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- Creators: Tongay, Sefaattin
Description
Carbon nanomaterials have caught tremendous attention in the last few decades due to their unique physical and chemical properties. Tremendous effort has been made to develop new synthesis techniques for carbon nanomaterials and investigate their properties for different applications. In this work, carbon nanospheres (CNSs), carbon foams (CF), and single-walled carbon nanotubes (SWNTs) were studied for various applications, including water treatment, energy storage, actuators, and sensors.
A facile spray pyrolysis synthesis technique was developed to synthesize individual CNSs with specific surface area (SSA) up to 1106 m2/g. The hollow CNSs showed adsorption of up to 300 mg rhodamine B dye per gram carbon, which is more than 15 times higher than that observed for conventional carbon black. They were also evaluated as adsorbents for removal of arsenate and selenate from water and displayed good binding to both species, outperforming commercial activated carbons for arsenate removal in pH > 8. When evaluated as supercapacitor electrode materials, specific capacitances of up to 112 F/g at a current density of 0.1 A/g were observed. When used as Li-ion battery anode materials, the CNSs achieved a discharge capacity of 270 mAh/g at a current density of 372 mA/g (1C), which is 4-fold higher than that of commercial graphite anode.
Carbon foams were synthesized using direct pyrolysis and had SSA up to 2340 m2/g. When used as supercapacitor electrode materials, a specific capacitance up to 280 F/g was achieved at current density of 0.1 A/g and remained as high as 207 F/g, even at a high current density of 10 A/g.
A printed walking robot was made from common plastic films and coatings of SWNTs. The solid-state thermal bimorph actuators were multifunctional energy transducers powered by heat, light, or electricity. The actuators were also investigated for photo/thermal detection. Electrochemical actuators based on MnO2 were also studied for potential underwater applications.
SWNTs were also used to fabricate printable electrodes for trace Cr(VI) detection, which displayed sensitivity up to 500 nA/ppb for Cr(VI). The limit of detection was shown to be as low as 5 ppb. A flow detection system based on CNT/printed electrodes was also demonstrated.
A facile spray pyrolysis synthesis technique was developed to synthesize individual CNSs with specific surface area (SSA) up to 1106 m2/g. The hollow CNSs showed adsorption of up to 300 mg rhodamine B dye per gram carbon, which is more than 15 times higher than that observed for conventional carbon black. They were also evaluated as adsorbents for removal of arsenate and selenate from water and displayed good binding to both species, outperforming commercial activated carbons for arsenate removal in pH > 8. When evaluated as supercapacitor electrode materials, specific capacitances of up to 112 F/g at a current density of 0.1 A/g were observed. When used as Li-ion battery anode materials, the CNSs achieved a discharge capacity of 270 mAh/g at a current density of 372 mA/g (1C), which is 4-fold higher than that of commercial graphite anode.
Carbon foams were synthesized using direct pyrolysis and had SSA up to 2340 m2/g. When used as supercapacitor electrode materials, a specific capacitance up to 280 F/g was achieved at current density of 0.1 A/g and remained as high as 207 F/g, even at a high current density of 10 A/g.
A printed walking robot was made from common plastic films and coatings of SWNTs. The solid-state thermal bimorph actuators were multifunctional energy transducers powered by heat, light, or electricity. The actuators were also investigated for photo/thermal detection. Electrochemical actuators based on MnO2 were also studied for potential underwater applications.
SWNTs were also used to fabricate printable electrodes for trace Cr(VI) detection, which displayed sensitivity up to 500 nA/ppb for Cr(VI). The limit of detection was shown to be as low as 5 ppb. A flow detection system based on CNT/printed electrodes was also demonstrated.
