Artículo

Boyd, J.; Pagola, G.I.; Caputo, M.C.; Ferraro, M.B.; Lazzeretti, P. "Calculation of hypershielding contribution to isotropic nitrogen shielding in strong magnetic fields" (2009) Journal of Chemical Theory and Computation. 5(5):1343-1349
La versión final de este artículo es de uso interno. El editor solo permite incluir en el repositorio el artículo en su versión post-print. Por favor, si usted la posee enviela a
Consulte el artículo en la página del editor
Consulte la política de Acceso Abierto del editor

Abstract:

Hypershielding contributions to magnetic shielding of the nitrogen N nucleus have been evaluated for some nitroso (RNO) and isodiazene (R 1 R 2 NN) compounds in the presence of an external spatially uniform, time-independent magnetic field, accounting for cubic response via Rayleigh-Schrödinger perturbation theory. Numerical estimates have been obtained at the coupled Hartree-Fock level of accuracy within the conventional common-origin approach. Medium-size basis sets of gaugeless (that is, without gauge-including phase factors) Gaussian functions have been employed in a numerical test to show that the isotropic hypershielding contribution τ N B N , τ N = 1/2〈Σ N αβγδ 〉, eqs 2-4 in the text, to average nitrogen shielding in PhNO (τ N ≈ 1.1 × 10 -5 ppm T -2 ), (CH 3 ) 3 CNO (τ N ≈ 2.3 × 10 -5 ppm T -2 ), and (CH 3 ) 2 NN (τ N ≈ 4.4 × 10 -5 ppm T -2 ) are similar and quite large. For 15 N at the highest currently available high-resolution NMR field strength of 22.3 T (ω H /2π = 950 MHz, ω 15N / 2π = 96.3 MHz) the change due to the additional shielding contribution for these compounds is between ∼0.5 and ∼2 Hz to lower frequency (upfield). Employing modern NMR instrumentation, shielding perturbations of this magnitude are, in principle, within detection limits, although instrumental instabilities and other field-dependent shielding phenomena make unambiguous detection at different field strengths difficult. © 2009 American Chemical Society.

Registro:

Documento: Artículo
Título:Calculation of hypershielding contribution to isotropic nitrogen shielding in strong magnetic fields
Autor:Boyd, J.; Pagola, G.I.; Caputo, M.C.; Ferraro, M.B.; Lazzeretti, P.
Filiación:Department of Biochemistry, South Parks Road, Oxford, 0X1 3QU, United Kingdom
Departamento de Física, Facultad de Ciencias Exactas y Naturales, Ciudad Universitaria, Pab. I, (1428) Buenos Aires, Argentina
Dipartimento di Chimica, Università degli Studi di Modena e Reggio Emilia, Via Campi 183, 41100 Modena, Italy
Carrera del Investigador del CONICET, Argentina
Año:2009
Volumen:5
Número:5
Página de inicio:1343
Página de fin:1349
DOI: http://dx.doi.org/10.1021/ct900034d
Título revista:Journal of Chemical Theory and Computation
Título revista abreviado:J. Chem. Theory Comput.
ISSN:15499618
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_15499618_v5_n5_p1343_Boyd

Referencias:

