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1. Benchmarking the semi-stochastic CC( P ; Q ) approach for singlet–triplet gaps in biradicals

   https://doi.org/10.1063/5.0100165  

   Chakraborty, Arnab; Yuwono, Stephen H.; Deustua, J. Emiliano; Shen, Jun; Piecuch, Piotr (October 2022, The Journal of Chemical Physics)

   We recently proposed a semi-stochastic approach to converging high-level coupled-cluster (CC) energetics, such as those obtained in the CC calculations with singles, doubles, and triples (CCSDT), in which the deterministic CC(P;Q) framework is merged with the stochastic configuration interaction Quantum Monte Carlo propagations [J. E. Deustua, J. Shen, and P. Piecuch, Phys. Rev. Lett. 119, 223003 (2017)]. In this work, we investigate the ability of the semi-stochastic CC(P;Q) methodology to recover the CCSDT energies of the lowest singlet and triplet states and the corresponding singlet–triplet gaps of biradical systems using methylene, (HFH)−, cyclobutadiene, cyclopentadienyl cation, and trimethylenemethane as examples. 

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2. Ab initio metadynamics calculations of dimethylamine for probing p K _b variations in bulk vs. surface environments

   https://doi.org/10.1039/D0CP03832F  

   Biswas, Sohag; Kwon, Hyuna; Barsanti, Kelley C.; Myllys, Nanna; Smith, James N.; Wong, Bryan M. (November 2020, Physical Chemistry Chemical Physics)

   null (Ed.)

   The basicity constant, or p K b , is an intrinsic physical property of bases that gives a measure of its proton affinity in macroscopic environments. While the p K b is typically defined in reference to the bulk aqueous phase, several studies have suggested that this value can differ significantly at the air–water interface (which can have significant ramifications for particle surface chemistry and aerosol growth modeling). To provide mechanistic insight into surface proton affinity, we carried out ab initio metadynamics calculations to (1) explore the free-energy profile of dimethylamine and (2) provide reasonable estimates of the p K b value in different solvent environments. We find that the free-energy profiles obtained with our metadynamics calculations show a dramatic variation, with interfacial aqueous dimethylamine p K b values being significantly lower than in the bulk aqueous environment. Furthermore, our metadynamics calculations indicate that these variations are due to reduced hydrogen bonding at the air–water surface. Taken together, our quantum mechanical metadynamics calculations show that the reactivity of dimethylamine is surprisingly complex, leading to p K b variations that critically depend on the different atomic interactions occurring at the microscopic molecular level. 

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3. Erratum: “Quasiparticle electronic structure of phthalocyanine:TMD interfaces from first-principles GW ” [J. Chem. Phys. 155, 214702 (2021)]

   https://doi.org/10.1063/5.0230977  

   Kafle, Gyanu P; Liu, Zhen-Fei (August 2024, The Journal of Chemical Physics)
4. Erratum: “Non-adiabatic mapping dynamics in the phase space of the SU ( N ) Lie group” [J. Chem. Phys. 157, 084105 (2022)]

   https://doi.org/10.1063/5.0138797  

   Bossion, Duncan; Ying, Wenxiang; Chowdhury, Sutirtha N.; Huo, Pengfei (July 2023, The Journal of Chemical Physics)
5. “Freedom of design” in chemical compound space: towards rational in silico design of molecules with targeted quantum-mechanical properties

   https://doi.org/10.1039/D3SC03598K  

   Medrano_Sandonas, Leonardo; Hoja, Johannes; Ernst, Brian G; Vázquez-Mayagoitia, Álvaro; DiStasio, Robert A; Tkatchenko, Alexandre (October 2023, Chemical Science)

   This work demonstrates that “freedom of design” is a fundamental and emergent property of chemical compound space. Such intrinsic flexibility enables rational design of distinct molecules sharing an array of targeted quantum-mechanical properties. 

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