ContributorsWang, Chengwei, Ph.D (Author) / Chan, Candace K. (Thesis advisor) / Tongay, Sefaattin (Committee member) / Wang, Qing Hua (Committee member) / Seo, Dong (Committee member) / Arizona State University (Publisher)
Created2015
Description
Since the discovery of graphene, two dimensional materials (2D materials) have become a focus of interest for material research due to their many unique physical properties embedded in their 2D structure. While they host many exciting potential applications, some of these 2D materials are subject to environmental instability issues induced by interaction between material and gas molecules in air, which poses a barrier to further application and manufacture. To overcome this, it is necessary to understand the origin of material instability and interaction with molecules commonly found in air, as well as developing a reproducible and manufacturing compatible method to post-process these materials to extend their lifetime. In this work, the very first investigation on environmental stability on Te containing anisotropic 2D materials such as GaTe and ZrTe3 is reported. Experimental results have demonstrated that freshly exfoliated GaTe quickly deteriorate in air, during which the Raman spectrum, surface morphology, and surface chemistry undergo drastic changes. Environmental Raman spectroscopy and XPS measurements demonstrate that H2O molecules in air interact strongly on the surface while O2, N2, and inert gases don't show any detrimental effects on GaTe surface. Moreover, the anisotropic properties of GaTe slowly disappear during the aging process. To prevent this gas/material interaction based surface transformation, diazonium based surface functionalization is adopted on these Te based 2D materials. Environmental Raman spectroscopy results demonstrate that the stability of functionalized Te based 2D materials exhibit much higher stability both in ambient and extreme conditions. Meanwhile, PL spectroscopy, angle resolved Raman spectroscopy, atomic force microscopy measurements confirm that many attractive physical properties of the material are not affected by surface functionalization. Overall, these findings unveil the degradation mechanism of Te based 2D materials as well as provide a way to significantly enhance their environmental stability through an inexpensive and reproducible surface chemical functionalization route.
ContributorsYang, Sijie (Author) / Tongay, Sefaattin (Thesis advisor) / Gould, Ian (Thesis advisor) / Trovitch, Ryan (Committee member) / Ghirlanda, Giovanna (Committee member) / Arizona State University (Publisher)
Created2017
Description
The world population is aging. Age-related disorders such as stroke and spinal cord injury are increasing rapidly, and such patients often suffer from mobility impairment. Wearable robotic exoskeletons are developed that serve as rehabilitation devices for these patients. In this thesis, a knee exoskeleton design with higher torque output compared to the first version, is designed and fabricated.
A series elastic actuator is one of the many actuation mechanisms employed in exoskeletons. In this mechanism a torsion spring is used between the actuator and human joint. It serves as torque sensor and energy buffer, making it compact and
safe.
A version of knee exoskeleton was developed using the SEA mechanism. It uses worm gear and spur gear combination to amplify the assistive torque generated from the DC motor. It weighs 1.57 kg and provides a maximum assistive torque of 11.26 N·m. It can be used as a rehabilitation device for patients affected with knee joint impairment.
A new version of exoskeleton design is proposed as an improvement over the first version. It consists of components such as brushless DC motor and planetary gear that are selected to meet the design requirements and biomechanical considerations. All the other components such as bevel gear and torsion spring are selected to be compatible with the exoskeleton. The frame of the exoskeleton is modeled in SolidWorks to be modular and easy to assemble. It is fabricated using sheet metal aluminum. It is designed to provide a maximum assistive torque of 23 N·m, two times over the present exoskeleton. A simple brace is 3D printed, making it easy to wear and use. It weighs 2.4 kg.
The exoskeleton is equipped with encoders that are used to measure spring deflection and motor angle. They act as sensors for precise control of the exoskeleton.
An impedance-based control is implemented using NI MyRIO, a FPGA based controller. The motor is controlled using a motor driver and powered using an external battery source. The bench tests and walking tests are presented. The new version of exoskeleton is compared with first version and state of the art devices.
A series elastic actuator is one of the many actuation mechanisms employed in exoskeletons. In this mechanism a torsion spring is used between the actuator and human joint. It serves as torque sensor and energy buffer, making it compact and
safe.
A version of knee exoskeleton was developed using the SEA mechanism. It uses worm gear and spur gear combination to amplify the assistive torque generated from the DC motor. It weighs 1.57 kg and provides a maximum assistive torque of 11.26 N·m. It can be used as a rehabilitation device for patients affected with knee joint impairment.
