Andreas Stoffers
2018
Stoffers, Andreas; Liebscher, Christian H; Alam, Masud; Lymperakis, Liverios; Cojocaru-Mirédin, Oana; Gault, Baptiste; Neugebauer, Jörg; Dehm, Gerhard; Scheu, Christina; Raabe, Dierk
Strain-Induced Asymmetric Line Segregation at Faceted Si Grain Boundaries Journal Article
In: Physical Review Letters, vol. 121, no. 1, pp. 015702 (1-5), 2018.
@article{Stoffers2018,
title = {Strain-Induced Asymmetric Line Segregation at Faceted Si Grain Boundaries},
author = {Andreas Stoffers and Christian H Liebscher and Masud Alam and Liverios Lymperakis and Oana Cojocaru-Mirédin and Baptiste Gault and Jörg Neugebauer and Gerhard Dehm and Christina Scheu and Dierk Raabe},
doi = {10.1103/PhysRevLett.121.015702},
year = {2018},
date = {2018-07-06},
journal = {Physical Review Letters},
volume = {121},
number = {1},
pages = {015702 (1-5)},
abstract = {The unique combination of atomic-scale composition measurements, employing atom probe tomog-raphy, atomic structure determination with picometer resolution by aberration-corrected scanning transmission electron microscopy, and atomistic simulations reveals site-specific linear segregation features at grain boundary facet junctions. More specific, an asymmetric line segregation along one particular type of facet junction core, instead of a homogeneous decoration of the facet planes, is observed. Molecular-statics calculations show that this segregation pattern is a consequence of the interplay between the asymmetric core structure and its corresponding local strain state. Our results contrast with the classical view of a homogeneous decoration of the facet planes and evidence a complex segregation patterning.},
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The unique combination of atomic-scale composition measurements, employing atom probe tomog-raphy, atomic structure determination with picometer resolution by aberration-corrected scanning transmission electron microscopy, and atomistic simulations reveals site-specific linear segregation features at grain boundary facet junctions. More specific, an asymmetric line segregation along one particular type of facet junction core, instead of a homogeneous decoration of the facet planes, is observed. Molecular-statics calculations show that this segregation pattern is a consequence of the interplay between the asymmetric core structure and its corresponding local strain state. Our results contrast with the classical view of a homogeneous decoration of the facet planes and evidence a complex segregation patterning.
2017
Stoffers, Andreas; Yu, Yuan; He, Dong-Sheng; Zhang, Siyuan; Cojocaru-Mirédin, Oana; Schwarz, Torsten; Wang, Xiao-Yu; Zheng, Shuqi; Zhu, Bin; Scheu, Christina; Wu, Di; He, Jia-Qing; Wuttig, Matthias; Huang, Zhong-Yue; Zu, Fang-Qiu
Simultaneous optimization of electrical and thermal transport properties of Bi 0.5 Sb 1.5 Te 3 thermoelectric alloy by twin boundary engineering Journal Article
In: Nano Energy, vol. 37, pp. 203-213, 2017.
