Backside absorbing layer microscopy: Watching graphene chemistry.

The rapid rise of two-dimensional nanomaterials implies the development of new versatile, high-resolution visualization and placement techniques. For example, a single graphene layer becomes observable on Si/SiO substrates by reflected light under optical microscopy because of interference effects when the thickness of silicon oxide is optimized. However, differentiating monolayers from bilayers remains challenging, and advanced techniques, such as Raman mapping, atomic force microscopy (AFM), or scanning electron microscopy (SEM) are more suitable to observe graphene monolayers. The first two techniques are slow, and the third is operated in vacuum; hence, in all cases, real-time experiments including notably chemical modifications are not accessible. The development of optical microscopy techniques that combine the speed, large area, and high contrast of SEM with the topological information of AFM is therefore highly desirable. We introduce a new widefield optical microscopy technique based on the use of previously unknown antireflection and absorbing (ARA) layers that yield ultrahigh contrast reflection imaging of monolayers. The BALM (backside absorbing layer microscopy) technique can achieve the subnanometer-scale vertical resolution, large area, and real-time imaging. Moreover, the inverted optical microscope geometry allows its easy implementation and combination with other techniques. We notably demonstrate the potentiality of BALM by in operando imaging chemical modifications of graphene oxide. The technique can be applied to the deposition, observation, and modification of any nanometer-thick materials.