Nonlinear optical spectroscopy of epitaxial magnetic garnet films

Nonlinear optical spectroscopy of epitaxial magnetic garnet films

Second and third harmonic optical spectra are studied in epitaxial magnetic thin films in the spectral ranges 1.7-3.2 eV and 2.4-4.2 eV, respectively. No significant increase of the intensity of the nonlinear spectra is found above the bandgap near 3.2 eV, where the linear absorption increases by tw...

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Дата:2002
Автори: Pavlov, V.V., Pisarev, R.V., Fiebig, M., Fröhlich, D.
Формат: Стаття
Мова:English
Опубліковано: Фізико-технічний інститут низьких температур ім. Б.І. Вєркіна НАН України 2002
Назва видання:Физика низких температур
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Магнетизм
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Цитувати:Nonlinear optical spectroscopy of epitaxial magnetic garnet films / V.V. Pavlov, R.V. Pisarev, M.Fiebig D. Fröhlich // Физика низких температур. — 2002. — Т. 28, № 7. — С. 733-738. — Бібліогр.: 20 назв. — англ.

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spelling irk-123456789-1302282018-02-10T03:04:25Z Nonlinear optical spectroscopy of epitaxial magnetic garnet films Pavlov, V.V. Pisarev, R.V. Fiebig, M. Fröhlich, D. Магнетизм Second and third harmonic optical spectra are studied in epitaxial magnetic thin films in the spectral ranges 1.7-3.2 eV and 2.4-4.2 eV, respectively. No significant increase of the intensity of the nonlinear spectra is found above the bandgap near 3.2 eV, where the linear absorption increases by two orders of magnitude. Large magnetic contributions to the second harmonic spectra and magnetic contrast as high as 100% are observed at selected photon energies. Contrary to that, no magnetic contribution to the third harmonic spectra is found. 2002 Article Nonlinear optical spectroscopy of epitaxial magnetic garnet films / V.V. Pavlov, R.V. Pisarev, M.Fiebig D. Fröhlich // Физика низких температур. — 2002. — Т. 28, № 7. — С. 733-738. — Бібліогр.: 20 назв. — англ. 0132-6414 PACS: 78.20.-e, 42.65.Ky, 75.50.Gg http://dspace.nbuv.gov.ua/handle/123456789/130228 en Физика низких температур Фізико-технічний інститут низьких температур ім. Б.І. Вєркіна НАН України
institution Digital Library of Periodicals of National Academy of Sciences of Ukraine
collection DSpace DC
language English
topic Магнетизм
Магнетизм
spellingShingle Магнетизм
Магнетизм
Pavlov, V.V.
Pisarev, R.V.
Fiebig, M.
Fröhlich, D.
Nonlinear optical spectroscopy of epitaxial magnetic garnet films
Физика низких температур
description Second and third harmonic optical spectra are studied in epitaxial magnetic thin films in the spectral ranges 1.7-3.2 eV and 2.4-4.2 eV, respectively. No significant increase of the intensity of the nonlinear spectra is found above the bandgap near 3.2 eV, where the linear absorption increases by two orders of magnitude. Large magnetic contributions to the second harmonic spectra and magnetic contrast as high as 100% are observed at selected photon energies. Contrary to that, no magnetic contribution to the third harmonic spectra is found.
format Article
author Pavlov, V.V.
Pisarev, R.V.
Fiebig, M.
Fröhlich, D.
author_facet Pavlov, V.V.
Pisarev, R.V.
Fiebig, M.
Fröhlich, D.
author_sort Pavlov, V.V.
title Nonlinear optical spectroscopy of epitaxial magnetic garnet films
title_short Nonlinear optical spectroscopy of epitaxial magnetic garnet films
title_full Nonlinear optical spectroscopy of epitaxial magnetic garnet films
title_fullStr Nonlinear optical spectroscopy of epitaxial magnetic garnet films
title_full_unstemmed Nonlinear optical spectroscopy of epitaxial magnetic garnet films
title_sort nonlinear optical spectroscopy of epitaxial magnetic garnet films
publisher Фізико-технічний інститут низьких температур ім. Б.І. Вєркіна НАН України
publishDate 2002
topic_facet Магнетизм
url http://dspace.nbuv.gov.ua/handle/123456789/130228
citation_txt Nonlinear optical spectroscopy of epitaxial magnetic garnet films / V.V. Pavlov, R.V. Pisarev, M.Fiebig D. Fröhlich // Физика низких температур. — 2002. — Т. 28, № 7. — С. 733-738. — Бібліогр.: 20 назв. — англ.
