ABSTRACT
The three-dimensional structure of oleic acid-capped CdSe and thiol-capped CdTe nanocrystals used as quantum dots has been determined by total synchrotron radiation x-ray diffraction and atomic pair distribution function analysis. Both CdSe and CdTe are found to exhibit the zinc-blende-type atomic ordering. It is only slightly distorted in CdSe implying the presence of nanosize domains and very heavily distorted in CdTe due to the presence of distinct core-shell regions. The results well demonstrate the great potential of the experimental approach and thus encourage its wider application in quantum dot research.
ACKNOWLEDGMENTS
The work was supported by NSF through Grant No. DMR 0304391(NIRT) and CMU through Grant No. REF C602281. Use of the Advanced Photon Source was supported by the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. One of the authors (C.W.) is grateful to the support of National Science Foundation for Distinguished Young Scholars of China (50525310).
- 1. M. Bruchez, M. Moronne, P. Gin, S. Weiss, and A. P. Alivisatos, Science https://doi.org/10.1126/science.281.5385.2013 281, 2013 (1998). Google ScholarCrossref, ISI
- 2. M. Han, X. Gao, J. Z. Su, and S. Nie, Nat. Biotechnol. https://doi.org/10.1038/90228 19, 631 (2001). Google ScholarCrossref, ISI
- 3. W. C. W. Chan, D. J. Maxwell, X. Gao, R. E. Bailey, M. Han, and S. Nie, Curr. Opin. Biotechnol. https://doi.org/10.1016/S0958-1669(02)00282-3 13, 40 (2002). Google ScholarCrossref, ISI
- 4. C. A. Leatherdale, W. K. Woo, F. V. Mikulec, and M. G. Bawendi, J. Phys. Chem. B https://doi.org/10.1021/jp025698c 106, 7619 (2002). Google ScholarCrossref, ISI
- 5. X. Gao, Y. Cui, R. M. Levenson, L. W. K. Chung, and S. Nie, Nat. Biotechnol. https://doi.org/10.1038/nbt994 22, 969 (2004). Google ScholarCrossref, ISI
- 6. V. L. Colvin, M. C. Schlamp, and A. P. Alivisatos, Nature (London) https://doi.org/10.1038/370354a0 370, 354 (1994). Google ScholarCrossref, ISI
- 7. V. I. Klimov, A. A. Mikhailovsky, S. Xu, A. Malko, J. A. Hollingsworth, C. A. Leatherdale, H. J. Eisler, and M. G. Bawendi, Science https://doi.org/10.1126/science.290.5490.314 290, 314 (2000). Google ScholarCrossref, ISI
- 8. N. C. Greenham, X. G. Peng, and A. P. Alivisatos, Phys. Rev. B https://doi.org/10.1103/PhysRevB.54.17628 54, 17628 (1996). Google ScholarCrossref, ISI
- 9. X. Peng, L. Manna, W. Yang, J. Wickham, E. Scher, A. Kadavanich, and A. Alivisatos, Nature (London) https://doi.org/10.1038/35003535 404, 59 (2000). Google ScholarCrossref, ISI
- 10. L. Manna, E. C. Scher, and A. P. Alivisatos, J. Am. Chem. Soc. https://doi.org/10.1021/ja003055+ 122, 12700 (2000). Google ScholarCrossref, ISI
- 11. B. O. Dabbousi, J. Rodriguez-Viejo, F. V. Mikulec, J. R. Heine, H. Mattoussi, R. Ober, K. F. Jensen, and M. G. Bawendi, J. Phys. Chem. B https://doi.org/10.1021/jp971091y 101, 9463 (1997). Google ScholarCrossref, ISI
- 12. M. A. Hines and Ph. Guyot-Sionnest, J. Phys. Chem. https://doi.org/10.1021/jp9530562 100, 468 (1996). Google ScholarCrossref, ISI
