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At least 1,477 records · Page 82

Electron energy distributions in a magnetized inductively coupled plasma

Optimizing and controlling electron energy distributions (EEDs) is a continuing goal in plasma materials processing as EEDs determine the rate coefficients for electron impact processes. There are many strategies to customize EEDs in low pressure inductively coupled plasmas (ICPs), for example, pulsing and choice of frequency, to produce the desired plasma properties. Recent experiments have shown that EEDs in low pressure ICPs can be manipulated through the use of static magnetic fields of sufficient magnitudes to magnetize the electrons and confine them to the electromagnetic skin depth. The EED is then a function of the local magnetic field as opposed to having non-local properties in the absence of the magnetic field. In this paper, EEDs in a magnetized inductively coupled plasma (mICP) sustained in Ar are discussed with results from a two-dimensional plasma hydrodynamics model. Results are compared with experimental measurements. We found that the character of the EED transitions from non-local to local with application of the static magnetic field. The reduction in cross-field mobility increases local electron heating in the skin depth and decreases the transport of these hot electrons to larger radii. The tail of the EED is therefore enhanced in the skin depth and depressed at large radii. Plasmas densities are non-monotonic with increasing pressure with the external magnetic field due to transitions between local and non-local kinetics.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

A new approach to entangling neutral atoms.

Our team has developed a new approach to entangling neutral atoms with a Rydberg-dressed interaction. Entangling neutral atoms is an essential key of quantum technologies such as quantum computation, many-body quantum simulation, and high-precision atomic sensors . The demonstrated Rydberg-dressed protocol involves adiabatically imposing a light shift on the ground state by coupling an excited Rydberg state with a tuned laser field. Using this technique, we have demonstrated a strong and tunable dipole - dipole interaction between two individually trapped atoms with energy shifts of order 1 MHz, which has been challenging to achieve in other protocols . During this program, we experimentally demonstrated Bell-state entanglement and the isomorphism to the Jaynes - Cumming model of a Rydberg-dressed two-atom system. Our theoretical calculations of a CPHASE quantum logic gate and arbitrary Dicke state quantum control in this system encourage further work.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Application of an Embedded Fracture and Borehole Modeling Approach to the Understanding of EGS Collab Experiment 1

EGS Collab is a series of meso-scale experiments and associated numerical simulation activities being funded by the United States Department of Energy, Geothermal Technologies Office (GTO) to investigate enhanced geothermal system processes under in-situ stress and slightly elevated temperature conditions. This project is designed to provide scientists and engineers with immediate access to impermeable rock at scales larger than possible in the laboratory, but generally smaller than those for commercial production. Immediate access to rock is provided via the existing drifts of the former Homestake Gold Mine, now operated as the Sanford Underground Research Facility in Lead, South Dakota. The objectives of the EGS Collab project are to develop well controlled fracture networks between injector and producer boreholes using normal and shear stimulation for permeability enhancement. The first experimental site was located off the West Access drift on the 4850 Level (4850 feet below ground surface) in phyllite of the Precambrian Poorman formation, and involved the creation of a fracture network comprising a combination of hydraulic and natural fractures. A second experimental site is now being considered near the battery alcove on the 4100 Level in amphibolite and rhyolite of the Yates Unit. Data generated during these experiments will be compared against predictions of a suite of computer codes specifically designed to solve problems involving coupled thermal, hydrological, geomechanical, and geochemical processes. Comparisons between experimental and numerical simulation results will provide code developers with direction for improvements and verification of process models, build confidence in the suite of available numerical tools, and ultimately identify critical future development needs for the geothermal modeling community. Moreover, conducting thorough comparisons of models, modelling approaches, measurement approaches and measured data, via the EGS Collab project, will serve to identify techniques that are most likely to succeed at the Frontier Observatory for Research in Geothermal Energy (FORGE), the GTO’s flagship EGS research effort. Experiment 1 has comprised a series of successful tests, including a long-term chilled-water circulation test, but the testbed has two atypical EGS elements. Active ventilation in the adjacent drift over a 50-year period cooled the testbed rock mass and hydraulic fracturing intersected monitoring boreholes making them conduits for fluid flow. Numerical simulations executed in support of the design of the EGS Collab Experiment 1, computed a radial temperature distribution and stress gradient orthogonal to the drift axis, resulting in the forecast of an oblong hydraulic fracture geometry, extended in the direction of the drift from the stimulation borehole. This paper describes the numerical simulation of long-term chilled-water circulation test with an embedded fracture and borehole modeling approach. The principal objective of the simulation work is show agreement between experimental observations in terms of production fluid temperatures, monitoring borehole temperatures, injection and production pressures, and tracer recoveries using a single conceptual model for the fracture network, using characterization and monitoring data generally available for EGS. A secondary objective is to improve the numerical simulation result comparisons with additional data available from the broader monitoring equipment within the testbed versus deeper, hotter, and more remote EGS. One complicating factor for comparisons between the numerical simulation results and experimental observations, is the Joule-Thomson heating associated with large pressure drops across the fracture network.

