Citation: FRANCO-PÉREZ Marco, GÁZQUEZ José L., AYERS Paul W., VELA Alberto. Thermodynamic Dual Descriptor[J]. Acta Physico-Chimica Sinica, ;2018, 34(6): 683-391. doi: 10.3866/PKU.WHXB201801031 shu

Thermodynamic Dual Descriptor

1.
Departamento de Química, Universidad Autónoma Metropolitana-Iztapalapa, Av. San Rafael Atlixco 186, Ciudad de México, 09340, México
2.
Department of Chemistry, McMaster University, Hamilton, Ontario, L8S 4M1, Canada
3.
Departamento de Química, Centro de Investigación y de Estudios Avanzados, Av. Instituto Politécnico Nacional 2508, Ciudad de México, 07360, México

Corresponding author: FRANCO-PÉREZ Marco, qimfranco@hotmail.com
Received Date: 16 November 2017
Revised Date: 27 December 2017
Accepted Date: 27 December 2017
Available Online: 3 June 2018
Fund Project: PWA thanks NSERC for support from the Canada Research Chairs, Compute Canada, and an NSERC Discovery Grant. MFP thanks Universidad Autónoma Metropolitana-Iztapalapa for a Visiting Professor Invitation. JLG and AV thank Conacyt for Grants 237045 and 128369, respectively

A new definition of the dual descriptor, namely, the thermodynamic dual descriptor, is developed within the grand canonical potential formalism. This new definition is formulated to describe the same physical phenomenon as the original definition proposed by Morell, Grand, and Toro-Labbé (J. Phys. Chem. A 2005, 109, 205), which is characterized by a second-order response of the electron density towards an electron flux. To formulate the new definition, we performed two successive partial derivatives of the average electron density, one with respect to the average number of electrons, and the other with respect to the chemical potential of the electron reservoir. When the derivative is expressed in terms of the three-state ensemble model, in the regime of low temperatures up to temperatures of chemical interest, one finds that the thermodynamic dual descriptor can be expressed as ∆f_T(r) = (β/2)C[f⁺(r)-f^-(r)], where β = 1/k_BT, C is a global quantity that depends on the temperature and global electronic properties of the molecule (the first ionization potential and the electron affinity), C = 1 for systems with zero fractional charge, and C = C_ω > 0 (albeit very close to zero) for systems with nonzero fractional charge, , and f⁺(r) and f^-(r) are the nucleophilic and electrophilic Fukui functions, respectively. The quantity within the square brackets is the original definition of the dual descriptor. As the local terms (the ones containing regioselectivity information) are equal to those of the dual descriptor, ∆f_T(r) has the same regioselectivity information, multiplied by the global quantity (β/2)C. This implies that the regioselectivity information contained in the original dual descriptor is preserved at all temperatures different from zero, and for any value of C > 0. One of the most important features of this new definition is that it avoids the undesired Dirac delta behavior observed when the second order partial derivative of the average density is taken with respect to the average number of electrons, using the exact density dependence of the average number of electrons.
- Dual descriptor,
- Chemical stability,
- Finite temperature chemical reactivity theory,
- Fractional average number of electrons,
- Amphiphilicity
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