Fe intercalated TaS2 single crystals exhibit interesting domain patterns at room temperature with... more Fe intercalated TaS2 single crystals exhibit interesting domain patterns at room temperature with the concentration of 1/4 and 1/3. In this work, we measured the optical spectrum and Raman response of Fe1=4TaS2 and Fe1=3TaS2, and compared this data with the parent compound 2H-TaS2: The optical conductivity data indicates a strong free carrier response, and Fe intercalation induced both dd excitations and new phonon modes compared to the parent compound that are strongly related to the symmetry breaking of the parent compound. Our ndings were in good agreement with rst principle calculations.
The interplay between charge, structure, magnetism, and orbitals leads to rich physics and exotic... more The interplay between charge, structure, magnetism, and orbitals leads to rich physics and exotic cross-coupling in multifunctional materials. Superlattices provide a superb platform to study the complex interactions between different degrees of freedom. In this dissertation, I present a spectroscopic investigation of natural and engineered superlattices including FexTaS2 and (LuFeO3)m/(LuFe2O4)1 under external stimuli of temperature and magnetic field as well as chemical substitution. Studying the phase transitions, symmetry-breaking, and complex interface interactions from a microscopic viewpoint enhances fundamental understanding of coupling mechanism between different order parameters and the exciting properties. In FexTaS2, we use optical spectroscopies to analyze the electronic properties. Strikingly, Fe intercalation dramatically changes the metallic character, revealing two separate free carrier responses in the Fe monolayer and TaS2 slabs, respectively. Signatures of chiral...
Hafnia (HfO2) is a promising material for emerging chip applications due to its high-κ dielectric... more Hafnia (HfO2) is a promising material for emerging chip applications due to its high-κ dielectric behavior, suitability for negative capacitance heterostructures, scalable ferroelectricity, and silicon compatibility. The lattice dynamics along with phononic properties such as thermal conductivity, contraction, and heat capacity are under-explored, primarily due to the absence of high quality single crystals. Herein, we report the vibrational properties of a series of HfO2 crystals stabilized with yttrium (chemical formula HfO2: xY, where x = 20, 12, 11, 8, and 0%) and compare our findings with a symmetry analysis and lattice dynamics calculations. We untangle the effects of Y by testing our calculations against the measured Raman and infrared spectra of the cubic, antipolar orthorhombic, and monoclinic phases and then proceed to reveal the signature modes of polar orthorhombic hafnia. This work provides a spectroscopic fingerprint for several different phases of HfO2 and paves the w...
Ferroic materials are well known to exhibit heterogeneity in the form of domain walls. Understand... more Ferroic materials are well known to exhibit heterogeneity in the form of domain walls. Understanding the properties of these boundaries is crucial for controlling functionality with external stimuli and for realizing their potential for ultra-low power memory and logic devices as well as novel computing architectures. In this work, we employ synchrotron-based near-field infrared nano-spectroscopy to reveal the vibrational properties of ferroelastic (90$${}^{\circ }$$∘ ferroelectric) domain walls in the hybrid improper ferroelectric Ca$${}_{3}$$3Ti$${}_{2}$$2O$${}_{7}$$7. By locally mapping the Ti-O stretching and Ti-O-Ti bending modes, we reveal how structural order parameters rotate across a wall. Thus, we link observed near-field amplitude changes to underlying structural modulations and test ferroelectric switching models against real space measurements of local structure. This initiative opens the door to broadband infrared nano-imaging of heterogeneity in ferroics.
Hafnia (HfO2) is a promising material for emerging chip applications due to its high-k dielectric... more Hafnia (HfO2) is a promising material for emerging chip applications due to its high-k dielectric behaviour, suitability for negative capacitance heterostructures, scalable ferroelectricity, and silicon compatibility. The lattice dynamics along with phononic properties such as thermal conductivity, contraction, and heat capacity are under-explored, primarily due to the absence of high quality single crystals. Herein, we report the vibrational properties of a series of HfO2 crystals stabilized with yttrium (chemical formula HfO2:xY, where x = 20, 12, 11, 8, and 0%) and compare our findings with a symmetry analysis and lattice dynamics calculations. We untangle the effects of Y by testing our calculations against the measured Raman and infrared spectra of the cubic, antipolar orthorhombic, and monoclinic phases and then proceed to reveal the signature modes of polar orthorhombic hafnia. This work provides a spectroscopic fingerprint for several different phases of HfO2 and paves the w...
Interface materials offer a means to achieve electrical control of ferrimagnetism at room tempera... more Interface materials offer a means to achieve electrical control of ferrimagnetism at room temperature as was recently demonstrated in (LuFeO3)m/(LuFe2O4)1 superlattices. A challenge to understanding the inner workings of these complex magnetoelectric multiferroics is the multitude of distinct Fe centres and their associated environments. This is because macroscopic techniques characterize average responses rather than the role of individual iron centres. Here, we combine optical absorption, magnetic circular dichroism and first-principles calculations to uncover the origin of high-temperature magnetism in these superlattices and the charge-ordering pattern in the m = 3 member. In a significant conceptual advance, interface spectra establish how Lu-layer distortion selectively enhances the Fe2+ → Fe3+ charge-transfer contribution in the spin-up channel, strengthens the exchange interactions and increases the Curie temperature. Comparison of predicted and measured spectra also identi...