A new version of exoskeleton design is proposed as an improvement over the first version. It consists of components such as brushless DC motor and planetary gear that are selected to meet the design requirements and biomechanical considerations. All the other components such as bevel gear and torsion spring are selected to be compatible with the exoskeleton. The frame of the exoskeleton is modeled in SolidWorks to be modular and easy to assemble. It is fabricated using sheet metal aluminum. It is designed to provide a maximum assistive torque of 23 N·m, two times over the present exoskeleton. A simple brace is 3D printed, making it easy to wear and use. It weighs 2.4 kg.
The exoskeleton is equipped with encoders that are used to measure spring deflection and motor angle. They act as sensors for precise control of the exoskeleton.
An impedance-based control is implemented using NI MyRIO, a FPGA based controller. The motor is controlled using a motor driver and powered using an external battery source. The bench tests and walking tests are presented. The new version of exoskeleton is compared with first version and state of the art devices.
ContributorsJhawar, Vaibhav (Author) / Zhang, Wenlong (Thesis advisor) / Sugar, Thomas G. (Committee member) / Lee, Hyunglae (Committee member) / Marvi, Hamidreza (Committee member) / Arizona State University (Publisher)
Created2018
Description
There has been a surge in two-dimensional (2D) materials field since the discovery of graphene in 2004. Recently, a new class of layered atomically thin materials that exhibit in-plane structural anisotropy, such as black phosphorous, transition metal trichalcogenides and rhenium dichalcogenides (ReS2), have attracted great attention. The reduced symmetry in these novel 2D materials gives rise to highly anisotropic physical properties that enable unique applications in next-gen electronics and optoelectronics. For example, higher carrier mobility along one preferential crystal direction for anisotropic field effect transistors and anisotropic photon absorption for polarization-sensitive photodetectors.
This dissertation endeavors to address two key challenges towards practical application of anisotropic materials. One is the scalable production of high quality 2D anisotropic thin films, and the other is the controllability over anisotropy present in synthesized crystals. The investigation is focused primarily on rhenium disulfide because of its chemical similarity to conventional 2D transition metal dichalcogenides and yet anisotropic nature. Carefully designed vapor phase deposition has been demonstrated effective for batch synthesis of high quality ReS2 monolayer. Heteroepitaxial growth proves to be a feasible route for controlling anisotropic directions. Scanning/transmission electron microscopy and angle-resolved Raman spectroscopy have been extensively applied to reveal the structure-property relationship in synthesized 2D anisotropic layers and their heterostructures.
This dissertation endeavors to address two key challenges towards practical application of anisotropic materials. One is the scalable production of high quality 2D anisotropic thin films, and the other is the controllability over anisotropy present in synthesized crystals. The investigation is focused primarily on rhenium disulfide because of its chemical similarity to conventional 2D transition metal dichalcogenides and yet anisotropic nature. Carefully designed vapor phase deposition has been demonstrated effective for batch synthesis of high quality ReS2 monolayer. Heteroepitaxial growth proves to be a feasible route for controlling anisotropic directions. Scanning/transmission electron microscopy and angle-resolved Raman spectroscopy have been extensively applied to reveal the structure-property relationship in synthesized 2D anisotropic layers and their heterostructures.
ContributorsChen, Bin, 1968- (Author) / Tongay, Sefaattin (Thesis advisor) / Bertoni, Mariana (Committee member) / Chang, Lan-Yun (Committee member) / Arizona State University (Publisher)
Created2018
Description
Layer structured two dimensional (2D) semiconductors have gained much interest due to their intriguing optical and electronic properties induced by the unique van der Waals bonding between layers. The extraordinary success for graphene and transition metal dichalcogenides (TMDCs) has triggered a constant search for novel 2D semiconductors beyond them. Gallium chalcogenides, belonging to the group III-VI compounds, are a new class of 2D semiconductors that carry a variety of interesting properties including wide spectrum coverage of their bandgaps and thus are promising candidates for next generation electronic and optoelectronic devices. Pushing these materials toward applications requires more controllable synthesis methods and facile routes for engineering their properties on demand.
