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At least 937 records · Page 52

Bi-directional tuning of thermal transport in SrCoO x with electrochemically induced phase transitions

Unlike the wide-ranging dynamic control of electrical conductivity, there does not exist an analogous ability to tune thermal conductivity by means of electric potential. The traditional picture assumes that atoms inserted into a material’s lattice act purely as a source of scattering for thermal carriers, which can only reduce thermal conductivity. In contrast, here we show that the electrochemical control of oxygen and proton concentration in an oxide provides a new ability to bi-directionally control thermal conductivity. On electrochemically oxygenating the brownmillerite SrCoO 2.5 to the perovskite SrCoO 3–δ , the thermal conductivity increases by a factor of 2.5, whereas protonating it to form hydrogenated SrCoO 2.5 effectively reduces the thermal conductivity by a factor of four. This bi-directional tuning of thermal conductivity across a nearly 10 ± 4-fold range at room temperature is achieved by using ionic liquid gating to trigger the ‘tri-state’ phase transitions in a single device. We elucidated the effects of these anionic and cationic species, and the resultant changes in lattice constants and lattice symmetry on thermal conductivity by combining chemical and structural information from X-ray absorption spectroscopy with thermoreflectance thermal conductivity measurements and ab initio calculations. This ability to control multiple ion types, multiple phase transitions and electronic conductivity that spans metallic through to insulating behaviour in oxides by electrical means provides a new framework for tuning thermal transport over a wide range.

36 MATERIALS SCIENCE↗

Modulating the Surface Ligand Orientation for Stabilized Anionic Redox in Li‐Rich Oxide Cathodes

Abstract Anionic redox chemistry is emerging as a key concept in the development of high‐energy lithium‐ion batteries, as it enables a nearly doubled charge storage capacity, aiding the development of high‐capacity batteries. However, the anionic reactivity is frequently irreversible from charge to discharge, leading to rapid decay of the capacity and voltage of batteries over long‐term cycling. Although the possibility of controlling the anionic redox reactions by tuning the geometric and electronic structures has recently been proposed, the implementation of this strategy is still a critical challenge. Herein, a strategy is proposed to improve the anionic redox reversibility of a model anionic redox active cathode material, Li 1.2 Ni 0.13 Co 0.13 Mn 0.54 O 2 , by tuning the surface ligand geometry via the growth of a lattice‐compatible spinel LiCoO 2 coating layer on the particle surface. Detailed local structure and first principles investigations reveal that the shape and orientation of the octahedral layer in the host lattice are modified. Accordingly, a two‐band oxygen redox behavior is triggered in the ligand‐orientation‐regulated Li‐rich cathode, leading to enhanced reversibility, and thus, remarkably improved capacity and voltage retention over cycling. This study highlights the importance of controllable ligand orientation, carving a new path for the development and design of Li‐rich cathodes in the future.

Liu, Yanchen↗

Engineering Globular Protein Vesicles through Tunable Self-Assembly of Recombinant Fusion Proteins

Vesicles assembled from folded, globular proteins have potential for functions different from traditional lipid or polymeric vesicles. However, they also present challenges in understanding the assembly process and controlling vesicle properties. From detailed investigation of the assembly behavior of recombinant fusion proteins, this work reports a simple strategy to engineer protein vesicles containing functional, globular domains. This is achieved through tunable self-assembly of recombinant globular fusion proteins containing leucine zippers and elastin-like polypeptides. The fusion proteins form complexes in solution via high affinity binding of the zippers, and transition through dynamic coacervates to stable hollow vesicles upon warming. The thermal driving force, which can be tuned by protein concentration or temperature, controls both vesicle size and whether vesicles are single or bi-layered. Lastly, these results provide critical information to engineer globular protein vesicles via self-assembly with desired size and membrane structure.

