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Chang-Beom Eom, Shane Lindemann and Mark Rzchowski
February 5, 2020

Layers without limits: Advance enables researchers to stack complex oxides at will

Written By: Renee Meiller

In the technology world, complex oxides are “wonder” materials that can have a wide array of electronic, magnetic and optical properties. As a result, they could enable next-generation electronics, data storage, sensing, energy technologies, biomedical devices, and many other applications.

Stacking ultrathin complex oxide single-crystal layers—or those composed of geometrically arranged atoms—allows researchers to create new heterostructures with hybrid properties and multiple functionalities. Now, a revolutionary platform developed by engineers at the University of Wisconsin-Madison and MIT will enable researchers to achieve these stacks in virtually unlimited combinations.

The team published details of the advance in the Feb. 5, 2020, issue of the journal Nature.

Epitaxy is the process for depositing one material on top of another in an orderly way. The researchers’ new platform overcomes a major challenge in conventional epitaxy—that each new complex oxide layer must be closely compatible with the atomic structure of the underlying layer. It’s sort of like stacking Lego blocks: The holes on the bottom of one block must align with the raised dots atop the other. If there’s a mismatch, the blocks won’t fit together properly.

Images of single-crystal oxides
To grow layers of single-crystal oxides for electronic components requires neighboring layers to interlock like Lego blocks. A new method throws out that limitation, producing new capabilities for data storage, sensing, energy technologies, biomedical devices and many other applications. Photo courtesy of Chang-Beom Eom.

“The advantage of the conventional method is that you can grow a perfect single crystal on top of a substrate, but you have a limitation,” says Chang-Beom Eom, a professor of materials science and engineering and physics at UW-Madison. “When you grow the next material, your structure has to be the same and your atomic spacing must be similar. That’s a constraint—and beyond that constraint, it doesn’t grow well.”

A couple of years ago, a team of MIT researchers developed an alternate approach. Led by Jeehwan Kim, an associate professor in mechanical engineering and materials science and engineering at MIT, the group added an ultrathin intermediate layer of a unique carbon material called graphene, then used epitaxy to grow a thin semiconducting material layer atop that. Just one molecule thick, the graphene acts like a peel-away backing due to its weak bonding. The researchers could remove the semiconductor layer from the graphene and what remained was an freestanding ultrathin sheet of semiconducting material.

Eom is a world expert in complex oxide materials, and says they are intriguing because they have a wide range of tunable properties—including multiple properties in one material—that many other materials do not.

So it made sense to apply the peel-away technique to complex oxides, which are much more challenging to grow and integrate. “If you have this kind of cut-and-paste growth and removal, combined with the different functionality of putting single-crystal oxide materials together, you have a tremendous possibility for making devices and doing science,” says Eom, who connected with mechanical engineers at MIT during a sabbatical there in 2014.

The Eom and Kim research groups combined their expertise to create ultrathin complex oxide single-crystal layers, again using graphene as the peel-away intermediate. More importantly, however, they conquered a previously insurmountable obstacle—the difference in crystal structure—in integrating different complex oxide materials. “Magnetic materials have one crystal structure, while piezoelectric materials have another,” says Eom. “So you cannot grow them on top of each other. When you try to grow them, it just becomes messy. Now we can grow the layers separately, peel them off, and integrate them.”

In their research, the team demonstrated the efficacy of the technique using materials such as perovskite, spinel and garnet, among several others. They also can stack single complex oxide materials and semiconductors.

The platform presents an opportunity for researchers to learn in ways they never could before. “This opens up the possibility for the study of new science, which has never been possible in the past because we could not grow it,” says Eom. “Stacking these was impossible, but now it is possible to imagine infinite combinations of materials. Now we can put them together.”

The advance also flings the door wide open for new materials with functionalities that could make vast improvements in future technologies. “What Dr. Eom and colleagues have done has essentially made it possible to arbitrarily stack layers of perfect materials without any loss of material quality,” says Evan Runnerstrom, program manager in materials design in the Army Research Office, which funded part of the research. “This advance, which would have been impossible using conventional thin film growth techniques, clears the way for nearly limitless possibilities in materials design. The ability to create perfect interfaces while coupling disparate classes of complex materials may enable entirely new behaviors and tunable properties, which could potentially be leveraged for new Army capabilities in communications, reconfigurable sensors, low power electronics, and quantum information science.”

Eom is the Raymond R. Holton Chair Professor and Theodore H. Geballe Professor in materials science and engineering and physics at UW-Madison.

Hyungwoo Lee and Shane Lindemann of UW-Madison and Hyun S. Kum and Sungkyu Kim of MIT all contributed equally to the paper. Other UW-Madison authors include Julian Irwin and Physics Professor Mark S. Rzchowski. Other MIT authors include Wei Kong, Kuan Qiao, Peng Chen, Jaewoo Shim, Sang-Hoon Bae, Chanyeol Choi, Luigi Ranno, Seungju Seo, Sangho Lee, Jackson Bauer and Caroline A. Ross. Additional authors include June Hyuk Lee of the Korea Atomic Energy Research Institute, Saien Xie and Darrell G. Schlom of Cornell University, Shruti Subramanian and Joshua A. Robinson of The Pennsylvania State University, Huashan Li of Sun Yat-Sen University in China, and Kyusang Lee of the University of Virginia.

The team at MIT and the University of Wisconsin-Madison acknowledge support by the Defense Advanced Research Projects Agency (DARPA) (award number 027049-00001, W. Carters and J. Gimlett). The work at the University of Wisconsin-Madison is also supported by the Army Research Office through grant W911NF-17-1-0462.