Two-photon transitions in systems with semiconductor quantum dots

Fëdorov, A. V.; Баранов, А. В.; Inoue, Kuon

doi:10.1103/physrevb.54.8627

Cited by 75 publications

(95 citation statements)

References 10 publications

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“…4,10 This approach allows one to find the QD electronic structure (e.g., transition energies) and its dependence on the dimensions for the QDs by solving the Schrödinger equation for each carrier, i.e. separately for electrons and holes, assuming spherical symmetry of the QD.…”

Section: Effective-mass and Sum-over-states Calculationsmentioning

confidence: 99%

“…Fewer opportunities for modification and NLO enhancement have been explored for QDs, as only limited experimental data are available on their NLO properties. [4][5][6][7][8][9] Various theoretical approaches [7][8][9][10][11] have been used to interpret these experimental data. These models, however, almost completely ignore the broad quantum chemistry approaches developed for organic molecules.…”

mentioning

confidence: 99%

“…2,3 Accordingly, the linear optical properties of colloidal QDs have been exhaustively studied both experimentally and theoretically. [4][5][6][7][8][9][10][11] The majority of QD theoretical studies are based on condensed matter approaches. For example, the parabolic band approximation for CdS (or CdSe) QDs 10 considers single conduction and three valence bands and ignores coupling between them.…”

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confidence: 99%

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Two-Photon Absorption in CdSe Colloidal Quantum Dots Compared to Organic Molecules

et al. 2014

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We discuss fundamental differences in electronic structure as reflected in one- and two-photon absorption spectra of semiconductor quantum dots and organic molecules by performing systematic experimental and theoretical studies of the size-dependent spectra of colloidal quantum dots. Quantum-chemical and effective-mass calculations are used to model the one- and two-photon absorption spectra and compare them with the experimental results. Currently, quantum-chemical calculations are limited to only small-sized quantum dots (nanoclusters) but allow one to study various environmental effects on the optical spectra such as solvation and various surface functionalizations. The effective-mass calculations, on the other hand, are applicable to the larger-sized quantum dots and can, in general, explain the observed trends but are insensitive to solvent and ligand effects. Careful comparison of the experimental and theoretical results allows for quantifying the range of applicability of theoretical methods used in this work. Our study shows that the small clusters can be in principle described in a manner similar to that used for organic molecules. In addition, there are several important factors (quality of passivation, nature of the ligands, and intraband/interband transitions) affecting optical properties of the nanoclusters. The larger-size quantum dots, on the other hand, behave similarly to bulk semiconductors, and can be well described in terms of the effective-mass models.

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Section: Effective-mass and Sum-over-states Calculationsmentioning

confidence: 99%

mentioning

confidence: 99%

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confidence: 99%

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Two-Photon Absorption in CdSe Colloidal Quantum Dots Compared to Organic Molecules

et al. 2014

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“…[5][6][7]). Hyper-Raman scattering is a nonlinear process with the absorption of two photons and the emission of one scattered photon with the simultaneous excitation of a vibrational mode.…”

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confidence: 97%

“…Present developments of sophisticated growth techniques made possible to obtain size selected II-VI semiconductor quantum dots (QDs) of nanoscale dimensions with good size distributions [3,4]. On the other hand, resonant Raman technique allows to study the optical vibrations modes and the characteristic of the electron-phonon interaction at an almost individual level [5][6][7]. The present contribution on the field is organized as follows: In Sec.…”

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Optical phonons and resonant Raman scattering in II–VI spheroidal quantum dots

Trallero‐Giner

2004

Physica Status Solidi (b)

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PACS 63. 22.+m, 78.30.Fs First order and multiphonon resonant Raman scattering processes from confined and interface polar optical phonons in II-VI nanocrystallites are analyzed. Fraehlich interaction between excitons and optical phonons has been considered and general selection rules for the exciton-phonon matrix elements of the scattering processes in the case of spheroidal quantum dots are given. A comparison is made between the Raman selection rules and non-linear hyper-Raman selection rules for spherical dots. It is shown that the relative intensities between phonon overtones in II-VI spherical quantum dots can be correctly described in the framework of excitonic model and the optical polar vibrational continuum model satisfying both the mechanical and electrostatic matching conditions at the interface. Detailed discussions of the surface optical phonons are provided in the case of a spherical Quantum-Dot/Quantum-Well (QD/QW) heterostructure. Their frequency dependence on the geometry, material parameters, as well as the electron-phonon interaction Hamiltonian are also reported. In addition, the interface optical phonons and the corresponding electron-phonon interaction in nanostructures with prolate and oblate spheroidal geometries and their contribution to the first order scattering process have been studied. This surface-optical phonon modes are strongly dependent on the nanocrystal geometry and new Raman selection rules are obtained given a plausible explanation for the observed low frequency shoulders present in the spectrum of several II-VI semiconductor nanostructures. [1] and reference therein). How do the optical phonon vibrations and their symmetry properties look like as the dimensions of the system change? Which is the behavior of the electron-optical phonon Hamiltonian as a function of the geometry and nanocristal size? These and other questions have attracted much attention in the last years due to their fundamental issues and the potential applications of the new generation of semiconductors. Several theoretical approaches have been considered to describe the confined and surface modes of colloidal nanostructures (see Refs. [1, 2] and reference therein). Weakly polar semiconductor compounds, in the form of slabs and spheres, were considered in pioneering works on the subject. Present developments of sophisticated growth techniques made possible to obtain size selected II-VI semiconductor quantum dots (QDs) of nanoscale dimensions with good size distributions [3,4]. On the other hand, resonant Raman technique allows to study the optical vibrations modes and the characteristic of the electron-phonon interaction at an almost individual level [5][6][7]. The present contribution on the field is organized as follows: In Sec. 2, a review of the optical longitudinal phonons and Raman selection rules in spherical quantum dots for the first and higher order is presented. Also, the non-linear hyper-Raman effect is discussed. The evolution of the surface optical

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Hyper‐Raman Spectroscopy

Ziegler

2001

Handbook of Vibrational Spectroscopy

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The essential phenomenological characteristics of the nonlinear spontaneous light scattering effect known as hyper‐Raman scattering (HRS) is described in this review. The salient features of the theoretical description of HRS are given within a susceptibility treatment of the induced electrical polarization. Symmetry selection rules and the relation of HRS to Raman scattering are highlighted in this theory section. Experimental considerations for the observation of this higher order Raman effect are considered. Recent applications of this technique to problems of chemical and physical interest are selected to illustrate the utility of this phenomenon. These include HRS studies of crystals, glasses, semiconductors, and liquids. The phenomenon of surface‐enhanced HRS and electronically resonance‐enhanced HRS are also described and illustrated.

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Two-photon transitions in systems with semiconductor quantum dots

Cited by 75 publications

References 10 publications

Two-Photon Absorption in CdSe Colloidal Quantum Dots Compared to Organic Molecules

Two-Photon Absorption in CdSe Colloidal Quantum Dots Compared to Organic Molecules

Optical phonons and resonant Raman scattering in II–VI spheroidal quantum dots

Hyper‐Raman Spectroscopy

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