series Физика низких температур
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AT frohlichd nonlinearopticalspectroscopyofepitaxialmagneticgarnetfilms
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fulltext Fizika Nizkikh Temperatur, 2002, v. 28, No. 7, p. 733 –738 Nonlinear optical spectroscopy of epitaxial magnetic garnet films V. V. Pavlov and R. V. Pisarev A. F. Ioffe Physical Technical Institute of the Russian Academy of Sciences, St. Petersburg, 194021 Russia E-mail: pisarev@pop.ioffe.rssi.ru M. Fiebig and D. Fröhlich Institut für Physik, Universität Dortmund, 44221 Dortmund, Germany Received February 1, 2002 Second and third harmonic optical spectra are studied in epitaxial magnetic thin films in the spectral ranges 1.7–3.2 eV and 2.4–4.2 eV, respectively. No significant increase of the in- tensity of the nonlinear spectra is found above the bandgap near 3.2 eV, where the linear ab- sorption increases by two orders of magnitude. Large magnetic contributions to the second harmonic spectra and magnetic contrast as high as 100% are observed at selected photon ener- gies. Contrary to that, no magnetic contribution to the third harmonic spectra is found. PACS: 78.20.–e, 42.65.Ky, 75.50.Gg 1. Introduction Bulk magnetic garnets and epitaxial magnetic garnet films are two well-known groups of materi- als characterized by a large variety of very useful magnetic, acoustic, optical, and magneto-optical properties [1–4]. For more than four decades they have remained one of the most actively studied magnetic dielectrics, both from the fundamental point of view as multi-sublattice ferrimagnets and for the purpose of technological applications. The prototype material of bulk crystals and thin films is yttrium iron garnet { [ ] ( )Y} Fe Fe O3 122 3 (YIG). The unit cell contains eight formula units. The rare-earth ions R3� enter 24c dodecahedral posi- tions 8 3{...} , while the Fe3� ions enter 16a octahe- dral positions 8 2[...] and 24d tetrahedral positions 8 3(...) . The superexchange interaction between the magnetic Fe3� ions leads to antiparallel ferrimag- netic ordering of the magnetic moments of the octa- hedral and tetrahedral iron sublattices. This strong interaction leads to a Curie temperature in the range of TC � 500–600 K. The superexchange inter- action between the rare-earth magnetic ions and the iron sublattices leads to an antiparallel orientation of the rare-earth magnetic moments with respect to the magnetization of the tetrahedral sublattice. A remarkable feature of magnetic garnets is the possi- bility of substituting ions in all three magnetic sublattices by many other magnetic and nonmag- netic ions from the periodic table of the elements. This degree of freedom allows one to vary practi- cally all of the physical properties of bulk crystals and epitaxial films over a very wide range. The magnetic iron garnets are highly transparent in the near infrared range 0.2–1.0 eV [5]. At lower energy the absorption rapidly increases due to lattice vibrations. The absorption increases progressively at photon energies higher than about 1 eV due to the intrinsic localized electronic transitions between the ( )3 5d levels of the Fe3� ions and, subsequently, above 3.2 eV due to intense charge-transfer and interband transitions, finally approaching absorp- tion coefficients as high as 5 105 1� �cm above 5 eV [6]. The linear magneto-optical properties of gar- nets, and in particular bismuth-substituted garnets, have attracted a lot of interest due to the fact that very high values of the specific Faraday rotation up to 105 deg/cm were observed at room temperature. To our knowledge, these values are probably the highest ever observed at room temperature due to a spontaneous magnetization. © V. V. Pavlov, R. V. Pisarev, M. Fiebig, and D. Fröhlich, 2002 Bulk crystals of magnetic garnets belong to the centrosymmetric cubic point group m3m (space group Ia3d). In the thin films, however, the obser- vation of a linear magneto-electric effect proved that the inversion symmetry is broken [7]. This is related to the fact that the films, which are grown by a liquid-phase epitaxial method on substrates cut from bulk cubic crystals of gadolinium gallium garnet Gd Ga O3 