Asymmetric, mixed-valence molecules for spectroscopic readout of quantum-dot cellular automata

Mixed-valence compounds may provide molecular devices for an energy-efficient, low-power, general-purpose computing paradigm known as quantum-dot cellular automata (QCA). Multiple redox centers on mixed-valence molecules provide a system of coupled quantum dots. The configuration of mobile charge on a double-quantum-dot (DQD) molecule encodes a bit of classical information robust at room temperature. When arranged in non-homogeneous patterns (circuits) on a substrate, local Coulomb coupling between molecules enables information processing. While single-electron transistors (SETs) and single-electron boxes (SEBs) could provide low-temperature solutions for reading the state of a 1-nm-scale molecule, we propose a room-temperature read-out scheme. Here, DQD molecules are designed with slightly dissimilar quantum dots. Ab initio calculations show that the binary device states of an asymmetric molecule have distinct Raman spectra. Additionally, the dots are similar enough that mobile charge is not trapped on either dot, allowing device switching driven by the charge configuration of a neighbor molecule. A technique such as tip-enhanced Raman spectroscopy (TERS) could be used to detect the state of a circuit comprised of several QCA molecules.