36 MATERIALS SCIENCE↗

Molecular mechanism of reflectin’s tunable biophotonic control: Opportunities and limitations for new optoelectronics

Discovery that reflectin proteins fill the dynamically tunable Bragg lamellae in the reflective skin cells of certain squids has prompted efforts to design new reflectin-inspired systems for dynamic photonics. But new insights into the actual role and mechanism of action of the reflectins constrain and better define the opportunities and limitations for rationally designing optical systems with reflectin-based components. We and our colleagues have discovered that the reflectins function as a signal-controlled molecular machine, regulating an osmotic motor that tunes the thickness, spacing, and refractive index of the tunable, membrane-bound Bragg lamellae in the iridocytes of the loliginid squids. The tunable reflectin proteins, characterized by a variable number of highly conserved peptide domains interspersed with positively charged linker segments, are restricted in intra- and inter-chain contacts by Coulombic repulsion. Physiologically, this inhibition is progressively overcome by charge-neutralization resulting from acetylcholine (neurotransmitter)-induced, site-specific phosphorylation, triggering the simultaneous activation and progressive tuning of reflectance from red to blue. Details of this process have been resolved through in vitro analyses of purified recombinant reflectins, controlling charge-neutralization by pH-titration or mutation as surrogates for the in vivo phosphorylation. Results of these analyses have shown that neutralization overcoming the Coulombic inhibition reversibly and cyclably triggers condensation and secondary folding of the reflectins, with the emergence of previously cryptic, phase-segregated hydrophobic domains enabling hierarchical assembly. This tunable, reversible, and cyclable assembly regulates the Gibbs-Donnan mediated osmotic shrinking or swelling of the Bragg lamellae that tunes the brightness and color of reflected light. Our most recent studies have revealed a direct relationship between the extent of charge neutralization and the size of the reflectin assemblies, further explaining the synergistic effects on the intensity and wavelength of reflected light. Mutational analyses show that the “switch” controlling reflectins’ structural transitions is distributed along the protein, while detailed comparisons of the sequences and structures of the recently evolved tunable reflectins to those of their ancestral, non-tunable homologs are helping to identify the specific structural determinants governing tunability.

47 OTHER INSTRUMENTATION↗

Molecular Assembly-Induced Charge Transfer for Programmable Functionalities

The donor–acceptor interface within molecular charge transfer (CT) solids plays a vital role in the hybridization of molecular orbitals to determine their carrier transport and electronic delocalization. In this study reported herein, we demonstrate molecular assembly-driven bilayer and crystalline solids, consisting of electron donor dibenzotetrathiafulvalene (DBTTF) and acceptor C 60 , in which interfacial engineering-induced CT degree control is a key parameter for tuning its optical, electronic, and magnetic performance. Compared to the DBTTF/C 60 bilayer structure, the DBTTFC 60 cocrystalline solids show a stronger degree of charge transfer for broad CT absorption and a large dielectric constant. In addition, the DBTTFC 60 cocrystals exhibit distinct CT arrangement-driven anisotropic electron mobility and spin characteristics, which further enables the development of high-penetration and high-energy $γ$-ray photodetectors. The results presented in this paper provide a basis for the design and control of molecular charge transfer solids, which facilitates the integration of such materials into molecular electronics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Innovative Patient Room Lighting System with Integrated Spectrally Adaptive Control

