In order to determine the molecular dipole moment (mu), polarizability (alpha), and first hyperpolarizability (beta) of L-arginine trifluoroacetate (LATF) crystals, a series of basis sets including polarized and diffuse functions have been employed at the framework of Hartree-Fock and second order Moller-Plesset perturbation theory methods. The MP2/6-311++G(d,p) model predicts for the converged value of in-crystal dipole moment, polarizability and first hyperpolarizability are 21.2 D, 20.0 x 10(-24) esu and 50.0 x 10(-31) esu, respectively. The calculated HOMO and LUMO energies show that charge transfer occur within the molecule. Electronic excitation properties are discussed within the framework of the two-level model on the basis of an orbital analysis. The coupled perturbed Hartree-Fock (CPHF) procedure yields information on the dispersion behavior of first hyperpolarizability terms. The magnitudes of the various hyperpolarizability terms which describe the various second-order nonlinear processes show the following trend: beta(-2 omega;omega,omega)>beta(0;omega,-omega)>beta(0,0,0). By using the molecular structures and the molecular first hyperpolarizability, the components of second harmonic tensor coefficient d of the crystals were evaluated by the oriented-gas model. (C) 2013 Elsevier B.V. All rights reserved.