Superlattices and Microstructures, Vol. 15, No. 3, 1994 339 PHOTO- AND ELECTROREFLECTANCE SPECTRA FROM SPATI- ALLY INHOMOGENEOUS HETEROSTRUCTURES CALCULATED BY MEANS OF A NEW METHOD D.Beliaev, R. Enderlein, J.A.N.T Soares, L-M.R. Scolfaro, A. Marti Ceschin, A.A. Quivy, and JR, Leite Instituto de Fisica da Universidade de Séo Paulo, Caiza Postal 20516, 01452-990 Séo Paulo,SP, Brazil (Received 22 Angust 1994) ‘The problem of calculating photo- and electro-reflectance spectra from weakly in homogeneous layers of semiconductor heterostructures is solved by combining two former approaches; the transfer matrix method and the perturbation theoretical treatment of the weak inhomogeneity. The electric field profile and its perturbation by pump light is calculated from an integral equation. ‘The method is applied to several heterostructures based on (Ca,Al)As. Due to its speed and accuracy the method is capable of onfine simulation of PR and ER spectra. Introduction Electro- (BR) and Photoreflectance (PR) spectrosco py are powerful tools for the investigation of the elec tronic states of heterostructures including plana semi conductor devices. Such systems consist of various lay. crs of either macroscopic or, in the case of quantum wells ‘and superlattices, mesoscopic widths, and of homoge- neous material compositions. Within a certain macro- scopie layer, weak spatial inhomogeneities of optical con- stants may occur due to non-zero space charge dist ‘butions and inhomogeneous electrical potential profiles In any case, such intra-layer inhomogeneities will arise from the modulating ER or PR perturbations. The weak intre-layer inhomogeneities are superimposed by the generally much stronger variations of optical con- stants between different layers ‘The problem of calculating optical reflectance spectra from such inhornogencous heterostructures has been ad- dressed in [1-3]. The heterostructure was divided in a number of thin layers, which were each narrow enough to be treated as spatially homogeneous. The transfer matrix method [4] was ssed in order to caleulate the reflectance of the whole multilayer structure, This ap- proach works well for sufficiently weak frequency dis persions and spatial inhomogeneities of the optical con stants, but runs into difficulties if these conditions are ‘not met [1.2]. Besides the numerieat problems this me- (0749-6036/94/030339-+05 $08.00/0 thod has the conceptional drawback of treating the weak intra-layer and strong inter-layer inhomogeneities on the same footing. In the present paper we will demonstrate that itis possible to treat. each kind of inhomogeneity by its own appropriate method, the intre-layer inhomo: geneity by means of a generalization of the perturba- tional method developed in [5] for the ease of an infinite half space, and the interlayer inhomogeneity by means of the transfer matrix method. We will prove that a certain weakly inhomogeneous layer, in first order with respect to the small inhomogeneous part of the complex dielectric function, may be characterized by a transfer matrix which incorporates the inhomogeneity in an in- tegral way. For calculating the reflectance of the het- cerostructure, thus only one matrix is necessary per layer. ‘This means a drastic reduction of the number of matr- ces as compared to [1-3], and allows the calculation of precise reflectance spectra for any frequency dispersions and spatial inhomogeneities, provided the electric field distribution in the heterostructure is known without and with pump light. 2. Method 2.1, Reflection coefficient For the calculation of the reflection coefficient, the semiconductor heterostructure may be treated as a lay- © 1994 Academic Press Limited340 ered plate embedded between two infinite half spaces, the lower one filled with the substrate material, and the upper one with vacuum. Let the normal to the layer, directed to the vacuum side, be the z-axis ofa cartesian coordinate system, and number the layers consecutively by an integer n, starting with n = I for the uppermsot layer and running to WV for the lowermost. ‘The n-th layer extends between z = 25-1 and z = Z». The lower boundary ofthe vacuum half space is taken to be 29 = 0. Each layer consists of a certain homogeneous semicon- ductor material characterized by its dielectric fanction (DF). By e) ve denote that of the material of layer m in absence of any perturbation. The spatially inhomo geneous electri feld of the heterostructure will change &*) by a small z-dependent contribution Ae™(2). Due lo it the total DF of the n-th layer becomes a smooth function (2) =) AH), «) of 2. The spatially varying DF ¢(z) of the whole hete- rostructure equals ¢(")(z) for 2n-1 > > zn. It exhibits abrupt spatial changes if 2 passes an interface, and weak changes if 2 varies within a certain layer. The DF's of the two half spaces are 1 for the upper and <"™) for the lower. ‘The heterostructure is exposed to linearly polarized mo- nochromatic light, incoming from the