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Aleksandar D. Rakic ´ , Aleksandra B. Djuris ˇ ic ´ , Jovan M. Elazar, and Marian L. Majewski
We present models for the optical functions of 11 metals used as mirrors and contacts in optoelectronic and optical devices: noble metals ͑Ag, Au, Cu͒, aluminum, beryllium, and transition metals ͑Cr, Ni, Pd, Pt, Ti, W͒. We used two simple phenomenological models, the Lorentz–Drude ͑LD͒ and the Brendel– Bormann ͑BB͒, to interpret both the free-electron and the interband parts of the dielectric response of metals in a wide spectral range from 0.1 to 6 eV. Our results show that the BB model was needed to describe appropriately the interband absorption in noble metals, while for Al, Be, and the transition metals both models exhibit good agreement with the experimental data. A comparison with measurements on surface normal structures conﬁrmed that the reﬂectance and the phase change on reﬂection from semiconductor–metal interfaces ͑including the case of metallic multilayers͒ can be accurately described by use of the proposed models for the optical functions of metallic ﬁlms and the matrix method for multilayer calculations. © 1998 Optical Society of America OCIS codes: 160.4760, 310.6860, 160.3380, 250.7260.
It is well known that the performances of optoelectronic devices are strongly inﬂuenced by the choice of their ohmic contacts. Recently semiconductor lasers and light-emitting diodes with metallic mirrors have received much attention. In vertical-cavity-surface-emitting lasers ͑VCSEL’s͒ a metallic layer is commonly deposited on top of a semiconductor distributed Bragg reﬂector ͑DBR͒ mirror to increase the reﬂectivity of the mirror and to serve as a contact.1–5 Asymmetric cladding separate conﬁnement heterostructure lasers rely on the surface metal to form an adequate waveguide for transverse conﬁnement of the optical mode. Consequently, the modal properties are a strong function of the choice of metals ͑and metal thickness͒ for the p-type contact.6 – 8 Metallic layers are not only interesting for lasers, they are also useful in a new generation of optical devices called resonant-cavity light-emitting diodes ͑RCLED’s͒. The RCLED’s have structures similar to VCSEL’s, but they require mirror reﬂec-
A. D. Rakic ´ and M. L. Majewski are with the Department of Computer Science and Electrical Engineering, The University of Queensland, Brisbane QLD 4072, Australia. A. B. Djuris ˇ ic ´ and J. M. Elazar are with the Faculty of Electrical Engineering, University of Belgrade, P.O. Box 816, Belgrade, Yugoslavia. Received 22 December 1997. 0003-6935͞98͞225271-13$15.00͞0 © 1998 Optical Society of America
tivity of only 90 –95%. This reﬂectivity can be achieved by using the metallic layer instead of the technologically more involved semiconductor DBR mirror. RCLED’s have been demonstrated with either one9 –11 or both metallic mirrors.12,13 The RC scheme was also successfully applied to photodetectors with metallic ͑Ag, Al͒ mirrors.14,15 In all cases the needed high mirror reﬂectivity can be attained by using pure noble metals or Al, whereas the good ohmic contact and reliable adhesion are achieved by using layers of wetting metals ͑Ti, Pd, Cr͒ between the semiconductor and the high-reﬂectivity metal layer. For metal͞GaAs ohmic contacts, the preferred metal is usually Au. Unfortunately, a pure Au contact has two major disadvantages; it has very poor adhesion and it diffuses rapidly into the semiconductor. To rectify these shortcomings of a p-type semiconductor͞Au contact, a thin layer of Ti is usually employed to improve adhesion, while the thin layer of Pt serves as a diffusion barrier.6 Several other metallization schemes for GaAs devices are also in use: nonalloyed AuZn͞Au for p-type ohmic contact and alloyed AuGe͞Ni͞Au for n-type ohmic contact,13 Ag͞Au͞ Ti͞Au for p-type and AuGe for n-type contact,10 Ag͞ CdSnO for p-type semitransparent contacts.11 The metal͞InP ohmic contact design concepts are very similar to those suggested for metal͞GaAs systems. Traditionally, Au-based alloy contacts ͑AuZn, AuZnNi, AuBe, AuGe, AuNi, AuCr, AuCd, AuMg, AuMn͒ have been used as well as nonalloyed Ti͞Pt͞Au and Ti͞Au metallization schemes for both contacts.14,16,17 How1 August 1998 ͞ Vol. 37, No. 22 ͞ APPLIED OPTICS 5271
22–24 Although there are several compilations of the optical properties of metals. for example. For example. In Section 2 we describe the LD and the BB models. The intraband part ⑀ ˆ r͑ f ͒͑͒ of the dielectric function is described by the well-known free-electron or Drude model37. strength fj . Therefore the purpose of this paper is twofold: ͑a͒ to present a comprehensive and accurate parameterization of the optical properties of metals for optoelectronic applications in a wide spectral range and ͑b͒ to compare 5272 APPLIED OPTICS ͞ Vol. which is not adequate in the near-IR and the visible wavelength range. k is the number of oscillators with frequency j . B. Material Models A. Often models for ⑀r͑͒ that are closely related to the electronic band structure prove to be exceedingly complicated for practical use or are restricted to a certain material.21 based on the damped harmonic oscillator approximation. The amplitude and the phase of the reﬂection coefﬁcient can be calculated from the optical constants ͓refractive index n͑͒ and extinction coefﬁcient k͔͑͒ or from the complex optical dielectric function ⑀r͑͒ ϭ ⑀r1͑͒ Ϫ i⑀r2͑͒. It has been shown. The phase change on reﬂection at the metal–semiconductor interface in the near-IR and visible wavelength range is always less than 180°. In Appendix A we outline the derivation of our analytic form of the BB model. In Section 4 we compare our results with recent measurements performed on vertical cavity structures. while ⍀p ϭ ͌f0p is the plasma frequency associated with intraband transitions with oscillator strength f0 and damping constant ⌫0. 