Gaussian 16 is proprietary, commercial software and is for general public use. Obtaining the software legally requires a valid license from Gaussian, Inc. .
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Psi4 is an open-source suite of quantum chemistry programs designed to be efficient, user-friendly, and reliable. It is written in C++ and Python, making it accessible to both users and developers. Psi4 supports a wide range of methods, including Hartree-Fock, DFT, MP2, and coupled-cluster, and has been shown in some benchmarks to produce results very close to those of Gaussian 16. It is entirely free and open-source, making it an excellent choice for those who value transparency and community-driven development.