In December of 2013, the U.S. Department of Energy’s SSL R&D Program released a Funding Opportunity Announcement (FOA), that for the first time, contained opportunities for comprehensive application-specific system development. The FOA included opportunities for two applications, one of which was a Patient Room. Philips Lighting Research North America, submitted a proposal for the Patient Room application, and was selected for the complete project award. The award amount was for $497,127, with a Philips Research co-funding commitment 165,709 dollars. The total project value was 662,836 dollars. This project sought to redefine lighting for the patient room application. The goal was to deliver an innovative LED patient suite (patient room and bathroom) lighting system solution that was 40% more energy-efficient than traditional fluorescent incumbent technologies, and would meet all the visual and non-visual needs of patients, caregivers and visitors, and improve the patient experience. State-of-the-art multichannel LED platforms and control technologies that would provide spectral tuning and become part of an intelligent, connected lighting system drove the solution. The project was scoped into four main task areas that included a) System Concept Creation, b) Identification of the Luminaire Portfolio, c) Development of the Connected Lighting Infrastructure, and d) System Performance Validation. Each of the four main tasks were completed and validated extensively over the course the 2 ½ year project. The system concept was created by first developing a lighting design that demonstrated best practices for patient room lighting – illuminance and uniformity for task performance, reduced glare, and convenient controls, in addition to giving patients control over the lighting in their environment. A framework was defined to deliver circadian support via software behaviors. Through that process luminaires were identified from the Philips portfolio that were adaptable – by their form, dimensions, and optical materials – to mix multicolor LED platforms uniformly and deliver target design lumen levels. The Blue Sky luminaire was selected for the patient bed area to give the illusion of skylight while providing white light on the patient bed. Luminaires used existing 2-channel tunable white LED boards, and newly developed 4-channel LED boards. Red-Orange, Blue, Green, and Blue-shifted Yellow LED chips were selected based on spectral characteristics and their ability to produce high quality white light. 4-channel Power over Ethernet (PoE) drivers were developed and firmware written so they would communicate with both 2- and 4-channel boards. These components formed the backbone of the connected lighting infrastructure. Software, flexible and nuanced in its complexity, was written to set behaviors for myriad lighting scenes in the room throughout the 24 hour day – and all could be overridden by manual controls. This included a dynamic tunable white program, three color changing automatic programs that simulated degrees of sunrise to sunset palettes, and an amber night lighting system that offered visual cues for postural stability to minimize the risk of falls. All programs were carefully designed to provide visual comfort for all occupants, support critical task performance for staff, and to support the patient’s 24hr rhythms. A full scale mockup room was constructed in the Philips Cambridge Lab. The lighting system was installed, tested and functionality demonstrated to ensure smooth operation of system components – luminaires, drivers, PoE switches, wall controls, patient remote, and daylight and occupancy sensors. How did the system perform? It met visual criteria, confirmed by calculations, simulations and measurements in the field. It met non-visual criteria, confirmed by setting circadian stimulus (CS) targets and performing calculations using the calculator developed by the Lighting Research Center. Finally, human factors validation studies were conducted to gain insight from real end users in the healthcare profession; surveys were administered, data analyzed, and audio comments captured. The general consensus was positive, with requests to pilot the system in their hospitals. The importance of the research completed under this grant is that it allowed the exploration and development of a unique lighting system, one that would deliver a blend of visual and non-visual criteria in patient room design for today’s healthcare environment. The research investigated the area of multichannel LED technology, multichannel Power over Ethernet (PoE) drivers and their integration with automatic and manual controls as a system – uncovering and meeting challenges along the way. It married visual needs of patients and staff with support for 24 hour rhythms, placing value on the wellbeing of the patient – while successfully saving energy over incumbent technologies. Indications are that the market is ready and willing to invest – multiple healthcare facilities are in line to pilot this system, recognizing its value beyond energy to patient and staff well-being. Its value to the public can best be expressed by a patient support coordinator who, after spending several hours in the room being immersed in the lighting, analyzing all its features, commented: “This re-writes lighting for healthcare”.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Tuning extreme ultraviolet emission for optimum coupling with multilayer mirrors for future lithography through control of ionic charge states

