Implementing
parallel and multivalued logic operations at the molecular
scale has the potential to improve the miniaturization and efficiency
of a new generation of nanoscale computing devices. Two-dimensional
photon-echo spectroscopy is capable of resolving dynamical pathways
on electronic and vibrational molecular states. We experimentally
demonstrate the implementation of molecular decision trees, logic
operations where all possible values of inputs are processed in parallel
and the outputs are read simultaneously, by probing the laser-induced
dynamics of populations and coherences in a rhodamine dye mounted
on a short DNA duplex. The inputs are provided by the bilinear interactions
between the molecule and the laser pulses, and the output values are
read from the two-dimensional molecular response at specific frequencies.
Our results highlights how ultrafast dynamics between multiple molecular
states induced by light–matter interactions can be used as
an advantage for performing complex logic operations in parallel,
operations that are faster than electrical switching.