Abstract
We have explored lowest energy minima structures of gold atom clusters both, charged and neutral (Au\hbox{$_{n}^{\nu}$}νn with n = 20, 28, 34, 38, 55, 75, 101, 146, 147, 192, 212 atoms and ν = 0, ±1). The structures have been obtained from first principles generalized gradient approximation, density functional theory (DFT) calculations based on norm-conserving pseudopotentials and numerical atomic basis sets. We have found two new disordered or defective isomers lower in energy than their ordered counterparts for n = 101, 147. The purpose of this work is to systematically study the difference between the electronic properties of the two lowest ordered and disordered isomers for each size. Our results agree with previous first principle calculations and with some recent experimental results (Au20 and Au101). For each case we report total energies, binding energies, ionization potentials, electron affinities, density of states, highest occupied molecular orbital-lowest unoccupied molecular orbital (HOMO-LUMO) gaps, Housdorff chirality measure index and their simulated image in a high resolution transmission electron microscopy (HRTEM). The calculated properties of the two low lying (ordered and disordered) isomers show clear differences as to be singled out in a suitable experimental setting. An extensive discussion on the evolution with size of the cohesive energy, the ionization potentials, the electron affinities, the HOMO-LUMO gaps and their index of chirality to determine the crossover between them is given.
Similar content being viewed by others
References
N. Lidgi-Guigui, C. Leung, R.E. Palmer, Surf. Sci. 602, 1006 (2008)
R.E. Palmer, C. Leung, Trends Biotechnol. 25, 48 (2006)
R.P. Andres, T. Bein, M. Dorogi, S. Feng, J.I. Henderson, C.P. Kubiak, W. Mahoney, R.G. Osifchin, R. Reiefenberger, Science 272, 1323 (1996)
R.P. Andres, J.D. Bielefeld, J.I. Henderson, D.B. Janes, V.R. Kolagunta, C.P. Kubiak, W.J. Mahoney, R.G. Osifchin, Science 273, 1690 (1996)
P. Alivisatos, K.P. Johnsson, X. Peng, T.E. Wilson, C.J. Loweth, M.P. Bruchez, P.G. Schultz, Nature 382, 609 (1996)
A.P. Alivisatos, Science 271, 933 (1996)
P. Alivisatos, Nat. Biotechnol. 22, 47 (2004)
M. Haruta, Catal. Today 36, 153 (1997)
R.J.C. Batista, H. Chacham, M.S.C. Mazzoni, I.L. Garzón, M.R. Beltrán, Phys. Rev. Lett. 96, 116802 (2006)
R.J.C. Batista, P. Ordejón, H. Chacham, E. Artacho, Phys. Rev. B 75, 041402 (2007)
A. Sanchez, S. Abbet, U. Heiz, W.D. Schneider, H. Häkkinen, R.N. Barnett, U. Landman. J. Phys. Chem. A 103, 9573 (1999)
T.P. Martin, Phys. Rev. 273, 199 (1993)
S.J.L. Billinge, I. Levin, Science 316, 561 (2007)
P.D. Jadzinsky, G. Calero, C.J. Ackerson, D.A. Bushnell, R.D. Kornberg, Science 318, 430 (2007)
O. Lopez-Acevedo, H. Tsunoyama, T. Tsukuda, H. Häkkinen, C.M. Aikens, J. Am. Chem. Soc. 132, 8210 (2010)
