Artículo
Weht, R.O.; Kohanoff, J.; Estrin, D.A.; Chakravarty, C. "An ab initio path integral Monte Carlo simulation method for molecules and clusters: Application to Li4 and Li5+" (1998) Journal of Chemical Physics. 108(21):8848-8858
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Abstract:
A novel method for simulating the statistical mechanics of molecular systems in which both nuclear and electronic degrees of freedom are treated quantum mechanically is presented. The scheme combines a path integral description of the nuclear variables with a first-principles adiabatic description of the electronic structure. The electronic problem is solved for the ground state within a density functional approach, with the electronic orbitals expanded in a localized (Gaussian) basis set. The discretized path integral is computed by a METROPOLIS Monte Carlo sampling technique on the normal modes of the isomorphic ring polymer. An effective short-time action correct to order τ4 is used. The validity and performance of the method are tested by studying two small lithium clusters, namely Li4 and Li5+. Structural and electronic properties computed within this fully quantum-mechanical scheme are presented and compared to those obtained within the classical nuclei approximation. Quantum delocalization effects turn out to be significant as shown by the fact that quantum simulation results at 50 K approximately correspond to those of classical simulations carried out at 150 K. The scaling factor depends, however, on the specific physical property, thus evidencing the different character of quantum and thermal correlations. Tunneling turns out to be irrelevant in the temperature range investigated (50-200 K). © 1998 American Institute of Physics.
Registro:
| Documento: | Artículo |
| Título: | An ab initio path integral Monte Carlo simulation method for molecules and clusters: Application to Li4 and Li5+ |
| Autor: | Weht, R.O.; Kohanoff, J.; Estrin, D.A.; Chakravarty, C. |
| Filiación: | Intl. Centre for Theoretical Physics, Strada Costiera 11, I-34014 Trieste, Italy Comn. Nac. de Ener. Atómica, Avenida Libertador 8250, 1429, Buenos Aires, Argentina Depto. Quim. Inorg., Analitica y Q., Fac. de Ciencias Exactas y Naturales, Pabellón 11, 1428, Buenos Aires, Argentina Department of Chemistry, Indian Inst. Technol.-Delhi Hauz K., New Delhi 110016, India |
| Año: | 1998 |
| Volumen: | 108 |
| Número: | 21 |
| Página de inicio: | 8848 |
| Página de fin: | 8858 |
| DOI: | http://dx.doi.org/10.1063/1.476331 |
| Título revista: | Journal of Chemical Physics |
| Título revista abreviado: | J Chem Phys |
| ISSN: | 00219606 |
| CODEN: | JCPSA |
| PDF: | https://bibliotecadigital.exactas.uba.ar/download/paper/paper_00219606_v108_n21_p8848_Weht.pdf |
| Registro: | https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00219606_v108_n21_p8848_Weht |
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Citas:
---------- APA ----------
Weht, R.O., Kohanoff, J., Estrin, D.A. & Chakravarty, C. (1998) . An ab initio path integral Monte Carlo simulation method for molecules and clusters: Application to Li4 and Li5+. Journal of Chemical Physics, 108(21), 8848-8858.http://dx.doi.org/10.1063/1.476331
---------- CHICAGO ----------
Weht, R.O., Kohanoff, J., Estrin, D.A., Chakravarty, C. "An ab initio path integral Monte Carlo simulation method for molecules and clusters: Application to Li4 and Li5+" . Journal of Chemical Physics 108, no. 21 (1998) : 8848-8858.http://dx.doi.org/10.1063/1.476331
---------- MLA ----------
Weht, R.O., Kohanoff, J., Estrin, D.A., Chakravarty, C. "An ab initio path integral Monte Carlo simulation method for molecules and clusters: Application to Li4 and Li5+" . Journal of Chemical Physics, vol. 108, no. 21, 1998, pp. 8848-8858.http://dx.doi.org/10.1063/1.476331
---------- VANCOUVER ----------
Weht, R.O., Kohanoff, J., Estrin, D.A., Chakravarty, C. An ab initio path integral Monte Carlo simulation method for molecules and clusters: Application to Li4 and Li5+. J Chem Phys. 1998;108(21):8848-8858.http://dx.doi.org/10.1063/1.476331
