Mirror, mirror on the wall…

…. Now we know there are chiral phonons for sure

Findings published in Nature settle the dispute: phonons can be chiral. This fundamental concept, discovered using circular X-ray light, sees phonons twisting like a corkscrew through quartz.

Throughout nature, at all scales, you can find examples of chirality – or handedness. Imagine trying to eat a sandwich with two hands that were not enantiomers – non-superimposable mirror images – of each other. Consider the pharmacological disasters caused by administering the wrong drug enantiomer or, at a subatomic scale, the importance of the concept of parity in particle physics. Now, thanks to a new study led by researchers at PSI, we know that phonons can also possess this property.

A phonon is a quasiparticle that describes the collective vibrational excitations of the atoms in a crystal lattice; imagine it as the Irish Riverdance of the atoms. Physicists have predicted that if phonons can demonstrate chirality they could have important implications on the fundamental physical properties of materials. With the rapid rise in recent years of research into topological materials that exhibit curious electronic and magnetic surface properties, interest in chiral phonons has grown. Yet, experimental proof for their existence has remained elusive.

What makes phonons chiral is the steps of their dance. In the new study, the atomic vibrations dance a twist that moves forwards like a corkscrew. This corkscrew motion is one of the reasons there has been such a drive to discover the phenomenon. If phonons can revolve in this way, like the coil of wire that forms a solenoid, perhaps they could create a magnetic field in a material.  

A new slant on the problem

It is this possibility that motivated the group of Urs Staub at PSI, who led the study. “It is because we are at the juncture between ultrafast X-ray science and materials research that we could approach the problem from a different angle,” he says. The researchers are interested in manipulating chiral modes of materials using chiral light – light that is circularly polarised.

It was using such light that the researchers could make their proof. Using quartz, one of the best-known minerals whose atoms – silicon and oxygen – form a chiral structure, they showed how circularly polarised light coupled to chiral phonons. To do this, they used a technique known as resonant inelastic X-ray scattering (RIXS) at the Diamond Light Source in the UK. This was complemented with supporting theoretical descriptions of how the process would create and enable the detection of chiral phonons from groups at the ETH Zurich (Carl Romao and Nicola Spaldin) and MPI Dresden (Jeroen van den Brink).

Read more on the PSI website

Image: To prove the existence of chiral phonons, researchers used resonant inelastic X-rays scattering (RIXS). Circularly polarised light shines on quartz. The angular momentum of the photons is transferred to a crystal, causing a revolution in this case of anions (orange spheres with p orbitals) relative to their neighbouring cations (green spheres).

Credit: Paul Scherrer Institute / Hiroki Ueda and Mahir Dzambegovic

RIXS Shows Flat-Band Stoner Excitations in a Kagome Semimetal

A sensitive synchrotron technique uncovers exotic behaviour important to next-gen electronics

Topological materials (including topological insulators, Dirac and Weyl semimetals and skyrmions) are a hot topic in science at the moment. A gold rush of sorts is underway, to discover and investigate the exotic physical properties of these materials, which could be the key that unlocks next-generation energy-efficient electronic devices and quantum computing. In some materials, geometrical confinement of electrons can give rise to electronic correlations that manifest as dispersionless ‘flat’ bands. These flat bands are of particular interest, as they can result in unconventional ferromagnetic and transport behaviour. However, there have been few characterisations of flat bands and their magnetism. In work recently published in Nature Communications, scientists from Diamond’s I21 beamline used resonant inelastic X-ray scattering (RIXS) to investigate the ferromagnetic Kagome semimetal Co3Sn2S2, reporting the first observation of flat-band Stoner excitations in this material. Their results also demonstrate that RIXS can clarify the magnon-Stoner interactions in itinerant correlated flat band systems. 

Mirian Garcia-Fernandez’s #My1stLight

Diamond’s I21 Resonant Inelastic X-ray Scattering (RIXS) beamline achieved first light in 2016. Mirian’s #My1st Light contribution shows the I21 team in the Diamond Control Room observing this fantastic achievement.

I21 is a dedicated Resonant Inelastic soft X-ray Scattering (RIXS) beamline that provides a highly monochromatised, focused and tunable X-ray beam onto materials, while detecting and energy-analysing scattered X-rays using a spatially-resolved two-dimensional detector. By studying the energy and momentum differences between the incident and the outgoing X-rays, one can obtain information such as the local lattice structure (local crystal field), electron orbitals (orbital excitations), collective lattice vibration (phonons), magnetic (spinons/magnons) and charge excitations of the material under investigation.