22 ͞ 1 August 1998 the LD model with the new BB model on several examples. are still frequently used. 37. nonalloyed composite coatings are much preferred when contact serves also as part of the optical cavity.39. 2.18. acting at the same time as semitransparent mirrors. and lifetime 1͞⌫j . ͑ Ϫ i⌫0͒ (2) The interband part of the dielectric function ⑀ ˆ r͑b͒͑͒ is described by the simple semiquantum model resembling the Lorentz result for insulators: ⑀ ˆ r͑b͒͑͒ ϭ ͚ jϭ1 k fj p2 . the optical functions of the noble metals are not amenable to such interpretation. No. have been found suitable for CdHgTe and CdZnTe devices.36 that a complex dielectric function ⑀r͑͒ can be expressed in the following form: ˆ r͑ f ͒͑͒ ϩ ⑀ ˆ r͑b͒͑͒. Accordingly.40 however. ͑j2 Ϫ 2͒ ϩ i⌫j (3) where p is the plasma frequency. Lorentz–Drude Model First we brieﬂy discuss the LD model often used for parameterization of the optical constants of metals. In Section 3 we give an overview of the optical dielectric functions of the metals used in this study and provide parameterizations of these optical functions in terms of LD and BB models. the Lorentzian broadening function has higher and more extended wings compared with the Gaussian one.32–34 It has been shown35. We present parameterization of the large number of metals for optoelectronic applications. If the same strength and full width at halfmaximum are assumed for both absorption line shapes.25–30 authors know of no systematic parameterization. We also give a new derivation of this ﬂexible phenomenological model and present a BB model in two different analytic forms suitable for implementation on a computer. Brendel–Bormann Model Let us now concentrate on the interband part ⑀ ˆ r͑b͒͑͒ of the dielectric function. Furthermore it can be a very sensitive function of wavelength in the vicinity of interband transitions of the employed metal ͑see.19 In contrast. it is necessary to determine precisely the phase and the amplitude of the reﬂection coefﬁcient of such a metal–semiconductor interface to design the resonator properly.38: ⑀ ˆ r͑ f ͒͑͒ ϭ 1 Ϫ ⍀p2 .9 Because metallic mirrors are the elements of the resonant cavity of VCSEL’s and RCLED’s.ever. other than studies in which the free-electron Drude model was used. Taking into account the phase change on reﬂection on the metal–semiconductor interface enables one to calculate the thickness of the last semiconductor layer ͑the phase-matching layer͒ before the metal to match the phase characteristic of DBR at the design wavelength. Usually the Lorentz model employs oscillators at major critical points ͑CP’s͒ in the joint density of states that correspond to interband transition energies បj . with some additional oscillators to model absorption between CP’s. which can be used to describe optical properties of an arbitrary solid. Pure gold contacts. Materials such as W and W alloys are certainly suitable candidates for obtaining abrupt metal– semiconductor interfaces. that usually the Gaussian line shape is a much better approximation for the broadening function than the Lorentzian line shape. Therefore simple phenomenological models such as the Lorentz-Drude ͑LD͒ oscillator model20 or Erman’s model. using ͑a͒ a simple LD model and ͑b͒ a recent model by Brendel and Bormann31 ͑BB͒. all the models based on the Lorentzian broadening function exhibit excessive absorption far from the CP’s. Ref. Brendel and . one can express the bulk ﬁlm optical dielectric function of Al by using the Ashcroft and Sturm model. Recently. 18 and references therein͒. ⑀ ˆ r͑͒ ϭ ⑀ (1) which separates explicitly the intraband effects ͑usually referred to as free-electron effects͒ from interband effects ͑usually referred to as bound-electron effects͒. Therefore there is need for a study that would provide a description of the optical functions of metals in terms of a simple model and that would cover all the metals used for optoelectronic applications.