5 12 (GGG) or substituted GGG (SGGG), possess a lattice parameter different from that of the substrate, which leads to a distorted noncubic crystal structure. Previous studies of sec- ond harmonic generation (SHG) in magnetic garnet films were restricted to a few selected photon ener- gies determined by the pump lasers, such as 1.17 eV (Nd:YAG lasers) or ~� 1.5 eV (Ti–sapphire lasers) [8]. Though breaking of inversion is not important in the analysis of the magnetic properties, it plays an essential role for the electro-optical and nonli- near optical properties. In particular, it allows crystallographic and the magnetic contributions to SHG in the electric dipole approximation. Obvi- ously, studies at selected photon energies could not clarify relations between observed SHG signals and particular features of electronic structure, absorp- tion spectra and magneto-optical spectra. In the present paper we report first results on a spectro- scopic study of SHG and third harmonic generation (THG) in magnetic garnet films below and above the fundamental band gap near 3.2 eV. 2. Electronic transitions in iron garnets Optical absorption and reflection spectra of con- centrated and diluted iron garnets have been studied in a large number of publications and the most im- portant data are summarized in Ref. 4. In spite of numerous publications along these lines, the assign- ments of spectral features remain doubtful in most cases due to the complexity of the spectra. Experi- mental data and crystal field calculations are sum- marized in Fig. 1. In its middle part Fig. 1 shows experimentally observed transition energies in YIG as reported in several papers [5,6,9–15]. The elec- tronic structure of iron garnets has been a subject of calculations based on crystal field theory and molecular orbital theory [5,9,14,16–18]. The left panels of Fig. 1 show the localized states of the Fe3� ions in the tetrahedral and octahedral sub- lattices. These states are given according to crystal field calculations which take into account tetra- gonal distortions in the tetrahedral sublattice and trigonal distortions in the octahedral sublattice [18].The calculations show that the relevant split- tings and shifts of the electronic states may of the order of 0.5 eV and therefore comparable to the splitting of the states in the cubic crystal fields of Td and Oh symmetry. Below the band gap the electronic transitions could be studied by transmission methods based on optical and magneto-optical techniques, whereas for transitions above the band gap of � 3.2 eV re- flection methods are in general more favorable [9,11,12]. With the use of very thin YIG films (t = = 0.26 �m) absorption spectra could be obtained up to 5.0 eV [6]. It should be noticed that all optical transitions between the localized states of the Fe3� ions are spin-forbidden. In addition, the transitions in the octahedral sublattice are parity-forbidden in the electric-dipole approximation and become al- lowed due to interaction with odd phonons. Optical absorption of YIG in the near infrared spectral range commences at about 1.2 eV and is due to the localized electronic transition 6 1 4 1A Tg g� between the ( )3 5d levels of the Fe3� ions in the octahedral sublattice. This transition is magnetic-dipole-allowed and leads to two very 734 Fizika Nizkikh Temperatur, 2002, v. 28, No. 7 V. V. Pavlov, R. V. Pisarev, M. Fiebig, and D. Fröhlich Tetrahedral calculated Absorption observed Octahedral calculated � � �� � � � � � � � � g � �g � � � �g g � � g � g � � g � � � g � ��g � g � �g � �� � � � � � 0 1 2 3 4 5 �� � �� 6 Pump THGSHG P h o to n e n e rg y, e V Fig. 1. The two columns on the left show the crystal field energy states of the Fe3+ ion in the distorted tetra- hedral and octahedral positions in the garnet structure. The column in the middle shows the experimentally ob- served electronic transitions and the continuous absorp- tion at higher photon energy. The right part of the fi- gure shows the energy range of the pump beam and that of the SH and TH spectra. weak absorption lines [10]. It is readily seen from Fig. 1 that at higher energy the transitions in the octahedral and the tetrahedral sublattices are over- lapping, so that