In this dissertation, vapor phase transport is used to synthesize layer structured gallium chalcogenide nanomaterials with highly controlled structure, morphology and properties, with particular emphasis on GaSe, GaTe and GaSeTe alloys. Multiple routes are used to manipulate the physical properties of these materials including strain engineering, defect engineering and phase engineering. First, 2D GaSe with controlled morphologies is synthesized on Si(111) substrates and the bandgap is significantly reduced from 2 eV to 1.7 eV due to lateral tensile strain. By applying vertical compressive strain using a diamond anvil cell, the band gap can be further reduced to 1.4 eV. Next, pseudo-1D GaTe nanomaterials with a monoclinic structure are synthesized on various substrates. The product exhibits highly anisotropic atomic structure and properties characterized by high-resolution transmission electron microscopy and angle resolved Raman and photoluminescence (PL) spectroscopy. Multiple sharp PL emissions below the bandgap are found due to defects localized at the edges and grain boundaries. Finally, layer structured GaSe1-xTex alloys across the full composition range are synthesized on GaAs(111) substrates. Results show that GaAs(111) substrate plays an essential role in stabilizing the metastable single-phase alloys within the miscibility gaps. A hexagonal to monoclinic phase crossover is observed as the Te content increases. The phase crossover features coexistence of both phases and isotropic to anisotropic structural transition.
Overall, this work provides insights into the controlled synthesis of gallium chalcogenides and opens up new opportunities towards optoelectronic applications that require tunable material properties.
In this dissertation, vapor phase transport is used to synthesize layer structured gallium chalcogenide nanomaterials with highly controlled structure, morphology and properties, with particular emphasis on GaSe, GaTe and GaSeTe alloys. Multiple routes are used to manipulate the physical properties of these materials including strain engineering, defect engineering and phase engineering. First, 2D GaSe with controlled morphologies is synthesized on Si(111) substrates and the bandgap is significantly reduced from 2 eV to 1.7 eV due to lateral tensile strain. By applying vertical compressive strain using a diamond anvil cell, the band gap can be further reduced to 1.4 eV. Next, pseudo-1D GaTe nanomaterials with a monoclinic structure are synthesized on various substrates. The product exhibits highly anisotropic atomic structure and properties characterized by high-resolution transmission electron microscopy and angle resolved Raman and photoluminescence (PL) spectroscopy. Multiple sharp PL emissions below the bandgap are found due to defects localized at the edges and grain boundaries. Finally, layer structured GaSe1-xTex alloys across the full composition range are synthesized on GaAs(111) substrates. Results show that GaAs(111) substrate plays an essential role in stabilizing the metastable single-phase alloys within the miscibility gaps. A hexagonal to monoclinic phase crossover is observed as the Te content increases. The phase crossover features coexistence of both phases and isotropic to anisotropic structural transition.
Overall, this work provides insights into the controlled synthesis of gallium chalcogenides and opens up new opportunities towards optoelectronic applications that require tunable material properties.
ContributorsCai, Hui, Ph.D (Author) / Tongay, Sefaattin (Thesis advisor) / Dwyer, Christian (Committee member) / Zhuang, Houlong (Committee member) / Arizona State University (Publisher)
Created2018
Description
Wearable robotics has gained huge popularity in recent years due to its wide applications in rehabilitation, military, and industrial fields. The weakness of the skeletal muscles in the aging population and neurological injuries such as stroke and spinal cord injuries seriously limit the abilities of these individuals to perform daily activities. Therefore, there is an increasing attention in the development of wearable robots to assist the elderly and patients with disabilities for motion assistance and rehabilitation. In military and industrial sectors, wearable robots can increase the productivity of workers and soldiers. It is important for the wearable robots to maintain smooth interaction with the user while evolving in complex environments with minimum effort from the user. Therefore, the recognition of the user's activities such as walking or jogging in real time becomes essential to provide appropriate assistance based on the activity.
This dissertation proposes two real-time human activity recognition algorithms intelligent fuzzy inference (IFI) algorithm and Amplitude omega ($A \omega$) algorithm to identify the human activities, i.e., stationary and locomotion activities. The IFI algorithm uses knee angle and ground contact forces (GCFs) measurements from four inertial measurement units (IMUs) and a pair of smart shoes. Whereas, the $A \omega$ algorithm is based on thigh angle measurements from a single IMU.
