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Carbon's Crystal Crawl Caught
Apr 2009
BERKELEY, Calif., April 1, 2009 — Carbon atoms moving along the edge of a graphene crystal have been captured on film, the first-ever live recording of the dynamics of carbon atoms in graphene. The work could lead to a new level of understanding and control of nanomaterials, such as those needed to advance artificial photosynthesis.

Graphene – single-layered sheets of carbon atoms arranged like chicken wire – may hold the key to the future of the electronics industry.
3-D rendering of a graphene hole imaged on TEAM 0.5 showing that the carbon atoms along the edge assume either a zigzag or an armchair configuration. The zigzag is the more stable configuration and shows promise for future spintronic technologies. (Image: Berkeley Lab)
Researchers with the Lawrence Berkeley National Laboratory (Berkeley Lab), working with TEAM (transmission electron aberration-corrected microscope) 0.5, the world’s most powerful transmission electron microscope, made the movie, which shows in real time carbon atoms repositioning themselves around the edge of a hole punched into a graphene sheet. Viewers can observe how chemical bonds break and form as the suddenly volatile atoms are driven to find a stable configuration.

“The atom-by-atom growth or shrinking of crystals is one of the most fundamental problems of solid-state physics, but is especially critical for nanoscale systems where the addition or subtraction of even a single atom can have dramatic consequences for mechanical, optical, electronic, thermal and magnetic properties of the material,” said physicist Alex Zettl, who led the research. “The ability to see individual atoms move around in real time and to see how the atomic configuration evolves and influences system properties is somewhat akin to a biologist being able to watch as cells divide and a higher order structure with complex functionality evolves.”

This Quick Time movie produced with the TEAM 0.5 microscope shows the growth of a hole and the atomic edge reconstruction in a graphene sheet. An electron beam focused to a spot on the sheet blows out the exposed carbon atoms to make the hole. The carbon atoms then reposition themselves to find a stable configuration.
Zettl holds joint appointments with Berkeley Lab’s Materials Sciences Division (MSD) and the Physics Department at the University of California (UC) Berkeley, where he is the director of the Center of Integrated Nanomechanical Systems. He is the principal author of a paper describing this work which appeared in the March 27 issue of the journal Science.

The newest instrument at Berkeley Lab’s National Center for Electron Microscopy (NCEM) - a DoE national user facility and the country’s premier center for electron microscopy and microcharacterization - TEAM 0.5 is capable of producing images with half angstrom resolution, which is less than the diameter of a single hydrogen atom.

“The real-time observation of the movements of edge atoms could lead to a new level of understanding and control of nanomaterials," said NCEM Director Ulrich Dahmen. "With further advances in electron-optical correctors and detectors it may become possible to increase the sensitivity and speed of such observations, and begin to see a live view of many other reactions at the atomic scale.”

Rubbing graphene off the end of a pencil tip and suspending the specimen in an observation grid, Zettl and his colleagues used prolonged irradiation from TEAM 0.5’s electron beam (set at 80 kV) to introduce a hole into the graphene’s pristine hexagonal carbon lattice. Focusing the beam to a spot on the sheet blows out the exposed carbon atoms to create the hole.

Since atoms at the edge of the hole are continually being ejected from the lattice by electrons from the beam, the size of the hole grows. The researchers used the same TEAM 0.5 electron beam to record for analysis a movie showing the growth of the hole and the rearrangement of the carbon atoms.

“Atoms that lose their neighbors become highly volatile, and move around rapidly, continually repositioning themselves from one metastable configuration to the next,” said Zettl. “Although configurations come and go, we found a zigzag configuration to be the most stable. It occurs more often and over longer length scales along the edge than the other most common configuration, which we called the armchair.”

The atomic dynamics of the hole in graphene was simulated via a kinetic monte carlo method. Probabilities for atomic migration, insertion and ejection were determined by ab-initio calculation. The simulation starts with a predefined hole in a graphene sheet. As it proceeds, the hole grows and the atoms along the edge rearrange themselves. The zigzag configuration is found to dominate the armchair one.
Understanding which of these atomic configurations is the most stable is one of the keys to predicting and controlling the stability of a device that utilizes graphene edges. The discovery of strong stability in the zigzag configuration is particularly promising news for the spintronic dreams of the computer industry.

Two years ago, co-authors Marvin Cohen and Steven Louie, theorists who hold joint appointments with Berkeley Lab’s Materials Sciences Division and UC Berkeley, calculated that nanoribbons of graphene can conduct a spin current and could therefore serve as the basis for nanosized spintronic devices. Spin, a quantum mechanical property arising from the magnetic field of a spinning electron, carries a directional value of either “up” or “down” that can be used to encode data in the 0s and 1s of the binary system. Spintronic devices promise to be smaller, faster and far more versatile than today’s devices because – among other advantages – data storage does not disappear when the electric current stops.
Alex Zettl, a physicist who holds joint appointments with Berkeley Lab and UC Berkeley, led the first live recording of carbon atoms in action at graphene edge. His previous accomplishments included the first fully functional radio from a single carbon nanotube, and a nanoscale mass sensor that can weigh individual atoms. (Photo: Berkeley Lab)
“Our calculations showed that zigzag graphene nanoribbons are magnetic and can carry a spin current in the presence of a sufficiently large electric field. By carefully controlling the electric field, it should be possible to generate, manipulate, and detect electron spins and spin currents in spintronics applications,” said Cohen.

“If electric fields can be made to produce and manipulate a 100-percent spin-polarized carrier system through a chosen geometric structure, it will revolutionize spintronics technology,” said Louie.

For Zettl and his movie-making collaborators, next up they will correlate the atomic dynamics in graphene that they can now observe in real time with such properties as electrical conduction, optical response and magnetism. This will be a major advance towards fully understanding and applying graphene to spintronic technology as well as other electronic and photovoltaic devices.

“While graphene is particularly exciting, our experimental methods should be applicable to other materials, including other 2-D systems as well,” Zettl said. “We are vigorously pursuing these areas of research in collaboration with the theorists and the staff at NCEM.”

"The ability to observe the dynamics of single carbon atoms is a dream come true that reaches beyond investigations of graphene. In fact it gets us one step closer to understanding artificial photosynthesis, which is considered to be an ultimate energy technology and is being pursued at Berkeley Lab through the Helios Project," said NCEM principal investigator and paper co-author Christian Kisielowski.

Other co-authors on the paper, “Graphene at the Edge: Stability and Dynamics,” were Çaglar Girit, Jannik Meyer, Rolf Erni, Marta Rossell, Li Yang, Cheol-Hwan Park, and Michael Crommie.

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A solid with a structure that exhibits a basically symmetrical and geometrical arrangement. A crystal may already possess this structure, or it may acquire it through mechanical means. More than 50 chemical substances are important to the optical industry in crystal form. Large single crystals often are used because of their transparency in different spectral regions. However, as some single crystals are very brittle and liable to split under strain, attempts have been made to grind them very...
A charged elementary particle of an atom; the term is most commonly used in reference to the negatively charged particle called a negatron. Its mass at rest is me = 9.109558 x 10-31 kg, its charge is 1.6021917 x 10-19 C, and its spin quantum number is 1/2. Its positive counterpart is called a positron, and possesses the same characteristics, except for the reversal of the charge.
The technology of generating and harnessing light and other forms of radiant energy whose quantum unit is the photon. The science includes light emission, transmission, deflection, amplification and detection by optical components and instruments, lasers and other light sources, fiber optics, electro-optical instrumentation, related hardware and electronics, and sophisticated systems. The range of applications of photonics extends from energy generation to detection to communications and...
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