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Title: Structure and spectroscopy of Cr{sup 3+} defects in KMgF{sub 3}, KZnF{sub 3}, and CsCaF{sub 3} crystals. An ab initio model potential embedded cluster study

Abstract

The ab initio model potential (AIMP) method has been proven to produce effective one-electron operators that accurately represent the embedding effects of the cations and anions that constitute crystalline lattices like the KMgF{sub 3}, KZnF{sub 3}, and CsCaF{sub 3} cubic fluoroperovskites. The combination of these quantum mechanical embedding potentials with highly sophisticated molecular quantum chemical calculations of the CrF{sub 6}{sup 3{minus}} defect cluster enables theoretical study of the structure and spectroscopy of promising laser materials like the Cr{sup 3+}-doped KMgF{sub 3}, KZnF{sub 3}, and CsCaF{sub 3} crystals at the level of quality attainable in molecular quantum chemistry. The combination of the theoretical results with available experimental data [electron paramagnetic resonance (EPR), electron spin resonance (ESR), absorption, and emission spectra at ambient and high pressures] can contribute to clarifying the electronic structure of these systems, where the difficulty associated with the existence of cubic, trigonal, and tetragonal Cr{sup 3+} defects contributing to the spectra. The results of AIMP embedded-cluster studies of the cubic defects are presented here as one more useful and independent source of information that serves to clarify the divergent assignments and to provide new spectroscopic information, which shows that the laser emission of Cr{sub 3+} defects in allmore » three crystals should be free from excited state absorption losses if the pumping process is done through selective excitation to the {sup 4}T{sub 2g} laser level, below the {sup 2}E{sub g} higher excited state. Since the Cr{sup 3+} substitutional impurities create an excess positive charge, the effects of lattice site relaxation and dipole polarization on the local structure have been investigated and are presented here.« less

Authors:
; ;
Publication Date:
Research Org.:
Univ. Autonoma de Madrid (ES)
OSTI Identifier:
20020821
Alternate Identifier(s):
OSTI ID: 20020821
Resource Type:
Journal Article
Journal Name:
International Journal of Quantum Chemistry
Additional Journal Information:
Journal Volume: 77; Journal Issue: 6; Other Information: PBD: 5 May 2000; Journal ID: ISSN 0020-7608
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 42 ENGINEERING; CRYSTAL DEFECTS; POTASSIUM FLUORIDES; MAGNESIUM FLUORIDES; ZINC FLUORIDES; CESIUM FLUORIDES; CALCIUM FLUORIDES; CHROMIUM FLUORIDES; CRYSTAL LATTICES; LASER MATERIALS; DOPED MATERIALS; OPTICAL PROPERTIES

Citation Formats

Lopez-Moraza, S., Seijo, L., and Barandiaran, Z. Structure and spectroscopy of Cr{sup 3+} defects in KMgF{sub 3}, KZnF{sub 3}, and CsCaF{sub 3} crystals. An ab initio model potential embedded cluster study. United States: N. p., 2000. Web. doi:10.1002/(SICI)1097-461X(2000)77:6<961::AID-QUA4>3.0.CO;2-A.
Lopez-Moraza, S., Seijo, L., & Barandiaran, Z. Structure and spectroscopy of Cr{sup 3+} defects in KMgF{sub 3}, KZnF{sub 3}, and CsCaF{sub 3} crystals. An ab initio model potential embedded cluster study. United States. doi:10.1002/(SICI)1097-461X(2000)77:6<961::AID-QUA4>3.0.CO;2-A.
Lopez-Moraza, S., Seijo, L., and Barandiaran, Z. Fri . "Structure and spectroscopy of Cr{sup 3+} defects in KMgF{sub 3}, KZnF{sub 3}, and CsCaF{sub 3} crystals. An ab initio model potential embedded cluster study". United States. doi:10.1002/(SICI)1097-461X(2000)77:6<961::AID-QUA4>3.0.CO;2-A.
@article{osti_20020821,
title = {Structure and spectroscopy of Cr{sup 3+} defects in KMgF{sub 3}, KZnF{sub 3}, and CsCaF{sub 3} crystals. An ab initio model potential embedded cluster study},
author = {Lopez-Moraza, S. and Seijo, L. and Barandiaran, Z.},
abstractNote = {The ab initio model potential (AIMP) method has been proven to produce effective one-electron operators that accurately represent the embedding effects of the cations and anions that constitute crystalline lattices like the KMgF{sub 3}, KZnF{sub 3}, and CsCaF{sub 3} cubic fluoroperovskites. The combination of these quantum mechanical embedding potentials with highly sophisticated molecular quantum chemical calculations of the CrF{sub 6}{sup 3{minus}} defect cluster enables theoretical study of the structure and spectroscopy of promising laser materials like the Cr{sup 3+}-doped KMgF{sub 3}, KZnF{sub 3}, and CsCaF{sub 3} crystals at the level of quality attainable in molecular quantum chemistry. The combination of the theoretical results with available experimental data [electron paramagnetic resonance (EPR), electron spin resonance (ESR), absorption, and emission spectra at ambient and high pressures] can contribute to clarifying the electronic structure of these systems, where the difficulty associated with the existence of cubic, trigonal, and tetragonal Cr{sup 3+} defects contributing to the spectra. The results of AIMP embedded-cluster studies of the cubic defects are presented here as one more useful and independent source of information that serves to clarify the divergent assignments and to provide new spectroscopic information, which shows that the laser emission of Cr{sub 3+} defects in all three crystals should be free from excited state absorption losses if the pumping process is done through selective excitation to the {sup 4}T{sub 2g} laser level, below the {sup 2}E{sub g} higher excited state. Since the Cr{sup 3+} substitutional impurities create an excess positive charge, the effects of lattice site relaxation and dipole polarization on the local structure have been investigated and are presented here.},
doi = {10.1002/(SICI)1097-461X(2000)77:6<961::AID-QUA4>3.0.CO;2-A},
journal = {International Journal of Quantum Chemistry},
issn = {0020-7608},
number = 6,
volume = 77,
place = {United States},
year = {2000},
month = {5}
}