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Promethium bound: Rare earth element’s secrets exposed



Promethium bound: Rare earth element’s secrets exposed

Scientists have uncovered the properties of a rare earth element that was first discovered 80 years ago at the very same laboratory, opening a new pathway for the exploration of elements critical in modern technology, from medicine to space travel.

Promethium was discovered in 1945 at Clinton Laboratories, now the Department of Energy’s Oak Ridge National Laboratory, and continues to be produced at ORNL in minute quantities. Some of its properties have remained elusive despite the rare earth element’s use in medical studies and long-lived nuclear batteries. It is named after the mythological Titan who delivered fire to humans and whose name symbolizes human striving.

“The whole idea was to explore this very rare element to gain new knowledge,” said Alex Ivanov, an ORNL scientist who co-led the research. “Once we realized it was discovered at this national lab and the place where we work, we felt an obligation to conduct this research to uphold the ORNL legacy.”

The ORNL-led team of scientists prepared a chemical complex of promethium, which enabled its characterization in solution for the first time. Thus, they exposed the secrets of this extremely rare lanthanide, whose atomic number is 61, in a series of meticulous experiments.

Their landmark study, published in the journal Nature, marks a significant advance in rare earth research and might rewrite chemistry textbooks.

“Because it has no stable isotopes, promethium was the last lanthanide to be discovered and has been the most difficult to study,” said ORNL’s Ilja Popovs, who co-led the research. Most rare earth elements are lanthanides, elements from 57 — lanthanum — to 71 — lutetium — on the periodic table. They have similar chemical properties but differ in size.

The other 14 lanthanides are well understood. They are metals with useful properties that make them indispensable in many modern technologies. They are workhorses of applications such as lasers, permanent magnets in wind turbines and electric vehicles, X-ray screens and even cancer-fighting medicines.

“There are thousands of publications on lanthanides’ chemistry without promethium. That was a glaring gap for all of science,” said ORNL’s Santa Jansone-Popova, who co-led the study. “Scientists have to assume most of its properties. Now we can actually measure some of them.”

The research relied on unique resources and expertise available at DOE national laboratories. Using a research reactor, hot cells and supercomputers, as well as the accumulated knowledge and skills of 18 scientists in different fields, the authors detailed the first observation of a promethium complex in solution.

The ORNL scientists bound, or chelated, radioactive promethium with special organic molecules called diglycolamide ligands. Then, using X-ray spectroscopy, they determined the properties of the complex, including the length of the promethium chemical bond with neighboring atoms — a first for science and a longstanding missing piece to the periodic table of elements.

Promethium is very rare; only about a pound occurs naturally in the Earth’s crust at any given time. Unlike other rare earth elements, only minute quantities of synthetic promethium are available because it has no stable isotopes.

For this study, the ORNL team produced the isotope promethium-147, with a half-life of 2.62 years, in sufficient quantities and at a high enough purity to study its chemical properties. ORNL is the United States’ only producer of promethium-147.

Notably, the team provided the first demonstration of a feature of lanthanide contraction in solution for the whole lanthanide series, including promethium, atomic number 61. Lanthanide contraction is a phenomenon in which elements with atomic numbers between 57 and 71 are smaller than expected. As the atomic numbers of these lanthanides increase, the radii of their ions decrease. This contraction creates distinctive chemical and electronic properties because the same charge is limited to a shrinking space. The ORNL scientists got a clear promethium signal, which enabled them to better define the shape of the trend — across the series.

“It’s really astonishing from a scientific viewpoint. I was struck once we had all the data,” said Ivanov. “The contraction of this chemical bond accelerates along this atomic series, but after promethium, it considerably slows down. This is an important landmark in understanding the chemical bonding properties of these elements and their structural changes along the periodic table.”

Many of these elements, such as those in the lanthanide and actinide series, have applications ranging from cancer diagnostics and treatment to renewable energy technologies and long-lived nuclear batteries for deep space exploration.

The achievement will, among other things, ease the difficult job of separating these valuable elements, according to Jansone-Popova. The team has long worked on separations for the whole series of lanthanides, “but promethium was the last puzzle piece. It was quite challenging,” she said. “You cannot utilize all these lanthanides as a mixture in modern advanced technologies, because first you need to separate them. This is where the contraction becomes very important; it basically allows us to separate them, which is still quite a difficult task.”

