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Large, valley-exclusive Bloch-Siegert shift in monolayer WS2

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Science  10 Mar 2017:
Vol. 355, Issue 6329, pp. 1066-1069
DOI: 10.1126/science.aal2241

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Going way off resonance

Single atomic layers of transition metal dichalcogenide (TMD) materials have two nonequivalent valleys in their electronic structure. When researchers shine visible light on these monolayers, left-circularly polarized light modifies the electronic levels in one valley but not the other. Sie et al. studied the material WS2. They found that in the infrared regime, if the frequency of the light was far away from the resonance, energy levels in both valleys were affected. The so-called Bloch-Siegert effect could explain the energy shift in the “wrong” valley. The findings should be important for the manipulation of valleytronic properties of TMDs.

Science, this issue p. 1066

Abstract

Coherent interaction with off-resonance light can be used to shift the energy levels of atoms, molecules, and solids. The dominant effect is the optical Stark shift, but there is an additional contribution from the so-called Bloch-Siegert shift that has eluded direct and exclusive observation in solids. We observed an exceptionally large Bloch-Siegert shift in monolayer tungsten disulfide (WS2) under infrared optical driving. By controlling the light helicity, we could confine the Bloch-Siegert shift to occur only at one valley, and the optical Stark shift at the other valley, because the two effects obey opposite selection rules at different valleys. Such a large and valley-exclusive Bloch-Siegert shift allows for enhanced control over the valleytronic properties of two-dimensional materials.

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