Tag Archives: Klaas-Jan Tielrooij

A graphene joke (of sorts): What did the electron ‘say’ to the phonon in the graphene sandwich?

Unfortunately, there isn’t a punch line but I appreciate the effort to inject a little lightness into the description of a fairly technical achievement, from a February 12, 2024 news item on Nanowerk, Note: A link has been removed,

Electrons carry electrical energy, while vibrational energy is carried by phonons. Understanding how they interact with each other in certain materials, like in a sandwich of two graphene layers, will have implications for future optoelectronic devices.

Key Takeaways

Twisted graphene layers exhibit unique electrical properties.

Electron-phonon interactions crucial for energy loss in graphene.

Discovery of a new physical process involving electron-phonon Umklapp scattering.

Potential implications for ultrafast optoelectronics and quantum applications.

A February 9, 2024 Eindhoven University of Technology (TU/e; Netherlands) press release, which originated the news item, is reproduced here in its entirety, Note: Links have been removed,

Electrons carry electrical energy, while vibrational energy is carried by phonons. Understanding how they interact with each other in certain materials, like in a sandwich of two graphene layers, will have implications for future optoelectronic devices. Recent work has revealed that graphene layers twisted relative to each other by a small ‘magic angle’ can act as perfect insulator or superconductor. But the physics of the electron-phonon interactions are a mystery. As part of a worldwide international collaboration, TU/e researcher Klaas-Jan Tielrooij has led a study on electron-phonon interactions in graphene layers. And they have made a startling discovery.

What did the electron say to the phonon between two layers of graphene?

This might sound like the start of a physics meme with a hilarious punchline to follow. But that’s not the case according to Klaas-Jan Tielrooij. He’s an associate professor at the Department of Applied Physics and Science Education at TU/e and the research lead of the new work published in Science Advances.

“We sought to understand how electrons and phonons ‘talk’ to each other within two twisted graphene layers,” says Tielrooij.

Electrons are the well-known charge and energy carriers associated with electricity, while a phonon is linked to the emergence of vibrations between atoms in an atomic crystal.

“Phonons aren’t particles like electrons though, they’re a quasiparticle. Yet, their interaction with electrons in certain materials and how they affect energy loss in electrons has been a mystery for some time,” notes Tielrooij.

But why would it be interesting to learn more about electron-phonon interactions? “These interactions can have a major effect on the electronic and optoelectronic properties of devices, made from materials like graphene, which we are going to see more of in the future.”

Twistronics: Breakthrough of the Year 2018

Tielrooij and his collaborators, who are based around the world in Spain, Germany, Japan, and the US, decided to study electron-phonon interactions in a very particular case – within two layers of graphene where the layers are ever-so-slightly misaligned.

Graphene is a two-dimensional layer of carbon atoms arranged in a honeycomb lattice that has several impressive properties such as high electrical conductivity, high flexibility, and high thermal conductivity, and it is also nearly transparent.

Back in 2018, the Physics World Breakthrough of the Year award went to Pablo Jarillo-Herrero and colleagues at MIT [Massachusetts Institute of Technology] for their pioneering work on twistronics, where adjacent layers of graphene are rotated very slightly relative to each other to change the electronic properties of the graphene.

Twist and astound!

“Depending on how the layers of graphene are rotated and doped with electrons, contrasting outcomes are possible. For certain dopings, the layers act as an insulator, which prevents the movement of electrons. For other doping, the material behaves as a superconductor – a material with zero resistance that allows the dissipation-less movement of electrons,” says Tielrooij.

Better known as twisted bilayer graphene, these outcomes occur at the so-called magic angle of misalignment, which is just over one degree of rotation. “The misalignment between the layers is tiny, but the possibility for a superconductor or an insulator is an astounding result.”

How electrons lose energy

For their study, Tielrooij and the team wanted to learn more about how electrons lose energy in magic-angle twisted bilayer graphene, or MATBG for short.

To achieve this, they used a material consisting of two sheets of monolayer graphene (each 0.3 nanometers thick), placed on top of each other, and misaligned relative to each other by about one degree.

Then using two optoelectronic measurement techniques, the researchers were able to probe the electron-phonon interactions in detail, and they made some staggering discoveries.

“We observed that the energy vanishes very quickly in the MATBG – it occurs on the picosecond timescale, which is one-millionth of one-millionth of a second!” says Tielrooij.

This observation is much faster than for the case of a single layer of graphene, especially at ultracold temperatures (specifically below -73 degrees Celsius). “At these temperatures, it’s very difficult for electrons to lose energy to phonons, yet it happens in the MATBG.”

Why electrons lose energy

So, why are the electrons losing the energy so quickly through interaction with the phonons? Well, it turns out the researchers have uncovered a whole new physical process.

“The strong electron-phonon interaction is a completely new physical process and involves so-called electron-phonon Umklapp scattering,” adds Hiroaki Ishizuka from Tokyo Institute of Technology in Japan, who developed the theoretical understanding of this process together with Leonid Levitov from Massachusetts Institute of Technology in the US.

Umklapp scattering between phonons is a process that often affects heat transfer in materials, because it enables relatively large amounts of momentum to be transferred between phonons.