@article{Stoffers2017,
title = {Simultaneous optimization of electrical and thermal transport properties of Bi 0.5 Sb 1.5 Te 3 thermoelectric alloy by twin boundary engineering},
author = {Andreas Stoffers and Yuan Yu and Dong-Sheng He and Siyuan Zhang and Oana Cojocaru-Mirédin and Torsten Schwarz and Xiao-Yu Wang and Shuqi Zheng and Bin Zhu and Christina Scheu and Di Wu and Jia-Qing He and Matthias Wuttig and Zhong-Yue Huang and Fang-Qiu Zu},
doi = {10.1016/j.nanoen.2017.05.031},
year = {2017},
date = {2017-05-01},
journal = {Nano Energy},
volume = {37},
pages = {203-213},
abstract = {The strong interdependence between the Seebeck coefficient, the electrical and thermal conductivity makes it difficult to obtain a high thermoelectric figure of merit, ZT. It is of critical significance to design a novel structure that manages to decouple these parameters. Here, we combine a liquid state manipulation method for solidified Bi0.5Sb1.5Te3 alloy with subsequent melt spinning, ball milling, and spark plasma sintering processes, to construct dedicated microstructures containing plenty of 60° twin boundaries. These twin boundaries firstly scatter the very low-energy carriers and lead to an enhancement of the Seebeck coefficient. Secondly, they provide a considerable high carrier mobility, compensating the negative effect of the reduced hole concentration on the electrical conductivity. Thirdly, both experimental and calculated results demonstrate that the twin-boundary scattering dominates the conspicuous decrease of the lattice thermal conductivity. Consequently, the highest ZT value of 1.42 is achieved at 348 K, which is 27% higher than that of the sample with less twin boundary treated without liquid state manipulation. The average ZT value from 300 K to 400 K reaches 1.34. Our particular sample processing methods enabling the twin-dominant microstructure is an efficient avenue to simultaneously optimize the thermoelectric parameters.},
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pubstate = {published},
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The strong interdependence between the Seebeck coefficient, the electrical and thermal conductivity makes it difficult to obtain a high thermoelectric figure of merit, ZT. It is of critical significance to design a novel structure that manages to decouple these parameters. Here, we combine a liquid state manipulation method for solidified Bi0.5Sb1.5Te3 alloy with subsequent melt spinning, ball milling, and spark plasma sintering processes, to construct dedicated microstructures containing plenty of 60° twin boundaries. These twin boundaries firstly scatter the very low-energy carriers and lead to an enhancement of the Seebeck coefficient. Secondly, they provide a considerable high carrier mobility, compensating the negative effect of the reduced hole concentration on the electrical conductivity. Thirdly, both experimental and calculated results demonstrate that the twin-boundary scattering dominates the conspicuous decrease of the lattice thermal conductivity. Consequently, the highest ZT value of 1.42 is achieved at 348 K, which is 27% higher than that of the sample with less twin boundary treated without liquid state manipulation. The average ZT value from 300 K to 400 K reaches 1.34. Our particular sample processing methods enabling the twin-dominant microstructure is an efficient avenue to simultaneously optimize the thermoelectric parameters.
Stoffers, Andreas; Barthel, Juri; Liebscher, Christian H; Gault, Baptiste; Cojocaru-Mirédin, Oana; Scheu, Christina; Raabe, Dierk
In: Microscopy and microanalysis, vol. 23, no. 2, pp. 291-299, 2017.
@article{Stoffers2017b,
title = {Correlating Atom Probe Tomography with Atomic-Resolved Scanning Transmission Electron Microscopy: Example of Segregation at Silicon Grain Boundaries},
author = {Andreas Stoffers and Juri Barthel and Christian H Liebscher and Baptiste Gault and Oana Cojocaru-Mirédin and Christina Scheu and Dierk Raabe},
doi = {10.1017/S1431927617000034},
year = {2017},
date = {2017-02-20},
journal = {Microscopy and microanalysis},
volume = {23},
number = {2},
pages = {291-299},
abstract = {In the course of a thorough investigation of the performance-structure-chemistry interdependency at silicon grain boundaries, we successfully developed a method to systematically correlate aberration-corrected scanning transmission electron microscopy and atom probe tomography. The correlative approach is conducted on individual APT and TEM specimens, with the option to perform both investigations on the same specimen in the future. In the present case of a Σ9 grain boundary, joint mapping of the atomistic details of the grain boundary topology, in conjunction with chemical decoration, enables a deeper understanding of the segregation of impurities observed at such grain boundaries.},
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In the course of a thorough investigation of the performance-structure-chemistry interdependency at silicon grain boundaries, we successfully developed a method to systematically correlate aberration-corrected scanning transmission electron microscopy and atom probe tomography. The correlative approach is conducted on individual APT and TEM specimens, with the option to perform both investigations on the same specimen in the future. In the present case of a Σ9 grain boundary, joint mapping of the atomistic details of the grain boundary topology, in conjunction with chemical decoration, enables a deeper understanding of the segregation of impurities observed at such grain boundaries.