beryllium. However. and W͒.43. The expression for the complete optical dielectric function now reads ⑀ ˆ r͑͒ ϭ 1 Ϫ k ⍀p2 j ͑͒. Integral ͑4͒ can be solved analytically ͑see Appendix A͒ to obtain j ϭ i ͱ fj p2 2 ͱ2 aj j where k is the number of BB oscillators used to interpret the interband part of the spectrum. Eq. 2 2 and where n0 is the refractive index of the incident ˆ 1 ϭ n1 Ϫ ik1 is the medium ͑semiconductor͒ and N refractive index of the substrate ͑metal͒. U͑1͞2. 1͞2. the amplitude reﬂection coefﬁcient and the phase are well deﬁned. Equations ͑13͒ and ͑14͒ imply that the incident medium is lossless owing to the well-known problems of deﬁning reﬂectivity for the wave incident from the lossy medium. Ϫ ͫ ͭͫ U 1͞2. trying always to engage 1 August 1998 ͞ Vol. Ni. 2 (9) we obtain j ϭ 2 ͱ2 aj j ifj p2 ϩ U 1͞2. ͓͑⑀r12 ϩ ⑀r22͒1͞2 Ϫ ⑀r1͔1͞2. can be calculated from the fractive index N complex optical dielectric function: nϭ kϭ ͑Im͓ z͔ Ͼ 0͒.Bormann31 have proposed a model for a dielectric function of solids that replaces a Lorentz oscillator with a superposition of an inﬁnite number of oscillators. Results for 11 Metals aj ϩ j 2 j (10) When we keep in mind that special functions of complex arguments are now readily available through languages such as Mathematica. energy.43 However. deﬁned by ͓see Ref. ͑n0 ϩ n1͒2 ϩ k12 (13) z A solution satisfying the condition aj Љ Ͼ 0 is aj Ј ϭ aj Љ ϭ ͱ2 ͱ2 ͕͓1 ϩ ͑⌫k͒͞2͔1͞2 ϩ 1͖1͞2.3͔͒ w͑ z͒ ϭ eϪz erfc͑Ϫiz͒ 2 1͞2 Refractive index n and extinction coefﬁcient k. z͒. C. being the real and the imaginary parts of the complex reˆ ϭ n Ϫ ik. Ϫ ͩ ͱ ͪͬ ͩ ͱ ͪ ͬͮ aj Ϫ j 2 j .42 or from various We have parameterized 11 most frequently used metals: noble metals ͑Ag. the Kummer functions of the second kind U͑a. For all the metals we have carefully chosen relevant optical data. Therefore a range of absorption function approximations with similar kernels and different wings can be obtained with Eq. 1͞2. even if the lossy incident medium ͑semiconductor͒ is assumed. 41.1. ͑11͒. and there are no problems in calculating the phase shift upon reﬂection needed in resonator design. this model is as easy to implement as a simple LD model. Pd. b. given by j ͑͒ ϭ Fortran and C libraries. while w͑ z͒ is the error integral of the complex argument. normal incidence reﬂectivity can be calculated by use of43 Rϭ ͑n0 Ϫ n1͒2 ϩ k12 . 1͞2. and Cu͒. This additional parameter allows for a continuous change in the absorption line shapes ranging from a purely Lorentzian for j Ϸ 0 to a nearly Gaussian for ⌫j Ϸ 0. we show that this model can be used to describe optical properties of a wide range of materials including metals. z2͒ ϭ ͱ ez erfc͑ z͒. By employing the relation between erfc͑ z͒ and U͑a. ͑5͒ also be expressed in terms of conﬂuent hypergeometric functions.39͔͒. Eq. ϩ ͑ Ϫ i⌫0͒ jϭ1 ͱ2j ϫ 1 ͐ ͫ ϩϱ Ϫϱ 2 exp Ϫ ͑ x Ϫ j ͒ 2j2 2 ͬ (4) ͚ (11) fj p d x.44 3. z͒ ͓cf. 41. In their original paper31 the authors suggested that the model is applicable to an amorphous solid in the far-IR part of the spectrum and constructed the model from a phenomenological point of view. ͑ x2 Ϫ 2͒ ϩ i⌫j The number of harmonic oscillators per frequency interval is determined by a Gaussian function. Optical Constants and Reﬂectivity ͫ ͩ ͱ ͪ ͩ ͱ ͪͬ w aj Ϫ j 2 j 2 ϩw aj ϩ j 2 j . aluminum. 37. (6) ͱ2 ͱ2 1 1 ͓͑⑀r12 ϩ ⑀r22͒1͞2 ϩ ⑀r1͔1͞2. ͑7. Thus an analytic function is obtained that satisﬁes the Kramers–Kronig ͑K–K͒ relations and has a ﬂexible shape of the absorption proﬁle. (5) where aj ϭ aj Ј ϩ iaj Љ ϭ ͑ Ϫ i⌫j ͒ and aj Љ Ͼ 0. (12) and erfc͑ z͒ is the complementary error function.6. This function. and some of the transition metals ͑Cr. (8) where the phase shift associated with the reﬂected beam is43 ϭ arctan 2n0 k1 ͑n0 Ϫ n12 Ϫ k12͒ 2 (14) We suggest that Eq. Ref. erfc͑ z͒ ϭ ͱ 2 ͐ ϩϱ exp͑Ϫt2͒dt. and linewidth. (7) For the simple semiconductor–metal interface. 22 ͞ APPLIED OPTICS 5273 . however. ͑13. Au. b. No. Pt. ͕͓1 ϩ ͑⌫k͒͞2͔1͞2 Ϫ 1͖1͞2. Ti. namely. introduces an additional parameter per each transition besides the strength.
555 0.084 0.336 0. even by an order of magnitude.292 6.3 to 26.100 4. Optimal values for LD model parameters. Of particular interest to our application is the study of The ` ye49 providing the dielectric function of Au in the 0. The values for oscillator strengths correspond to the plasma frequencies បp given in Table 1.030 0.314 0.249 — — — Ti 0. the highly efﬁcient move generation mechanism.121 0.580 2.802 4.082 0. A. whereas Table 3 presents optimal parameters for the BB model.333 0.096 0. 45.51 10. as depicted in Fig.166 1. we used K–K consistent sets of optical data in the whole range.291 0.149 2.18 — — — Al 0. B.01 9.032 0.830 0.054 0.576 8.706 3.545 0.47 agree well at ϳ3. To ﬁt the models ͑LD and BB͒ to the data.135 1.047 0.276 0.384 2.071 0.333 0.48 from 3.452 4.305 11.511 0.065 8. are given in Table 2.148 0.649 2.621 1.668 3.300 0. obtained by this algorithm.166 1.048 0.899 2.825 1.175 0. polarimetric measurements of Winsemius et al. we use the acceptance-probability-controlled simulated annealing algorithm ͑described in detail in Refs.75 15.304 4.083 5.48 and of Winsemius et al.969 0.227 0.130 1. morphology.174 0.22 algorithm has proved to be insensitive to initial parameter values and extremely efﬁcient in escaping local minima. 