Charging Quenches Multiple Exciton Generation in Semiconductor Nanocrystals: First-Principles Calculations on Small PbSe Clusters
Source abstract
Abstract
We demonstrate using symmetry adapted cluster theory with configuration interaction (SAC-CI) that charging of small PbSe nanocrystals (NCs) greatly modifies their electronic states and optical excitations. Conduction and valence band transitions that are not available in neutral NCs dominate low energy electronic excitations and show weak optical activity. At higher energies these transitions mix with both single excitons (SEs) and multiple excitons (MEs) associated with transitions across the band-gap. As a result, both SEs and MEs are significantly blue-shifted, and ME generation is drastically hampered. The overall contribution of MEs to the electronic excitations of the charged NCs is small even at very high energies. The calculations support the recent view that the observed strong dependence of the ME yields on the experimental conditions is likely due to the effects of NC charging.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Quantum Dots Synthesis And Properties · Chalcogenide Semiconductor Thin Films · Nanocluster Synthesis and Applications
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
Department of Chemistry, University of Washington, Seattle, Washington 98195-1700
References (40)
Show source-provided references
1. Beard M. C. · Nano Lett. · 2009 · 9 · 83610.1021/nl803600v ↗
2. Rabani E. · Nano Lett. · 2008 · 8 · 448810.1021/nl802443c ↗
3. Mcguire J. A. · Acc. Chem. Res. · 2008 · 41 · 181010.1021/ar800112v ↗
4. Trinh M. T. · Nano Lett. · 2008 · 8 · 171310.1021/nl0807225 ↗
5. Nozik A. J. · Chem. Phys. Lett. · 2008 · 457 · 310.1016/j.cplett.2008.03.094 ↗
6. Prezhdo O. V. · Chem. Phys. Lett. · 2008 · 460 · 110.1016/j.cplett.2008.03.099 ↗
7. Ben-Lulu M. · Nano Lett. · 2008 · 8 · 120710.1021/nl080199u ↗
8. Franceschetti A. · Phys. Rev. Lett. · 2008 · 100 · 13680510.1103/PhysRevLett.100.136805 ↗
9. Luo J.-W. · Nano Lett. · 2008 · 8 · 317410.1021/nl801459h ↗
10. Nair G. · Phys. Rev. B · 2008 · 78 · 12532510.1103/PhysRevB.78.125325 ↗
11. Nair G. · Phys. Rev. B · 2007 · 76 · 0813410.1103/PhysRevB.76.081304 ↗
12. Nozik A. J. · Annu. Rev. Phys. Chem. · 2001 · 52 · 19310.1146/annurev.physchem.52.1.193 ↗
13. Nozik A. J. · Physica E · 2002 · 14 · 11510.1016/S1386-9477(02)00374-0 ↗
14. Crooker S. · Phys. Rev. Lett. · 2002 · 89 · 18680210.1103/PhysRevLett.89.186802 ↗
15. Schaller R. D. · Phys. Rev. Lett. · 2004 · 92 · 18660110.1103/PhysRevLett.92.186601 ↗
16. Ellingson R. J. · Nano Lett · 2005 · 5 · 86510.1021/nl0502672 ↗
17. Schaller R. D. · Nat. Phys. · 2005 · 1 · 18910.1038/nphys151 ↗
18. Schaller R. D. · Appl. Phys. Lett. · 2005 · 87 · 25310210.1063/1.2142092 ↗