This dissertation also attempts to address the problem of online tuning of virtual impedance for an assistive robot based on real-time gait and activity measurement data to personalize the assistance for different users. An automatic impedance tuning (AIT) approach is presented for a knee assistive device (KAD) in which the IFI algorithm is used for real-time activity measurements. This dissertation also proposes an adaptive oscillator method known as amplitude omega adaptive oscillator ($A\omega AO$) method for HeSA (hip exoskeleton for superior augmentation) to provide bilateral hip assistance during human locomotion activities. The $A \omega$ algorithm is integrated into the adaptive oscillator method to make the approach robust for different locomotion activities. Experiments are performed on healthy subjects to validate the efficacy of the human activities recognition algorithms and control strategies proposed in this dissertation. Both the activity recognition algorithms exhibited higher classification accuracy with less update time. The results of AIT demonstrated that the KAD assistive torque was smoother and EMG signal of Vastus Medialis is reduced, compared to constant impedance and finite state machine approaches. The $A\omega AO$ method showed real-time learning of the locomotion activities signals for three healthy subjects while wearing HeSA. To understand the influence of the assistive devices on the inherent dynamic gait stability of the human, stability analysis is performed. For this, the stability metrics derived from dynamical systems theory are used to evaluate unilateral knee assistance applied to the healthy participants.
This dissertation proposes two real-time human activity recognition algorithms intelligent fuzzy inference (IFI) algorithm and Amplitude omega ($A \omega$) algorithm to identify the human activities, i.e., stationary and locomotion activities. The IFI algorithm uses knee angle and ground contact forces (GCFs) measurements from four inertial measurement units (IMUs) and a pair of smart shoes. Whereas, the $A \omega$ algorithm is based on thigh angle measurements from a single IMU.
This dissertation also attempts to address the problem of online tuning of virtual impedance for an assistive robot based on real-time gait and activity measurement data to personalize the assistance for different users. An automatic impedance tuning (AIT) approach is presented for a knee assistive device (KAD) in which the IFI algorithm is used for real-time activity measurements. This dissertation also proposes an adaptive oscillator method known as amplitude omega adaptive oscillator ($A\omega AO$) method for HeSA (hip exoskeleton for superior augmentation) to provide bilateral hip assistance during human locomotion activities. The $A \omega$ algorithm is integrated into the adaptive oscillator method to make the approach robust for different locomotion activities. Experiments are performed on healthy subjects to validate the efficacy of the human activities recognition algorithms and control strategies proposed in this dissertation. Both the activity recognition algorithms exhibited higher classification accuracy with less update time. The results of AIT demonstrated that the KAD assistive torque was smoother and EMG signal of Vastus Medialis is reduced, compared to constant impedance and finite state machine approaches. The $A\omega AO$ method showed real-time learning of the locomotion activities signals for three healthy subjects while wearing HeSA. To understand the influence of the assistive devices on the inherent dynamic gait stability of the human, stability analysis is performed. For this, the stability metrics derived from dynamical systems theory are used to evaluate unilateral knee assistance applied to the healthy participants.
ContributorsChinimilli, Prudhvi Tej (Author) / Redkar, Sangram (Thesis advisor) / Zhang, Wenlong (Thesis advisor) / Sugar, Thomas G. (Committee member) / Lee, Hyunglae (Committee member) / Marvi, Hamidreza (Committee member) / Arizona State University (Publisher)
Created2018
Description
Lower-limb wearable assistive robots could alter the users gait kinematics by inputting external power, which can be interpreted as mechanical perturbation to subject normal gait. The change in kinematics may affect the dynamic stability. This work attempts to understand the effects of different physical assistance from these robots on the gait dynamic stability.