22 ͞ 1 August 1998 5274 .151 3.056 2. we used the data tabulated in Ref.185 0.663 2.970 0.312 1.206 0.393 2.916 9.03 10.453 3. For our ﬁts we used data between 0.840 0.777 0.638 4.031 1.92 9.72 9.601 2.664 0.715 — — — Pt 0. Values of the LD Model Parameters Metal Parameters f0 ⌫0 f1 ⌫1a 1a f2 ⌫2 2 f3 ⌫3 3 f4 ⌫4 4 f5 ⌫5 5 a Ag 0.760 0. Silver the measurements obtained on ﬁlms similar ͑in terms of geometry.241 0.213 5. the replacement of the temperature control of the cooling schedule with direct control of acceptance probability.125 and 0.191 0.162 0.419 20.395 1.104 1.590 5.43 — — — W 0.47 between 0.597 0.5 eV.236 5.836 7.121 0.29 Au 0.305 0.65–1 eV͒. No attempt has been made here to constrain the values of the oscillator strengths and linewidths in the ﬁtting procedure. No.214 13.183 0.4 eV where they meet.382 3.080 0.98 18.010 0.415 0.351 1.5– 6-eV range from the measurements of the reﬂectance and the transmittance of semitransparent Table 2. The absorption data ͑⑀r2͒ of the same groups continue well at ϳ1 eV with a somewhat steeper slope in the data of Winsemius et al.140 3.29 13.509 0.178 1. The data of Leveque et al. 32 and 34͒.65 and 3.089 — — — Pd 0.030 3.808 0.517 9.957 0.582 0. which was speciﬁcally designed for solving parameter estimation problems.838 1.638 4.150 1.3 eV. and the process of growth͒ to the ﬁlms used in optoelectronic devices. Gold Gold has been the subject of extensive optical studies.659 1. (15) To minimize the merit ͑or cost͒ function.47 Our model dielectric function agrees well in slope and magnitude with both data sets.454 3.98 eV. This For parameterization of the optical constants of silver.494 4.950 0.917 0.008 0.004 0. wherever possible.125 and 6 eV.024 0.604 — — — Cr 0.124 0.59 7.498 — — — In electron volts. The algorithm has two independent features that make it superior to other simulated annealing algorithms in terms of convergence rate and robustness: ﬁrst.106 2. The dispersion data ͑⑀r1͒ of Dold and Mecke46 have the same slope but slightly lower values than the data of Winsemius et al.646 2.048 0.83 14.335 8.481 0.816 0.064 0.053 0.047 0.187 1.775 — — — Ni 0.050 0. second.011 0.345 0.780 0. 1.32 Cu 0.100 0. This composite set consists of the polarimetric data of Dold and Mecke46 between 0.676 1. APPLIED OPTICS ͞ Vol.575 0. and K–K analyzed in situ reﬂectance measurements of Leveque et al.Table 1.035 0.518 1. Values of the Plasma Frequencies បp ͑eV͒ Metal Ag Au Cu Al Be Cr Ni Pd Pt Ti W បp 9.334 0. we employed the following objective function: iϭN ϭ 2 ͚ iϭ1 ͫͯ ⑀r1͑i ͒ Ϫ ⑀r1exp͑i ͒ ⑀r2͑i ͒ Ϫ ⑀r2exp͑i ͒ ϩ exp ⑀r1 ͑i ͒ ⑀r2exp͑i ͒ ͯ ͯ ͯͬ 2 .544 0.517 0.168 0.870 2.332 3.762 19.47 in the region of overlap ͑0.001 1.523 0.886 0.501 0.141 3.659 0.729 6.065 3.723 3. Also.530 4.281 1.330 0.061 0.547 3.543 1.473 — — — Be 0. 37.845 0.378 0.530 1.
825 0.379 0.805 0.962 0.214 2.742 0.454 0.136 1.060 0.809 1.799 0.120 1.179 27.047 2.817 2.050 0.030 0.894 0.446 0.042 0.069 0.080 0.648 0.956 0.096 0.022 0.246 1.903 — — — — Ni 0.86 2. At ϳ2 eV.97 1.562 0.49 1 August 1998 ͞ Vol.498 0.252 0.506 0.469 0.059 0.031 0.398 2. 2.133 0.851 1.526 0.346 2.854 — — — — W 0.416 0.827 0.317 0.338 4.985 0.039 0.172 8.170 4.182 1.885 0.819 1.551 2.495 1.587 1.167 0.131 0.849 0.261 3.100 2.459 0.997 4.083 4.197 0.050 0.962 0.009 0.277 0.822 4.562 0.076 0.0 eV.782 0.035 2.137 1. The results on wellcrystallized ﬁlms of thicknesses from 10 to 25 nm evaporated in ultrahigh vacuum ͑10Ϫ11 Torr͒ show good agreement with data obtained on bulk samples.013 0.555 5.637 8.584 0.057 0.081 0.035 0.025 1.067 0.919 0.877 1.000 0. 22 ͞ APPLIED OPTICS 5275 .409 0.126 0.983 6.754 0.067 3.093 0.726 0.225 0.136 1.311 3. Figure 2 shows the real and the imaginary part of the dielectric function of gold versus photon energy between 0.357 2.312 0. Real and imaginary parts of the optical dielectric function of Au: solid curves.163 0.019 4.273 2.113 4.583 0.769 2. Also shown are selected experimental data points from Dold and Mecke46 and The ` ye.467 0.56 0.821 0.117 9.146 — — — — Ti 0.131 0.333 0.324 0.665 1.027 0.987 1.048 0. values that we calculated using the BB model.615 0. the LD model.054 0.719 0.049 0.218 1.189 2.083 0. Real and imaginary parts of the optical dielectric function of Ag: solid curves.022 2.957 0.98-eV region and the data of The ` ye49 between 1.689 0.561 0.469 3.893 — — — — Cr 0.820 0.891 8.502 0.256 0.022 0. No.218 0.665 0.066 2.006 3. Both data sets were tabulated in Ref. 1.912 — — — — In electron volts. the LD model.052 18. 45.0002 4.330 0.218 0.167 0.661 0.236 1.317 0.770 0.481 3.256 0.49 In our analysis we used the ellipsometric data of Dold and Mecke46 in the 0.185 0.115 0.510 — — — — Pd 0.694 0.904 4.513 0.081 0..189 0. Values of the BB Model Parameters Metal Parameter f0 ⌫0 f1 ⌫1a 1a 1a f2 ⌫2 2 2 f3 ⌫3 3 3 f4 ⌫4 4 4 f5 ⌫5 5 5 a Ag 0.154 0. A detailed analysis of these samples indicated that it is possible to produce very thin but continuous ﬁlms with the same properties as the bulk material.014 2.186 0. dashed curves.059 1.067 5.654 6.0 and 6.735 — — — — Be 0. Also shown are the selected experimental data points from Dold and Mecke.051 0.189 0.343 0.281 0.074 0.46 Winsemius et al.119 5.48 Fig.Table 3.318 0. ﬁlms of various thicknesses.349 0.604 3.312 0.827 1.766 2.719 — — — — Al 0.830 0.463 0.427 1.309 2.343 0.125– 0.105 6.056 0.050 0.331 — — — — Pt 0.213 0.442 1. values that we calculated using the BB model. the BB model ﬁts the data much better than the LD model. dashed curves.433 1.315 1.109 19. This better set can Fig.432 1.125 6.497 0. 37.066 0.2 and 5 eV.47 and Leveque et al.795 Cu 0.516 Au 0. where the lowest-laying interband transitions occur in Au.127 1.648 4.047 0.277 0.145 4.606 0.
