying it can reveal valuable clues about the nucleus. For example, the nuclear magnetic dipole moment can provide information on how protons and neutrons are distributed inside the nucleus.

In most experiments, physicists treat electron-nucleus interactions as taking place at (relatively) long ranges. With RaF, that’s not the case. Udrescu describes the radium atom’s electrons as being “squeezed” within the molecule, which increases the probability that they will interact with, and penetrate, the radium nucleus. This behaviour manifests itself as a slight shift in the energy levels of the radium atom’s electrons, and the team’s precision measurements – combined with state-of-the-art molecular structure calculations – confirm that this is indeed what happens.

“We see a clear breakdown of this [long-range interactions] picture because the electrons spend a significant amount of time within the nucleus itself due to the special properties of this radium molecule,” Wilkins explains. “The electrons thus act as highly sensitive probes to study phenomena inside the nucleus.”

Searching for violations of fundamental symmetries

According to Udrescu, the team’s work “lays the foundations for future experiments that use this molecule to investigate nuclear symmetry violation and test the validity of theories that go beyond the Standard Model of particle physics.” In this model, each of the matter particles we see around us – from baryons like protons to leptons such as electrons – should have a corresponding antiparticle that is identical in every way apart from its charge and magnetic properties (which are reversed).

The problem is that the Standard Model predicts that the Big Bang that formed our universe nearly 14 billion years ago should have generated equal amounts of antimatter and matter – yet measurements and observations made today reveal an almost entirely matter-based universe. Subtler differences between matter particles and their antimatter counterparts might explain why the former prevailed, so by searching for these differences, physicists hope to explain antimatter-matter asymmetry.

Wilkins says the team’s work will be important for future such searches in species like RaF. Indeed, Wilkins, who is now at Michigan State University’s Facility for Rare Isotope Beams (FRIB), is building a new setup to cool and slow beams of radioactive molecules to enable higher-precision spectroscopy of species relevant to nuclear structure, fundamental symmetries and astrophysics. His long-term goal, together with other members of the RaX collaboration (which includes FRIB and the MIT team as well as researchers at Harvard University and the California Institute of Technology), is to implement advanced laser-based techniques using radium-containing molecules.

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New high-precision laser spectroscopy measurements on thorium-229 nuclei could shed more light on the fine structure constant, which determines the strength of the electromagnetic interaction, say physicists at TU Wien in Austria.

The electromagnetic interaction is one of the four known fundamental forces in nature, with the others being gravity and the strong and weak nuclear forces. Each of these fundamental forces has an interaction constant that describes its strength in comparison with the others. The fine structure constant, α, has a value of approximately 1/137. If it had any other value, charged particles would behave differently, chemical bonding would manifest in another way and light-matter interactions as we know them would not be the same.

“As the name ‘constant’ implies, we assume that these forces are universal and have the same values at all times and everywhere in the universe,” explains study leader Thorsten Schumm from the Institute of Atomic and Subatomic Physics at TU Wien. “However, many modern theories, especially those concerning the nature of dark matter, predict small and slow fluctuations in these constants. Demonstrating a non-constant fine-structure constant would shatter our current understanding of nature, but to do this, we need to be able to measure changes in this constant with extreme precision.”

With thorium spectroscopy, he says, we now have a very sensitive tool to search for such variations.

Nucleus becomes slightly more elliptic

The new work builds on a project that led, last year, to the worlds’s first nuclear clock, and is based on precisely determining how the thorium-229 (²²⁹Th) nucleus changes shape when one of its neutrons transitions from a ground state to a higher-energy state. “When excited, the ²²⁹Th nucleus becomes slightly more elliptic,” Schumm explains. “Although this shape change is small (at the 2% level), it dramatically shifts the contributions of the Coulomb interactions (the repulsion between protons in the nucleus) to the nuclear quantum states.”

The result is a change in the geometry of the ²²⁹Th nucleus’ electric field, to a degree that depends very sensitively on the value of the fine structure constant. By precisely observing this thorium transition, it is therefore possible to measure whether the fine-structure constant is actually a constant or whether it varies slightly.

After making crystals of ²²⁹Th doped in a CaF₂ matrix at TU Wien, the researchers performed the next phase of the experiment in a JILA laboratory at the University of Colorado, Boulder, US, firing ultrashort laser pulses at the crystals. While they did not measure any changes in the fine structure constant, they did succeed in determining how such changes, if they exist, would translate into modifications to the energy of the first nuclear excited state of ²²⁹Th.

“It turns out that this change is huge, a factor 6000 larger than in any atomic or molecular system, thanks to the high energy governing the processes inside nuclei,” Schumm says. “This means that we are by a factor of 6000 more sensitive to fine structure variations than previous measurements.”

Increasing the spectroscopic accuracy of the ²²⁹Th transition

Researchers in the field have debated the likelihood of such an “enhancement factor” for decades, and theoretical predictions of its value have varied between zero and 10 000. “Having confirmed such a high enhancement factor will now allow us to trigger a ‘hunt’ for the observation of fine structure variations using our approach,” Schumm says.

Andrea Caputo of CERN’s theoretical physics department, who was not involved in this work, calls the experimental result “truly remarkable”, as it probes nuclear structure with a precision that has never been achieved before. However, he adds that the theoretical framework is still lacking. “In a recent work published shortly before this work, my collaborators and I showed that the nuclear-clock enhancement factor K is still subject to substantial theoretical uncertainties,” Caputo says. “Much progress is therefore still required on the theory side to model the nuclear structure reliably.”

Schumm and colleagues are now working on increasing the spectroscopic accuracy of their ²²⁹Th transition measurement by another one to two orders of magnitude. “We will then start hunting for fluctuations in the transition energy,” he reveals, “tracing it over time and – through the Earth’s movement around the Sun – space.

The present work is detailed in Nature Communications.

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