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The extreme electro-optical contrast between crystalline and amorphous statesin phase change materials is routinely exploited in optical data storage andfuture applications include universal memories, flexible displays,reconfigurable optical circuits, and logic devices. Optical contrast isbelieved to arise due to a change in crystallinity. Here we show that theconnection between optical properties and structure can be broken. Using aunique combination of single-shot femtosecond electron diffraction and opticalspectroscopy, we simultaneously follow the lattice dynamics and dielectricfunction in the phase change material Ge2Sb2Te5 during an irreversible statetransformation. The dielectric function changes by 30% within 100 femtosecondsdue to a rapid depletion of electrons from resonantly-bonded states. Thisoccurs without perturbing the crystallinity of the lattice, which heats with a2 ps time constant. The optical changes are an order-of-magnitude larger thanthose achievable with silicon and present new routes to manipulate light on anultrafast timescale without structural changes.

Time-Domain Separation of Optical Properties From Structural Transitions in Resonantly Bonded Materials