54 Fig. Aluminum be attributed to the Gaussian broadening in the interband part of the spectrum. BB model. Beryllium There have been only a few studies of optical properties of Be.50 and Ordal et al. and they produced different results. LD model͒. Results of this analysis are tabulated in Refs. with data from various sources36. dashed curves. The values of Nash and Sambles for ⑀r2͑͒ are smaller than the majority of other data in the visible range. 22 ͞ 1 August 1998 To ﬁt the models to data for Al we used results from a recent study of Rakic ´ . Recent research of Nguyen et al. tabulated data. Real and imaginary parts of the optical dielectric function of Cu: solid curves.18 D. 50 was obtained by combining original transmission measurements.2 meV͒ to 0.18 In Ref..26 pertinent in the IR and far-IR range.50 Ordal et al. E.50 and Ordal et al. values that we calculated using the BB model.54 5276 APPLIED OPTICS ͞ Vol. Figure 4 shows excellent agreement between tabulated data18 ͑open circles͒ and models ͑solid curves. Also shown are selected data from Rakic ´ . The data of Ordal et al. self-consistent algorithm presenting the combination of the K–K analysis and the LD model application. the BB model. onto the high-quality silica grating with a well-deﬁned pitch ͑800 nm͒ and a proﬁle.56 shows that for high-rate-evaporated aluminum the electron mean free path increases by nearly an order of magnitude over the thickness range of 5. 4. are obtained from the K–K analysis of their reﬂectance data.54 They thermally deposited copper ﬁlm. dashed curves. 37. solid curves. Film was covered by a 50nm-thick layer of silicon monoxide without being removed from vacuum. 18 optical and electron-energy-loss data for evaporated aluminum ﬁlms have been critically analyzed and used in an iterative. authors have claimed that this is due to the absence of contamination in their protected copper ﬁlms. New values for the optical functions of aluminum have been reported in the wide spectral range from 200 m ͑6.51–53 to provide an absorption spectrum large enough for a K–K analysis. Also shown are tabulated data from Hagemann et al.26 from 0.55 dc conductivity measurements. In Fig. transitions that dominate the bulk-material interband spectrum are noticeable. We used the data of Ordal et al. and are in good agreement with both the peak position and the linewidth of the electron-energy-loss data.. espe- . dashed curves.12 nm ͑10 keV͒. C. the LD model.87 eV and data of Hagemann et al. 3. An interesting new result is the surface plasmon– polariton study of Nash and Sambles.1 to 0. 45 and 25.5– 6 nm. For thicknesses over the 6-nm parallel-band. 3 we compare several experimental data sets for Cu. showing that the values of Nash and Sambles for ⑀r1 closely agree with the data of Hagemann et al. which becomes dominant in this region. Real and imaginary parts of the optical dielectric function of Al: solid curves.50 from 1 to 6 eV. dashed curves. Figure 3 depicts the real and the imaginary part of the dielectric function as a function of energy ͑open circles.26 in the region of overlap. These functions are in accordance with recent calculations of Lee and Chang. LD model. values calculated by use of the BB model. The results are examined for internal consistency by inertial and f-sum rules. performed on ﬁlms evaporated in the conventional vacuum. Copper Data for the copper that we used in this research are from the studies of Hagemann et al.26 The composite data set reported in Ref. we expect the bulk dielectric function of aluminum presented here to be a reasonably good approximation for aluminum thin-ﬁlm dielectric function.26 and Nash and Sambles. No. the LD model͒. representing a transition of the particle ﬁlm in the continuous ﬁlm with single-crystalline grains that span the thickness of the ﬁlm.Fig.. 350 nm thick. Keeping in mind that aluminum layers used in optoelectronic devices are usually more than 10 nm thick.