- 13. X. Peng, M. C. Schlamp, A. V. Kadavanich, and A. P. Alivisatos, J. Am. Chem. Soc. https://doi.org/10.1021/ja970754m 119, 7019 (1997). Google ScholarCrossref, ISI
- 14. G. M. Dalpian, M. L. Tiago, M. L. Puerto, and J. R. Chelikovsky, Nano Lett. https://doi.org/10.1021/nl0525094 6, 501 (2006). Google ScholarCrossref
- 15. J. Rockenberger, L. Troger, A. L. Rogach, M. Tischer, M. Grundmann, A. Eychmuller, and H. Weller, J. Chem. Phys. https://doi.org/10.1063/1.476216 108, 7807 (1998). Google ScholarScitation, ISI
- 16. A. Eychmuller and A. L. Rorach, Pure Appl. Chem. 72, 179 (2000). Google ScholarCrossref
- 17. A. C. Carter, C. E. Bouldin, K. M. Kemner, M. I. Bell, J. C. Woicik, and S. A. Majetich, Phys. Rev. B https://doi.org/10.1103/PhysRevB.55.13822 55, 13822 (1997). Google ScholarCrossref
- 18. D. S. Yang, D. R. Fazzini, T. I. Morrison, L. Troger, and G. Bunker, J. Non-Cryst. Solids https://doi.org/10.1016/S0022-3093(96)00577-7 210, 275 (1997). Google ScholarCrossref
- 19. J. McBride, J. Treadway, L. C. Feldman, S. J. Pennycook, and S. J. Rosenthal, Nano Lett. 7, 1496 (2006). Google ScholarCrossref
- 20. J. McBride, T. Kippeny, S. J. Pennycook, and S. J. Rosenthal, Nano Lett. https://doi.org/10.1021/nl049406q 4, 1279 (2004). Google ScholarCrossref
- 21. Z. T. Deng, L. Cao, F. Q. Tang, and B. S. Zou, J. Phys. Chem. B https://doi.org/10.1021/jp052484x 109, 16671 (2005). Google ScholarCrossref, ISI
- 22. H. Zhang, L. Wang, H. Xiong, L. Hu, B. Yang, and W. Li, Adv. Mater. (Weinheim, Ger.) 15, 1712 (2003). Google ScholarCrossref
- 23. J. Gao, W. Yang, and C. Wang, J. Phys. Chem. B 109, 17467 (2005). Google ScholarCrossref
- 24. V. Petkov, I. -K. Jeong, J. S. Chung, M. F. Thorpe, S. Kycia, and S. J. L. Billinge, Phys. Rev. Lett. https://doi.org/10.1103/PhysRevLett.83.4089 83, 4089 (1999). Google ScholarCrossref
- 25. T. Egami and S. J. L. Billinge, Underneath the Bragg Peaks. Structural Analysis of Complex Materials (Pergamon, Oxford, 2003). Google Scholar
- 26. V. Petkov, P. Y. Zavalji, S. Lutta, M. S. Whittingham, V. Parvanov, and S. Shastri, Phys. Rev. B https://doi.org/10.1103/PhysRevB.69.085410 69, 085410 (2004). Google ScholarCrossref
- 27. M. Gateshki, V. Petkov, G. Williams, S. K. Pradhan, and Y. Ren, Phys. Rev. B https://doi.org/10.1103/PhysRevB.71.224107 71, 224107 (2005). Google ScholarCrossref
- 28. H. P. Klug and L. E. Alexander, X-ray Diffraction Procedures for Polycrystalline Materials (Wiley, New York, 1974). Google Scholar
- 29. Y. Waseda, The Structure of Nanosrystalline Materials (McGraw-Hill, New York, 1980). Google Scholar
- 30. V. Petkov, J. Appl. Crystallogr. https://doi.org/10.1107/S0021889889002104 22, 387 (1989). Google ScholarCrossref
- 31. H. Zhang, B. Gilbert, N. Huang, and J. F. Banfield, Nature (London) https://doi.org/10.1038/nature01845 424, 1025 (2003). Google ScholarCrossref, ISI