vacuum side at normal incidence. It, will be reflected at the plane 2 = 0. Let B(2) be the electric field component in polarization direction, and ky = w/c the wave number in vacuum. In the heterostructure, £(} has to be calculated from the vwave equation and the electromagnetic boundary con- ditions. The solution (2) and is frst derivative £'(2) say be gencrated from the intial values (0), £"(0) by raeans of te teansfec matrix M = My Myre. May O) where M, are the transfer matrices of the various layers (4]. The latter matrices are defined as = ( Ex(en) B-(e) m= (25 e): ® with By (2), B-(2) as the two indepenent solution ofthe wave equation for the canonical boundary conditions [4]. In linear approximation with respect to Ae(z) they read_ Byte) = 3 [er eer], a pela ge fen], with pale) = Fhle~ te) he wie trot) EE), 6) Superlattices and Microstructures, Vol. 15, No. 3, 1994 and k, = VéTky. By means of M, and using the vee- tors €9 = (1,~iko),en = (—iel™ko,1), the reflection coefficient R may be written in the compact form ‘ent M | eo) IF = Teen ea) o 2.2. Field profile For the caleulation of the electric field profile all layers| are assumed to be homogeneously doped. ‘The electric field aud the potential (2) are supposed to vanish at oo, At : = 0 the potential takes the surface value . The total charge density p{z) is calculated from the expression Ate) = ING) m(2)-Nel2) +012], () where mp, Nj, Ny are, respectively, the electron, bole, ionized donor, and ionized acceptor concentrations. Com plete ionization of the dopant atoms is not assumed. ‘The standard formula for n,p,Nj..Nq are used in or- der to express these quantities in terms of the potential (plz) - The latter obeys Poisson's equation which here is transformed to an integral equation ween far [Par ae ‘The boundary conditions (0) = Vy and yoo) = 0 are automatically guaranteed by this relation. Since p ‘enters the right hand side, equation (9) has to be solved self-consistently. 3. Results By means of the methods developed above we ealeu Jate PR spectra from three different structures being y first, an infinite half space filled with GaAs, second, a AlasGarsAs/GaAs heterostructure with an alloy layer thickness of 3.5um, and third the same heterastruc- ture as before but with an alloy layer thickness of lam only. For the infinite half space we assume a surface depletion layer of varying width, This corresponds to electri feld profiles decaying linearly into the sample with different gradients. For the 3.5ym heterostructure the fied profile is ealeulated from eq.(9) by assuming both the alloy, buffer and substrate layers to be of r type, with a concentration Np = 10"an-* in the alloy and Np 10Mem~* in the buffer and substrate layers. These values are chosen in order to compare with experimental and theoretical PR spectea from (61) ‘The dopant concentration of the Ij heterostructure is taken in accordance with the parameters of « sampleSuperlattices and Microstructures, Vol. 15, No. 3. 1994 grown in our laboratory, The n-doped alloy layer of concentration Np = 3.6» 10"em™* js followed by a p- doped buffer layer of 300A width. ‘The field profile is varied until the calculated PR spectrum coincides with, the measured, In all three cases the calculations are done under the assumption that the PR signals result entirely from the light induced modulation of the elec tric field inside the sample. The unperturbed complex dielectric functions of GaAs and Al;Gai-rAs/GaAs are taken from the experimental data in [7]. Peample 1 For the electric field induced change Ae(u) of the DF wwe take the well-known Airy-function expression (8), Aelia) = O(e6"!){[Ai(n) Bi'(n) — n(n) Bn) (10) 451Ai%(n) ~ 9A%9)] 42°) ‘of the complex argument 7 = (u—w+iT')/9, valid at an Me-ctitical point. Here w,,T and @ = (eF?/2m>A)", denote, respectively, the gap, damping and electro-op- tical frequencies; F means the electric field strength, and mt, the reduced effective mass, ‘The value of Cin (10) has been determined by fitting the experimental ey spectra in the photon energy range from 1.4 to 1.6 eV with the zero-field expression for ¢. An electri field modulation through zero has been assumed in the cal- culations, The influence of the field gradient on PR line shapes is illustrated in Fig.1. Spectrum (a) corresponds to the weakest gradient. ‘The line shape has approxi rately the form of the electro-optical function Gas in the case of a homogeneous half space. Increasing the aradient the subsidiary oscillations in curves (b), (c)s (€) become more and more damped. Spectrum (b) ex: hibits beating-like structures caused by the interference between light waves reflected from different parts of the inhomogeneous half space. The calculations of (AR/R)- line shapes under the conditions of example 1 have been repeated by means of the method developed in (5) for ‘an inhomogeneous half space. The results are identical -with those in Fig Example 2 ‘The interpretation of the PR spectra taken from the 