19. Beard M. C. · Nano Lett. · 2007 · 7 · 250910.1021/nl071486l ↗
20. Schaller R. D. · Nano Lett. · 2007 · 7 · 346910.1021/nl072046x ↗
21. Pijpers J. J. H. · J. Phys. Chem. C · 2007 · 111 · 414610.1021/jp066709v ↗
22. Califano M. · Nano Lett. · 2004 · 4 · 52510.1021/nl049869w ↗
23. Pandey A. · Science · 2008 · 322 · 92910.1126/science.1159832 ↗
24. Schaller R. D. · Phys. Rev. Lett. · 2005 · 95 · 19640110.1103/PhysRevLett.95.196401 ↗
25. Harbold J. M. · Phys. Rev. B · 2005 · 72 · 19531210.1103/PhysRevB.72.195312 ↗
26. Kilina S. V. · J. Phys. Chem. C · 2007 · 111 · 487110.1021/jp0669052 ↗
27. Kilina S. V. · ACS Nano · 2009 · 3 · 9310.1021/nn800674n ↗
28. Cooney R. R. · Phys. Rev. Lett. · 2007 · 98 · 17740310.1103/PhysRevLett.98.177403 ↗
29. Isborn C. M. · J. Phys. Chem. C · 2008 · 112 · 1829110.1021/jp807283j ↗
30. Peterson J. J. · Nano Lett. · 2006 · 6 · 51010.1021/nl0525756 ↗
31. Kamisaka H. · Nano Lett. · 2006 · 6 · 229510.1021/nl0617383 ↗
32. Habenicht B. F. · Nano Lett. · 2007 · 7 · 326010.1021/nl0710699 ↗
33. Kamisaka H. · J. Phys. Chem. C · 2008 · 112 · 780010.1021/jp710435q ↗
34. Nakatsuji H. · J. Chem. Phys. · 1978 · 68 · 205310.1063/1.436028 ↗
35. Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; Scuseria, G. E.; Robb, M. A.; Cheeseman, J. R.; Montgomery, J. A., Jr.; Vreven, T.; Kudin, K. N.; Burant, J. C.; Millam, J. M.; Iyengar, S. S.; Tomasi, J.; Barone, V.; Mennucci, B.; Cossi, M.; Scalmani, G.; Rega, N.; Petersson, G. A.; Nakatsuji, H.; Hada, M.; Ehara, M.; Toyota, K.; Fukuda, R.; Hasegawa, J.; Ishida, M.; Nakajima, T.; Honda, Y.; Kitao, O.; Nakai, H.; Klene, M.; Li, X.; Knox, J. E.; Hratchian, H. P.; Cross, J. B.; Bakken, V.; Adamo, C.; Jaramillo, J.; Gomperts, R.; Stratmann, R. E.; Yazyev, O.; Austin, A. J.; Cammi, R.; Pomelli, C.; Ochterski, J. W.; Ayala, P. Y.; Morokuma, K.; Voth, G. A.; Salvador, P.; Dannenberg, J. J.; Zakrzewski, V. G.; Dapprich, S.; Daniels, A. D.; Strain, M. C.; Farkas, O.; Malick, D. K.; Rabuck, A. D.; Raghavachari, K.; Foresman, J. B.; Ortiz, J. V.; Cui, Q.; Baboul, A. G.; Clifford, S.; Cioslowski, J.; Stefanov, B. B.; Liu, G.; Liashenko, A.; Piskorz, P.; Komaromi, I.; Martin, R. L.; Fox, D. J.; Keith, T.; Al-Laham, M. A.; Peng, C. Y.; Nanayakkara, A.; Challacombe, M.; Gill, P. M. W.; Johnson, B.; Chen, W.; Wong, M. W.; Gonzalez, C.; Pople, J. A. Gaussian 03, revision C.02; Gaussian, Inc.: Wallingford, CT, 2004.
36. Petersilka M. · Phys. Rev. Lett. · 1996 · 76 · 121210.1103/PhysRevLett.76.1212 ↗
37. Craig C. F. · Phys. Rev. Lett. · 2005 · 95 · 16300110.1103/PhysRevLett.95.163001 ↗
38. Dreuw A. · Chem. Phys. · 2005 · 104 · 4009
39. Levine B. G. · Mol. Phys. · 2006 · 104 · 103910.1080/00268970500417762 ↗
40. Pijpers J. J. H. · J. Phys. Chem. B · 2007 · 111 · 4146