Figure 7 shows the real and the imaginary part of the optical dielectric function versus photon energy ͑open circles. 25. This indicates 1 August 1998 ͞ Vol. We used their data between 0. agreed with each other well within the estimated experimental error. dashed curves.57 They obtained a consistent set of optical constants by performing a K–K analysis in the wide spectral range from 0. No. probably because of this agreement among the published optical functions of Ni is good. they noted that the values of the conductivities increased with ﬁlm thickness. In this paper we used the data from Weaver and Benbow62 in the 0. Also shown are tabulated data from Bos and Lynch58 and Kirillova and Noskov.64 – 6. data from Arakawa et al. addresses the change in optical constants with ﬁlm thickness.41 eV.1– 0.46 and 5 eV.069 and 0. One result of their research.and 26-nm-thick ﬁlms showed a slight increase in n with decreasing ﬁlm thickness. 6. 22 ͞ APPLIED OPTICS 5277 . BB model.58 tabulated in Ref. depending strongly on sample preparation and the method for the analysis of experimental data.60 cially in the visible range of the spectrum. the successive differences were not more than the assumed experimental error. probably due to the ﬁnegrain structure and voids in the ﬁlms. and the bulksample ellipsometric data of Kirillova and Noskov. Real and imaginary parts of the optical dielectric function of Cr: solid curves. with thicknesses of 40 and 50 nm. Fig. The optical constants of Cr measured on two ﬁlms. These data are also tabulated in the review of Borghesi and Piaggi. We used their data between 0. show lower reﬂectance values.2 nm thick.06 to 26 eV. solid curves. measurements on 36.4.08 to 50 eV. 5. which is particularly important to our application.61 measured in the 0. Unfortunately. the BB model.6 and 6 eV. the LD model. the BB model. LD model͒. 37. Chromium inary part of the dielectric function of chromium.069 – 4. 57. In the case of the three thickest ﬁlms. The data that we used for ﬁtting are from the excellent study of Arakawa et al. Palladium The optical properties of palladium have been the subject of several investigations. Nickel In our research we used the K–K-analysis data of Bos and Lynch.6-eV range and from Johnson and Christy61 between 0. although their K–K analysis extends further.60 tabulated in Ref.Fig.63 Johnson and Christy61 reported the systematic dependence of optical constants on ﬁlm thickness. Figure 6 shows our calculated values for the real and the imag- Nickel does not behave as a free-electron metal for wavelengths shorter than ϳ20 m.7. Figure 5 shows the real and the imaginary part of the optical dielectric function as a function of energy. and 41. 59. using normalincidence reﬂectance data from various sources. Here we used data from the research of Lynch and Hunter.57.45 This consistent set of optical functions is obtained by K–K inversion of reﬂectance and absorptance data from a number of sources in the range from 0. 29. the LD model͒. dashed curves. dashed curves.61 However. Good agreement with experimental data can be observed for both models. F. Real and imaginary parts of the optical dielectric function of Be versus photon energy ͑open circles.2. Kirillova and Noskov60 reported measurements in the 0. The frequently quoted data of Johnson and Christy.095 eV in the IR. results disagree as to the magnitude of the optical functions. tabulated data. 32. Analyzing ﬁlms 16. solid curves. H.9-eV range. the solid curves. and the dashed curves. The measurements of Bos and Lynch58 extend to 0. Open circles represent data from Ref.2 to 5 eV. whereas the value of k was almost unaffected. For our ﬁts we have employed data from 0. The inconsistency in the results can be attributed to the difﬁculty of sample preparation. the LD model. G. values that we calculated using the BB model.60-eV range. Good agreement between tabulated data and both models can be observed.
9. that. 9.1 to 30 eV. As the other transition metals do. Also shown are tabulated data from Weaver and Benbow62 and Johnson and Christy. Interband transitions for platinum are expected. Real and imaginary parts of the optical dielectric function of Pd: solid curves. data from Weaver64. 70 the paper by Johnson and Christy61 is quoted as a source of data. 71 ͑pp. The ⑀r1 values from Kirillova and coworkers are in reasonably good agreement with the data of Johnson and Christy61 in the region of overlap.70 reported reﬂectivity and absorptivity measurements of mechanically polished and electropolished bulk Ti samples in the energy range from 0. The prominent maximum in the ⑀r1 values of Lynch et al.6 eV. 7. 12–145͒.4 and 9. the LD model. Kirillova and coworkers72–74 used an ellipsometric technique to measure the optical constants of mechanically and chemically polished polycrystalline samples from 0.06 to 2. K–K analysis was used to invert the measured spectrum to the optical dielectric function. 7. Also shown are tabulated data from Lynch and Hunter. at ϳ6. The ⑀r2 values from Kirillova and coworkers are noticeably lower ͑for photon energies greater than 1 eV͒. This data set is tabulated in Ref. for thicknesses of more than 20 nm. A fast evaporation rate was used to insure the surface smoothness of the ﬁlms. Real and imaginary parts of the optical dielectric function of Ni: solid curves.Fig. 22 ͞ 1 August 1998 Johnson and Christy61 investigated the reﬂectivity and the transmissivity of thin titanium ﬁlms ͑29. dashed curves.46 eV is absent in the data of Kirillova and coworkers. although all the energies of the structures do not agree well. solid curves.72–74 The weaker peak in the ⑀r1 values of .70 at ϳ0. dashed curves. Figure 8 shows excellent agreement between our ﬁts ͑for both models͒ and tabulated values of the real and the imaginary part of the optical dielectric function. LD model͒. The structure of optical constants64 is evident at approximately 7.61 5278 APPLIED OPTICS ͞ Vol. BB model. solid curves.8 eV. BB model.64 Weaver used reﬂectance65– 67 and transmittance68 data from a number of sources to obtain n and k by the K–K technique. 69.45 Fig. instead of Ref.3.8 eV. Figure 9 shows a dielectric function versus energy for platinum ͑open circles. and 10. Real and imaginary parts of the optical dielectric function of Pt versus photon energy ͑open circles. platinum possesses the characteristic minimum in ⑀r2 with an additional structure at higher energy.8 –35 nm thick͒ evaporated in a conventional vacuum from a tungsten ﬁlament. dashed curves. bulklike values of optical constants represent a good approximation. J. 37. 8.3. values that we calculated using the BB model.8. Lynch et al. according to Ref. we used the tabulation of the optical constants of Pt given in 45 based on the study of Weaver. No. tabulated data. values that we calculated using the BB model. but owing to an error. Titanium Fig. Platinum To ﬁt our model to data. dashed curves. I. the LD model. LD model͒.