3.5urn heterostructure in [6] has raised some contro- versy (1]. Here we reinvestigate this problem. Fig.2a shows the calculated potential and field profiles without and with light modulation at T = 300K. We assume the change of the surface barrier to be the dominant ‘effect of pump light [9]. As Fig.2a indicates, there is practically no field modulation in GaAs due to this ef: fect. ‘The intesity of pump light (wave length in vacuum 341 AR/R 1 J NO 174 4.87 2 Energy (eV) L 135° 1.48 Fig.l, Calculated PR spectra for bulk GaAs with an electric field Fo(1— |2|/w) decaying linearly in a deple- tion region of width w. Fp = 60kV/om;I = 10meV, (a) w = 3um, (b) w = Yum; (6) w = 034m; (a) 05pm. {622.8nm), which penetrates upto the interface, amounts to explI0.2] = 3.6 x 10™* times the incoming inten: sity only. Modulation due to it will be neglected. Then the experimental PR spectral features close to the fun- ‘damental band gap of GaAs cannot be attributed to the field-induced changes of the DF of GaAs. However, it turns out that PR structures at the GaAs gap may arise from changes of the alloy DF. These changes cannot, of ‘course, be explained by the Franz-Keldysh effect since they occur at photon energies far below the gap. A mod: ulation mechanism which is known to be quite efficient in this spectral range is the change of the energy gap due to the piezo-electric effect. By adopting this mechanism ‘and assuming a light induced surface barrier modula tion of 100% we get the PR spectrum of Fig.2b. The structures between the GaAs and AlGaAs gaps are ‘due to the Fabry-Perot oscillations of the heterosiru ture. The period of these oscillations is modulated by the field induced DF changes in the alloy region. Thus PR signal is produced whove line shape is given by the fist derivative ofthe Fabry-Perot spectrum without342 ‘Superlattices and Microstructures, Vol. 15, No. 3, 1994 8 8 é Gaga AlyAs| uns & (a2) renumiog lectric Field (kV/em) & § z(um) =a yon Tt L L | (ar/Ryx10* -2 4 tb) boii r sii 1314 45 16 17 18 19° 2 Eneray (eV) Fig2. (a) Potential and field profiles for the 3.5um - -GrozsAlozr As/GaAs heterostructure described in the text, without modulation and with 100% modulation ‘of the surface barrier. Part (b) shows the corresponding calculated PR spectrum. The Franz-Keldysh response of the alloy isnot included. T’ = 20meV for GaozsAloarAs, and 10meV for GaAs, modulation. The calculated oscillation period isin good agreement with that observed experimentally [6]. An interpretation of the experimental PR. spectzum from {6] in terms of an interference rather than the Franz- Keldysh effect has already been attempted in [1] assum- ing the Franz-Keldysh effect in GaAs to be the dom- inating modulation mechanism. An AlzxGanAs layer width of 2.5m had to be assumed, however, instead of 3.5um reported in [6], in order to obtain the experimen tally observed oscillation period, Example 9 Fig.3 shows the experimental PR spectrum taken at T = 300K from the AlasGaraAs/GaAs heterostructure grown by MBE in our laboratory. Due to the alloy layer width of lum only, the pump light will cause stronger L Ftx10% vem) 3 g e S L L L 1 1 448~«CtTSCSC«iSSC Energy (eV) Fig.3. Experimental (a) and calculated (b) PR spectra of the Iym-GarzAlagAs/GaAs heterostructure as de- scribed in the text. The insert shows the unperturbed field profile field modulation in the GaAs buffer and substrate layers than in example 2. Accordingly, the theoretical curve in Fig has been calculated by assuming the Franz Keldysh effect in GaAs to be the dominating modulation mechanism. With the unperturbed electrie feld profile shown in the insert of Fig.3, and a modulation of the surface field by 100% and the interface field by 5% a remarkably good agreement between calculated and ex- perimental spectra is obtained. This indicates that the ‘oscillations below the fundamental band gap of the alloy are probably due to the GaAs buffer layer / substrate interface. In conclusion, the above examples demonstrate that PR spectra from heterostructures are essentially determined by the actual field profiles without and with light mod- lation. Methods for calculating such profiles and the corresponding modulated reflectance spectra are, there fore, highly desirable. ‘The present paper has provided such methods. Acknowledgements ‘The authors would like to thank CNPq and CAPES (Brazilian funding agencies) for partial financial sup- port.Superlattices and Microstructures, Vol. 15, No. 3, 1994 References (1) R.A. Batchelor and A. Harnett, J.Appl.Phys. 71, 2414 (1992) [2] PLL. Jackson and E.G, Seebauer, J.Appl.Phys. 69, 943 (1991) {3] U. Behn and H. Roppischer, J.Phys. C 21, 5507 (1988) [4] M. Born, and E. Wolf, Principles of Optics, Pergamon Press Oxford, 1964 343 (5] D.B. Aspnes and A. Frova, Solid State Comm. 7, 155 (1968) [6] M. Sydor, N. Jahren, W.C. Mitchel, W.V. Lampert, TW. Haas, MY. Yen, $.M. Mudare, and DH. Tomich, J. Appl. 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