Information processing in parallel through directionally resolved molecular polarization components in coherent multidimensional spectroscopy.
We propose that information processing can be implemented by measuring the directional components of the macroscopic polarization of an ensemble of molecules subject to a sequence of laser pulses. We describe the logic operation theoretically and demonstrate it by simulations. The measurement of integrated stimulated emission in different phase matching spatial directions provides a logic decomposition of a function that is the discrete analog of an integral transform. The logic operation is reversible and all the possible outputs are computed in parallel for all sets of possible multivalued inputs. The number of logic variables of the function is the number of laser pulses used in sequence. The logic function that is computed depends on the chosen chromophoric molecular complex and on its interactions with the solvent and on the two time intervals between the three pulses and the pulse strengths and polarizations. The outputs are the homodyne detected values of the polarization components that are measured in the allowed phase matching macroscopic directions, kl, kl=∑iliki where ki is the propagation direction of the ith pulse and {li} is a set of integers that encodes the multivalued inputs. Parallelism is inherently implemented because all the partial polarizations that define the outputs are processed simultaneously. The outputs, which are read directly on the macroscopic level, can be multivalued because the high dynamical range of partial polarization measurements by nonlinear coherent spectroscopy allows for fine binning of the signals. The outputs are uniquely related to the inputs so that the logic is reversible.
Department de Chimie, B6c, Université de Liège, B4000 Liège, Belgium.
Tian-Min
TM
Yan
Department de Chimie, B6c, Université de Liège, B4000 Liège, Belgium.
Barbara
B
Fresch
The Fritz Haber Research Center for Molecular Dynamics, The Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem 91904, Israel.
R D
RD
Levine
Department de Chimie, B6c, Université de Liège, B4000 Liège, Belgium.
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F
Remacle
D003198:Computer Simulation; D007257:Information Theory; D007834:Lasers; D008128:Logic; D008958:Models, Molecular; D017711:Nonlinear Dynamics; D055620:Optical Phenomena; D013057:Spectrum Analysis