Find out more on the beamline’s webpage

Unravelling tautomeric mixtures

RIXS at BESSY II allows to see clearly

A team at HZB has developed a method of experimentally unravelling tautomeric mixtures. Based on resonant inelastic X-ray scattering (RIXS) at BESSY II, not only proportions of the tautomers can be deduced, but the properties of each individual tautomer can be studied selectively. This method could yield to detailed information on the properties of molecules and their biological function. In the present study, now advertised on the cover of “The Journal of Physical Chemistry Letters” the technique was applied to the prototypical keto-enol equilibrium.

Many (organic) molecules exist as a mixture of two almost identical molecules, with the same molecular formula but one important difference: A single hydrogen atom sits in a different position. The two isomeric forms transform into each other, creating a delicate equilibrium, a “tautomeric” mixture. Many amino acids are tautomeric mixtures, and since they are building blocks of proteins, they may influence their shape and function and thus their biological functions in organisms.

Until now: Mission impossible

Until now, it has been impossible to selectively investigate the electronic structure of such tautomeric mixtures experimentally: Classical spectroscopic methods “see” only the sum of the signals of each molecular forms – the details of the properties of the two individual tautomers cannot be determined.

Now at BESSY II: it works

A team led by HZB physicist Prof. Alexander Föhlisch has now succeeded in providing a method of experimentally unravelling tautomeric mixtures. Using inelastic X-ray scattering (RIXS) and a data processing/evaluation method newly developed at HZB, the individual proportions of the tautomers can be clearly deduced from the measured data. “We can experimentally separate the signal of each individual molecule in the mixture by X-ray scattering, which leads to a detailed insight into their functionality and chemical properties,” says Dr. Vinicíus Vaz Da Cruz, first author of the paper and postdoc in Föhlisch’s team.

Read more on the HZB website

Image: The illustration visualises the experimental method, here on the prototypical keto-enol equilibrium. It appears on the cover of “The Journal of Physical Chemistry Letters”.

Credit: © Martin Künsting / HZB

New discovery will have huge impact on the development of future battery cathodes

A new paper published today in Nature Energy reveals how a collaborative team of researchers have been able to fully identify the nature of oxidised oxygen in the important battery material – Li-rich NMC – using RIXS (Resonant Inelastic X-ray Scattering) at Diamond. This compound is being closely considered for implementation in next generation Li-ion batteries because it can deliver a higher energy density than the current state-of-the-art materials, which could translate to longer driving ranges for electric vehicles. They expect that their work will enable scientists to tackle issues like battery longevity and voltage fade with Li-rich materials.

The paper, ‘First cycle voltage hysteresis in Li-rich 3d cathodes associated with molecular O2 trapped in the bulk’ by a joint team from the University of Oxford, the Henry Royce and Faraday Institutions and Diamond, examines the results of their investigations to better understand the important compound known in the battery industry as Li-rich NMC (or Li1.2Ni0.13Co0.13Mn0.54O2).   

Principal Beamline Scientist on I21 RIXS at Diamond, Kejin Zhou,said:

Our work is much about understanding the mysterious first cycle voltage hysteresis in which the O-redox process cannot be fully recovered resulting in the loss of the voltage hence the energy density.

Read more on the Diamond website

Image: A previous study (Nature 577, 502–508 (2020)) into this process made by the same research team, at the I21 beamline at Diamond, reported that, in Na-ion battery cathodes, the voltage hysteresis is related to the formation of molecular O2 trapped inside of the particles due to the migration of transition metal ions during the charging process.

Classic double-slit experiment in a new light

An international research team led by physicists from Collaborative Research Centre 1238, ‘Control and Dynamics of Quantum Materials’ at the University of Cologne has implemented a new variant of the basic double-slit experiment using resonant inelastic X-ray scattering at the European Synchrotron ESRF in Grenoble. This new variant offers a deeper understanding of the electronic structure of solids. Writing in Science Advances, the research group have now presented their results under the title ‘Resonant inelastic x-ray incarnation of Young’s double-slit experiment’.

The double-slit experiment is of fundamental importance in physics. More than 200 years ago, Thomas Young diffracted light at two adjacent slits, thus generating interference patterns (images based on superposition) behind this double slit. That way, he demonstrated the wave character of light. In the 20th century, scientists have shown that electrons or molecules scattered on a double slit show the same interference pattern, which contradicts the classical expectation of particle behaviour, but can be explained in quantum-mechanical wave-particle dualism. In contrast, the researchers in Cologne investigated an iridium oxide crystal (Ba3CeIr2O9) by means of resonant inelastic X-ray scattering (RIXS).

>Read more on the European Synchrotron website

Image: Beamline ID20, where the experiments took place.
Credit: P. Jayet.