A knee exoskeleton and ankle assistive device (Robotic Shoe) are developed and used to provide walking assistance. The knee exoskeleton provides personalized knee joint assistive torque during the stance phase. The robotic shoe is a light-weighted mechanism that can store the potential energy at heel strike and release it by using an active locking mechanism at the terminal stance phase to provide push-up ankle torque and assist the toe-off. Lower-limb Kinematic time series data are collected for subjects wearing these devices in the passive and active mode. The changes of kinematics with and without these devices on lower-limb motion are first studied. Orbital stability, as one of the commonly used measure to quantify gait stability through calculating Floquet Multipliers (FM), is employed to asses the effects of these wearable devices on gait stability. It is shown that wearing the passive knee exoskeleton causes less orbitally stable gait for users, while the knee joint active assistance improves the orbital stability compared to passive mode. The robotic shoe only affects the targeted joint (right ankle) kinematics, and wearing the passive mechanism significantly increases the ankle joint FM values, which indicates less walking orbital stability. More analysis is done on a mechanically perturbed walking public data set, to show that orbital stability can quantify the effects of external mechanical perturbation on gait dynamic stability. This method can further be used as a control design tool to ensure gait stability for users of lower-limb assistive devices.
A knee exoskeleton and ankle assistive device (Robotic Shoe) are developed and used to provide walking assistance. The knee exoskeleton provides personalized knee joint assistive torque during the stance phase. The robotic shoe is a light-weighted mechanism that can store the potential energy at heel strike and release it by using an active locking mechanism at the terminal stance phase to provide push-up ankle torque and assist the toe-off. Lower-limb Kinematic time series data are collected for subjects wearing these devices in the passive and active mode. The changes of kinematics with and without these devices on lower-limb motion are first studied. Orbital stability, as one of the commonly used measure to quantify gait stability through calculating Floquet Multipliers (FM), is employed to asses the effects of these wearable devices on gait stability. It is shown that wearing the passive knee exoskeleton causes less orbitally stable gait for users, while the knee joint active assistance improves the orbital stability compared to passive mode. The robotic shoe only affects the targeted joint (right ankle) kinematics, and wearing the passive mechanism significantly increases the ankle joint FM values, which indicates less walking orbital stability. More analysis is done on a mechanically perturbed walking public data set, to show that orbital stability can quantify the effects of external mechanical perturbation on gait dynamic stability. This method can further be used as a control design tool to ensure gait stability for users of lower-limb assistive devices.
ContributorsRezayat Sorkhabadi, Seyed Mostafa (Author) / Zhang, Wenlong (Thesis advisor) / Lee, Hyunglae (Committee member) / Artemiadis, Panagiotis (Committee member) / Arizona State University (Publisher)
Created2018
Description
Solid-state lithium-ion batteries are a major area of research due to their increased safety characteristics over conventional liquid electrolyte batteries. Lithium lanthanum zirconate (LLZO) is a promising garnet-type ceramic for use as a solid-state electrolyte due to its high ionic conductivity. The material exists in two dierent phases, one that is cubic in structure and one that is tetragonal. One potential synthesis method that results in LLZO in the more useful, cubic phase, is electrospinning, where a mat of nanowires is spun and then calcined into LLZO. A phase containing lanthanum zirconate (LZO) and amorphous lithium occursas an intermediate during the calcination process. LZO has been shown to be a sintering aid for LLZO, allowing for lower sintering temperatures. Here it is shown the eects of internal LZO on the sintered pellets. This is done by varying the 700C calcination time to transform diering amounts of LZO and LLZO in electrospun nanowires, and then using the same sintering parameters for each sample. X-ray diraction was used to get structural and compositional analysis of both the calcined powders and sintered pellets. Pellets formed from wires calcined at 1 hour or longer contained only LLZO even if the calcined powder had only undergone the rst phase transformation. The relative density of the pellet with no initial LLZO of 61.0% was higher than that of the pellet with no LZO, which had a relative density of 57.7%. This allows for the same, or slightly higher, quality material to be synthesized with a shorter amount of processing time.