2016
Stoffers, Andreas; Liebscher, Christian; Choi, Pyuck ‐ Pa; Herbig, Michael; Scheu, Christina; Dehm, Gerhard; Povstugar, Ivan; Raabe, Dierk
Correlative atom probe tomography and electron microscopy on energy materials Book Chapter
In: pp. 778-779, Wiley ‐ VCH Verlag GmbH & Co. KGaA, 2016.
@inbook{Stoffers2016,
title = {Correlative atom probe tomography and electron microscopy on energy materials},
author = {Andreas Stoffers and Christian Liebscher and Pyuck ‐ Pa Choi and Michael Herbig and Christina Scheu and Gerhard Dehm and Ivan Povstugar and Dierk Raabe},
doi = {10.1002/9783527808465.EMC2016.4442},
year = {2016},
date = {2016-11-30},
pages = {778-779},
publisher = {Wiley ‐ VCH Verlag GmbH & Co. KGaA},
abstract = {We present recent progress in correlative methods for the joint analysis of samples by Atom Probe Tomography (LEAP 3000, LEAP 5000) and Electron Microscopy (Cs corrected Titan Themis). Measurements are conducted on the same Atom Probe sample tips and in some cases atomic resolution is reached. Examples from functional and structural energy-related materials are presented including segregation effects in multicrystalline silicon solar cells and their relation to cell efficiency (Fig. 1), superalloys for advanced turbines and high strength steels (Fig. 2).},
type = {inbook},
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We present recent progress in correlative methods for the joint analysis of samples by Atom Probe Tomography (LEAP 3000, LEAP 5000) and Electron Microscopy (Cs corrected Titan Themis). Measurements are conducted on the same Atom Probe sample tips and in some cases atomic resolution is reached. Examples from functional and structural energy-related materials are presented including segregation effects in multicrystalline silicon solar cells and their relation to cell efficiency (Fig. 1), superalloys for advanced turbines and high strength steels (Fig. 2).
Stoffers, Andreas; Liebscher, CH; Cojocaru-Mirédin, Oana; Gault, Baptiste; Scheu, Christina; Dehm, Gerhard; Raabe, Dierk
Topological Impurity Segregation at Faceted Silicon Grain Boundaries Studied by Correlative Atomic-Resolution STEM and APT Journal Article
In: Microscopy and Microanalysis, vol. 22, no. S5, pp. 46-47, 2016.
@article{Stoffers2016b,
title = {Topological Impurity Segregation at Faceted Silicon Grain Boundaries Studied by Correlative Atomic-Resolution STEM and APT},
author = {Andreas Stoffers and CH Liebscher and Oana Cojocaru-Mirédin and Baptiste Gault and Christina Scheu and Gerhard Dehm and Dierk Raabe},
doi = {10.1017/S1431927616012253},
year = {2016},
date = {2016-11-01},
journal = {Microscopy and Microanalysis},
volume = {22},
number = {S5},
pages = {46-47},
abstract = {Topological Impurity Segregation at Faceted Silicon Grain Boundaries Studied by Correlative Atomic-Resolution STEM and APT - Volume 22 Issue S5 - CH Liebscher, A Stoffers, O Cojocaru-Mirédin, B Gault, C Scheu, G Dehm, D Raabe},
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Topological Impurity Segregation at Faceted Silicon Grain Boundaries Studied by Correlative Atomic-Resolution STEM and APT - Volume 22 Issue S5 - CH Liebscher, A Stoffers, O Cojocaru-Mirédin, B Gault, C Scheu, G Dehm, D Raabe
2015
Stoffers, Andreas; Ziebarth, Benedikt; Barthel, Juri; Cojocaru-Mirédin, Oana; Elsässer, Christian; Raabe, Dierk
Complex Nanotwin Substructure of an Asymmetric Σ9 Tilt Grain Boundary in a Silicon Polycrystal Journal Article
In: Physical review letters, vol. 115, no. 23, pp. 235502, 2015.