The research team used several premier DOE facilities in the project. At ORNL, promethium was synthesized at the High Flux Isotope Reactor, a DOE Office of Science user facility, and purified at the Radiochemical Engineering Development Center, a multipurpose radiochemical processing and research facility. Then, the team performed X-ray absorption spectroscopy at the National Synchrotron Light Source II, a DOE Office of Science user facility at DOE’s Brookhaven National Laboratory, specifically working at the Beamline for Materials Measurement, which is funded and operated by the National Institute of Standards and Technology.

The team also performed quantum chemical calculations and molecular dynamics simulations at the Oak Ridge Leadership Computing Facility, a DOE Office of Science user facility at ORNL, using the lab’s Summit supercomputer, the only computational resource capable of providing the necessary calculations at the time. In addition, the researchers used resources of the Compute and Data Environment for Science at ORNL. They expect future calculations to be performed on ORNL’s Frontier, the world’s most powerful supercomputer and the first exascale system, which is able to perform more than a quintillion calculations each second.

Popovs emphasized that the ORNL-led accomplishments can be attributed to teamwork. Each of the Nature paper’s 18 authors was critical to the project, he said.

The achievement sets the stage for a new era of research, the scientists said. “Anything that we would call a modern marvel of technology would include, in one shape or another, these rare earth elements,” Popovs said. “We are adding the missing link.”

Besides Popovs, Ivanov and Jansone-Popova from ORNL’s Chemical Sciences Division, the paper’s co-authors include Darren Driscoll, Subhamay Pramanik, Jeffrey Einkauf, Santanu Roy and Thomas Dyke, also of ORNL’s Chemical Sciences Division; Frankie White, Richard Mayes, Laetitia Delmau, Samantha Cary, April Miller and Sandra Davern of ORNL’s Radioisotope Science and Technology Division; Matt Silveira and Shelley VanCleve of ORNL’s Isotope Processing and Manufacturing Division; Dmytro Bykov of the National Center for Computational Sciences at ORNL; and Bruce Ravel of the National Institute of Standards and Technology.

This work was primarily co-sponsored by DOE’s Office of Science for ligand synthesis, lanthanide complexation studies, crystallization processes, spectroscopic analyses and simulation efforts. The production, purification and preparation of the promethium sample were supported by the DOE Isotope Program, managed by the Office of Science for Isotope R&D and Production. The single-crystal X-ray diffraction data collection and refinement were supported by the DOE Office of Science.

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Are mixed emotions real? New research says yes




Are mixed emotions real? New research says yes

In Pixar’s latest film, Inside Out 2, complex feelings like envy and embarrassment join the cast of characters. Nostalgia, however, is hurried out the door to cries of “too early!” when she appears.

If animators wish to give nostalgia more consideration in a future film, new data from researchers at the USC Dornsife College of Letters, Arts and Sciences could guide them in determining how to animate this sort of “mixed emotion.”

What’s new: In a recent study, the USC Dornsife neuroscientists found that brains display distinct neural activity when experiencing emotions such as bittersweetness.

  • The advance could help solve a longstanding scientific debate: whether “mixed emotions” arise from unique activity in the brain, or if we’re just flip-flopping back and forth between positive and negative feelings.

Why it matters: Mixed emotions are a common experience, but they’ve been understudied scientifically for several reasons.

  • Emotions are often thought to exist only on a spectrum from negative to positive.
  • It’s easier to study one feeling at a time.

In his words: “It’s hard to evoke these complex emotions in a realistic way inside the lab,” says Jonas Kaplan, associate professor (research) of psychology and co-author of the study, published in the journal Cerebral Cortex in April.

Key findings:

  • Mixed feelings elicited unique neural activity in the amygdala and nucleus accumbens areas of the brain.
  • This activity was different than the brain activity seen when a subject reported a purely positive or negative emotion.

What else? The researchers could predict when someone was going to shift emotions.

  • Particular regions of the brain, like the insular cortex, displayed significant changes as subjects reported an emotional transition.

“Not only did we find brain activity that was correlated with mixed emotions, but we found that it held steady over time,” says Anthony Vaccaro, lead author of the study and a postdoctoral researcher at the Neuroendocrinology of Social Ties Lab at USC Dornsife. Vaccaro recently completed his PhD in psychology at USC Dornsife. “You’re not ping-ponging between negative and positive. It’s a very unique, mixed emotion over a long period.”