the unambiguous assignment of the states becomes difficult. In fact, the experimentally observed spectrum of YIG is characterized by a more complicated structure than expected from the- ory even if the case of very low symmetries is taken into account. Aside from their dependence on the cubic and noncubic crystal field parameters, the po- sitions of the electronic levels are also subject to several other parameters, such as the intra-atomic interaction parameters, spin–orbit coupling, ex- change interaction, etc. In strongly correlated sys- tems like iron garnets, paired transitions may lead to additional absorption bands in the optical spec- tra. For example, absorption bands in the spectral range around 2.5 eV are at least in part due to paired transitions. These factors, being sometimes of comparable magnitude or not exactly known, complicate the unique assignment of optical absorp- tion bands. Low-temperature optical and mag- neto-optical studies resolve the splittings of the transitions, revealing a rather complicated ener- gy-level structure. The exact position of the band gap remains not well defined and is usually assumed to lie near 3.2–3.4 eV, where the absorption coefficient of YIG starts to increase more rapidly, approaching values of � � � �5 105 1cm above 5 eV [6]. This ab- sorption value is typical for interband transitions in transition-metal oxides. The substitution of Bi3� for Y3� in iron garnets leads to a shift of the strong absorption edge to lower energy and to a huge in- crease of magneto-optical effects in the visible and ultraviolet spectral range. The suggested micro- scopic mechanisms of the enhanced magneto-optical Faraday and Kerr effects are assumed to originate in an increase of the spin–orbit interaction due to the formation of a molecular orbit between the 3d orbitals of the Fe3� ions and the 2p orbitals of O2�. This is further mixed with the 6p orbitals of Bi3� , which has a large spin–orbit interaction coefficient. A recent analysis shows that the most important electronic transitions responsible for the Faraday rotation in bismuth-substituted garnets lie at 2.6, 3.15, and 3.9 eV [19]. 3. Experiment In the present study we used thin films of mag- netic garnets grown by a liquid-phase epitaxial method. Films were grown on transparent nonmag- netic substrates cut from bulk cubic crystals of ga- dolinium gallium garnet Gd Ga O3 5 12 or substituted GGG. The films were grown on substrates with the four different orientations (001), (110), (111), and (210) and differed in their compositions, lattice pa- rameters, and thicknesses [8]. Optical absorption spectra were measured using a Cary 2300 spec- trophotometer and were found to be in agreement with published data. Absorption spectra measured at T = 15 K in three films are shown in Fig. 2. Op- tical densities higher than D = 4.5 are above the working range of the spectrophotometer and could not be measured. The setup for the SHG and THG experiments is shown in Fig. 3. A Nd: YAG laser system and a �-BaB O2 4 operated optical parametric oscillator Fizika Nizkikh Temperatur, 2002, v. 28, No. 7 735 Nonlinear optical spectroscopy of epitaxial magnetic garnet films � � � O p ti c a l d e n s it y , Fig. 2. Optical absorption spectra in the three garnet films studied in the paper. The films differ in their com- positions and thicknesses. Optical densities higher than D = 4.5 are out of the range of the spectrophotometer and could therefore not be measured. WP Lens F Lens Analyzer F OPO Mono- chromator Reference Idler Glan Prism Reference Lens EM S M M M M Fig. 3. Transmission setup for SH/TH spectroscopy. SHG/THG: second harmonic/third harmonic genera- tion; OPO: optical parametric oscillator; WP: wave plate; F: filter; S: sample; EM: electromagnet; PM: photomultiplier; PC: personal computer; M: mirror. (OPO) were used as the light source, the perfor- mance of which was monitored with a wavemeter. The pulse energy was measured for normalizing the observed SH and TH intensities. For proper nor- malization it was necessary to measure the absorp- tion of the fundamental beam by placing a pho- todiode behind the sample, since in all samples the absorption varies strongly as function of the