- 32. R. B. Neder and V. I. Korsunsiy, J. Phys.: Condens. Matter https://doi.org/10.1088/0953-8984/17/5/013 17, S125 (2005). Google ScholarCrossref
- 33. Th. Proffen and S. J. L. Billinge, J. Appl. Crystallogr. https://doi.org/10.1107/S0021889899003532 32, 572 (1999). Google ScholarCrossref
- 34. M. Kh. Rabadanov, I. A. Verin, Yu. M. Ivanov, and V. I. Simonov, Kristallografiya 46, 703 (2001). Google Scholar
- 35. L. E. Brus, Appl. Phys. A: Solids Surf. https://doi.org/10.1007/BF00331535 53, 465 (1991). Google ScholarCrossref
- 36.It may be noted that the agreement factors achieved with the PDF analyses appear somewhat higher when compared to those usually resulted from the Rietveld analyses of conventional diffraction data in reciprocal space. This reflects the fact that the atomic PDF differs from the conventional XRD pattern being a quantity much more sensitive to the local atomic ordering in materials. As a result, ’s between 10% and 20% are common for PDF analyses. The inherently higher absolute value of the goodness-of-fit factors resulted from PDF-based analyses does not affect their functional purpose as a residual quantity that must be minimized to find the best fit and as a quantity allowing to differentiate between competing structural models.
- 37. H. Weller, Adv. Mater. (Weinheim, Ger.) https://doi.org/10.1002/adma.19930050204 5, 88 (1993). Google ScholarCrossref
- 38. S. K. Vashist, R. Tewari, R. P. Bajpal, L. M. Bharadwaj, and R. Reiteri, Nanotechnology https://doi.org/10.1088/0957-4484/2/1/001 2, 1 (2006). Google ScholarCrossref
- 39. S. Ergun and S. R. Schehl, Carbon https://doi.org/10.1016/0008-6223(73)90063-8 11, 127 (1973). Google ScholarCrossref
- 40. P. D. Lao, Y. Guo, G. G. Siu, and S. C. Shen, Phys. Rev. B https://doi.org/10.1103/PhysRevB.48.11701 48, 11701 (1993). Google ScholarCrossref
- 41. G. Scamarcio, M. Lugara, and D. Manno, Phys. Rev. B https://doi.org/10.1103/PhysRevB.45.13792 45, 13792 (1992). Google ScholarCrossref, ISI
- 42. Y. Hwang, S. Shin, H. Park, S. Park, U. Kim, H. Jeong, E. Shin, and D. Kim, Phys. Rev. B https://doi.org/10.1103/PhysRevB.54.15120 54, 15120 (1996). Google ScholarCrossref
- 43. N. Herron, J. Calabrese, W. Farneth, and Y. Wang, Science 259, 1426 (1993). Google ScholarCrossref
- 44. Y. Wang and N. Herron, Phys. Rev. B https://doi.org/10.1103/PhysRevB.42.7253 42, 7253 (1990). Google ScholarCrossref, ISI
- 45. J.-Yu. Zhang, X.-Yo Wang, M. Xiao, L. Qu, and X. Peng, Appl. Phys. Lett. https://doi.org/10.1063/1.1507613 81, 2076 (2002). Google ScholarScitation, ISI
- 46. D. Rodic, V. Spasojevic, A. Bajorek, and P. Oennerud, J. Magn. Magn. Mater. 152, 159 (1996). Google ScholarCrossref
- 47. H. Borchert, D. V. Talapin, N. Gopanik, C. McGinley, S. Adam, A. Lobo, T. Moller, and H. Weller, J. Phys. Chem. B https://doi.org/10.1021/jp0352884 107, 9662 (2003). Google ScholarCrossref
Please Note: The number of views represents the full text views from December 2016 to date. Article views prior to December 2016 are not included.