We report on the identification of the optimum plasma conditions for a laser-produced plasma source for efficient coupling with multilayer mirrors at 6.x nm for beyond extreme ultraviolet lithography. A small shift to lower energies of the peak emission for Nd:YAG laser-produced gadolinium plasmas was observed with increasing laser power density. Charge-defined emission spectra were observed in electron beam ion trap (EBIT) studies and the charge states responsible identified by use of the flexible atomic code (FAC). The EBIT spectra displayed a larger systematic shift of the peak wavelength of intense emission at 6.x nm to longer wavelengths with increasing ionic charge. This combination of spectra enabled the key ion stage to be confirmed as Gd{sup 18+}, over a range of laser power densities, with contributions from Gd{sup 17+} and Gd{sup 19+} responsible for the slight shift to longer wavelengths in the laser-plasma spectra. The FAC calculation also identified the origin of observed out-of-band emission and the charge states responsible.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Mode Orientation Control For Sapphire Dielectric Ring Resonator

Small sapphire tuning wedge used in technique for solving mode-purity problem associated with sapphire dielectric-ring resonator part of cryogenic microwave frequency discriminator. Breaks quasi-degeneracy of two modes and allows selective coupling to just one mode. Wedge mounted on axle entering resonator cavity and rotated while resonator cryogenically operating in vacuum. Furthermore, axle moved vertically to tune resonant frequency.

Santiago, David G.↗

Note: Control of liquid helium supply to cryopanels of Kolkata superconducting cyclotron

The Kolkata superconducting cyclotron utilises liquid helium to cool the main magnet niobium-titanium (NbTi) coil and the cryopanels. Three liquid helium cooled cryopanels, placed inside the dees of the radio-frequency system, maintain the high vacuum in the acceleration region of the superconducting cyclotron. The small cryostat placed inside the cryogenic distribution manifold located at the basement of the superconducting cyclotron building supplies liquid helium in parallel branches to three cold heads, used for cooling their associated cryopanels. The level in the cryostat has to be maintained at an optimum value to ensure uninterrupted flow of liquid helium to these three cold heads. This paper describes the transfer function of the overall system, its tuning parameters, and discusses the actual control of cryostat level by using these parameters.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Atmospheric Tracer Depletion Testing for Unfiltered Air In-Leakage Determination at the Wolf Creek Nuclear Power Plant

Atmospheric Tracer Depletion tests were conducted at the Wolf Creek Nuclear Power Plant to quantify the unfiltered in-leakage (UI) into the Control Room (CR), Control Building (CB), and Equipment Rooms (ER) at the Wolf Creek Nuclear Power Plant. Wolf Creek has two independent charcoal filter Emergency Ventilation Systems (EVS) that can be used to purify air entering the control building and control room. The Bravo System contains a filtration system in Room 1501 in the Auxiliary Building for the Control Room and another filtration system (FGK02B) on Elevation 2016 for the Control Building. The Alpha system contains a filtration system in Room 1512 in the Auxiliary Building for the Control Room and another filtration system (FGK02A) on Elevation 2016 for the Control Building.The Atmospheric Tracer Depletion (ATD) test is a technique to measure in-leakage using the concentration of perfluorocarbon compounds that have a constant atmospheric background. These levels are present in the Control Room and Control Building under normal operating conditions. When air is supplied by either of the EVS, most of the PFTS are removed by the charcoal filters. If the concentrations of the PFTs measured in protected areas are the same as the levels at the output of the EVS, the in-leakage of outside air into the protected area would be zero. If the concentration is higher in the protected area than at the output of the filter system, there is in-leakage and the in-leakage can be quantified by the difference.Sampling was performed using state-of-the-art Brookhaven Atmospheric Tracer Samplers (BATS) air sampling equipment and analysis performed on Brookhaven National Laboratory (BNL) dedicated PFT analytical systems. In the Alpha test two tracers PMCH and mcPDCH were used to determine in-leakage into the control building. The analytical system was tuned to maximize sensitivity after initial analysis of the Alpha test. The increased sensitivity permitted accurate quantification of five isomers of the PFT PDCH (mtPDCH, pcPDCH, otPDCH, mcPDCH, and ptPDCH). These isomers were quantified in the low concentration samples in the Alpha test and in all samples in the Bravo test.The best estimates of UI (Rui) for the four zones are provided in Table ES-1. For the CB, this estimate averages the four tracers at the four elevations. For the CR, this estimate uses the four sampling units located in the Control Room.