photon energy. Wave plates, polarizers, and optical filters were used to set the polarization of the fundamen- tal light, analyze the polarization of the SH and TH light, and separate the fundamental light from the SH and TH light behind the sample. In some cases, a monochromator was included in the setup in order to exclude the possibility of two-photon luminescence contributions to the observed signals. By a telephoto lens the signal light was projected on a cooled CCD camera or a photomultiplier. The data were corrected for the spectral response of the filters and the detection system. The magnetic con- trast was determined from the normalized differ- ence between the SH intensity for opposite orienta- tions of the saturating transverse magnetic field. 4. Nonlinear optical susceptibilities In magnetically ordered materials the relation between the induced polarization P and the electric field E( )� of the fundamental beam in the electric dipole approximation can be written as P = E E E E E E � � � � � � � � � � 0 1 2 3 ( � � � ( ) ( ) ( ) ( ) + + ( ) ( ) + + ( ) ( ) ( )...). (1) In the electric-dipole approximation, odd tensors � ( )� 1 , � ( )� 3 , ... are allowed in all media, whereas even tensors � ( )� 2 , � ( )� 4 , ... are allowed only in noncentro- symmetric media. For crystals with a spontaneous or a magnetic-field-induced magnetization M the optical susceptibility tensors contain crystallogra- phic (nonmagnetic) contributions and magnetic contributions: � � � ( )� � �n m� �cr M . (2) The intensity of SH and TH signals can be written as I E M I E m( ) | � ( ; , ) � ( ; , , ) | , ( ) 2 2 2 0 3 0 4 2 0 � � � � � � � � � � � � � � � cr 6 23 3 0| � ( ; , , ) � ( ; , , , ) | ,� � � � � � � � � �cr � � �m M (3) V. V. Pavlov, R. V. Pisarev, M. Fiebig, and D. Fröhlich 736 Fizika Nizkikh Temperatur, 2002, v. 28, No. 7 � S H in te n s it y a rb . u n it s . � � , , Fig. 4. SH spectra in the YIG/GGG(111) film for op- posite orientations of the transverse magnetic field. The upper and lower panels depict SH spectra for two sides of the film. Table Nonzero components of the nonlinear optical tensors � ijkl cr and � ijklm m relevant for the point group 3m m x( )� in the geometry k z| | (films of (111) type) �ijkl cr �ijklm m 1 3 1 3 yyyy xxxx xxyy yxxy� � � yyyyx yxyyy yxxyx, , xxxxx yyyyx yxyyy yxxyx� � � � 1 2 1 2 xxxyy yyyyx yxxyx� � 1 2 1 2 xxyyx yyyyx yxyyy yxxyx� � � � 1 2 1 2 xyyyy yyyyx yxxyx� � 1 2 yxxxy yyyyx yxyyy yxxyx� � � yxyyz xxxyz xyyyz yxxxz� � � � � 1 3 1 3 where the crystallographic and magnetic contri- butions are described by polar tensors ��cr and axial tensors �� m , respectively. The sign � refers to the opposite projections of the magnetization M. The symmetry properties of the tensors ��cr and �� m are strictly defined by the crystallographic point group. Nonzero components of ��cr and �� m are given in Ref. 8 for SHG and in Table for THG for the case of 3m symmetry. If nonlinear optical waves of crystallographic and magnetic origin are both present, their interference will lead to different SH and TH intensities for opposite orientations of the magnetization and thus to a magnetic contrast between oppositely magnetized regions. 5. Experimental results and discussion Figure 4 shows the SH spectra in a YIG/GGG (111) film for two opposite orientations of the mag- netization M in transverse geometry. The upper and lower panels show the results for the two cases with the SH signal being emitted directly from the free film surface (film-to-photodetector case) and from the surface of the film attached to the sub- strate (film-to-laser case). The two geometries lead to different SH spectra. In particular, a split transi- tion near 2.4 eV is well resolved for the free film surface and smeared out for the more strained sur- face attached to the substrate. Note that magnetic contrast varies from 0 to 100%. According to the energy level diagram in Fig. 1, some features in the SH spectrum can be assigned to the crystal-field transitions in the two iron sublattices. Two other sharp absorption features near 2.57 eV (presumably due to the 6 1 4 4 1A E A� , transition in the tetra- hedral sublattice) and 2.66 eV (presumably due to the 6 1 4 4 1A E A� , transition