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Journal of Nanomedicine & Nanotechnology

On the correct form of the nonlinear optical susceptibility in strongly-driven semiconductor quantum dots

John Boviatsis, Emmanuel Paspalakis

Published Aug 27, 2015• 0 citations
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Abstract

I recent years, significant attention has been given to nonlinear optical phenomena, such as nonlinear optical absorption and dispersion, derived from a driven quantum transition of semiconductor nanostructures, such as semiconductor quantum wells, quantum disks and mainly quantum dots. An important issue that is widely studied is the effect of probe electromagnetic field intensity on the total (nonlinear) absorption coefficient and on the total (nonlinear) index of refraction. Some of the phenomena that are commonly found for large electromagnetic field intensities are the creation of a strong dip in the absorption spectrum near or at resonance (the so-called bleaching effect), negative absorption near or at resonance that leads to optical gain and the change of the slope of the total index of refraction near or at resonance from negative to positive that changes the behavior of the system from fast to slow light. Unfortunately, these phenomena do not exist and are artifacts of a common abuse of the theoretical methodology for the study of the total absorption coefficient and the total index of refraction. The main error is that the total absorption coefficient and the total index of refraction was initially derived from density matrix equations using perturbation theory and includes first-order (linear) as well as third-order (nonlinear) terms. This method gives correct results for small electromagnetic field intensities and it leads to saturation of absorption and dispersion in this regime. However, for larger intensities it gives the misleading results mentioned above due to either failure of the order of perturbation theory considered in the derivation of the total absorption coefficient and the total index of refraction or even failure of perturbation theory at all in the treatment of the problem. In this work, we revisit the problem of the total absorption coefficient and the total index of refraction in a symmetric semiconductor quantum dot structure (we choose the example of a core-shell quantum dot) under a strong probe field excitation. We use the two-level model, solve the relevant density matrix equations under the rotating wave approximation and under steady state conditions, and obtain the correct form of the nonlinear optical susceptibility that is then used for the derivation of the formulae of the total absorption coefficient and the total index of refraction under the interaction with a strong probe field. Actually, the commonly used perturbation theory formulae can be obtained by our formulae using a series expansion and keeping terms up to second order in electric field amplitude. We also derive the electronic structure of the quantum dot system by solving numerically the time-independent Schrodinger equation, under the effective mass approximation, using the potential morphing method and obtain the energy difference and the electric dipole matrix element for the relevant transitions of the quantum dot system. Then, for the specific quantum dot system we compare the results of the total absorption coefficient and the total index of refraction for the two methodologies (the perturbation result and our result) for different electromagnetic field intensities.