G. Chen, Q. Wang, Q. Sun, Y. Kawazoe, P. Jena, J. Chem. Phys. 132, 194306 (2010)
J. Wang, G. Wang, J. Zhao, Phys. Rev. B 66, 035418 (2002)
S. Bulusu, X. Li, S. Wang, X.C. Zeng, Porc. Natl. Acad. Sci. USA 103, 8326 (2006)
S. Bulusu, X.C. Zeng, J. Chem. Phys. 125, 154303 (2006)
X. Xing, B. Yoon, U. Landman, J.H. Parks, Phys. Rev. B 74, 165423 (2006)
J.P.K. Doye, D.J. Wales, Phys. Rev. Lett. 80, 1357 (1998)
J.P.K. Doye, D.J. Wales, Phys. Rev. Lett. 86, 5719 (2001)
D.J. Wales, Energy Landscapes with Applications to Clusters, Biomolecules and Glasses (Cambridge University Press, Cambridge, 2003)
X. Gu, M. Ji, S.H. Wei, X.G. Gong, Phys. Rev. B 70, 205401 (2004)
O.D. Haberlen, S.C. Chung, N. Rosch, Ber. Bunsen-Ges. Phys. Chem. 98, 882 (1994)
I.L. Garzón, K. Michaelian, M.R. Beltrán, A. Posada-Amarillas, P. Ordejón, E. Artacho, D. Sánchez Portal, J. Soler, Phys. Rev. Lett. 81, 1600 (1998)
I.L. Garzón, A. Posada-Amarillas, Phys. Rev. B 54, 11796 (1996)
I.L. Garzón, K. Michaelian, M.R. Beltrán, A. Posada-Amarillas, P. Ordejón, E. Artacho, D. Sánchez Portal, J. Soler, Eur. Phys. J. D 9, 211 (1999)
J.A. Ascencio, C. Gutiérrez-Wing, M.E. Espinosa, M. Marín, S. Tehuacanero, C. Zorrilla, M. José-Yacamán, Surf. Sci. 396, 349 (1998)
C.L. Cleveland, U. Landman, T.G. Schaaff, M.N. Shafigullin, P.W. Stephens, R.L. Whetten, Phys. Rev. Lett. 79, 1873 (1997)
R.L. Whetten, J.T. Khoury, M.M. Alvarez, S. Murthy, I. Vezmar, Z.L. Wang, P.W. Stephens, C.L. Cleveland, W.D. Luedtke, U. Landman, Adv. Mat. 8, 428 (1996)
F. Baletto, R. Ferrando, A. Fortunelli, F. Montalenti, C. Mottet, J. Chem. Phys. 116, 3856 (2002)
K. Michaelian, N. Rendón, I.L. Garzón, Phys. Rev. B 60, 2000 (1999)
R.P. Gupta, Phys. Rev. B 23, 6265 (1981)
P. Ordejón, E. Artacho, J.M. Soler, Phys. Rev. B 53, 10 441 (1996)
D. Sánchez-Portal, P. Ordejón, E. Artacho, J.M. Soler, Int. J. Quantum Chem. 65, 453 (1997)
E. Artacho, D. Sánchez-Portal, P. Ordejón, A. García, J.M. Soler, Phys. Status Solidi B 215, 809 (1999)
W. Khon, L.J. Sham, Phys. Rev. 140, 1133 (1965)
J.M. Soler, M.R. Beltrán, K. Michaelian, I.L. Garzon, P. Ordejón, D. Sanchez-Portal, E. Artacho, Phys. Rev. B 61, 5771 (2000)
I.L. Garzón, J.A. Reyes, J.I.L. Rodríguez Hernámdez, I. Sigal, M.R. Beltrán, K. Michaelian, Phys. Rev. B 66, 073403 (2002)
I.L. Garzón, E. Artacho, M.R. Beltrán, A. García, J. Junquera, K. Michaelian, P. Ordejón, D. Sánchez-Portal, J.M. Soler, Nanotechnology 12, 126 (2001)
T.G. Schaaff, R.L. Whetten. J. Phys. Chem. B 104, 2630 (2000)
H. Häkkinen, M. Moseler, O. Kostko, N. Morgner, M. Astruc Hoffmann, B.V. Issendorff, Phys. Rev. Lett. 93, 093401 (2004)
H. Häkkinen, M. Walter, H. Grönbeck, J. Phys. Chem. B 110, 9927 (2006)
A.B. Buda, K. Mislow, J. Am. Chem. Soc. 114, 6006 (1992)
A.B. Buda, T. Auf def Heyde, K. Mislow, Angew. Chem. Int. Ed. Engl. 31, 989 (1992)