in the octahedral sub- lattice) are also observed in the SH spectrum. Two more spectral features in the absorption spectrum are observed at 2.9 and 3.2 eV, with oscillator strengths an order of magnitude higher than those for the tetrahedral transitions. However, the rele- vant features in the SH spectrum are of the same order of magnitude as for the transitions with the lower optical absorption. Figure 5 shows the SH spectra of a bismuth- substituted Bi-YIG/SGGG(210) film. As a rule bismuth-substituted films show the strongest SH signals [8]. The present sample was studied in a spectral range beginning at 1.7 eV and at low tem- perature T = 6 K. It shows a well-resolved structure with five strong bands of varying magnetic con- trast. We note that the spectra for two sides of the film are different, as it was the case for the YIG/GGG(111) film. As in the previous case, the increase of the linear optical absorption does not lead to a noticeable increase of the SH intensity. Figure 6 shows the third harmonic spectra in the three magnetic films. Note that even in the elec- Fizika Nizkikh Temperatur, 2002, v. 28, No. 7 737 Nonlinear optical spectroscopy of epitaxial magnetic garnet films � � � S H in te n s it y , a rb . u n it s , Fig. 5. SH spectra in the Bi-YIG/SGGG(210) film. T H in te n s it y , a rb . u n it s T = 293 K YIG/GGG(111) Bi-YIG/GGG(111) Bi-YIG/SGGG(210) TH energy, eV 4.23.83.43.02.6 0 1 2 0 1 2 0 1 2 3 Fig. 6. TH spectra in YIG/GGG(111), Bi-YIG/GGG(111), and Bi-YIG/SGGG(210) films. tric-dipole approximation a breaking of space inver- sion symmetry is not required for the observation of a TH signal. Although the optical absorption and the magnitudes of the linear magneto-optical sig- nals are very different in the three films, their third harmonic spectra are similar. The tetrahedral tran- sition 6 1 4 2A T� centered near 2.4 eV is well re- solved in the TH spectrum, and in particular in the YIG/GGG(111) film. Note that the strong in- crease of the linear absorption above 3 eV is not ac- companied by a similar increase of the TH spectra. Contrary to the SH spectra, no difference in the TH spectra is observed within the experimental ac- curacy upon a reorientation of the magnetization or upon a variation of the magnetic field. This is sur- prising, because according to a phenomenological analysis a magnetic contribution to the THG is al- lowed both in the longitudinal and transverse ge- ometries. In conclusion, the SH spectra of various aniso- tropic magnetic garnet films were measured in a range of photon energies stretching from 1.7–3.2 eV and thus, below the fundamental band gap at � 3.2 eV. The spectra revealed contributions of nonmagnetic and magnetic type to the total SH intensity. We also report the TH spectra in the range of 2.4–4.2 eV and thus, below and above the band gap. No studies along these lines for the mag- netic transition-metal oxides have been reported so far with the only recent exception of third har- monic spectroscopy of La CuO2 4 [20]. While the intensity of linear absorption grows progressively as a function of photon energy, the intensity of the SH and TH spectra does not show a similar beha- vior. We may assume that this is due to the fact that only localized d–d transitions contribute to the nonlinear spectra, with the relevant contribu- tion vanishing for charge-transfer and interband transitions. A very interesting and puzzling result is the observation of a very large magnetic contribu- tion to the SH spectra with a magnetic contrast of up to 100%. By contrast, no magnetic contribution is found in the TH spectra. All these observations demonstrate a strong necessity for further experi- mental and theoretical studies of nonlinear optical properties of magnetic garnet materials. 6. Acknowledgments This work was supported by the Deutsche For- schungsgemeinschaft, the Russian Foundation for Basic Research, and the Alexander-von-Hum- boldt-Stiftung. We thank H.-J. Weber for the help in optical absorption measurements. 1. Physics of Magnetic Garnets, A. Paoletti (ed.), North Holland, Amsterdam (1978). 2. G. Winkler, Magnetic garnets, Vieweg, Braun- schweig (1981). 3. 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