246 PublicacionesMOVILLA, PLANELLES, AND JASKÓLSKIPHYSICAL REVIEW B 73, 035305 2006also be stressed that the angular localization is certainly acorrelation effect it becomes important only in case B ofhigh correlation, but the radial localization is mainly a monoelectroniceffect coming from the strong localization in theself-polarization well of the energetically low-lying singleparticleeigenfunctions radial localization is important inboth cases A and B, regardless of low/high correlation.In summary, we have investigated the role of imagecharges on the correlation effects in a system of two electronsin a spherical quantum dot embedded in high out=80 and low out =1 permittivity media. Our findingsshow that a transition from almost independent particles toWigner-type localization of the conduction band electronsmay be attained by tuning an appropriate dielectric responseof the surrounding medium.FIG. 3. Angular correlation density Z corresponding to thesame cases as in Fig. 2.ACKNOWLEDGM<strong>EN</strong>TSFinancial support from MEC-DGI Contract No.CTQ2004-02315/BQU, UJI-Bancaixa Contract No. P1-B2002-01 Spain, and KBN-3T1104326 and PZB-MIN-008/P03/2003 Poland is gratefully acknowledged. A SpanishMECD FPU grant is also acknowledged by one of the authorsJ.L.M..*Electronic address: josep.planelles@exp.uji.es1 L. Bányai and S. W. Koch, Semiconductor Quantum Dots WorldScientific, Singapore, 1993.2 L. E. Brus, J. Chem. Phys. 80, 4403 1984.3 L. Bányai, P. Gilliot, Y. Z. Hu, and S. W. Koch, Phys. Rev. B 45,14136 1992.4 F. Stern, Phys. Rev. B 17, 5009 1978.5 P. G. Bolcatto and C. R. Proetto, J. Phys.: Condens. Matter 13,319 2001.6 J. L. Movilla and J. Planelles, Phys. Rev. B 71, 075319 2005.7 J. L. Movilla and J. Planelles, Comput. Phys. Commun. 170, 1442005.8 J. L. Movilla, G. Garcia-Belmonte, J. Bisquert, and J. Planelles,Phys. Rev. B 72, 153313 2005.9 A. Orlandi, G. Goldoni, F. Mangui, and E. Molinari, Semicond.Sci. Technol. 17, 1302 2002.10 A. Orlandi, M. Rontani, G. Goldoni, F. Manghi, and E. Molinari,Phys. Rev. B 63, 045310 2001.11 A. Franceschetti, A. Williamson, and A. Zunger, J. Phys. Chem.B 104, 3398 2000.12 S. M. Reimann, M. Koskinen, and M. Manninen, Phys. Rev. B62, 8108 2000; R. Egger, W. Häusler, C. H. Mak, and H.Grabert, Phys. Rev. Lett. 82, 3320 1999.13 L. G. G. V. Dias da Silva and M. A. M. de Aguiar, Phys. Rev. B66, 165309 2002.14 S. Bednarek, T. Chwiej, J. Adamowski, and B. Szafran, Phys.Rev. B 67, 205316 2003.15 A. Matulis and F. M. Peeters, Solid State Commun. 117, 6552001.16 D. C. Thompson and A. Alavi, Phys. Rev. B 66, 235118 2002.17 A. V. Filinov, M. Bonitz, and Y. E. Lozovik, Phys. Rev. Lett. 86,3851 2001.18 B. Szafran, S. Bednarek, and J. Adamowski, Phys. Rev. B 67,045311 2003.19 V. A. Fonoberov, E. P. Pokatilov, and A. A. Balandin, Phys. Rev.B 66, 085310 2002; L. Bányai, I. Galbraith, C. Ell, and H.Haug, ibid. 36, 6099 1987.20 <strong>It</strong> should be pointed out that dielectric and spatial confinementsare highly nonadditive Ref. 6. In particular, a large V 0 wouldprevent the self-polarization potential to confine the electronicdensity at the QD border in case B.21 We do not use the quantum-chemical definition of the correlationenergy and the correlation effects. In this paper correlation isunderstood as the contribution of excited configurations to theexact wave function in comparison to the ground configuration1s 2 .22 Despite this strong confinement, the system is, formally, in theweak confinement regime because the QD radius is larger thanthe effective Bohr radius a * B . An increasing of a * B , and thereforea formal transition to the strong confinement regime, while dotremained constant, can be achieved by means of a severe decreasingof the effective mass. This would yield a severe increasingof the kinetic energy so that the image charges wouldeventually be unable to recover the Wigner molecule limit.23 The enhancement of Coulomb interactions in systems embeddedin low permittivity media is a well-known phenomenon Refs. 1,2, and 19. However, in our case, the enhancement is extremelyhigh due to the fact that the electron density is strongly confinedin a thin shell, just beyond the QD border, where the dielectricconstant is unity.035305-4
Confinamiento dieléctrico 247PHYSICAL REVIEW B 76, 115312 2007Theory of dielectrically induced surface excitonic states in spherical quantum dotsF. Rajadell, J. L. Movilla, M. Royo, and J. Planelles*Departament de Química Física i Analítica, UJI, Box 224, E-12080 Castelló, SpainReceived 2 March 2007; published 12 September 2007The formation of quantum dot QD excitonic surface states induced by dielectric mismatch is theoreticallyexplored in spherical nanocrystals embedded in very high and in very low permittivity media. <strong>It</strong> is found thatthe transition from volume to surface exciton states V→S always parallels a sudden drop of exciton brightnessif the QD is embedded in low dielectric constant media. This is not the case of a QD buried in highpermittivity media. In this case, the V→S transition is monitored by a reduction in exciton brightness or notdepending on the m h * /m e * ratio between the effective masses of electron and hole. The presence of a hydrogenicdonor impurity at the QD center can drastically reduce the electron-hole density overlap and thus the excitonicbinding energy and the drop of brightness that parallels the formation of surface states.DOI: 10.1103/PhysRevB.76.115312PACS numbers: 71.35.Cc, 73.21.La, 73.22.f, 73.20.AtI. INTRODUCTIONMost of the active key components of modern informationtechnologies rely on semiconductor devices with electronicor optoelectronic functions. <strong>It</strong> is believed that quantum bits,which are generic quantum mechanical two-level systems,will become the basic building blocks of this technology inthe next future. One possible realization of these two-levelsystems is an exciton ground state in a quantum dot QD. 1The formation of QD excitons or electron-hole e-h pairs ande-h recombination leading to photoluminescence has receiveda great deal of attention in the literature. 