J. Jellinek, I.L. Garzón, Z. Phys. D 20, 239 (1991)
I.L. Garzón, J. Jellinek, Z. Phys. D 20, 235 (1991)
I.L. Garzón, J. Jellinek, Z. Phys. D 26, 316 (1993)
K. Michaelian, Am. J. Phys. 66, 231 (1998)
V. Rossato, M. Guillope, B. Legrand, Philos. Mag. A 59, 321 (1989)
N. Troullier, J.L. Martins, Phys. Rev. B 43, 1993 (1991)
L. Kleinman, D.M. Bylander, Phys. Rev. Lett. 48, 1425 (1982)
E.M. Fernández, J.M. Soler, I.L. Garzón, L.C. Balbás, Phys. Rev. B 70, 165403 (2004)
J.P. Perdew, K. Burke, M. Ernzerhof, Phys. Rev. B 77, 3865 (1996)
O.F. Sankey, D.J. Niklewski, Phys. Rev. B 40, 3979 (1989)
W.H. Press, S.A. Teukolsky, W.T. Vetterling, B.P. Flannery, Numerical Recipes. The Art of Scientific Computing (Cambridge University Press, Cambridge, 1992)
J.M. Soler, M.R. Beltrán, K. Michaelian, I.L. Garzón, P. Ordejón, D. Sánchez Portal, E. Artacho, Phys. Rev. B 61, 5771 (2000)
A.F. Jalbout, F.F. Contreras-Torres, L.A. Pérez, I.L. Garzón, J. Phys. Chem. A 112, 353 (2008)
I.E. Santizo, F. Hidalgo, L.A. Pérez, C. Noguez, I.L. Garzón, J. Phys. Chem. C 112, 17533 (2008)
R.M. Olson, M.S. Gordon, J. Chem. Phys. 126, 214310 (2007)
R.M. Olson, S. Varganov, M.S. Gordon, H. Metiu, S. Chretien, P. Piecuch, K. Kowalski, S. Kucharski, M. Musial, J. Am. Chem. Soc. 127, 1049 (2005)
I.L. Garzón, C. Rovira, K. Michaelian, M.R. Beltrán, P. Ordejón, J. Junquera, D. Sanchez-Portal, E. Artacho, J.M. Soler, Phys. Rev. Lett. 85, 5250 (2000)
A. Gómes Rodríguez, L.M. Beltrán del Rio, R. Herrera Becerra, Ultramicroscopy 110, 95 (2010)
J.M. Cowley, A.F. Moodie, Acta Cryst. 10, 609 (1957)
R.L. Whetten, R.C. Price, Science 318, 407 (2007)
X. Gu, S. Bulusu, X. Li, X.C. Zeng, J. Li, X.G. Gong, L.S. Wang, J. Phys. Chem. C 111, 8228 (2007)
J. Li, X. Li, H.J. Zhai, L.S. Wang, Science 299, 864 (2003)
C. Jackschath, I. Rabin, W. Ber Bunsenges Schulz, Phys. Chem. 86, 1200 (1992)
E.S. Kryachko, F. Remacle, Int. J. Quantum Chem. 107, 2922 (2007)
X. Xing, B. Yoon, U. Landman, J.H. Parks, Phys. Rev. B 74, 165423 (2006)
K.J. Taylor, C.L. Pettiette-Hall, O. Cheshnovsky, R.E. Smalley, J. Chem. Phys. 96, 3319 (1992)
G. Periyasami, F. Remacle, Nano Lett. 9, 3007 (2009)
P. Pyykkö, Chem. Soc. Rev. 37, 1967 (2008)
S.T. Arnold, J.G. Eaton, D. Patel-Misra, H.W. Sarkas, K.H. Bowen, Ion and Cluster Ion Spectroscopy and Structure (Elsevier, Amsterdam, 1988), p. 147
J. Wang, G. Wang, J. Zhao, Chem. Phys. Lett. 380, 716 (2003)
V.A. Spasov, Y. Shi, K.M. Ervin, Chem. Phys. 262, 75 (2000)
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Beltrán, M.R., Suárez Raspopov, R. & González, G. Structural evolution study of 1−2 nm gold clusters. Eur. Phys. J. D 65, 411–420 (2011). https://doi.org/10.1140/epjd/e2011-20273-2
Received:
Revised:
Published:
Issue Date:
DOI: https://doi.org/10.1140/epjd/e2011-20273-2