@article{Stoffers2015,
title = {Complex Nanotwin Substructure of an Asymmetric Σ9 Tilt Grain Boundary in a Silicon Polycrystal},
author = {Andreas Stoffers and Benedikt Ziebarth and Juri Barthel and Oana Cojocaru-Mirédin and Christian Elsässer and Dierk Raabe},
doi = {10.1103/PhysRevLett.115.235502},
year = {2015},
date = {2015-12-02},
journal = {Physical review letters},
volume = {115},
number = {23},
pages = {235502},
abstract = {Grain boundaries in materials have substantial influences on device properties, for instance on mechanical stability or electronic minority carrier lifetime in multicrystalline silicon solar cells. This applies especially to asymmetric, less ordered or faceted interface portions. Here, we present the complex atomic interface structure of an asymmetric Σ9 tilt grain boundary in silicon, observed by high resolution scanning transmission electron microscopy (HR-STEM) and explained by atomistic modeling and computer simulation. Structural optimization of interface models for the asymmetric Σ9 and related symmetrical Σ9 and Σ3 tilt grain boundaries, by means of molecular-statics simulations with empirical silicon potentials in combination with first-principles calculations, results in a faceted asymmetric interface structure, whose grain-boundary energy is so low that it is likely to exist. The simulated local atomic structures match the observed HR-STEM images very well.},
keywords = {},
pubstate = {published},
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Grain boundaries in materials have substantial influences on device properties, for instance on mechanical stability or electronic minority carrier lifetime in multicrystalline silicon solar cells. This applies especially to asymmetric, less ordered or faceted interface portions. Here, we present the complex atomic interface structure of an asymmetric Σ9 tilt grain boundary in silicon, observed by high resolution scanning transmission electron microscopy (HR-STEM) and explained by atomistic modeling and computer simulation. Structural optimization of interface models for the asymmetric Σ9 and related symmetrical Σ9 and Σ3 tilt grain boundaries, by means of molecular-statics simulations with empirical silicon potentials in combination with first-principles calculations, results in a faceted asymmetric interface structure, whose grain-boundary energy is so low that it is likely to exist. The simulated local atomic structures match the observed HR-STEM images very well.
Stoffers, Andreas; Ziebarth, Benedikt; Barthel, Juri; Cojocaru-Mirédin, Oana; Elsässer, Christian; Raabe, Dierk
Complex Nanotwin Substructure of an Asymmetric Σ9 Tilt Grain Boundary in a Silicon Polycrystal Journal Article
In: Physical review letters, vol. 115, no. 23, pp. 235502, 2015.
@article{Stoffers2015bb,
title = {Complex Nanotwin Substructure of an Asymmetric Σ9 Tilt Grain Boundary in a Silicon Polycrystal},
author = {Andreas Stoffers and Benedikt Ziebarth and Juri Barthel and Oana Cojocaru-Mirédin and Christian Elsässer and Dierk Raabe},
year = {2015},
date = {2015-12-02},
journal = {Physical review letters},
volume = {115},
number = {23},
pages = {235502},
abstract = {Grain boundaries in materials have substantial influences on device properties, for instance on mechanical stability or electronic minority carrier lifetime in multicrystalline silicon solar cells. This applies especially to asymmetric, less ordered or faceted interface portions. Here, we present the complex atomic interface structure of an asymmetric Σ9 tilt grain boundary in silicon, observed by high resolution scanning transmission electron microscopy (HR-STEM) and explained by atomistic modeling and computer simulation. Structural optimization of interface models for the asymmetric Σ9 and related symmetrical Σ9 and Σ3 tilt grain boundaries, by means of molecular-statics simulations with empirical silicon potentials in combination with first-principles calculations, results in a faceted asymmetric interface structure, whose grain-boundary energy is so low that it is likely to exist. The simulated local atomic structures match the observed HR-STEM images very well.},
keywords = {},
pubstate = {published},
tppubtype = {article}
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Grain boundaries in materials have substantial influences on device properties, for instance on mechanical stability or electronic minority carrier lifetime in multicrystalline silicon solar cells. This applies especially to asymmetric, less ordered or faceted interface portions. Here, we present the complex atomic interface structure of an asymmetric Σ9 tilt grain boundary in silicon, observed by high resolution scanning transmission electron microscopy (HR-STEM) and explained by atomistic modeling and computer simulation. Structural optimization of interface models for the asymmetric Σ9 and related symmetrical Σ9 and Σ3 tilt grain boundaries, by means of molecular-statics simulations with empirical silicon potentials in combination with first-principles calculations, results in a faceted asymmetric interface structure, whose grain-boundary energy is so low that it is likely to exist. The simulated local atomic structures match the observed HR-STEM images very well.