Graphs show consistent brain activity during positive, negative and mixed emotions, demonstrating that mixed emotions are distinct from other feelings. (Image: Jonas Kaplan.)

How they did it: As study subjects watched a poignant animated short film, researchers monitored their brain activity using a magnetic resonance imaging (MRI) machine.· The researchers chose One Small Step by TAIKO Studios for its ability to evoke simultaneous happy and sad feelings. · After the first viewing, participants rewatched the video without MRI and indicated when they experienced positive, negative or mixed emotions. The researchers then compared these reports with the MRI imaging results.

Opportunity: The study lays out practical groundwork for future scientific research into this understudied phenomenon, research that Kaplan says would also be beneficial for understanding human psychology.

  • “There’s a certain sophistication that’s required to sit with a mixed emotion and to allow yourself to feel positive and negative at the same time. Looking into that more, exploring the benefits of being able to accept positive and negativity at the same time within yourself, is something we think is worth study,” he says.

What’s next: Kaplan and Vaccaro will next look at how emotional reactions fluctuate in group settings, such as watching a movie together in a cinema.

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Paleontology: New fossil fish genus discovered




Paleontology: New fossil fish genus discovered

Gobies or Gobioidei are one of the most species-rich groups of marine and freshwater fish in Europe. Spending most of their lives on the bottom of shallow waterbodies, they make substantial contributions to the functioning of many ecosystems. With the identification of a new genus of a fossil freshwater goby, students of the international master program ‘Geobiology and Paleobiology’ at LMU and paleontologist Bettina Reichenbacher, professor at the Department of Earth and Environmental Sciences at LMU, have made a discovery that provides critical insights into the evolutionary history of these fish.

Measuring up to 34 mm, the small fish of the new genus †Simpsonigobius were discovered in 18-million-year-old rocks in Turkey and are marked by a distinct combination of morphological features, including otoliths (hearing stones) with a unique shape.

Modern research techniques elucidate position in family tree

To determine the relationships of †Simpsonigobius within the gobioid phylogenetic tree, the researchers utilized a “total-evidence” phylogenetic dataset, which they enhanced in order to combine a total of 48 morphological characters and genetic data from five genes for 48 living and 10 fossil species. In addition, the team employed “tip-dating” for fossil gobioid species for the first time. This is a phylogenetic method in which the age of the fossils (= tips) included in the phylogenetic tree is used to infer the timing of the evolutionary history of the entire group.

The results show that the new genus is the oldest skeleton-based member of the family Oxudercidae — which is classified among the “modern” gobies (families Gobiidae and Oxudercidae) — and the oldest freshwater goby within this modern group. The tip-dating analysis estimated the emergence of the Gobiidae at 34.1 million years ago and that of the Oxudercidae at 34.8 million years ago, which is consistent with previous dating studies using other methods. Moreover, stochastic habitat mapping, in which the researchers incorporated fossil gobies for the first time, revealed that the gobies probably possessed broad salinity tolerance at the beginning of their evolutionary history, which challenges previous assumptions.

“The discovery of †Simpsonigobius not only adds a new genus to the Gobioidei, but also provides vital clues about the evolutionary timeline and habitat adaptations of these diverse fishes. Our research highlights the importance of analyzing fossil records using modern methods to achieve a more accurate picture of evolutionary processes,” says Reichenbacher. First author Moritz Dirnberger, currently a doctoral candidate at the University of Montpellier, adds: “The findings are expected to pave the way for further studies on gobioid evolution and the role of environmental factors in shaping their diversity.”

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Ancient ocean slowdown warns of future climate chaos




Ancient ocean slowdown warns of future climate chaos

When it comes to the ocean’s response to global warming, we’re not in entirely uncharted waters. A UC Riverside study shows that episodes of extreme heat in Earth’s past caused the exchange of waters from the surface to the deep ocean to decline.

This system has been described as the “global conveyer belt,” because it redistributes heat around the globe through the movement of the ocean waters, making large portions of the planet habitable.

