TY  - GEN
AB  - The adsorption of simple gas molecules to metal oxide surfaces is a primary step in many heterogeneous catalysis applications. Quantum chemical modeling of these reactions is a challenge in terms of both cost and accuracy, and quantum-embedding methods are promising, especially for localized chemical phenomena. In this work, we employ density matrix embedding theory (DMET) for periodic systems to calculate the adsorption energy of CO to the MgO(001) surface. Using coupled-cluster theory with single and double excitations and second-order Møller–Plesset perturbation theory as quantum chemical solvers, we perform calculations with embedding clusters up to 266 electrons in 306 orbitals, with the largest embedding models agreeing to within 1.2 kcal/mol of the non-embedding references. Moreover, we present a memory-efficient procedure of storing and manipulating electron repulsion integrals in the embedding space within the framework of periodic DMET.
AD  - University of Chicago
AD  - University of Chicago
AD  - Brown University
AD  - University of Chicago
AD  - University of Chicago
AU  - Mitra, Abhishek
AU  - Hermes, Matthew R.
AU  - Cho, Minsik
AU  - Agarawal, Valay
AU  - Gagliardi, Laura
DA  - 2022-08-08
ID  - 5524
JF  - The Journal of Physical Chemistry Letters
L1  - https://knowledge.uchicago.edu/record/5524/files/Periodic-Density-Matrix-Embedding-for-CO-Adsorption-on-the-MgO-001-Surface.pdf
L1  - https://knowledge.uchicago.edu/record/5524/files/jz2c01915_si_001.pdf
L1  - https://knowledge.uchicago.edu/record/5524/files/jz2c01915_si_002.pdf
L2  - https://knowledge.uchicago.edu/record/5524/files/Periodic-Density-Matrix-Embedding-for-CO-Adsorption-on-the-MgO-001-Surface.pdf
L2  - https://knowledge.uchicago.edu/record/5524/files/jz2c01915_si_001.pdf
L2  - https://knowledge.uchicago.edu/record/5524/files/jz2c01915_si_002.pdf
L4  - https://knowledge.uchicago.edu/record/5524/files/Periodic-Density-Matrix-Embedding-for-CO-Adsorption-on-the-MgO-001-Surface.pdf
L4  - https://knowledge.uchicago.edu/record/5524/files/jz2c01915_si_001.pdf
L4  - https://knowledge.uchicago.edu/record/5524/files/jz2c01915_si_002.pdf
LA  - eng
LK  - https://knowledge.uchicago.edu/record/5524/files/Periodic-Density-Matrix-Embedding-for-CO-Adsorption-on-the-MgO-001-Surface.pdf
LK  - https://knowledge.uchicago.edu/record/5524/files/jz2c01915_si_001.pdf
LK  - https://knowledge.uchicago.edu/record/5524/files/jz2c01915_si_002.pdf
N2  - The adsorption of simple gas molecules to metal oxide surfaces is a primary step in many heterogeneous catalysis applications. Quantum chemical modeling of these reactions is a challenge in terms of both cost and accuracy, and quantum-embedding methods are promising, especially for localized chemical phenomena. In this work, we employ density matrix embedding theory (DMET) for periodic systems to calculate the adsorption energy of CO to the MgO(001) surface. Using coupled-cluster theory with single and double excitations and second-order Møller–Plesset perturbation theory as quantum chemical solvers, we perform calculations with embedding clusters up to 266 electrons in 306 orbitals, with the largest embedding models agreeing to within 1.2 kcal/mol of the non-embedding references. Moreover, we present a memory-efficient procedure of storing and manipulating electron repulsion integrals in the embedding space within the framework of periodic DMET.
PY  - 2022-08-08
T1  - Periodic Density Matrix Embedding for CO Adsorption on the MgO(001) Surface
TI  - Periodic Density Matrix Embedding for CO Adsorption on the MgO(001) Surface
UR  - https://knowledge.uchicago.edu/record/5524/files/Periodic-Density-Matrix-Embedding-for-CO-Adsorption-on-the-MgO-001-Surface.pdf
UR  - https://knowledge.uchicago.edu/record/5524/files/jz2c01915_si_001.pdf
UR  - https://knowledge.uchicago.edu/record/5524/files/jz2c01915_si_002.pdf
Y1  - 2022-08-08
ER  -