54 ENVIRONMENTAL SCIENCES↗

Atmospheric Tracer Depletion Testing for Unfiltered Air In-Leakage Determination at the Wolf Creek Nuclear Power Plant

Atmospheric Tracer Depletion tests were conducted at the Wolf Creek Nuclear Power Plant to quantify the unfiltered in-leakage (UI) into the Control Room (CR), Control Building (CB), and Equipment Rooms (ER) at the Wolf Creek Nuclear Power Plant. Wolf Creek has two independent charcoal filter Emergency Ventilation Systems (EVS) that can be used to purify air entering the control building and control room. The Bravo System contains a filtration system in Room 1501 in the Auxiliary Building for the Control Room and another filtration system (FGK02B) on Elevation 2016 for the Control Building. The Alpha system contains a filtration system in Room 1512 in the Auxiliary Building for the Control Room and another filtration system (FGK02A) on Elevation 2016 for the Control Building. The Atmospheric Tracer Depletion (ATD) test is a technique to measure in-leakage using the concentration of perfluorocarbon compounds that have a constant atmospheric background. These levels are present in the Control Room and Control Building under normal operating conditions. When air is supplied by either of the EVS, most of the PFTS are removed by the charcoal filters. If the concentrations of the PFTs measured in protected areas are the same as the levels at the output of the EVS, the in-leakage of outside air into the protected area would be zero. If the concentration is higher in the protected area than at the output of the filter system, there is in-leakage and the in-leakage can be quantified by the difference. Sampling was performed using state-of-the-art Brookhaven Atmospheric Tracer Samplers (BATS) air sampling equipment and analysis performed on Brookhaven National Laboratory (BNL) dedicated PFT analytical systems. In the Alpha test two tracers PMCH and mcPDCH were used to determine in-leakage into the control building. The analytical system was tuned to maximize sensitivity after initial analysis of the Alpha test. The increased sensitivity permitted accurate quantification of five isomers of the PFT PDCH (mtPDCH, pcPDCH, otPDCH, mcPDCH, and ptPDCH). These isomers were quantified in the low concentration samples in the Alpha test and in all samples in the Bravo test. The best estimates of UI (Rui) for the four zones are provided in Table ES-1. For the CB, this estimate averages the four tracers at the four elevations. For the CR, this estimate uses the four sampling units located in the Control Room.

54 ENVIRONMENTAL SCIENCES↗

Simple Monomers for Precise Polymer Functionalization During Ring-Opening Metathesis Polymerization

Controlling the monomer sequence of synthetic polymers is a grand challenge in polymer science. Conventional sequence control has been achieved in dispersed polymers by exploiting the kinetic tendencies of monomers and their order of addition. While the sequence of blocks in multiblock copolymers can be readily tuned using sequential addition of monomers (SAM), control over the sequence distribution is eroded as the targeted block size approaches a single monomer unit (i.e., X n ~ 1) due to the stochastic nature of chain-growth reactions. Thus, unique monomers are needed to ensure precise single additions. Herein, we investigate common classes of cyclic olefin monomers for ring-opening metathesis polymerization (ROMP) to identify monomers for single unit addition during sequential monomer addition synthesis. Through careful analysis of polymerization kinetics, we find that easily synthesized oxanorbornene imide monomers are suitable for single-addition reactions. With the identified monomers, we demonstrate the synthesis of multiblock copolymers containing up to three precise functionalization sites and singly cross-linked four-armed star copolymers. In conclusion, we envision that expanded kinetic analyses of monomer reactivities in ROMP reactions will enable novel polymer synthesis capabilities such as the autonomous synthesis of sequence-defined polymers or one-shot multiblock copolymer syntheses.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Robust highly durable solid oxide fuel cell cathodes – Improved materials compatibility & self-regulating surface chemistry