Using tiny, fossilized shells recovered from ancient deep-sea sediments, the study in the Proceedings of the National Academy of Sciences demonstrates how the conveyor belt responded around 50 million years ago. At that time, Earth’s climate resembled conditions predicted by the end of this century, if significant action is not taken to reduce carbon emissions.

Oceans play a crucial role in regulating Earth’s climate. They move warm water from the equator toward the north and south poles, balancing the planet’s temperatures. Without this circulation system, the tropics would be much hotter and the poles much colder. Changes in this system are linked to significant and abrupt climate change.

Furthermore, the oceans serve a critical role in removing anthropogenic carbon dioxide from the atmosphere. “The oceans are by far the largest standing pool of carbon on Earth’s surface today,” said Sandra Kirtland Turner, vice-chair of UCR’s Department of Earth and Planetary Sciences and first author of the study.

“Today, the oceans contain nearly 40,000 billion tons of carbon — more than 40 times the amount of carbon in the atmosphere. Oceans also take up about a quarter of anthropogenic CO2 emissions,” Kirtland Turner said. “If ocean circulation slows, absorption of carbon into the ocean may also slow, amplifying the amount of CO2 that stays in the atmosphere.”

Previous studies have measured changes in ocean circulation in Earth’s more recent geologic past, such as coming out of the last ice age; however, those do not approximate the levels of atmospheric CO2 or warming happening to the planet today. Other studies provide the first evidence that deep ocean circulation, particularly in the North Atlantic, is already starting to slow.

To better predict how ocean circulation responds to greenhouse gas-driven global warming, the research team looked to the early Eocene epoch, between roughly 49 and 53 million years ago. Earth then was much warmer than today, and that high-heat baseline was punctuated by spikes in CO2 and temperature called hyperthermals.

During that period, the deep ocean was up to 12 degrees Celsius warmer than it is today. During the hyperthermals, the oceans warmed an additional 3 degrees Celsius.

“Though the exact cause of the hyperthermal events is debated, and they occurred long before the existence of humans, these hyperthermals are the best analogs we have for future climate change,” Kirtland Turner said.

By analyzing tiny fossil shells from different sea floor locations around the globe, the researchers reconstructed patterns of deep ocean circulation during these hyperthermal events. The shells are from microorganisms called foraminifera, which can be found living throughout the world’s oceans, both on the surface and on the sea floor. They are about the size of a period at the end of a sentence.

“As the creatures are building their shells, they incorporate elements from the oceans, and we can measure the differences in the chemistry of these shells to broadly reconstruct information about ancient ocean temperatures and circulation patterns,” Kirtland Turner said.

The shells themselves are made of calcium carbonate. Oxygen isotopes in the calcium carbonate are indicators of temperatures in the water the organisms grew in, and the amount of ice on the planet at the time.

The researchers also examined carbon isotopes in the shells, which reflect the age of the water where the shells were collected, or how long water has been isolated from the ocean surface. In this way, they can reconstruct patterns of deep ocean water movement.

Foraminifera can’t photosynthesize, but their shells indicate the impact of photosynthesis of other organisms nearby, like phytoplankton. “Photosynthesis occurs in the surface ocean only, so water that has recently been at the surface has a carbon-13 rich signal that is reflected in the shells when that water sinks to the deep ocean,” Kirtland Turner said.

“Conversely, water that has been isolated from the surface for a long time has built up relatively more carbon-12 as the remains of photosynthetic organisms sink and decay. So, older water has relatively more carbon-12 compared to ‘young’ water.”

Scientists often make predictions about ocean circulation today using computer climate models. They use these models to answer the question: ‘how is the ocean going to change as the planet keeps warming?’ This team similarly used models to simulate the ancient ocean’s response to warming. They then used the foraminifera shell analysis to help test results from their climate models.

During the Eocene, there were about 1,000 parts per million (ppm) of carbon dioxide in the atmosphere, which contributed to that era’s high temperatures. Today, the atmosphere holds about 425 ppm.

However, humans emit nearly 37 billion tons of CO2 into the atmosphere each year; if these emission levels continue, similar conditions to the Early Eocene could occur by the end of this century.

Therefore, Kirtland Turner argues it is imperative to make every effort to reduce emissions.

“It’s not an all-or-nothing situation,” she said. “Every incremental bit of change is important when it comes to carbon emissions. Even small reductions of CO2 correlate to less impacts, less loss of life, and less change to the natural world.”

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