Quantum Calculations

Erica Vander Mause and Rob Hodgson
March 11, 2014

Abstract

This experiment uses three different ab initio basis sets, 6-21G, 6-31G, and DZV, to predict the molecular properties is Br2, NHF2 and nitrobenzene.  Comparing the calculated characteristics to experimental data, it was found that 6-31G(a smaller basis set than DZV) more accurately predicted the properties of BR2.  As expected the largest basis set, DZV, most accurately predicted the properties of the other two molecules nitrobenzene and NHF2. 

Introduction

    The goal of this experiment is to successfully describe the overall electronic structure of the molecule at study. Three different molecules will be examined: Br2, NHF2, and Nitrobenzene. Accurately describing the most probable locations of electrons and their energies available, will predict useful properties of the molecule such as dipole moment, polarizability, vibrational frequencies,absorption of visible light. Software was used to aid in the calculation intensive process of describing electrons.  Avogadro was used to build the molecules, wxMacMolplt to optimize geometry, GamessQ ran all of the calculations, and then Jmol analyzed the characteristics of interest in the calculations made in GamessQ.
    The calculations set up in wxMacMolplt consisted of different levels of theory. The levels of theory (basis sets) that we will be using for our calculations are 6-21G (3-21G for Br2 only), 6-31G, and DZV (which is in order of increasing size of calculations taken). By using these different levels of theory we will look into the intuitive nature of electronic structure within a molecule.
    Each theory of calculations used a different number of Gaussian functions to describe the electron wave function.  The first number in each theory level signifies the number of Gaussian’s added together to describe inner electrons.  The number following the dash describes the number of Gaussian’s used to describe the valance electrons in each atom of the molecule.  More Gaussian’s were used to more accurately model the behavior of the valance electrons because those are the most important for bonding.  For example, in the 6-21G 6 Gaussian’s were added together to describe the inner electrons.  The DZV or double zeta valance basis set is the biggest basis set used in this procedure. 
    Each of these basis sets was evaluated using Harte-Frock Self Consistent Field calculations.  A single electron in the molecule was chosen.  All of the other electrons in the molecule were treated as single electronic field acting on the selected electron.  Based off of the coulomb interactions with the all electron encompassing electronic field and the nuclei, the lowest energy position for electron and nuclei were found.  Then another electron was chosen and the process was repeated until the energy of the molecule reached a minimum.  

Molecules 

Use the following links to navigate to the calculations of each molecule.  

di-bromine

NHF2

nitrobenzene
      


Conclusion

    Computational results are useful when there is little or no reliable experimental data on a molecule.  Computations may be useful when making predicitons about reactions that use expensive materials.  Unsuccessful reactions and reagent waste could be avoided if computional models were used to find reactions that are likely to take place.  Computational results could also be useful if the molecule is dangerous to handle or synthesize.  Computational results also provide a visual of the molecule that cannot be seen experimentally.  This can lead to a greater understanding of what is going on at the molecular level.  As discussed in this report, the accuracy of the calculated results vary, and a bigger basis set does not always improve accuracy.  Experimental results are necessary to back up the computational results.