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The molecular dipole moment plays a significant role in governing important phenomena like molecular interactions, molecular configuration, and charge transfer, which are important in several electronic, electrochemical, and optoelectronic systems. Here, the effect of the change in the dipole moment of a tethered molecule on the carrier properties of (functionalized) trilayer graphene--a stack of three layers of sp(2)-hybridized carbon atoms--is demonstrated. It is shown that, due to the high carrier confinement and large quantum capacitance, the trans-to-cis isomerisation of 'covalently attached' azobenzene molecules, with a change in dipole moment of 3D, leads to the generation of a high effective gating voltage. Consequently, 6 units of holes are produced per azobenzene molecule (hole density increases by 440 000 holes μm(-2)). Based on Raman and X-ray photoelectron spectroscopy data, a model is outlined for outer-layer, azobenzene-functionalized trilayer graphene with current modulation in the inner sp(2) matrix. Here, 0.097 V are applied by the isomerisation of the functionalized azobenzene. Further, the large measured quantum capacitance of 72.5 μF cm(-2) justifies the large Dirac point in the heavily doped system. The mechanism defining the effect of dipole modulation of covalently tethered molecules on graphene will enable future sensors and molecular-machine interfaces with graphene.

Nonspecific binding (NSB), a random adsorption of biocomponents such as proteins and bacteria on noncomplementary materials,isoneofthebiggestproblemsinbiological applications including biosensors, protein chips, surgical instruments, drug delivery, and biomedicine. Polyoxyethylene sorbitan laurate (TWEEN), a commercially available chemical with aliphatic ester chains, has shown promise as a medical material and in overcomingproblems associated withNSB. [1‐4] However,stability during solution-based processing and uniformity of the materials that have TWEEN coating on flat substrates or nanomaterials using the selfassembled-monolayer (SAM) method has been an important issue. Further, biocompatible materials with high strength are important for several medical applications including stents, nail implants, and strong invasive instruments. Here, we present the production of a free-standing ‘‘paperlike’’ material composed of TWEEN and reduced graphene oxide (RGO) platelets and obtained by simple filtration of a homogeneous aqueous colloidal suspension of TWEEN/RGO hybrid. The ‘‘TWEEN paper’’ was highly stable in water without leakage of TWEEN and is compliant and sufficiently robust to be handled by hand without breaking. Furthermore, the TWEEN paper was noncytotoxic to three mammalian cell lines and biocompatible, inhibiting nonspecific binding of Gram-positive bacteria. [5] In contrast, RGO paper without TWEEN showed nonspecific bacterial binding. TWEEN is composed ofthree chemical parts (Fig. 1a): aliphatic esterchains that can prevent NSB ofbiomolecules, three-terminal hydroxyl groups that are hydrophilic and can be chemically modified for further applications, and an aliphatic chain that can easily be adsorbed on a hydrophobic surface by noncovalent interaction. Protein microarrays on flat substrates with SAM of TWEEN [4] and highly sensitive biosensors, [1‐3] built using field-effect transistor (FET) behavior of individual carbon nanotube (CNT) strands coated with TWEEN, have demonstrated that TWEEN can be effectively used to overcome NSB.