Stoffers, Andreas; Mirédin, Oana Cojocaru ‐; Seifert, Winfried; Zaefferer, Stefan; Riepe, Stephan; Raabe, Dierk
Grain boundary segregation in multicrystalline silicon: Correlative characterization by EBSD, EBIC, and atom probe tomography Journal Article
In: Progress in Photovoltaics: Research and Applications, vol. 23, no. 12, pp. 1742-1753, 2015.
@article{Stoffers2015b,
title = {Grain boundary segregation in multicrystalline silicon: Correlative characterization by EBSD, EBIC, and atom probe tomography},
author = {Andreas Stoffers and Oana Cojocaru ‐ Mirédin and Winfried Seifert and Stefan Zaefferer and Stephan Riepe and Dierk Raabe},
doi = {10.1002/pip.2614},
year = {2015},
date = {2015-05-01},
journal = {Progress in Photovoltaics: Research and Applications},
volume = {23},
number = {12},
pages = {1742-1753},
abstract = {This study aims to better understand the influence of crystallographic structure and impurity decoration on the recombination activity at grain boundaries in multicrystalline silicon. A sample of the upper part of a multicrystalline silicon ingot with intentional addition of iron and copper has been investigated. Correlative electron-beam-induced current, electron backscatter diffraction, and atom probe tomography data for different types of grain boundaries are presented. For a symmetric coherent Σ3 twin boundary, with very low recombination activity, no impurities are detected. In case of a noncoherent (random) high-angle grain boundary and higher order twins with pronounced recombination activity, carbon and oxygen impurities are observed to decorate the interface. Copper contamination is detected for the boundary with the highest recombination activity in this study, a random high-angle grain boundary located in the vicinity of a triple junction. The 3D atom probe tomography study presented here is the first direct atomic scale identification and quantification of impurities decorating grain boundaries in multicrystalline silicon. The observed deviations in chemical decoration and induced current could be directly linked with different crystallographic structures of silicon grain boundaries. Hence, the current work establishes a direct correlation between grain boundary structure, atomic scale segregation information, and electrical activity. It can help to identify interface–property relationships for silicon interfaces that enable grain boundary engineering in multicrystalline silicon.},
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pubstate = {published},
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This study aims to better understand the influence of crystallographic structure and impurity decoration on the recombination activity at grain boundaries in multicrystalline silicon. A sample of the upper part of a multicrystalline silicon ingot with intentional addition of iron and copper has been investigated. Correlative electron-beam-induced current, electron backscatter diffraction, and atom probe tomography data for different types of grain boundaries are presented. For a symmetric coherent Σ3 twin boundary, with very low recombination activity, no impurities are detected. In case of a noncoherent (random) high-angle grain boundary and higher order twins with pronounced recombination activity, carbon and oxygen impurities are observed to decorate the interface. Copper contamination is detected for the boundary with the highest recombination activity in this study, a random high-angle grain boundary located in the vicinity of a triple junction. The 3D atom probe tomography study presented here is the first direct atomic scale identification and quantification of impurities decorating grain boundaries in multicrystalline silicon. The observed deviations in chemical decoration and induced current could be directly linked with different crystallographic structures of silicon grain boundaries. Hence, the current work establishes a direct correlation between grain boundary structure, atomic scale segregation information, and electrical activity. It can help to identify interface–property relationships for silicon interfaces that enable grain boundary engineering in multicrystalline silicon.