11.73 in the energy range from 0. GaAs–Al. Comparisons and Conclusions Most measurements of the optical functions of tungsten are in good agreement. BB model. In the IR and visible wavelength range. data from Weaver et al.3 eV can be noticed in the data of Johnson and Christy61 at ϳ1. Interference between these two ﬁelds causes the high reﬂectivity of the metal. 15͑a͔͒ and the one terminating on a metallic layer ͓Figs. 10. Real and imaginary parts of the optical dielectric function of Ti: solid curves. 76. and GaAs–Pt interfaces.. the reﬂectivity R is also less than one.70 Fig.73 Bolotin et al. This phase difference of a half-period is a delay between the time when the incident ﬁeld is absorbed and the time when it is reradiated by the medium. and for GaAs we used our model for N͑͒ ϭ n͑͒ Ϫ ik͑͒ described in Ref.15 eV and in the data of Kirillova and coworkers at ϳ1 eV ͑see Fig. 15͑b͒ and 15͑c͔͒. Figure 14 depicts the phase change on reﬂection for the same four interfaces in the same wavelength range.74 If one treats a metal as a perfect conductor. GaAs–Au. the LD model.70 located at 1.68 Figure 12 shows the real and the imaginary part of the dielectric function of W versus photon energy ͑open circles. the phase change on reﬂection from real metal is always less than and can be strongly frequency dependent in the vicinity of the interband transition frequencies.2 m͒. In Fig. We employed models for the optical constants of metals ͓N͑͒ ϭ n͑͒ Ϫ ik͔͑͒ described in Section 3. solid curves.4 – 0. 22 ͞ APPLIED OPTICS 5279 . 12. Tungsten Ref.73 and Bolotin et al. dashed curves. BB model.74 Johnson and Christy. Material response is out of phase with respect to the electric ﬁeld incident on the metal.Fig. 45.72. Real and imaginary parts of the optical dielectric function of Ti: experimental data points. Real and imaginary parts of the optical dielectric function of W versus photon energy ͑open circles.61 and Lynch et al. LD model͒.75. Lynch et al. 11 we compare the real and the imaginary part of the model dielectric function of Ti against the pertinent experimental data. 37. dashed curves. one needs only to enforce the tangential component of the electric ﬁeld Etan ϭ 0 on its surface since there is no ﬁeld penetration into it. K. Figure 13 shows reﬂectivities for GaAs–Ag. Let us now compare the DBR mirror terminating on air ͓Fig. tabulated data. dashed curves.1 to 6 eV ͑12. In our ﬁts we used data from Kirillova and Charikov72. solid curves. Also shown are tabulated data from Kirillova and Charikov72. In this paper we used the optical constants of Weaver et al. Kirillova and Charikov.75 tabulated in Fig. Consequently. If the semiconductor layers comprising the DBR are of a quarter1 August 1998 ͞ Vol.6 eV. values that we calculated using the BB model. Optical constants were obtained by the K–K inversion of reﬂectivity data in combination with the absorption spectrum from Haensel et al. LD model͒. 4. No.06 to 2. 10͒. To illustrate this we calculated R͑͒ and ͑͒ for four semiconductor–metal interfaces in the spectral range from 0.
The additional highindex QWOT layer ͑the phase-matching layer͒ is needed between the last semiconductor layer and the perfectly conductive metallic layer ͓see Fig. In this paper we present. the wave reﬂected from interface 1. Calculated reﬂectivities for four GaAs–metal interfaces: GaAs͞100 nm Ag. while n and d are the refractive index and the physical thickness of the phase-matching layer. one needs to have a matching layer with phase thickness ␦ satisfying Ϫ2␦ ϩ ϭ 0 ͓see Fig. ͑14͒. DBR mirror terminating on ͑a͒ air. Reference 77 presents the measured reﬂectance for two F–P cavities: ͑a͒ air– GaAs ͑1000 nm͒–wax and ͑b͒ air–GaAs ͑1000 nm͒– Ti͞Au ͑2 nm͞170 nm͒–wax. GaAs͞100 nm Au. Therefore the round-trip phase shift Ϫ in the phase-matching layer cancels the phase change on reﬂection at the semiconductor–metal interface. is in phase with the wave reﬂected from interface 2. Results are depicted in Fig. 15͑b͔͒ to keep the waves reﬂected from interfaces 1 and 2 in phase.77 describes a method for direct measurement of that uses the speciﬁcally designed cavity. wave optical thickness ͑QWOT͒. 15͑a͔͒. If we now consider the real metal with the complex refractive index N ϭ n Ϫ ik. which experiences a phase shift ␦ ϭ Ϫ while making a round trip through the last high-index layer ͑GaAs͒ and no phase change on reﬂection. ϭ . 2 0 (16) where 0 is the vacuum wavelength. 15. 37. To keep the waves reﬂected from interfaces 1 and 2 in phase. ͑b͒ perfectly conductive metal. GaAs͞100 nm Al. Therefore the required phase thickness of the phase-matching layer is ␦ϭ 2 ϭ nd. the dashed curves show the experimental data from 77. No. They recorded the reﬂectance spectra of Fabry–Perot ͑F–P͒ resonators formed by semiconductor layers clad by ͑a͒ air on one side and a dielectric on the other and ͑b͒ air on one side and a metal multilayer on the other. 76. A recent paper of Babic ´ et al. where Ͻ at all wavelengths. Again. and GaAs͞ 100 nm Pt. Fig. GaAs͞100 nm Au. 5280 APPLIED OPTICS ͞ Vol. GaAs͞100 nm Al. for the ﬁrst time to our . The phase change on reﬂection at 1550 nm estimated from the experiment ͑exp Ϸ 137°͒ is in accordance with our calculated phase calc ϭ 139°. for the optical constants of metals we used the models from Section 3 and for the GaAs model described in Ref.Fig. 15͑c͔͒. The solid curves are from the transfer-matrix calculations. The needed thickness d is therefore dϭ 0 ϭ ͑QWOT͒. and ͑c͒ real metal. 22 ͞ 1 August 1998 It is important therefore that we know precisely the phase change on reﬂection from the metal– semiconductor interface ͑͒ to be able to calculate the thickness of the phase-matching layer. the phase change on reﬂection is determined by Eq. and GaAs͞100 nm Pt. 16. which undergoes the phase change on reﬂection ϭ ͓see Fig. 14. 13. We used a transfermatrix method to calculate the reﬂectivity of structures ͑a͒ and ͑b͒. Calculated phase changes on reﬂection for four GaAs͞ metal interfaces: GaAs͞100 nm Ag. 4n ͩͪ (17) Fig.
