TY - JOUR

T1 - Enhancing NMR Quantum Computation by Exploring Heavy Metal Complexes as Multiqubit Systems

T2 - a Theoretical Investigation

AU - Boreli Dos Reis Lino, Jessica

AU - Sauer, Stephan P. A.

AU - Ramalho, Teodorico Castro

PY - 2020/6/18

Y1 - 2020/6/18

N2 - Assembled together with the most common qubits used in NMR quantum computation experiments, spin--1/2 nuclei, such as 113Cd, 199Hg, 125Te and 77Se could leverage the prospective scalable quantum computer architectures, enabling many and heteronuclear qubits for NMR quantum information processing (QIP) implementations. A computational design strategy for prescreening recently synthesized complexes of cadmium, mercury, tellurium, selenium and phosphorus (called MRE complexes) as suitable qubit molecules for NMR QIP is reported. Chemical shifts and spin--spin coupling constants in five MRE complexes were examined using the spin--orbit zeroth order regular approximation (ZORA) at the density functional theory (DFT) level and the four--component relativistic Dirac-Kohn-Sham approach. In particular the influence of different conformers, basis sets, exchange-correlation functionals and methods to treat the relativistic as well as solvent effects were studied. The differences in the chemical shifts and spin--spin coupling constants between different low energy conformers of the studied complexes were found to be very small. The TZ2P basis set was found to be the optimum choice for the studied chemical shifts, while the TZ2P--J basis set was the best for the couplings studied in this work. The PBE0 exchange-correlation functional exhibited the best performance for the studied MRE complexes. The addition of solvent effects has not improved on the gas phase results in comparison to experiment, with the exception of the phosphorus chemical shift. The use of MRE complexes as qubit molecules for NMR QIP could face the challenges in single qubit control and multiqubit operations. They exhibit chemical shifts appropriately dispersed, allowing qubit addressability and exceptional large spin--spin couplings, which could reduce the time of quantum gate operations and likely preserve the coherence.

AB - Assembled together with the most common qubits used in NMR quantum computation experiments, spin--1/2 nuclei, such as 113Cd, 199Hg, 125Te and 77Se could leverage the prospective scalable quantum computer architectures, enabling many and heteronuclear qubits for NMR quantum information processing (QIP) implementations. A computational design strategy for prescreening recently synthesized complexes of cadmium, mercury, tellurium, selenium and phosphorus (called MRE complexes) as suitable qubit molecules for NMR QIP is reported. Chemical shifts and spin--spin coupling constants in five MRE complexes were examined using the spin--orbit zeroth order regular approximation (ZORA) at the density functional theory (DFT) level and the four--component relativistic Dirac-Kohn-Sham approach. In particular the influence of different conformers, basis sets, exchange-correlation functionals and methods to treat the relativistic as well as solvent effects were studied. The differences in the chemical shifts and spin--spin coupling constants between different low energy conformers of the studied complexes were found to be very small. The TZ2P basis set was found to be the optimum choice for the studied chemical shifts, while the TZ2P--J basis set was the best for the couplings studied in this work. The PBE0 exchange-correlation functional exhibited the best performance for the studied MRE complexes. The addition of solvent effects has not improved on the gas phase results in comparison to experiment, with the exception of the phosphorus chemical shift. The use of MRE complexes as qubit molecules for NMR QIP could face the challenges in single qubit control and multiqubit operations. They exhibit chemical shifts appropriately dispersed, allowing qubit addressability and exceptional large spin--spin couplings, which could reduce the time of quantum gate operations and likely preserve the coherence.

KW - Faculty of Science

KW - Quantum Computing

KW - NMR spectrocopy

KW - chemical shift

KW - Spin-spin coupling constant

KW - ZORA

KW - cadmium

KW - mercury

KW - tellurium

KW - Selenium

KW - Phosphorus

U2 - 10.1021/acs.jpca.0c01607

DO - 10.1021/acs.jpca.0c01607

M3 - Journal article

C2 - 32463687

VL - 124

SP - 4946

EP - 4955

JO - Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory

JF - Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory

SN - 1089-5639

IS - 24

ER -