"Gold-Standard" Δ-Machine Learned Transferable Potential for Linear Alkanes

线性烷烃的“黄金标准”Δ-机器学习可迁移势

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Abstract

The conformational properties of linear alkanes, C(n)H(2n+2), have been of intense interest for many years. Experiments and corresponding electronic structure calculations were first reported in the mid-2000s and continue to the present time. These focus on the minimum chain length where the transition from the linear minimum to the hairpin minimum occurs. We recently reported a transferable, many-body permutationally invariant polynomial (MB-PIP) potential for linear alkanes trained on roughly 253 000 B3LYP electronic energies for C(14)H(30). Here we report a Δ-ML approach to elevate this B3LYP-based and a new PBE0+MBD MB-PIP potential using roughly 4500 Pair Natural Orbital Local Coupled Cluster (PNO-LCCSD(T)-F12) energies. The new Δ-corrected potentials predict the difference in these minima accurately, compared to benchmark PNO-LCCSD(T)-F12 energies results, over the range C(12)H(28) to C(28)H(58). Vibrational power spectra are also reported for C(14)H(30) using the original B3LYP-based and Δ-ML corrected potentials. These new MB-PIP potentials for linear alkanes are the most accurate ones currently available and can be used in studies of properties of linear alkanes.

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