Fe intercalated TaS2 single crystals exhibit interesting domain patterns at room temperature with... more Fe intercalated TaS2 single crystals exhibit interesting domain patterns at room temperature with the concentration of 1/4 and 1/3. In this work, we measured the optical spectrum and Raman response of Fe1=4TaS2 and Fe1=3TaS2, and compared this data with the parent compound 2H-TaS2: The optical conductivity data indicates a strong free carrier response, and Fe intercalation induced both dd excitations and new phonon modes compared to the parent compound that are strongly related to the symmetry breaking of the parent compound. Our ndings were in good agreement with rst principle calculations.
The interplay between charge, structure, magnetism, and orbitals leads to rich physics and exotic... more The interplay between charge, structure, magnetism, and orbitals leads to rich physics and exotic cross-coupling in multifunctional materials. Superlattices provide a superb platform to study the complex interactions between different degrees of freedom. In this dissertation, I present a spectroscopic investigation of natural and engineered superlattices including FexTaS2 and (LuFeO3)m/(LuFe2O4)1 under external stimuli of temperature and magnetic field as well as chemical substitution. Studying the phase transitions, symmetry-breaking, and complex interface interactions from a microscopic viewpoint enhances fundamental understanding of coupling mechanism between different order parameters and the exciting properties. In FexTaS2, we use optical spectroscopies to analyze the electronic properties. Strikingly, Fe intercalation dramatically changes the metallic character, revealing two separate free carrier responses in the Fe monolayer and TaS2 slabs, respectively. Signatures of chiral...
Hafnia (HfO2) is a promising material for emerging chip applications due to its high-κ dielectric... more Hafnia (HfO2) is a promising material for emerging chip applications due to its high-κ dielectric behavior, suitability for negative capacitance heterostructures, scalable ferroelectricity, and silicon compatibility. The lattice dynamics along with phononic properties such as thermal conductivity, contraction, and heat capacity are under-explored, primarily due to the absence of high quality single crystals. Herein, we report the vibrational properties of a series of HfO2 crystals stabilized with yttrium (chemical formula HfO2: xY, where x = 20, 12, 11, 8, and 0%) and compare our findings with a symmetry analysis and lattice dynamics calculations. We untangle the effects of Y by testing our calculations against the measured Raman and infrared spectra of the cubic, antipolar orthorhombic, and monoclinic phases and then proceed to reveal the signature modes of polar orthorhombic hafnia. This work provides a spectroscopic fingerprint for several different phases of HfO2 and paves the w...
Ferroic materials are well known to exhibit heterogeneity in the form of domain walls. Understand... more Ferroic materials are well known to exhibit heterogeneity in the form of domain walls. Understanding the properties of these boundaries is crucial for controlling functionality with external stimuli and for realizing their potential for ultra-low power memory and logic devices as well as novel computing architectures. In this work, we employ synchrotron-based near-field infrared nano-spectroscopy to reveal the vibrational properties of ferroelastic (90$${}^{\circ }$$∘ ferroelectric) domain walls in the hybrid improper ferroelectric Ca$${}_{3}$$3Ti$${}_{2}$$2O$${}_{7}$$7. By locally mapping the Ti-O stretching and Ti-O-Ti bending modes, we reveal how structural order parameters rotate across a wall. Thus, we link observed near-field amplitude changes to underlying structural modulations and test ferroelectric switching models against real space measurements of local structure. This initiative opens the door to broadband infrared nano-imaging of heterogeneity in ferroics.
Hafnia (HfO2) is a promising material for emerging chip applications due to its high-k dielectric... more Hafnia (HfO2) is a promising material for emerging chip applications due to its high-k dielectric behaviour, suitability for negative capacitance heterostructures, scalable ferroelectricity, and silicon compatibility. The lattice dynamics along with phononic properties such as thermal conductivity, contraction, and heat capacity are under-explored, primarily due to the absence of high quality single crystals. Herein, we report the vibrational properties of a series of HfO2 crystals stabilized with yttrium (chemical formula HfO2:xY, where x = 20, 12, 11, 8, and 0%) and compare our findings with a symmetry analysis and lattice dynamics calculations. We untangle the effects of Y by testing our calculations against the measured Raman and infrared spectra of the cubic, antipolar orthorhombic, and monoclinic phases and then proceed to reveal the signature modes of polar orthorhombic hafnia. This work provides a spectroscopic fingerprint for several different phases of HfO2 and paves the w...
Interface materials offer a means to achieve electrical control of ferrimagnetism at room tempera... more Interface materials offer a means to achieve electrical control of ferrimagnetism at room temperature as was recently demonstrated in (LuFeO3)m/(LuFe2O4)1 superlattices. A challenge to understanding the inner workings of these complex magnetoelectric multiferroics is the multitude of distinct Fe centres and their associated environments. This is because macroscopic techniques characterize average responses rather than the role of individual iron centres. Here, we combine optical absorption, magnetic circular dichroism and first-principles calculations to uncover the origin of high-temperature magnetism in these superlattices and the charge-ordering pattern in the m = 3 member. In a significant conceptual advance, interface spectra establish how Lu-layer distortion selectively enhances the Fe2+ → Fe3+ charge-transfer contribution in the spin-up channel, strengthens the exchange interactions and increases the Curie temperature. Comparison of predicted and measured spectra also identi...
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