4͔͒ I1 ϭ ͐ ϩϱ Ϫϱ eϪt aj Ϫ j 2 . Au.Appendix A The Brendel–Borman model requires the integration of Eq. while for aluminum and the transition metals both models exhibit good agreement with the experimental data. experimental curves from Ref. we can solve the second integral ͑ x Ϫ j ͒2 ϩϱ 2j2 I2 ϭ dx ͑aj Ϫ j ͒ ϩ ͑ x Ϫ j ͒ Ϫϱ ͐ exp Ϫ ͫ ͬ (A6) by introducing t ϭ ͑ x Ϫ j ͒͑͌͞2j ͒ and z2 ϭ ͑aj ϩ j ͒͑͌͞2j ͒: I2 ϭ ϭ ͐ tϭϩϱ tϭϪϱ eϪ t dt ϭ z2 ϩ t 2 ͐ tϭϩϱ tϭϪϱ eϪt dt z2 Ϫ t 2 aj ϩ j Ϫz22 e erfc͑Ϫiz2͒ ϭ w . ͱ2j fj p fj p2 ͐ exp Ϫ ϩϱ ͫ Ϫϱ ͑ x Ϫ j ͒2 2j2 d x. and some of the transition metals ͑Cr. ͑7. beryllium. Ti. 41. Au. Eqs. ͑aj Ϫ j ͒ Ϫ ͑ x Ϫ j ͒ Ϫϱ ͐ exp Ϫ ͬ (A4) By introducing t ϭ ͑ x Ϫ j ͒͑͌͞2j ͒ and z1 ϭ ͑aj Ϫ j ͒͑͌͞2j ͒. dt ϭ eϪz1 erfc͑Ϫiz1͒ ϭ w z1 Ϫ t i i ͱ2j (A5) 2 ͩ ͪ Using a similar approach. 16. Ni. ͑ x Ϫ 2͒ ϩ i⌫j We deﬁne aj2 ϭ 2 Ϫ i⌫j with Im͓aj ͔ Ͼ 0 and obtain j ͑͒ ϭ Ϫ Fig. 77. we ﬁnd that ͓see Ref.3͒ and ͑7.1 to 6 eV. Comparison with the measurements on surface normal structures conﬁrmed that the reﬂectance and the phase change on reﬂection from semiconductor–metal interfaces ͑including the case of metallic multilayers͒ can be accurately calculated by use of the proposed models for the optical functions of metals and the transfer matrix theory. Pd. 37. namely. ϩ ͐ exp Ϫ ϩϱ ͫ Ά͐ ͫ exp Ϫ ϩϱ ͫ Ϫϱ Ϫϱ ͑ x Ϫ j ͒2 2j2 dx . Measured and calculated reﬂectivity of metal clad ͑air– GaAs–Ti͞Au͒ and dielectric clad ͑air–GaAs–wax͒ F–P cavities: reﬂectance that we calculated using the transfer matrix method. We used two simple phenomenological models.1. Cu͒. No. In such a case it is physically justiﬁed and computationally simpler to employ a single Gaussian-like BB oscillator instead. aluminum. Although it is known that the optical constants of thick ﬁlms ͑bulk͒ can differ from the optical constants of thin metallic ﬁlms. and the growth process͒ to the ﬁlms used in optoelectronic devices. ͑4͒ in closed form. The integral to be solved is j ͑͒ ϭ ͱ2j ϫ 2 1 ͐ ͫ ϩϱ Ϫϱ exp Ϫ ͑ x Ϫ j ͒2 2j2 ͬ (A1) fj p2 d x. This is in accordance with our initial assumptions. unless a large number of oscillators were used to describe that transition. 22 ͞ APPLIED OPTICS . and W͒. the optical constants of evaporated ﬁlms still provide a good approximation. solid curves. morphology. the LD and the BB models to interpret both the freeelectron and the interband parts of the dielectric response of real metals in the wide spectral range from 0. aj ϩ x ͬ ͑ x Ϫ j ͒2 2j2 dx aj Ϫ x ͬ · (A3) Now the ﬁrst integral can be written as ͑ x Ϫ j ͒2 ϩϱ 2j2 I1 ϭ d x. Pt. trying always to use the measurements obtained on ﬁlms similar ͑in terms of geometry. a comprehensive parameterization of the optical functions for 11 metals for applications in optoelectronic and optical devices: noble metals ͑Ag. The LD model due to the extended absorption of the Lorentz oscillators can hardly describe a sharp absorption edge. For all the metals we carefully chose relevant optical data. dashed curves. Our results show that the BB model was needed for an appropriate description of the onset of interband absorption in noble metals ͑Ag. i i ͱ2j ͩ ͪ (A7) 5281 1 August 1998 ͞ Vol. and Cu͒. 2 aj Ϫ x2 ͬ (A2) 2 j ͑͒ ϭ Ϫ 2 ͱ2 aj j knowledge.1.
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