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The general idea of using ultrashort light pulses to control ferroic orderparameters has recently attracted attention as a means to achieve control overmaterial properties on unprecedented time scales. Much of the challenge in suchwork is in understanding the mechanisms by which this control can be achieved,and in particular how observables can be connected to structural and electronicproperties. Here we report on a combination of experimental and computationalmethods to study the electronic structure of the semiconducting ferroelectricGeTe when driven out of equilibrium by absorption of a femtosecond pulse oflight. We observe coherent modulations of second harmonic generations on theorder of 50%, which we attribute to a combination of atomic and electronicstructure changes due to a coherently excited soft mode. Comparison of theobserved experimental data with model calculations indicates that this effectis predominantly due to an ultrafast modulation of the covalency of the bondingbetween Ge and Te ions. This stands in contrast to previously held assumptionsin other systems, indicating that care should be exercised in using indirectmeasurements of electronic structure to make strong conclusions about themagnitude of nuclear motions.

Ultrafast modulation of covalency in GeTe driven by a ferroelectric soft mode