2014
Stoffers, Andreas; Cojocaru-Mirédin, Oana; Breitenstein, Otwin; Seifert, Winfried; Zaefferer, Stefan; Raabe, Dierk
2014 IEEE 40th Photovoltaic Specialist Conference (PVSC), IEEE, 2014.
@conference{Stoffers2014,
title = {Grain boundary characterization in multicrystalline silicon using joint EBSD, EBIC, and atom probe tomography},
author = {Andreas Stoffers and Oana Cojocaru-Mirédin and Otwin Breitenstein and Winfried Seifert and Stefan Zaefferer and Dierk Raabe},
doi = {10.1109/PVSC.2014.6925089},
year = {2014},
date = {2014-06-09},
booktitle = {2014 IEEE 40th Photovoltaic Specialist Conference (PVSC)},
pages = {0042-0046},
publisher = {IEEE},
abstract = {The efficiency of multicrystalline silicon solar cells suffers from the presence of extended defects like dislocations and grain boundaries. In fact, the defects themselves do not implicitly have to be harmful, but their interaction with impurities makes them detrimental for the cell efficiencies. Here, we present a systematic method to correlate the grain boundary charge recombination activity with local grain boundary properties and the site specific segregation information. For that, electron beam induced current is used to characterize the recombination activity at the grain boundaries, while electron backscatter diffraction is used to map the grain boundary crystallography. Atom probe tips containing the desired grain boundary are cut by using a novel site-specific sample preparation. Finally, atom probe tomography is used to reveal the 3D distribution of the impurities at the selected grain boundary. In conclusion, this work is one of the first studies based on understanding the correlation between the charge recombination activity and structural as well as chemical properties at grain boundaries in multicrystalline silicon solar cells.},
keywords = {},
pubstate = {published},
tppubtype = {conference}
}
The efficiency of multicrystalline silicon solar cells suffers from the presence of extended defects like dislocations and grain boundaries. In fact, the defects themselves do not implicitly have to be harmful, but their interaction with impurities makes them detrimental for the cell efficiencies. Here, we present a systematic method to correlate the grain boundary charge recombination activity with local grain boundary properties and the site specific segregation information. For that, electron beam induced current is used to characterize the recombination activity at the grain boundaries, while electron backscatter diffraction is used to map the grain boundary crystallography. Atom probe tips containing the desired grain boundary are cut by using a novel site-specific sample preparation. Finally, atom probe tomography is used to reveal the 3D distribution of the impurities at the selected grain boundary. In conclusion, this work is one of the first studies based on understanding the correlation between the charge recombination activity and structural as well as chemical properties at grain boundaries in multicrystalline silicon solar cells.
2011
Stoffers, Andreas; Oberdorfer, Christian; Schmitz, Guido
Controlled Field Evaporation of Fluorinated Self-Assembled Monolayers Journal Article
In: Langmuir : the ACS journal of surfaces and colloids, vol. 28, no. 1, pp. 56-59, 2011.
@article{Stoffers2011,
title = {Controlled Field Evaporation of Fluorinated Self-Assembled Monolayers},
author = {Andreas Stoffers and Christian Oberdorfer and Guido Schmitz},
doi = {10.1021/la204126x},
year = {2011},
date = {2011-12-02},
journal = {Langmuir : the ACS journal of surfaces and colloids},
volume = {28},
number = {1},
pages = {56-59},
abstract = {Self-assembled monolayers of amino-undecanethiol and perfluoro-decanethiol are studied by atom probe tomography based on laser-assisted controlled field desorption. In the case of hydrogenated chains the identification of detected molecular species is difficult because of residual hydrocarbons. By contrast, fractions of the fluorinated chains can be unequivocally identified. Although chemically similar, the evaporation of both chains appears in significantly different molecular fractions. For the fluorinated chains, a well-ordered evaporation sequence is determined that allows conclusions to be drawn about the strength of bonds under field conditions and may lay the basis for the future numerical reconstruction of the chemical structure of such films.},
keywords = {},
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Self-assembled monolayers of amino-undecanethiol and perfluoro-decanethiol are studied by atom probe tomography based on laser-assisted controlled field desorption. In the case of hydrogenated chains the identification of detected molecular species is difficult because of residual hydrocarbons. By contrast, fractions of the fluorinated chains can be unequivocally identified. Although chemically similar, the evaporation of both chains appears in significantly different molecular fractions. For the fluorinated chains, a well-ordered evaporation sequence is determined that allows conclusions to be drawn about the strength of bonds under field conditions and may lay the basis for the future numerical reconstruction of the chemical structure of such films.