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Ultrafast sonograms shed new light on rapid phase transitions

Vanadium dioxide crystal lattice (A. Julia St盲hler / Fritz Haber Institute)

An international team of physicists has developed a method for taking ultrafast “sonograms” that can track the structural changes that take place within solid materials in trillionth-of-a-second intervals as they go through an important physical process called a phase transition.

Common phase transitions include the melting of candle wax before it burns and dissolving sugar in water. They are purely structural changes that produce dramatic changes in a material鈥檚 physical properties and they play a critical role both in nature and in industrial processes ranging from steel making to chip fabrication.

The researchers have applied this method to shed new light on the manner in which vanadium dioxide, the material that undergoes the fastest phase transition known, shifts between its transparent and reflective phases.

Many of these transitions, like that in vanadium dioxide, take place so rapidly that scientists have had difficulty catching them in the act. 鈥淭his means that there is a lot that we still don鈥檛 know about the dynamics of these critical processes,鈥 said Professor of Physics , who directed the team of Vanderbilt researchers who were involved.

To build a more complete picture of this phenomenon in vanadium dioxide (VO2), one of the most unusual phase-change materials known, Vanderbilt researchers collaborated with physicists at the in Berlin, who have developed the powerful new technique for obtaining a more complete picture of ultrafast phase changes. Details of the method, which can track the structural changes that take place within materials at intervals of less than a trillionth of a second, are in the Mar. 6 issue of the journal .

New details on nature鈥檚 quickest phase-change artist

Vanadium dioxide shifts from a transparent, semiconducting phase to a reflective, metallic phase in the time it takes a beam of light to travel a tenth of a millimeter. This phase change can be caused by heating the material above 150 degrees Fahrenheit (65 degrees Celsius) or by hitting it with a pulse of laser light.

Lost vibrations: In the insulating state, the VO2 crystal structure vibrates at four well-defined frequencies when hit by a low power laser pulse. These vibrations modulate the reflectivity over time as shown in the left image. In the right image, the power of the laser has been turned up and the VO2 has stopped vibrating, indicating that the phase transition has occurred. (Courtesy of Fritz Haber Institute)

VO2 is one of a class of materials now being considered for use in faster computer memory. When mixed with suitable additives, it makes a window coating that blocks infrared transmission on hot days and reduces heat loss during cool periods. In addition, it has potential applications in optical shutters, sensors and cameras.

鈥淲ith this new technique, we were able to see a lot of details that we鈥檝e never seen before,鈥 said Haglund. These details include how the electrons in the material rearrange first and then are followed by the movement of the much more massive atoms as the material shifts from its semiconductor to metallic-phase orientation. These details provide new information that can be used to design high-speed optical switches using this unique material.

Laser-based method tracks phase changes in ultra-short intervals

The new method is a variation on a standard method known as 鈥榩ump-and-probe.鈥 It uses an infrared laser that can produce powerful pulses of light that only last for femtoseconds (millionths of a trillionth of a second). When these pump pulses strike the surface of the target material, they generate high-frequency atomic vibrations determined by the material鈥檚 composition and phase. These vibrations change during a phase transition so they can be used to identify and track the transition in time.

Richard Haglund in the laboratory. (Joe Howell/Vanderbilt)

At the same time, the physicists split off a small fraction of the infrared beam (the probe), convert it into white light and use it to illuminate the surface of the target. It turns out that these lattice vibrations produce changes in the material鈥檚 surface reflectivity. As a result, the physicists can track what is happening inside the material by mapping the changes taking place on its surface.

The situation is analogous to hitting a gong with thousands of tiny microscopic hammers. The sound each hammer makes depends on the composition and arrangement of the atoms in the part of the gong where it hits. If the composition and arrangement of the atoms changes in one of these areas, then the sound the hammer makes also changes.

鈥淭he real power of this technique is that it is sensitive to atomic changes inside the material which are usually observed using expensive large-scale X-ray sources. Now we can do the experiment optically and in the lab on a tabletop,鈥 said , an Alexander von Humbolt fellow at the Fritz Haber Institute.

The Fritz Haber Institute group (left to right): Simon Wall, Laura Foglia, Daniel Wegkamp and Julia Staehler. (Courtesy of Fritz Haber Institute)

Vanderbilt graduate students and fabricated and characterized the vanadium dioxide thin films; , , , and at the Fritz Haber Institute directed the laser experiments and subsequent data analysis.

The project was funded by grants from the and the .