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Chinese Journal of Luminescence•Jan 1, 2006•0 citations
I recent years, significant attention has been given to nonlinear optical phenomena, such as nonlinear optical absorption and dispersion, derived from a driven quantum transition of semiconductor nanostructures, such as semiconductor quantum wells, quantum disks and mainly quantum dots. An important issue that is widely studied is the effect of probe electromagnetic field intensity on the total (nonlinear) absorption coefficient and on the total (nonlinear) index of refraction. Some of the phenomena that are commonly found for large electromagnetic field intensities are the creation of a strong dip in the absorption spectrum near or at resonance (the so-called bleaching effect), negative absorption near or at resonance that leads to optical gain and the change of the slope of the total index of refraction near or at resonance from negative to positive that changes the behavior of the system from fast to slow light. Unfortunately, these phenomena do not exist and are artifacts of a common abuse of the theoretical methodology for the study of the total absorption coefficient and the total index of refraction. The main error is that the total absorption coefficient and the total index of refraction was initially derived from density matrix equations using perturbation theory and includes first-order (linear) as well as third-order (nonlinear) terms. This method gives correct results for small electromagnetic field intensities and it leads to saturation of absorption and dispersion in this regime. However, for larger intensities it gives the misleading results mentioned above due to either failure of the order of perturbation theory considered in the derivation of the total absorption coefficient and the total index of refraction or even failure of perturbation theory at all in the treatment of the problem. In this work, we revisit the problem of the total absorption coefficient and the total index of refraction in a symmetric semiconductor quantum dot structure (we choose the example of a core-shell quantum dot) under a strong probe field excitation. We use the two-level model, solve the relevant density matrix equations under the rotating wave approximation and under steady state conditions, and obtain the correct form of the nonlinear optical susceptibility that is then used for the derivation of the formulae of the total absorption coefficient and the total index of refraction under the interaction with a strong probe field. Actually, the commonly used perturbation theory formulae can be obtained by our formulae using a series expansion and keeping terms up to second order in electric field amplitude. We also derive the electronic structure of the quantum dot system by solving numerically the time-independent Schrodinger equation, under the effective mass approximation, using the potential morphing method and obtain the energy difference and the electric dipole matrix element for the relevant transitions of the quantum dot system. Then, for the specific quantum dot system we compare the results of the total absorption coefficient and the total index of refraction for the two methodologies (the perturbation result and our result) for different electromagnetic field intensities.
In recent years,the subject of optical nonlinearity in semiconductor quantum confined structures such as quantum wires and quantum dots has attracted a considerable attention because of their relevance for studying practical applications and as a probe for the electronic structure of media.It has been shown that the low dimensional quantum systems present very large nonlinear optical susceptibilities .Theoretically,most of the studies on quantum dots are focused on spherical quantum dots for simplicity.The shape of quantum dot depends on growth conditions.In fact,quantum dots are better described as thin disk or cylinder.In the present work third order nonlinear optical susceptibilities in disk shaped quantum dots due to resonant intersubband transition are analyzed by a compact density matrix approach.It has rarely been discussed in literatures.Firstly,we consider an electron moving in a quantum disk whose radius R is very large compared to its thickness d .For simplicity,we assume that the isotropic effective mass approximation is valid within the disk and that the inner potential is null while the outer confining potential is approximately infinite.Using the adiabatic approximation we solve the three dimensional Schrdinger equation and obtain the analytical expressions of wave functions and energy levels in cylindrical coordinates.Secondly,we consider the system is excited by an electromagnetic field with frequency ω. The electromagnetic field is incident with a polarization vector normal to the disk.We treat H′=ezE(t) as a perturbation term.By using the compact density matrix method,we derive a general formula for third order nonlinear optical susceptibilites employing a four level model in quantum disk.Finally,numerical results are illustrated for a typical GaAs quantum disk.We calculate the third order nonlinear optical susceptibilities as a function of the disk thickness.It is shown that the third order nonlinear optical susceptibilities in quantum disk are 10～100 times larger than that in quantum well for various disk thickness.Furthermore,if we choose an optimized thickness of quantum disk,we could obtain a quite large refractive index with a comparatively small absorption coefficient.Therefore,we suggest that the quantum dots would be an excellent system in the field of optical communications and optical switching.
We study nonlinear optical absorption and nonlinear optical rectification in an asymmetric semiconductor quantum dot structure under a strong probe field excitation. We apply a form of the rotating wave approximation for asymmetric quantum systems, solve the relevant density matrix equations under steady state conditions, and derive the formulae for nonlinear optical absorption and nonlinear optical rectification under the interaction with a strong probe field. The differences between our formulae and those of a previous study are also presented for the case of an electron confined in an asymmetric double quantum dot nanostructure.
Analytical expressions for the linear and nonlinear optical susceptibilities of spherical quantum dots are obtained using the Schrödinger equation. To solve the Schrödinger equation, the Nikiforov-Uvarov method was used, assuming that electrons isolated in the medium are associated with the Gelman inverse quadratic potential. Using the density matrix formalism, analytical expressions were obtained for the coefficients of linear and nonlinear absorption and changes in the refractive index of quantum dots. Elements of the matrix of the electric dipole moment l=± 1 and m = 0 are obtained according to the selection rules. To demonstrate the results obtained, we used the real physical characteristics of quantum dots obtained from gallium arsenide (GaAs).
Transient optical nonlinearities of semiconductor quantum dots in the strongly confined regime are studied, in which the exciton, biexciton and magnetic field effects are taken into account. The photo induced band-to-band electronic transitions are considered from both the heavy-hole (hh) and light-hole (lh) valence bands to the lowest (1s) exciton state below the fundamental absorption edge. The time dependent perturbation technique for a three-level system, under the near band gap resonant excitation regime, has been employed; with the incorporation of the relaxation and dephasing mechanisms phenomenologically. The induced polarization is calculated from where the real and imaginary parts of the third-order nonlinear optical susceptibility, responsible for the occurrence of nonlinear refraction and nonlinear absorption respectively, have been derived. The temporal and detuning spectra of nonlinear refraction and absorption; and their dependence on density of biexcitons and a moderately strong magnetic field, have been analyzed. It is observed that the nonlinear refraction and nonlinear absorption enhance with increasing magnetic field in small CdS quantum dots.
Abstract The optical properties of the CdSe/ZnS spherical core/shell quantum dot (CSQD), related to the laser-driven transitions 1 s → 1 p − 1 and 1 s → 2 p − 1 , are the subject of this study. We investigate in detail how transition energies, oscillator strengths, imaginary and real parts of the total, linear and third-order susceptibilities change with the variation of the model parameters, such as CSQD radius, core radius, relaxation rates and laser intensity. The energy levels and wave functions, needed for the calculations of the model parameters, were obtained by solving the radial Schrödinger equation in the effective mass approximation with the corresponding boundary conditions. The interaction of CSQD with laser light was studied in a density matrix approach using a two-level model and, for the first time, a five-level model. Optical Bloch equations were derived under dipole and rotating wave approximations and solved in the steady-state regime to obtain an analytic expression for susceptibility. Special attention was paid to the cases in which nonlinear susceptibility prevailed over linear susceptibility, leading to the appearance of the window in the absorption peak. It was found that susceptibility is more sensitive to the change in the core radius than to the change in the CSQD radius and that a greater laser intensity is needed to change the nature of the absorption and dispersion curves for 1 s → 2 p − 1 then for 1 s → 1 p − 1 transition.
In the past few years advance in nanofabrication techniques have made it possible to make well-like compound semiconductor structures of low nanometer size.In these structures,the state of the electron in the direction perpendicular to the length of the well is quantized with sufficiently large separation in energy levels and the motion of the electron parallel to the length is that of a quasi-free electron.One of the most remarkable properties of these one-dimensional electron system is that the optical transitions between the size-quantized subbands are feasible.The result shows there is a large optical nonlinearities in asymmetric quantum wells.The problem of optical saturation of intersubband absorption has recently attracted considerable attention.The problem is very important to the development of superlattice devices such as fast infrared detectors and(modulators) because one needs to know the range of input optical intensities for which linear operation is(possible.) The analytical expression of the linear and the third-order nonlinear optical intersubband absorption coefficients are obtained in Pschl-Teller wells using the density matrix formalism taking into account the(intrasubband) relaxation.Since there are two adjustable parameters κ and λ in Pschl-Teller wells,the shapes of the wells will change with the change of the parameters κ and λ,accordingly the linear and the third-order nonlinear optical absorption coefficients will change with the parameters κ and λ.It is shown that the optical absorption coefficient depends on the parameter,and the optical intensity strongly. The absorption saturation will occur with I increase.Numerical results are presented for a typical AlGaAs/GaAs Pschl-Teller well.