The boundary between a substance’s liquid and solid phases may not be as clear-cut as previously believed. A new state of matter that is a hybrid of both has emerged in research by scientists at the University of Nottingham, UK and the University of Ulm, Germany, and they say the discovery could have applications in catalysis and other thermally-activated processes.

In liquids, atoms move rapidly, sliding over and around each other in a random fashion. In solids, they are fixed in place. The transition between the two states, solidification, occurs when random atomic motion transitions to an ordered crystalline structure.

At least, that’s what we thought. Thanks to a specialist microscopy technique, researchers led by Nottingham’s Andrei Khlobystov found that this simple picture isn’t entirely accurate. In fact, liquid metal nanoparticles can contain stationary atoms – and as the liquid cools, their number and position play a significant role in solidification.

Some atoms remain stationary

The team used a method called spherical and chromatic aberration-corrected high-resolution transmission electron microscopy (Cc/Cs-corrected HRTEM) at the low-voltage SALVE instrument at Ulm to study melted metal nanoparticles (such as platinum, gold and palladium) deposited on an atomically thin layer of graphene. This carbon-based material acted a sort of “hob” for heating the particles, says team member Christopher Leist, who was in charge of the HRTEM experiments. “As they melted, the atoms in the nanoparticles began to move rapidly, as expected,” Leist says. “To our surprise, however, we found that some atoms remained stationary.”

At high temperatures, these static atoms bind strongly to point defects in the graphene support. When the researchers used the electron beam from the transmission microscope to increase the number of these defects, the number of stationary atoms within the liquid increased, too. Khlobystov says that this had a knock-on effect on how the liquid solidified: when the stationary atoms are few in number, a crystal forms directly from the liquid and continues to grow until the entire particle has solidified. When their numbers increase, the crystallization process cannot take place and no crystals form.

“The effect is particularly striking when stationary atoms create a ring (corral) that surrounds and confines the liquid,” he says. “In this unique state, the atoms within the liquid droplet are in motion, while the atoms forming the corral remain motionless, even at temperatures well below the freezing point of the liquid.”

Unprecedented level of detail

The researchers chose to use Cc/Cs-corrected HRTEM in their study because minimizing spherical and chromatic aberrations through specialized hardware installed on the microscope enabled them to resolve single atoms in their images.

“Additionally, we can control both the energy of the electron beam and the sample temperature (the latter using MEMS-heated chip technology),” Khlobystov explains. “As a result, we can study metal samples at temperatures of up to 800 °C, even in a molten state, without sacrificing atomic resolution. We can therefore observe atomic behaviour during crystallization while actively manipulating the environment around the metal particles using the electron beam or by cooling the particles. This level of detail under such extreme conditions is unprecedented.”

Effect could be harnessed for catalysis

The Nottingham-Ulm researchers, who report their work in ACS Nano, say they obtained their results by chance while working on an EPSRC-funded project on 1-2 nm metal particles for catalysis applications. “Our approach involves assembling catalysts from individual metal atoms, utilizing on-surface phenomena to control their assembly and dynamics,” explains Khlobystov. “To gain this control, we needed to investigate the behaviour of metal atoms at varying temperatures and within different local environments on a support material.

“We suspected that the interplay between vacancy defects in the support and the sample temperature creates a powerful mechanism for controlling the size and structure of the metal particles,” he tells Physics World. “Indeed, this study revealed the fundamental mechanisms behind this process with atomic precision.”

The experiments were far from easy, he recalls, with one of the key challenges being to identify a thin, robust and thermally conductive support material for the metal. Happily, graphene meets all these criteria.

“Another significant hurdle to overcome was to be able to control the number of defect sites surrounding each particle,” he adds. “We successfully accomplished this by using the TEM’s electron beam not just as an imaging tool, but also as a means to modify the environment around the particles by creating defects.”

The researchers say they would now like to explore whether the effect can be harnessed for catalysis. To do this, Khlobystov says it will be essential to improve control over defect production and its scale. “We also want to image the corralled particles in a gas environment to understand how the phenomenon is influenced by reaction conditions, since our present measurements were conducted in a vacuum,” he adds.

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Physicists in the UK have succeeded in routing and teleporting entangled states of light between two four-user quantum networks – an important milestone in the development of scalable quantum communications. Led by Mehul Malik and Natalia Herrera Valencia of Heriot-Watt University in Edinburgh, Scotland, the team achieved this milestone thanks to a new method that uses light-scattering processes in an ordinary optical fibre to program a circuit. This approach, which is radically different from conventional methods based on photonic chips, allows the circuit to function as a programmable entanglement router that can implement several different network configurations on demand.

The team performed the experiments using commercially-available optical fibres, which are multi-mode structures that scatter light via random linear optical processes. In simple terms, Herrera Valencia explains that this means the light tends to ricochet chaotically through the fibres along hundreds of internal pathways. While this effect can scramble entanglement, researchers at the Institut Langevin in Paris, France had previously found that the scrambling can be calculated by analysing how the fibre transmits light. What is more, the light-scattering processes in such a medium can be harnessed to make programmable optical circuits – which is exactly what Malik, Herrera Valencia and colleagues did.

“Top-down” approach

The researchers explain that this “top-down” approach simplifies the circuit’s architecture because it separates the layer where the light is controlled from the layer in which it is mixed. Using waveguides for transporting and manipulating the quantum states of light also reduces optical losses. The result is a reconfigurable multi-port device that can distribute quantum entanglement between many users simultaneously in multiple patterns, switching between different channels (local connections, global connections or both) as required.

A further benefit is that the channels can be multiplexed, allowing many quantum processors to access the system at the same time. The researchers say this is similar to multiplexing in classical telecommunications networks, which makes it possible to send huge amounts of data through a single optical fibre using different wavelengths of light.

Access to a large number of modes

Although controlling and distributing entangled states of light is key for quantum networks, Malik says it comes with several challenges. One of these is that conventional methods based on photonics chips cannot be scaled up easily. They are also very sensitive to imperfections in how they’re made. In contrast, the waveguide-based approach developed by the Heriot-Watt team “opens up access to a large number of modes, providing significant improvements in terms of achievable circuit size, quality and loss,” Malik tells Physics World, adding that the approach also fits naturally with existing optical fibre infrastructures.

Gaining control over the complex scattering process inside a waveguide was not easy, though. “The main challenge was the learning curve and understanding how to control quantum states of light inside such a complex medium,” Herrera Valencia recalls. “It took time and iteration, but we now have the precise and reconfigurable control required for reliable entanglement distribution, and even more so for entanglement swapping, which is essential for scalable networks.”

While the Heriot-Watt team used the technique to demonstrate flexible quantum networking, Malik and Herrera Valencia say it might also be used for implementing large-scale photonic circuits. Such circuits could have many applications, ranging from machine learning to quantum computing and networking, they add.

Looking ahead, the researchers, who report their work in Nature Photonics, say they are now aiming to explore larger-scale circuits that can operate on more photons and light modes. “We would also like to take some of our network technology out of the laboratory and into the real world,” says Malik, adding that Herrera Valencia is leading a commercialization effort in that direction.

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