Solid oxide fuel cells (SOFCs) are electrochemical conversion devices that directly transform hydrogen or hydrocarbon fuels to electricity, with energy efficiencies as high as 90%, coupled with reduced emissions. Several factors, however, remain to be addressed when considering scale-up of SOFC technology, including the need to overcome decreased performance due to sluggish rates of the oxygen reduction reaction (ORR) at the cathode under reduced temperatures and susceptibility to degradation in performance from surface poisoning e.g. from chromia, while limiting the use of critical raw materials (lanthanides and transition metals) present in high performing mixed ionic electronic conducting electrodes like (La,Sr)CoO 3 (LSC). In this project we explored the key descriptors for determining ORR activity in SOFC electrodes and tried to recover performance degradation by applying them to SOFC electrodes. In order to do this, we first selected a model mixed ionic electronic conducting (MIEC) oxide, Pr-doped CeO 2 (Pr 0.1 Ce 0.9 O 2-δ , PCO), which is a chemically stable fluorite and free of inherent poison sources (e.g. Sr segregation in LSC) that potentially react with external impurities such as Cr-species vaporized from the interconnect. The three approaches originally planned in this project are as follows: 1) evaluation of scavenger exsolution characteristics, 2) study of scavengers gettering efficacy following Cr and Si poisoning and 3) integration of new compositions into porous electrodes. Among them, exceptional progress has been made in 2) and 3), especially understanding the role of surface infiltrants in impacting electrode performance and degradation of PCO materials. We found that the Smith acidity scale for binary oxides serves as a powerful descriptor for tuning and predicting the oxygen exchange kinetics on MIEC PCO surfaces. As a result, with infiltration with binary oxides, ranging from strongly basic (Li 2 O) to strongly acidic (SiO 2 ) onto the surface of porous PCO, it was possible to systematically vary the chemical surface exchange coefficient (k chem ) by 6 orders of magnitude! L i2 O increased k chem by nearly 1,000 times over that of pristine PCO, while SiO 2 decreased k chem by nearly the same factor. Strikingly, although the pre-exponential of k chem scales linearly with the acidity of the infiltrated binary oxide, there is nearly no change in the activation energy. With this insight, we attributed the origin of these dramatic changes in k chem values to the systematic increase and decrease in the surface electron density induced by infiltrated binary oxides. More interestingly, although both Cr 2 O 3 and SiO 2 were determined to be acidic by Smith, suggesting that this feature could likely be the primary reason that these compounds serve to poison the ORR on SOFC cathodes, the effect of poisoning could be subsequently tuned by adding multiple infiltrants and controlling their relative surface acidities. We also systematically examined the effect of serial infiltration of basic and acidic oxides. It turned out that serial infiltration of Li not only recovers approximately 20-fold degraded k chem of PCO by acidic Cr 2 O 3 but its k chem is enhanced even beyond that of the non-infiltrated PCO by more than three orders of magnitude. This was further verified with a screen-printing PCO symmetric cell in terms of the electrode performance (area-specific resistance, ASR) related to approach 3). These observations point to acidity as a key descriptor not only in tuning and predicting the ORR activity of SOFC cathodes that largely determines the overall performance of SOFC, but in mitigating and reactivating poisoned electrode performance. This work provides novel guidelines for making the electrode performance much more active and robust in SOFCs, which can further be applied to all applications requiring oxygen exchange reaction, such as electrolyzers, permeation membranes and gas sensors.

30 DIRECT ENERGY CONVERSION↗

Design and implementation of fuzzy logic controllers

The main objectives of our research are to present a self-contained overview of fuzzy sets and fuzzy logic, develop a methodology for control system design using fuzzy logic controllers, and to design and implement a fuzzy logic controller for a real system. We first present the fundamental concepts of fuzzy sets and fuzzy logic. Fuzzy sets and basic fuzzy operations are defined. In addition, for control systems, it is important to understand the concepts of linguistic values, term sets, fuzzy rule base, inference methods, and defuzzification methods. Second, we introduce a four-step fuzzy logic control system design procedure. The design procedure is illustrated via four examples, showing the capabilities and robustness of fuzzy logic control systems. This is followed by a tuning procedure that we developed from our design experience. Third, we present two Lyapunov based techniques for stability analysis. Finally, we present our design and implementation of a fuzzy logic controller for a linear actuator to be used to control the direction of the Free Flight Rotorcraft Research Vehicle at LaRC.

