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Electromagnetics

Three-Level Description of Optical Nonlinearities in Semiconductors

John M. Arnold, David C. Hutchings

Published Nov 1, 1999• 4 citations
Publisher

Abstract

A description of the second–order nonlinear optical susceptibility of semiconductor materials is considered. The Lie algebra su(3) arises from a 3–level quantum model for each state in the Brillouin zone, which is obtained by truncation of the true infinite–dimensional basis. The accuracy of several approximations inherent in this approach is analysed, in particular the electric dipole and minimal replacement Hamiltonians which specify the electrodynainical interaction in a finite–dimensional quantum system. The three–level model is extended by adding relaxation processes and utilising the rotating wave approximation to account for resonant nonlinear effects. Analytical forms for the transition rates associated with two–photon absorption and electromagnetically induced transparency are derived.

DOI
10.1080/02726349908908669

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Journal of the Optical Society of America B•Jul 1, 1985•14 citations
A description of the second–order nonlinear optical susceptibility of semiconductor materials is considered. The Lie algebra su(3) arises from a 3–level quantum model for each state in the Brillouin zone, which is obtained by truncation of the true infinite–dimensional basis. The accuracy of several approximations inherent in this approach is analysed, in particular the electric dipole and minimal replacement Hamiltonians which specify the electrodynainical interaction in a finite–dimensional quantum system. The three–level model is extended by adding relaxation processes and utilising the rotating wave approximation to account for resonant nonlinear effects. Analytical forms for the transition rates associated with two–photon absorption and electromagnetically induced transparency are derived.
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.
Optical-intensity-dependent gain and mixing susceptibilities of amplifying semiconductor materials have been calculated using the density-matrix approach. The model, which takes intraband relaxation and carrier-injection rate into account, allows for numerical computation of these susceptibilities, whatever the medium saturation is. As a simplification, an equivalent two-level system is derived which represents the gain and nearly degenerate four-wave mixing susceptibilities. Such an equivalence, which leads to the same field-induced polarization as the conventional rate equation model, also connects the two-level (or rate equation) parameters to the real characteristics of the semiconductor material.>
This dissertation addresses both fundamental aspects of Coulomb correlations in semiconductor quantum wells and more practical aspects of theoretical analysis of semiconductor optoelectronic devices. After introducing the subject, we present and evaluate a state-of-the-art theory of the third order coherent optical response of a semiconductor quantum well based on the Dynamics Controlled Truncation (DCT) scheme. Already in the third order (the so-called chi (3)) regime, semiconductors exhibit a number of many-body Coulomb correlation effects. Their manifestation in various multi-pulse experimental configurations, customarily used in ultrafast semiconductor spectroscopy, has been an important component of this thesis. Coherent optical effects in a semiconductor 3-band system based on the heavy-hole, light-hole and conduction bands were investigated. The quantum beats in the time-integrated differential transmission signal were analyzed and compared with experimental data obtained at the University of Iowa. Fundamental differences from corresponding quantum beats in atomic 3-level systems were found. Also, the analysis of experimental data (obtained at the University of Arizona) of the coupled heavy-hole-light-hole optical Stark shift revealed evidence of intervalence band coherences, an analog of Raman coherences in atomic 3-levels systems. A scheme for realization of electromagnetically-induced transparency (EIT) based on the interference of excitonic and biexcitonic coherences was proposed. Corresponding experiments performed at the University of Oregon showed indeed a considerable coherent reduction of excitonic absorption. Furthermore, an extension of the chi(3) analysis revealed an energy renormalization of the biexciton, in good agreement with the corresponding experiment. A microscopic analysis of polarization dynamics in time-resolved four-wave mixing signals was performed, revealing interesting implications for the biexciton dephasing in addition to the significance of many-body correlations. In the case of four-wave mixing in semiconductor microcavities, our theoretical analysis in conjunction with experimental data obtained at the University of Tokyo gave us indications for a significant shortcoming of the second Born approximation (2nd BA) applied to two-exciton Coulomb correlations in a thin semiconductor quantum well, in agreement with the general knowledge of the qualitative failure of the 2nd BA in systems with short-range interaction in two dimensions. We also analyzed a novel all-optical switching technique based on the nonlinear polarization rotation. Apart from identifying the many-particle processes relevant for the switch operation in the chi(3) regime, we proposed ways to further optimize the switch.
In the past few years, with developing the technology of electromagnetically induced transparency (EIT) and improving the semiconductor technology, it has become possible to realize the application of optical soliton to communication device. Studies show the reduction of group velocity of the optical soliton in EIT medium under weak driving condition, which possibly realizes the storing of optical pulses in information storage. More importantly, semiconductor quantum wells have the inherent advantages such as large electric dipole moments of the transitions, high nonlinear optical coefficients, small size, easily operating and integrating. So it is considered to be the most potential EIT medium to realize the application of quantum devices. The optical soliton behavior in the semiconductor quantum well is studied, which can provide a certain reference value for the practical application of information transmission and processing together quantum devices. Although there has been a series of researches on both linear and nonlinear optical properties in semiconductor quantum wells structures, few publications report the effects of the cross-coupling longitude-optical phonon (CCLOP) relaxation on its linear and nonlinear optical properties. However, to our knowledge, the electron-longitude-optical phonon scattering rate can be realized experimentally by varying the sub-picosecond range to the order of a picosecond. According to this, we in the paper study the effects of the CCLOP relaxation on its linear and nonlinear optical properties in a cascade-type three-level EIT semiconductor quantum well. According to the current experimental conditions, we first propose a cascade-type three-level EIT semiconductor quantum well model. And in this model we consider the longitudinal optical phonons coupling between the bond state and anti-bond state. Subsequently, by using the multiple-scale method, we analytically study the dynamical properties of solitons in the cascade-type three-level EIT semiconductor quantum well with the CCRLOP. It is shown that when the CCRLOP strength is smaller, there exhibits the dark soliton in the EIT semiconductor quantum well. Only if the strength of the CCRLOP is larger, will in the system there exists bright soliton. That is to say, with increasing the strength of the CCRLOP, the soliton type of the system is converted from dark to bright soliton little by little. So, the temporal soliton type can be effectively controlled by the strength of the CCRLOP. In addition, we also find that the group velocity of the soliton can also be controlled by the strength of CCRLOP and the control light. These results may provide a theoretical basis for manipulating experimentally the dynamics of soliton in semiconductor quantum wells.
The strong optical nonlinearity of biexcitons in semiconductors necessitates a nonperturbative calculation of the nonlinear-optical susceptibility of the semiconductor and of the propagation equation of the light wave. Such calculations are possible for all light-beam geometries within a simple model in which excitons and biexcitons are treated quantum mechanically as bosons, with no reference to their internal structure. This simple model can account for most experimental observations, while when dephasing and population effects are considered it predicts the appearance of a dephasing-induced extra resonance analogous to that observed in gases or molecular crystals.