  • Bachtold, A., Strunk, C., Salvetat, J.-P., Bonard, J.-M., Forró, L., Nussbaumer, T., Schöneberger, C., Aharonov-Bohm oscillations in carbon nanotubes (1999) Nature (London), 397, p. 673
  • Zaric, S., Ostojic, G.N., Kono, J., Shaver, W., Moore, V.C., Strano, M.S., Hauge, R.H., Wei, X., Optical Signatures of the Aharonov-Bohm Phase in Single-Walled Carbon Nanotubes (2004) Science, 304, p. 1129
  • Coskun, U.C., Wei, T.-C., Vishveshwara, S., Goldbart, P.M., Bezryadin, A., The Magnetic Flux Modulation of the Energy Gap in Nanotube Quantum Dots (2004) Science, 304, p. 1132
  • Compernolle, S., Chibotaru, L.F., Ceulemans, A., Novel type of magnetic response in carbon nanomaterials (2006) Chem. Phys. Lett, 428, p. 119
  • Compernolle, S., Chibotaru, L.F., Ceulemans, A., Vortices and their relation to ring currents and magnetic moments in nanographenes in high magnetic field (2006) J. Chem,. Phys. B, 110, p. 19340
  • Rasolt, M., Tesanovic, Z., Theoretical aspects of supercon-ductivity in very high magnetic fields (1992) Rev. Mod. Phys, 64, p. 709
  • Lai, D., Matter in strong magnetic fields (2001) Rev. Mod. Phys, 73, p. 629
  • Proceedings of the 172nd WE-Heraeus-Seminar on Atoms and Molecules in Strong External Fields, Bad Honnef, Germany, April 7-11, 1997. In Atoms and Molecules in Strong External Fields, 2nd ed.; Schmeicher, P., Schweizer, W., Eds.; Springer: New York, USA, 1998; Runge, K., Sabin, J.R., Introduction to the Workshop on Properties of Molecules in Strong Magnetic Fields (1997) Int. J. Quantum Chem, 64, p. 495. , and references therein
  • Ramsey, N.F., Possibility of Field-Dependent Nuclear Magnetic Shielding (1970) Phys. Rev. A, 1, p. 1320
  • Vaara, J., Manninen, P., Lounila, J., Magnetic Field-Dependence of Nuclear Magnetic Shielding in Closed-Shell Atomic Systems (2003) Chem. Phys. Lett, 372, p. 750
  • Manninen, P., Vaara, J., Magnetic-field dependence of 59 Co nuclear magnetic shielding in Co(III) complexes (2004) Phys. Rev. A, 69, p. 022503
  • Pagola, G.L., Caputo, M.C., Ferraro, M.B., Lazzeretti, P., Calculation of the fourth-rank hypermagnetizability of some small molecules (2004) J. Chem. Phys, 120, p. 9556
  • Pagola, G.L., Caputo, M.C., Ferraro, M.B., Lazzeretti, P., Non-linear ring currents: Effect of strong magnetic fields on π-electron circulation (2004) Chem. Phys. Lett, 400, p. 133
  • Pagola, G.L., Caputo, M.C., Ferraro, M.B., Lazzeretti, P., Nonlinear response of the benzène molecule to strong magnetic fields (2005) J. Chem. Phys, 112, p. 074318
  • Pagola, G.L., Caputo, M.C., Ferraro, M.B., Lazzeretti, P., Fourth-rank hypermagnetizability of medium-size planar conjugated molecules and Mierene (2005) Phys. Rev. A, 72. , 033401:1
  • Pagola, G.L., Caputo, M.C., Ferraro, M.B., Lazzeretti, P., Sum rules for invariance of the fourth-rank hypermagnetis-ability in a gauge translation (2005) Chem. Phys. Lett, 408, p. 403
  • Pagola, G.L., Caputo, M.C., Ferraro, M.B., Lazzeretti, P., Calculation of the fourth-rank nuclear magnetic hypershielding of some small molecules (2006) Phys. Rev. A, 74, p. 022509
  • Žaucer, M., Aḿan, A., Magnetic Field-Dependent Molecular Susceptibility (1977) Phys. Rev. A, 16, p. 475
  • Soncini, A., Fowler, P.W., Non-linear ring currents: Effect of strong magnetic fields on π-electron circulation (2004) Chem. Phys. Lett, 400, p. 213
  • Tellgren, E.L., Soncini, A., Helgaker, T., Nonperturbative ab initio calculations in strong magnetic fields using London orbitals (2008) J. Chem. Phys, 129, p. 154114
  • Ramsey, N.F., Magnetic Shielding of Nuclei in Molecules (1950) Phys. Rev, 78, p. 699
  • Abragam, A., (1961) The Principles of Nuclear Magnetism, p. 279. , Oxford: Clarendon Press: London
  • Epstein, S.T., (1974) The Variation Method in Quantum Chemistry; California University, , Academic Press: New York
  • Bothner-By, A.A., Magnetic Field Induced Alignment of Molecules (1995) Encyclopedia of Nuclear Magnetic Resonance, pp. 2932-2938. , Grant, D. M, Harris, R. K, Eds, John Wiley & Sons: Chichester
  • Ottiger, M., Tjandra, N., Bax, A., Magnetic Field Dependent Amide 15 N Chemical Shifts in a Protein-DNA Complex Resulting from Magnetic Ordering in Solution (1997) J. Am. Chem. Soc, 119, p. 9825
  • Lipari, G., Szabo, A., Model-free approach to the interpretation of nuclear magnetic resonance (1982) J. Am. Chem. Soc, 104, p. 4546
  • Lipari, G., Szabo, A., Model-free approach to the interpretation of nuclear magnetic resonance relaxation in macromolecules. 2. Analysis of experimental results (1982) J. Am. Chem. Soc, 104, p. 4559
  • Werbelow, L.G., Dynamic Frequency Shift (1995) Encyclopedia of Nuclear Magnetic Resonance, pp. 1776-1783. , Grant, D. M, Harris, R. K, Eds, John Wiley & Sons: Chichester
  • Baker, M.R., Anderson, C.H., Ramsey, N.F., Nuclear Magnetic Antishielding of Nuclei in Molecules. Magnetic Moments of F19, N14, and N15 (1964) Phys. Rev, 133, pp. A1533