Abihana, Osama A.↗

Gradient-Descent-Based Learning Gain for Backstepping Controller and Disturbance Observer of Nonlinear Systems

This paper proposes a gradient-descent-based learning (GL) gain for backstepping controller and disturbance observer (DOB) of nonlinear system. The proposed method consists of the GL gain update law, controller, and DOB. The GL gain update law is proposed to adapt the control gain and DOB gain according to the direction that minimizes the cost function. The mathematical analysis reveals that the GL gain always has a positive sign and upper bound. The controller is designed via a backstepping procedure to track the desired output with GL control gain. The DOB is designed to estimate the unknown external disturbance with the GL DOB gain. Because the control and DOB gains are simultaneously tuned to achieve improved performance, the time consumption for tuning can be reduced. In addition, the peaking phenomenon can be avoided initially by a small initial value of GL gains. The stability of the closed-loop system is guaranteed using the input-to-state stability property. The performance of the proposed method was validated via simulations and experiments using a DC motor.

42 ENGINEERING↗

Achieving Long-Lived Triplet States in Intramolecular SF Films through Molecular Engineering

Tuning singlet fission (SF) dynamics in the solid states in a controllable way is vitally important yet still a challenge due to the electronic coupling, which is highly sensitive to molecular packing. Here, we demonstrate a molecular engineering approach to independently optimize the triplet generation and decay process in intramolecular SF films by using terphenyl-bridged TIPS-pentacene tetramers. By controlling the degree of steric hindrance within individual tetramers, we can systematically tune the degree of intermolecular coupling in thin films. Taking advantage of both the intra- and intermolecular SF processes allows us to maintain a rapid triplet pair generation process, even in the case of weak intermolecular coupling. This approach allows us to maintain a picosecond triplet generation process while simultaneously varying the rate constants for triplet-triplet annihilation over three orders of magnitude.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Reaching quantum critical point by adding nonmagnetic disorder in single crystals of superconductor (Ca 𝑥 ⁢Sr 1−𝑥 ) 3 ⁢Rh 4 ⁢Sn 13

The Remeika series superconductor, (Ca 𝑥 ⁢Sr 1−𝑥 ) 3 ⁢Rh 4 ⁢Sn 13 , shows a rare nonmagnetic quantum critical point (QCP) associated with the continuous charge-density wave (CDW) and structural transition under the “dome” of superconductivity achieved by tuning composition and applying pressure. Here, we use a nonmagnetic pointlike disorder induced by 2.5 MeV electron irradiation to suppress the CDW and drive the system to and even beyond the QCP. This conclusion is based on a clear evolution of temperature-dependent resistivity, 𝜌⁡(𝑇), from the Fermi liquid to the non-Fermi liquid regime with increasing amount of disorder. Starting on the CDW side, below the suggested QCP concentration of 𝑥 𝑐 =0.9, added disorder resulted in a progressively larger linear term and a reduced quadratic term in 𝜌⁡(𝑇). Nearly perfect 𝑇−linear dependence is observed at the dose at which long-range CDW order is suppressed to 𝑇=0, consistent with the expectations. We refine the QCP location in this system and place it in the interval between 𝑥=0.75 and 0.85. Our results strongly support the concept that the disorder can tune the system to the quantum critical regime and even beyond. It follows from the argument by Imry and Ma that any ordered phase is unstable toward quenched disorder. Introduced in a controlled way, this disorder becomes a nonthermal tuning parameter likely applicable to a variety of different systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