ContributorsLondon, Nathan Harry (Author) / Chan, Candace (Thesis director) / Tongay, Sefaattin (Committee member) / Department of Physics (Contributor) / Materials Science and Engineering Program (Contributor) / Barrett, The Honors College (Contributor)
Created2017-05
Description
Prosthetic sockets are a static interface for dynamic residual limbs. As the user's activity level increases, the volume of the residual limb decreases by up to 11% and increases by as much as 7% after activity. Currently, volume fluctuation is addressed by adding/removing prosthetic socks to change the profile of the residual limb. However, this is time consuming. These painful/functional issues demand a prosthetic socket with an adjustable interface that can adapt to the user's needs. This thesis presents a prototype design for a dynamic soft robotic interface which addresses this need. The actuators are adjustable depending on the user's activity level, and their structure provides targeted compression to the soft tissue which helps to limit movement of the bone relative to the socket. The engineering process was used to create this design by defining system level requirements, exploring the design space, selecting a design, and then using testing/analysis to optimize that design. The final design for the soft robotic interface meets the applicable requirements, while other requirements for the electronics/controls will be completed as future work. Testing of the prototype demonstrated promising potential for the design with further refinement. Work on this project should be continued in future research/thesis projects in order to create a viable consumer product which can improve lower limb amputee's quality of life.
ContributorsHolmes, Breanna Swift (Author) / Zhang, Wenlong (Thesis director) / Polygerinos, Panagiotis (Committee member) / Mechanical and Aerospace Engineering Program (Contributor) / Barrett, The Honors College (Contributor)
Created2018-05
Description
This thesis presents systematic studies on angle dependent Raman and Photoluminescence (PL) of a new class of layered materials, Transition Metal Trichalcogenides (TMTCs), which are made up of layers possessing anisotropic structure within the van-der-Waals plane. The crystal structure of individual layer of MX3 compounds consists of aligned nanowire like 1D chains running along the b-axis direction. The work focuses on the growth of two members of this family - ZrS3 and TiS3 - through Chemical Vapor Transport Method (CVT), with consequent angle dependent Raman and PL studies which highlight their in-plane optically anisotropic properties. Results highlight that the optical properties of few-layer flakes are highly anisotropic as evidenced by large PL intensity variation with polarization direction (in ZrS3) and an intense variation in Raman intensity with variation in polarization direction (in both ZrS3 and TiS3).
Results suggest that light is efficiently absorbed when E-field of the polarized incident excitation laser is polarized along the chain (b-axis). It is greatly attenuated and absorption is reduced when field is polarized perpendicular to the length of 1D-like chains, as wavelength of the exciting light is much longer than the width of each 1D chain. Observed PL variation with respect to the azimuthal flake angle is similar to what has been previously observed in 1D materials like nanowires. However, in TMTCs, since the 1D chains interact with each other, it gives rise to a unique linear dichroism response that falls between 2D and 1D like behavior. These results not only mark the very first demonstration of high PL polarization anisotropy in 2D systems, but also provide a novel insight into how interaction between adjacent 1D-like chains and the 2D nature of each layer influences the overall optical anisotropy of Quasi-1D materials. The presented results are anticipated to have impact in technologies involving polarized detection, near-field imaging, communication systems, and bio-applications relying on the generation and detection of polarized light.
Results suggest that light is efficiently absorbed when E-field of the polarized incident excitation laser is polarized along the chain (b-axis). It is greatly attenuated and absorption is reduced when field is polarized perpendicular to the length of 1D-like chains, as wavelength of the exciting light is much longer than the width of each 1D chain. Observed PL variation with respect to the azimuthal flake angle is similar to what has been previously observed in 1D materials like nanowires. However, in TMTCs, since the 1D chains interact with each other, it gives rise to a unique linear dichroism response that falls between 2D and 1D like behavior. These results not only mark the very first demonstration of high PL polarization anisotropy in 2D systems, but also provide a novel insight into how interaction between adjacent 1D-like chains and the 2D nature of each layer influences the overall optical anisotropy of Quasi-1D materials. The presented results are anticipated to have impact in technologies involving polarized detection, near-field imaging, communication systems, and bio-applications relying on the generation and detection of polarized light.
ContributorsPant, Anupum (Author) / Tongay, Sefaattin (Thesis advisor) / Alford, Terry Lynn (Committee member) / He, Ximin (Committee member) / Arizona State University (Publisher)
Created2016