“We see the effects of phonon-phonon Umklapp scattering all the time as it affects the ability for (non-metallic) materials at room temperature to conduct heat. Just think of an insulating material on the handle of a pot for example,” says Ishizuka. “However, electron-phonon Umklapp scattering is rare. Here though we have observed for the first time how electrons and phonons interact via Umklapp scattering to dissipate electron energy.”

Challenges solved together

Tielrooij and collaborators may have completed most of the work while he was based in Spain at the Catalan Institute of Nanoscience and Nanotechnology (ICN2), but as Tielrooij notes. “The international collaboration proved pivotal to making this discovery.”

So, how did all the collaborators contribute to the research? Tielrooij: “First, we needed advanced fabrication techniques to make the MATBG samples. But we also needed a deep theoretical understanding of what’s happening in the samples. Added to that, ultrafast optoelectronic measurement setups were required to measure what’s happening in the samples too.”

Tielrooij and the team received the magic-angle twisted samples from Dmitri Efetov’s group at Ludwig-Maximilians-Universität in Munich, who were the first group in Europe able to make such samples and who also performed photomixing measurements, while theoretical work at MIT in the US and at Tokyo Institute of Technology in Japan proved crucial to the success of the research.

At ICN2, Tielrooij and his team members Jake Mehew and Alexander Block used cutting-edge equipment particularly time-resolved photovoltage microscopy to perform their measurements of electron-phonon dynamics in the samples.

The future

So, what does the future look like for these materials then? According to Tielrooij, don’t expect anything too soon.

“As the material is only being studied for a few years, we’re still some way from seeing magic-angle twisted bilayer graphene having an impact on society.”

But there is a great deal to be explored about energy loss in the material.

“Future discoveries could have implications for charge transport dynamics, which could have implications for future ultrafast optoelectronics devices,” says Tielrooij. “In particular, they would be very useful at low temperatures, so that makes the material suitable for space and quantum applications.”

The research from Tielrooij and the international team is a real breakthrough when it comes to how electrons and phonons interact with each other.

But we’ll have to wait a little longer to fully understand the consequences of what the electron said to the phonon in the graphene sandwich.

Illustration showing the control of energy relaxation with twist angle. Image: Authors

Here’s a link to and a citation for the paper,

Ultrafast Umklapp-assisted electron-phonon cooling in magic-angle twisted bilayer graphene by Jake Dudley Mehew, Rafael Luque Merino, Hiroaki Ishizuka, Alexander Block, Jaime Díez Mérida, Andrés Díez Carlón, Kenji Watanabe, Takashi Taniguchi, Leonid S. Levitov, Dmitri K. Efetov, and Klaas-Jan Tielrooij. Science Advances 9 Feb 2024 Vol 10, Issue 6 DOI: 10.1126/sciadv.adj1361

This paper is open access.

Water talks to electrons in graphene (i.e., carbon)?

Institutions from Spain, Germany, and England collaborated on the study announced in this June 23, 2023 news item on Nanowerk, Note: A link has been removed,

For the last 20 years, scientists have been puzzled by how water behaves near carbon surfaces. It may flow much faster than expected from conventional flow theories or form strange arrangements such as square ice.

Now, an international team of researchers from the Max Plank Institute for Polymer Research of Mainz (Germany), the Catalan Institute of Nanoscience and Nanotechnology (ICN2, Spain), and the University of Manchester (England), reports in a study published in Nature Nanotechnology (“Electron cooling in graphene enhanced by plasmon–hydron resonance”) that water can interact directly with the carbon’s electrons: a quantum phenomenon that is very unusual in fluid dynamics.

Pictured above: Water-graphene quantum friction (Credits: Lucy Reading-Ikkanda / Simons Foundation)

There are two press releases with almost identical text, the June 22, 2023 Max Planck Institute press release with its additional introductory paragraph is below,

Water and carbon make a quantum couple: the flow of water on a carbon surface is governed by an unusual phenomenon dubbed quantum friction. A work published in ‘Nature Nanotechnology’ experimentally demonstrates this phenomenon – which was predicted in a previous theoretical study— at the interface between liquid water and graphene, a single layer of carbon atoms. Advanced ultrafast techniques were used to perform this study. These results could lead to applications in water purification and desalination processes and maybe even to liquid-based computers.

A liquid, such as water, is made up of small molecules that randomly move and constantly collide with each other. A solid, in contrast, is made of neatly arranged atoms that bathe in a cloud of electrons. The solid and the liquid worlds are assumed to interact only through collisions of the liquid molecules with the solid’s atoms: the liquid molecules do not “see” the solid’s electrons. Nevertheless, just over a year ago, a paradigm-shifting theoretical study proposed that at the water-carbon interface, the liquid’s molecules and the solid’s electrons push and pull on each other, slowing down the liquid flow: this new effect was called quantum friction. However, the theoretical proposal lacked experimental verification.