2 A veryinteresting feature of semiconductor QDs spectra is the shiftof excitonic peaks as compared to bulk values. This originatesfrom two usually opposite contributions. On the onehand, the single-particle band gap is shifted to higher energiesdue to the quantum size effect. On the other hand, theCoulomb attraction between the e-h pair created by photoexcitationadds a redshift correction. Both corrections are sizedependent and generally result in an overall blueshift of theoptical band gap as compared to the bulk. 3 Since the pioneeringwork by Brus, 4,5 the influence of QD surface dielectricpolarization on energy and density distribution of carriers hasbeen taken into account for a proper comparison betweentheory and experiments. This surface polarization is especiallystrong for QDs in a glass matrix, liquid solution, air, ora vacuum, where the background dielectric constant of theQD and the surrounding medium are substantially different.Two contributions to the energy originate from the dielectricmismatch, namely, single-particle contributions coming fromthe interaction of carriers with their own induced chargesself-polarization energy and two-particle contributionscoming from the interaction of a carrier with the charge inducedby the other one polarization of the Coulomb interaction.By assuming infinitely or very high confinementbarriers and steplike dielectric functions, the dielectric mismatchcorrections on excitonic energies in spherical QDs almosttotally cancel each other out. 4,6–9 However, dielectricmismatch corrections on excitonic energies no longer cancelout if finite confining barrier heights are considered. 10 Underspecific conditions, the attractive self-polarization potentialwell originated from the dielectric mismatch is even able toconfine carriers in surface states. 11–15 Dielectrically inducedexciton surface states in semiconductor QDs were predictedfor the first time by Bányai et al. 11,17 using a model whereelectron and hole are confined in a QD by a common lowpotential height barrier and have a large effective e-h massratio m h * /m e * =10, the QD being subject to a strong dielectricmismatch QD / out =10.In this Brief Report, we explore the possible formation ofexcitonic surface states in two different situations, i aspherical QD in air, where the hole confining barrier height ismuch higher than the electron one, and ii a QD buried in amatrix with a higher dielectric constant in this case, as isusual, we will assume that the confinement barrier height forholes is about 1/2 that corresponding to electrons. We willshow that in both cases, a dielectric mismatch-induced transitionfrom a volume to a surface state involving an opticalband gap redshift with respect to the case of no dielectricmismatch can be reached under specific conditions. Relevantdifferences between the two cases are found. Thus, incase i, only the electron can be confined in the selfpolarizationpotential well, beyond the QD border. However,the hole, despite its heavier mass, as it is subject to a higherconfining barrier, cannot overcome the spatial confinementand remains within the QD but close to the border due to thee-h attraction. The transition from volume to surface statescan be monitored in this case by a sudden change in theoverlap between electron and hole wave functions, i.e., by adecrease in the exciton brightness. A quite different situationholds in case ii because the self-polarization potential wellis now located on the inner side of the QD border so that nospatial confining barrier prevents localization of particles init. In this case, we find that the transition from volume tosurface states can be monitored by a reduction in the excitonicbrightness or not, depending on the m h * /m e * ratio. Inaddition, the influence of an on-center shallow donor impurityon the binding energy and oscillator strength of the fundamentalexciton is also addressed. <strong>It</strong> results in an almosttotal suppression of binding and brightness.II. THEORY AND COMPUTATIONAL DETAILSWe deal with the fundamental exciton of spherical QDs. <strong>It</strong>has been reported 2,16 that this exciton basically involves the1098-0121/2007/7611/1153125115312-1©2007 The American Physical Society
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BIBLIOGRAFÍA 297[48] M.G. Burt,
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BIBLIOGRAFÍA 299[71] W.H. Press, S
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BIBLIOGRAFÍA 301[97] U.H. Lee, D.
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BIBLIOGRAFÍA 303[121] S.W. Chung,
- Page 327 and 328:
BIBLIOGRAFÍA 305[145] R. Blossey y
- Page 329 and 330:
BIBLIOGRAFÍA 307[169] F. Suárez,
- Page 331 and 332:
BIBLIOGRAFÍA 309[194] C. Delerue,
- Page 333 and 334:
BIBLIOGRAFÍA 311[220] J.L. Zhu y X
- Page 335 and 336:
BIBLIOGRAFÍA 313[245] L.M. Peter,
- Page 337 and 338:
BIBLIOGRAFÍA 315[266] P. Rinke, K.
- Page 339 and 340:
BIBLIOGRAFÍA 317[289] Y. Wang, L.
- Page 341 and 342:
BIBLIOGRAFÍA 319[314] A. Wójs y P