  • Saika, A., Slichter, C.P., A Note on the Fluorine Resonance Shifts (1954) J. Chem. Phys, 22, p. 26
  • Herbison-Evans, D., Richards, R.E., 14N chemical shifts in organic compounds (1964) Mol. Phys, 8, p. 19
  • Lambert, J. B.; Roberts, J. D. Nitrogen-15 Magnetic Resonance Spectroscopy. V. Oxygen-Nitrogen Compounds. J. Am. Chem. Soc. 1965, 87, 4087; Dervan, P. B.; Squillacote, M. E.; Lahti, P. M.; Sylwester, A. P.; Roberts, J. D. Nitrogen-15 NMR spectrum of a 1,1-diazene. N-(2,2,6,6- tetramethylpiperidyl)nitrene. J. Am. Chem. Soc. 1981, 103, 1120; Witanowski, M., Biedrzycka, Z., Webb, G.A., Solvent Effects on the Nitrogen NMR Shielding of 2-Methyl-2-nitrosopropane and its Azodioxy Dimer (1996) Maen. Reson. Chem, 34, p. 233
  • http://www.kjemi.uio.no/software/dalton, DALTON, An electronic structure program, Release 2.0; accessed Feb 24, 2006, 2005; Dunning Jr., T.H., Gaussian Basis Set for Use in Correlated Molecular Calculations. I. The Atoms Boron through Neon and Hydrogen (1989) J. Chem. Phys, 90, p. 1007
  • Woon, D.E., Dunning Jr., T.H., Gaussian basis sets for use in correlated molecular calculations. V. Coreion valence basis sets for boron through neon (1995) J. Chem. Phys, 103, p. 4572
  • Ligabue, A., Sauer, S.P.A., Lazzeretti, P., Correlated and gauge invariant calculations of nuclear magnetic shielding constants using the continuous transformation of the origin of the current density approach (2003) J. Chem. Phys, 118, p. 6830
  • The aug-cc-pCVTZ/CTOCD-uc and sp tt d tt f 2 /sp t d basis sets can be downlowed from http://fyskem.ki.ku.dk/sauer/BasisSets; Sauer, S.P.A., Paidarová, L., Oddershede, J., Correlated and Gauge Origin Independent Calculations of Magnetic Proper-ties. II. Shielding Constants of Simple Singly Bonded Molecules (1994) Theor. Chim. Acta, 88, p. 351
  • Sauer, S.P.A., Paidarová, L., Oddershede, J., Correlated and Gauge Origin Independent Calculations of Magnetic Proper-ties. I. Triply Bonded Molecules (1994) Mol. Phys, 81, p. 87
  • Huzinaga, S., Andzelm, J., Klobukowsi, M., Radzio-Andzelm, E., Sakai, Y., Tatewaki, H., (1984) Gaussian Basis Sets for Molecular Calculations, , Elsevier: Amsterdam
  • Lazzeretti, P., Malagoli, M., Zanasi, R., Sistemi informatici e calcolo parallelo Research Report, , Technical report on project, 1/67, CNR, 1991
  • Becke, A.D., Density-functional termochemistry. III. The role of exact exchange (1993) J. Chem. Phys, 98, p. 5648
  • Petersson, G.A., Bennett, A., Tensfeldt, T.G., Al-Laham, M.A., Shirley, W.A., Mantzaris, J., A complete basis set model chemistry. I. The total energies of closed-shell atoms and hydrides of the first-row elements (1988) J. Chem. Phys, 89, p. 2193
  • Petersson, G.A., Tensfeldt, T.G., Montgomery Jr., J.A., A complete basis set model chemistry. III. The complete basis set-quadratic configuration interaction family of methods (1991) J. Chem. Phys, 94, p. 6091
  • Keal, W., Tozer, D.J., The exchange-correlation potential in Kohn-Sham nuclear magnetic resonance shielding calculations (2003) J. Chem. Phys, 119, p. 3015
  • Keal, W., Tozer, D.J., A semiempirical generalized gradient approximation exchange-correlation functional (2004) J. Chem. Phys, 121, p. 5654
  • Ligabue, A., Sauer, S.P.A., Lazzeretti, P., Gauge invariant calculations of nuclear magnetic shielding constants using the continuous transformation of the origin of the current density approach. II. Density functional and coupled cluster theory (2007) J. Chem. Phys, 126, p. 154111
  • Kongsted, J., Aidas, K., Mikkelsen, K.V., Sauer, S.P.A., On the accuracy of density functional theory to predict shifts in nuclear magnetic resonance shielding constants due to hydrogen bonding (2008) J. Chem. Theor. Comput, 4, p. 267
  • Soffe, N., Boyd, J., Leonard, M., The construction of a high-resolution 750 MHz probehead (1995) J. Maen. Reson. A, 16, p. 117
  • Lumsden, M.D., Wu, G., Wasylishen, R.E., Curtis, R.D., Solid-state nitrogen-15 NMR studies of the nitroso group in the nitrosobenzene dimer and p-nitroso-N, N-dimethylaniline (1993) J. Am. Chem. Soc, 115, p. 2825
  • Boyd, J., Pagola, G.I., Caputo, M.C., Ferraro, M.B., Lazzeretti, P., To be published; Sturz, L., Dölle, A., Anisotropic Reorientational Dynamics of Toluène in Neat Liquid. A 13 C Nuclear Magnetic Relaxation Study (2001) J. Phys. Chem. A, 105, p. 5055
  • Mohr, P.J., Taylor, B.N., CODATA Recommended Values of the Fundamental Physical Constants: 2002 (2005) Rev. Mod. Phys, 77, p. 1
  • Andersson, L.O., Mason, J.B., van Bronswijk, W., Nitrogen Nuclear Magnetic Resonance. Part 1. The Nitroso(Nitrosyl) Group (1970) J. Chem. Soc. A, 1970, p. 296
  • Jameson, C.J., Jameson, A.K., Oppusunggu, D., Wille, S., Burrell, P.M., Mason, J., 15N Nuclear Magnetic Shielding Scale from Gas Phase Studies (1981) J. Chem. Phys, 74, p. 81
  • Witanowski, M., Biedrzycka, Z., Sicinska, W., Webb, G.A., Solvent-Induced Effects on the Nitrogen NMR Shieldings of Some Nitrosobenzene Systems (1997) Magn. Reson. Chem, 35, p. 262