“We have now used lasers to see quantum friction at work,” explains study lead author Dr Nikita Kavokine, a researcher at the Max Planck Institute in Mainz and the Flatiron Institute in New York. The team studied a sample of graphene – a single monolayer of carbon atoms arranged in a honeycomb pattern. They used ultrashort red laser pulses (with a duration of only a millionth of a billionth of a second) to instantaneously heat up the graphene’s electron cloud. They then monitored its cooling with terahertz laser pulses, which are sensitive to the temperature of the graphene electrons. This technique is called optical pump – terahertz probe (OPTP) spectroscopy.

To their surprise, the electron cloud cooled faster when the graphene was immersed in water, while immersing the graphene in ethanol made no difference to the cooling rate. “This was yet another indication that the water-carbon couple is somehow special, but we still had to understand what exactly was going on,” Kavokine says. A possible explanation was that the hot electrons push and pull on the water molecules to release some of their heat: in other words, they cool through quantum friction. The researchers delved into the theory, and indeed: water-graphene quantum friction could explain the experimental data.

“It’s fascinating to see that the carrier dynamics of graphene keep surprising us with unexpected mechanisms, this time involving solid-liquid interactions with molecules none other than the omnipresent water,” comments Prof Klaas-Jan Tielrooij from ICN2 (Spain) and TU Eindhoven (The Netherlands). What makes water special here is that its vibrations, called hydrons, are in sync with the vibrations of the graphene electrons, called plasmons, so that the graphene-water heat transfer is enhanced through an effect known as resonance.

The experiments thus confirm the basic mechanism of solid-liquid quantum friction. This will have implications for filtration and desalination processes, in which quantum friction could be used to tune the permeation properties of the nanoporous membranes. “Our findings are not only interesting for physicists, but they also hold potential implications for electrocatalysis and photocatalysis at the solid-liquid interface,” says Xiaoqing Yu, PhD student at the Max Planck Institute in Mainz and first author of the work.

The discovery was down to bringing together an experimental system, a measurement tool and a theoretical framework that seldom go hand in hand. The key challenge is now to gain control over the water-electron interaction. “Our dream is to switch quantum friction on and off on demand,” Kavokine says. “This way, we could design smarter water filtration processes, or perhaps even fluid-based computers.”   

The almost identical June 26, 2023 University of Manchester press release is here.

Here’s a link to and a citation for the paper,

Electron cooling in graphene enhanced by plasmon–hydron resonance by Xiaoqing Yu, Alessandro Principi, Klaas-Jan Tielrooij, Mischa Bonn & Nikita Kavokine. Nature Nanotechnology (2023) DOI: https://doi.org/10.1038/s41565-023-01421-3 Published: 22 June 2023

This paper is open access.

Converting light to electricity at femto speeds

This is a pretty remarkable (to me anyway) piece of research on speeding up the process of converting light to electricity. From an April 14, 2015 Institute of Photonic Science press release (also on EurekAlert but dated April 15, 2015),

The efficient conversion of light into electricity plays a crucial role in many technologies, ranging from cameras to solar cells. It also forms an essential step in data communication applications, since it allows for information carried by light to be converted into electrical information that can be processed in electrical circuits. Graphene is an excellent material for ultrafast conversion of light to electrical signals, but so far it was not known how fast graphene responds to ultrashort flashes of light.

The new device that the researchers developed is capable of converting light into electricity in less than 50 femtoseconds (a twentieth of a millionth of a millionth of a second). To do this, the researchers used a combination of ultrafast pulse-shaped laser excitation and highly sensitive electrical readout. As Klaas-Jan Tielrooij comments, “the experiment uniquely combined the ultrafast pulse shaping expertise obtained from single molecule ultrafast photonics with the expertise in graphene electronics. Facilitated by graphene’s nonlinear photo-thermoelectric response, these elements enabled the observation of femtosecond photodetection response times.”

The ultrafast creation of a photovoltage in graphene is possible due to the extremely fast and efficient interaction between all conduction band carriers in graphene. This interaction leads to a rapid creation of an electron distribution with an elevated electron temperature. Thus, the energy absorbed from light is efficiently and rapidly converted into electron heat. Next, the electron heat is converted into a voltage at the interface of two graphene regions with different doping. This photo-thermoelectric effect turns out to occur almost instantaneously, thus enabling the ultrafast conversion of absorbed light into electrical signals. As Prof. van Hulst states, “it is amazing how graphene allows direct non-linear detecting of ultrafast femtosecond (fs) pulses”.

The results obtained from the findings of this work, which has been partially funded by the EC Graphene Flagship, open a new pathway towards ultra-fast optoelectronic conversion. As Prof. Koppens comments, “Graphene photodetectors keep showing fascinating performances addressing a wide range of applications”.

Here’s a link to and a citation for the paper,

Generation of photovoltage in graphene on a femtosecond timescale through efficient carrier heating by K. J. Tielrooij, L. Piatkowski, M. Massicotte, A. Woessner, Q. Ma, Y. Lee,  K. S. Myhro, C. N. Lau, P. Jarillo-Herrero, N. F. van Hulst & F. H. L. Koppens. Nature Nanotechnology (2015) doi:10.1038/nnano.2015.54 Published online 13 April 2015

This paper is behind a paywall but there is a free preview via ReadCube Access.