Role of Symmetry Breaking on the Optical Transitions in Lead-Salt Quantum Dots
Padilha, Lazaro A.
Olszak, Peter D.
Hagan, David J.
Van Stryland, Eric W.
Sargent, Edward H.
KAUST Grant NumberKUS-I1-009-21
Permanent link to this recordhttp://hdl.handle.net/10754/599534
MetadataShow full item record
AbstractThe influence of quantum confinement on the one- and two-photon absorption spectra (1PA and 2PA) of PbS and PbSe semiconductor quantum dots (QDs) is investigated. The results show 2PA peaks at energies where only 1PA transitions are predicted and 1PA peaks where only 2PA transitions are predicted by the often used isotropic k•p four-band envelope function formalism. The first experimentally identified two-photon absorption peak coincides with the energy of the first one photon allowed transition. This first two-photon peak cannot be explained by band anisotropy, verifying that the inversion symmetry of the wave functions is broken and relaxation of the parity selection rules has to be taken into account to explain optical transitions in lead-salt QDs. Thus, while the band anisotropy of the bulk semiconductor plays a role in the absorption spectra, especially for the more anisotropic PbSe QDs, a complete model of the absorption spectra, for both 1PA and 2PA, must also include symmetry breaking of the quantum confined wave functions. These studies clarify the controversy of the origin of spectral features in lead-salt QDs. © 2010 American Chemical Society.
CitationNootz G, Padilha LA, Olszak PD, Webster S, Hagan DJ, et al. (2010) Role of Symmetry Breaking on the Optical Transitions in Lead-Salt Quantum Dots. Nano Lett 10: 3577–3582. Available: http://dx.doi.org/10.1021/nl1018673.
SponsorsThis material is based upon work supported in part by the U.S. Army Research Office under Contract/Grant 50372-CH-MUR, the Air Force Office of Sponsored Research MURI AFOSR Grant FA9550-06-1-0337, the DARPA ZOE program Grant W31R4Q-09-1-0012, and the Israel Ministry of Defense contract 993/54250-01 and by Award No. KUS-I1-009-21, made by King Abdullah University of Science and Technology (KAUST). We also would like to thank Frank W. Wise for helpful discussions.
PublisherAmerican Chemical Society (ACS)
CollectionsPublications Acknowledging KAUST Support
- Optimization of band structure and quantum-size-effect tuning for two-photon absorption enhancement in quantum dots.
- Authors: Padilha LA, Nootz G, Olszak PD, Webster S, Hagan DJ, Van Stryland EW, Levina L, Sukhovatkin V, Brzozowski L, Sargent EH
- Issue date: 2011 Mar 9
- Linear and nonlinear optical characterizations of a monomeric symmetric squaraine-based dye in solution.
- Authors: Toro C, De Boni L, Yao S, Ritchie JP, Masunov AE, Belfield KD, Hernandez FE
- Issue date: 2009 Jun 7
- Highly efficient multiple exciton generation in colloidal PbSe and PbS quantum dots.
- Authors: Ellingson RJ, Beard MC, Johnson JC, Yu P, Micic OI, Nozik AJ, Shabaev A, Efros AL
- Issue date: 2005 May
- Optical investigation of quantum confinement in PbSe nanocrystals at different points in the Brillouin zone.
- Authors: Koole R, Allan G, Delerue C, Meijerink A, Vanmaekelbergh D, Houtepen AJ
- Issue date: 2008 Jan
- Two-photon-induced blue shift of core and shell optical transitions in colloidal CdSe/CdS quasi-type II quantum rods.
- Authors: Allione M, Ballester A, Li H, Comin A, Movilla JL, Climente JI, Manna L, Moreels I
- Issue date: 2013 Mar 26