Abstract
Ab initio computational studies were performed for CdSe nanocrystals (NCs) over a wide variety of sizes ranging from 8 to 150 atoms in conjunction with recent experimental work. The density functional based calculations indicate substantial relaxations. Changes in coordination of surface atoms were found to play a crucial role in determining the NC stability and optical properties. While optimally (threefold) coordinated surface atoms resulted in stable closed-shell structures with large optical gaps, sub-optimal coordination gave rise to lower stability and negligible optical gaps. These computations are in qualitative agreement with recent chemical etching experiments suggesting that closed shell NCs contribute strongly to photoluminescence quantum yield while clusters with nonoptimal surface coordination do not.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
References
Murray C.B., Kagan C.R., Bawendi M.G. (2000). Annu. Rev. Mater. Sci. 30: 545
Alivisatos A.P. (1996). J. Phys. Chem. 100: 13226
Chan W.CW., Maxwell D.J., Gao X., Bailey R.E., Han M., Nie S. (2002). Curr. Opin. Biotechnol. 13: 40
Han M., Gao X., Su J.Z., Nie S. (2001). Nat. Biotechnol. 19: 631
Klimov V.I., Mikhailovsky A.A., Xu S., Malko A., Hollingsworth J.A., Leatherdale C.A., Eisler H.J. Bawendi M.G. (2000). Science 290, 314
Ispasoiu R.G., Lee J., Papadimitrakopoulos F., Goodson T. III (2001). Chem. Phys. Lett. 340: 7
Ispasoiu R.G., Jin Y., Lee J., Papadimitrakopoulos F., Goodson T. III (2002). Nano Lett. 2: 127
Huynh W.U., Dittmer J.J., Alivisatos A.P. (2002). Science 295: 2425
Peng X., Wickham J., Alivisatos A.P. (1998). J. Am. Chem. Soc. 120: 5343
Talapin D.V., Rogach A.L., Kornowski A., Haase M., Weller H. (2001). Nano. Lett. 1: 207
Li R., Lee J., Yang B., Horspool D.N., Aindow M., Papadimitrakopoulos F. (2005). J. Am. Chem. Soc. 127: 2524
Li R., Lee J., Kang D., Luo Z., Aindow M., Papadimitrakopoulos F. (2006). Adv. Funct. Mater. 16: 345
Talapin D.V., Rogach A.L., Shevchenko E.V., Kornowski A., Haase M., Weller H. (2002). J. Am. Chem. Soc. 124: 5782
Sarkar P., Springborg M. (2003). Phys. Rev. B 68: 235409
Rabani E. (2001). J. Chem. Phys. 115: 1493
Eichkorn K., Alrichs R. (1998). Chem. Phys. Lett. 288: 235
Wang L.W., Zunger A. (1996). Phys. Rev. B 53: 9579
Pokrant S., Whaley K.B. (1999). Eur. Phys. J. D 6: 255
Puzder A., Williamson A.J., Gygi F., Galli G. (2004). Phys. Rev. Lett. 92: 217401
Kasuya A., et al. (2004). Nature 3: 99
Troparevsky M.C., Kronik L., Chelikowsky J.R. (2002). Phys. Rev. B 65: 033311
Martin R. (2004) Electronic Structure: Basic Theory and Practical Methods. Cambridge University Press, New York
Soler J.M., Artacho E., Gale J., Garcia A., Junquera J., Ordejon P., Sanchez-Portal D. (2002). J. Phys.: Condens. Matter 14: 2745
Troullier N., Martins J.L. (1991). Phys. Rev. B 43: 1993
Zakharov O., Rubio A., Blasé X., Cohen M.L., Louie S.G. (1994). Phys. Rev. B 50: 10780
Hellwege, K.-H., Madelung, O.: Numerical Data and Functional Relationships in Science and Technology, Landolt-Bornstein, New Series, Group III, vol. 17a, 22a. Springer, Berlin Heidelberg, New York (1982)
Brus L.E. (1986). J. Phys. Chem. 90: 2555
Peng Z.A., Peng X. (2002). J. Am. Chem. Soc. 124: 3343
Soloviev V.N., Eichhöfer A., Fenske D., Banin U. (2000). J. Am. Chem. Soc. 122: 2673
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Yu, M., Fernando, G.W., Li, R. et al. Discrete size series of CdSe quantum dots: a combined computational and experimental investigation. J Computer-Aided Mater Des 14, 167–174 (2007). https://doi.org/10.1007/s10820-006-9040-y
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10820-006-9040-y