Ab initio Thermodynamics with Applications to Molecular Sensor Design

Mario Blanco, Michael Freund, William A. Goddard

California Institute of Technology

Abstract

First principles thermodynamic calculations will enable chemists to design chemical processes with unparalleled levels of optimization, leading to high purity synthesis, milder conditions, and the elimination of unwanted pollutants. Such ab initio thermodynamic calculations will also enable the design of new chemical sensing technologies that have remained largely untapped. We have shown how this information can be used for the development of chemical vapor polymer sensors for an artificial nose. This year we present how highly accurate predictions are required for the development of chemically reactive biosensors. We show how ab initio calculations, through the use of bond order (BOC) and exposed solvent surface (ESS) corrections, may begin to approach the level of accuracy required to predict chemical equilibrium constants in solution. An overview of these methods is given with one such example; the sensitivity and response time optimization of polyboronic acid based hydrogels for the measurement of glucose levels in chronic diabetes patients.