Tribute to Piergiorgio Casavecchia and Antonio Laganà

Balucani, Nadia; Bowman, Jay; Connor, J. N. L.; Lee, Y. T.

doi:10.1021/acs.jpca.6b05527

Cited by 3 publications

(4 citation statements)

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“…[6][7][8] The magnetic properties of transition metal complexes and materials can be controlled by light, temperature, and pressure by initiating spin-crossover transitions between the low-spin and high-spin states. [9][10][11][12] Among many examples of processes where intersystem crossings play a central role are combustion, [13,14] reactions in the atmosphere and in interstellar space, [5,15] transition metal-based catalysis, [16] and binding of small molecules to the active sites of metalloproteins. [17][18][19][20] Intersystem crossing has applications in photodynamic therapy, [21,22] free-radical polymerization reactions, [23] organic-light emitting diodes, [24][25][26] and metal-organic frameworks.…”

Section: Introductionmentioning

confidence: 99%

“…In principle, the rates of intersystem crossings can be calculated by solving the quantum Schr€ odinger or classical Newton equations for the nuclear motion on the multiple coupled electronic PESs using nonadiabatic ab initio molecular dynamics (NA-AIMD). In the most of the applications of NA-AIMD to intersystem crossings, the classical nuclear trajectories are propagated on the PESs prebuild [13,14,29,30] or calculated "on the-fly" along the nuclear trajectories. [26,28,[31][32][33][34] The last approach, also called direct dynamics, can be applied to relatively large systems with dozens of atoms.…”

Section: Introductionmentioning

confidence: 99%

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Nonadiabatic transition state theory: Application to intersystem crossings in the active sites of metal‐sulfur proteins

Lykhin

Kaliakin

dePolo

et al. 2016

Int J of Quantum Chemistry

139

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Nonadiabatic transition state theory (NA-TST) is a powerful tool to investigate the nonradiative transitions between electronic states with different spin multiplicities. The statistical nature of NA-TST provides an elegant and computationally inexpensive way to calculate the rate constants for intersystem crossings, spin-forbidden reactions, and spin-crossovers in large complex systems. The relations between the microcanonical and canonical versions of NA-TST and the traditional transition state theory are shown, followed by a review of the basic steps in a typical NA-TST rate constant calculation. These steps include evaluations of the transition probability and coupling between electronic states with different spin multiplicities, a search for the minimum energy crossing point (MECP), and computing the densities of states and partition functions for the reactant and MECP structures. The shortcomings of the spin-diabatic version of NA-TST related to ill-defined state coupling and state counting are highlighted. In three examples, we demonstrate the application of NA-TST to intersystem crossings in the active sites of metal-sulfur proteins focusing on [NiFe]-hydrogenase, rubredoxin, and Fe 2 S 2 -ferredoxin.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Nonadiabatic transition state theory: Application to intersystem crossings in the active sites of metal‐sulfur proteins

Lykhin

Kaliakin

dePolo

et al. 2016

Int J of Quantum Chemistry

139

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“…The longrange forces are properly considered in the DMBE PES. Qusi-classical trajectory (QCT) [17][18][19][20] and quantum mechanical (QM) [21][22][23][24][25][26] methods have been carried out on the BHL and DMBE PES, yielding cross sections and rate constants in good agreement with experiment. For the title reaction, Lin and Guo [27] have reported quantum wave packet studies and further confirmed the domination of the CD 1 H channel.…”

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confidence: 99%

Quantum reaction dynamics of C(¹D) + HD → CH(CD) + D(H) on the ground state potential energy surface

2017

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We present accurate quantum dynamic calculations of the reaction C(1D) + HD on the latest version of the 11A′ potential energy surface [Zhang et al., J. Chem. Phys. 140, 234301 (2014)]. Using a Chebyshev real wave packet method with full Coriolis coupling, we obtain the initial state‐specified ( vi=0, ji=0) reaction probabilities, integral cross sections, and rate constants. The resulting probabilities display oscillatory structures due to numerous long‐lived resonances supported by the deep potential well. The calculated rate constants and CD/CH product branching ratio at room temperature are in reasonably good agreement with the experimental measurements.

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“…Intermolecular potentials are the most importantinputs of molecular simulation [13] and the accuracy of the dynamics computations depends on the accuracy of the IPES. [14] Spectroscopic studies, [15,16] molecular beam scattering experiments [17][18][19][20][21][22] and speed of sound data [23] are some experimental methods from which information about intermolecular potentials may be obtained. However, it is still difficult to accurately determine the potential energy surfaces of interacting molecules only from these experimental methods.…”

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confidence: 99%

F₂ dimer: Improved intermolecular potential energy surface using ab initio calculations

Tashakor

Noorbala

Namazian

2016

Int J of Quantum Chemistry

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A computational study on the intermolecular potential energy of 44 different orientations of F2 dimers is presented. Basis set superposition error (BSSE) corrected potential energy surface is calculated using the supermolecular approach at CCSD(T) and QCISD(T) levels of theory. The interaction energies obtained using the aug‐cc‐pVDZ and aug‐cc‐pVTZ basis sets are extrapolated to the complete basis set limit using the latest extrapolation scheme. The basis set effect is checked and it is found that the extrapolated intermolecular energies provide the best compromise between the accuracy and computational cost. Among 1320 energy points of F2–F2 system covering more relative orientations, the most stable structure of the dimers was obtained with a well depth of −146.62 cm−1 that related to cross configuration, and the most unstable structure is related to linear orientation with a well depth of −52.63 cm−1. The calculated second virial coefficients are in good agreement with experimental data. The latest extrapolation scheme of the complete basis set limit at the CCSD(T) level of theory is used to determine the intermolecular potential energy surface of the F2 dimer. Comparing the results obtained by the latest scheme with those by older schemes show that the new approach provides the best compromise between accuracy and computational cost.

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Tribute to Piergiorgio Casavecchia and Antonio Laganà

Cited by 3 publications

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Nonadiabatic transition state theory: Application to intersystem crossings in the active sites of metal‐sulfur proteins

Nonadiabatic transition state theory: Application to intersystem crossings in the active sites of metal‐sulfur proteins

Quantum reaction dynamics of C(¹D) + HD → CH(CD) + D(H) on the ground state potential energy surface

F₂ dimer: Improved intermolecular potential energy surface using ab initio calculations

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Tribute to Piergiorgio Casavecchia and Antonio Laganà

Cited by 3 publications

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Nonadiabatic transition state theory: Application to intersystem crossings in the active sites of metal‐sulfur proteins

Nonadiabatic transition state theory: Application to intersystem crossings in the active sites of metal‐sulfur proteins

Quantum reaction dynamics of C(1D) + HD → CH(CD) + D(H) on the ground state potential energy surface

F2 dimer: Improved intermolecular potential energy surface using ab initio calculations

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Product

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Quantum reaction dynamics of C(¹D) + HD → CH(CD) + D(H) on the ground state potential energy surface

F₂ dimer: Improved intermolecular potential energy surface using ab initio calculations