Citas:

---------- APA ----------
Boyd, J., Pagola, G.I., Caputo, M.C., Ferraro, M.B. & Lazzeretti, P. (2009) . Calculation of hypershielding contribution to isotropic nitrogen shielding in strong magnetic fields. Journal of Chemical Theory and Computation, 5(5), 1343-1349.
http://dx.doi.org/10.1021/ct900034d
---------- CHICAGO ----------
Boyd, J., Pagola, G.I., Caputo, M.C., Ferraro, M.B., Lazzeretti, P. "Calculation of hypershielding contribution to isotropic nitrogen shielding in strong magnetic fields" . Journal of Chemical Theory and Computation 5, no. 5 (2009) : 1343-1349.
http://dx.doi.org/10.1021/ct900034d
---------- MLA ----------
Boyd, J., Pagola, G.I., Caputo, M.C., Ferraro, M.B., Lazzeretti, P. "Calculation of hypershielding contribution to isotropic nitrogen shielding in strong magnetic fields" . Journal of Chemical Theory and Computation, vol. 5, no. 5, 2009, pp. 1343-1349.
http://dx.doi.org/10.1021/ct900034d
---------- VANCOUVER ----------
Boyd, J., Pagola, G.I., Caputo, M.C., Ferraro, M.B., Lazzeretti, P. Calculation of hypershielding contribution to isotropic nitrogen shielding in strong magnetic fields. J. Chem. Theory Comput. 2009;5(5):1343-1349.
http://dx.doi.org/10.1021/ct900034d