numerical simulation, embedded fractures and boreh↗

Hygrothermal Simulation of Foundations: Part 1 - Soil Material Properties

The hygrothermal performance of soils coupled to buildings is a complicated process. A computational approach for heat transfer through the ground has been well defined (EN ISO 13370:2007, 2007), and simplified methods have been developed (Staszczuk, Radon, and Holm 2010). However, these approaches generally ignore the transfer of soil moisture, which is not negligible (Janssen, Carmeliet, and Hens 2004). This study is divided into several parts. The intention of the first part is to gather, comprehend and adapt soil properties from Soil Science. The obtained information must be applicable to related tasks in Building Science and validated with hygrothermal calculation tools. Future parts of this study will focus on the validation aspect of the soil properties to be implemented. Basic changes in the software code may be requested at this time. Different types of basement construction will be created with a hygrothermal calculation tool, WUFI. Simulations from WUFI will be compared with existing or ongoing measurements. The intentions of the first part of this study have been fulfilled. The soil properties of interest in Building Science have been defined for 12 different soil textures. These properties will serve as input parameters when performing hygrothermal calculations of building constructions coupled to soil materials. The reliability of the soil parameters will be further evaluated with measurements in Part 2.

Kehrer, Manfred↗

Evidence of Cu I /Cu II Redox Process by X‐ray Absorption and EPR Spectroscopy: Direct Synthesis of Dihydrofurans from β‐Ketocarbonyl Derivatives and Olefins

Abstract The Cu I /Cu II and Cu I /Cu III catalytic cycles have been subject to intense debate in the field of copper‐catalyzed oxidative coupling reactions. A mechanistic study on the Cu I /Cu II redox process, by X‐ray absorption (XAS) and electron paramagnetic resonance (EPR) spectroscopies, has elucidated the reduction mechanism of Cu II to Cu I by 1,3‐diketone and detailed investigation revealed that the halide ion is important for the reduction process. The oxidative nature of the thereby‐formed Cu I has also been studied by XAS and EPR spectroscopy. This mechanistic information is applicable to the copper‐catalyzed oxidative cyclization of β‐ketocarbonyl derivatives to dihydrofurans. This protocol provides an ideal route to highly substituted dihydrofuran rings from easily available 1,3‐dicarbonyls and olefins.

Yi, Hong↗

Diffusion Dominant Solute Transport Modelling in Fractured Media Under Deep Geological Environment - 12211

Deep geologic disposal of high activity and long-lived radioactive waste is gaining increasing support in many countries, where suitable low permeability geological formation in combination with engineered barriers are used to provide long term waste contaminant and minimise the impacts to the environment and risk to the biosphere. This modelling study examines the solute transport in fractured media under low flow velocities that are relevant to a deep geological environment. In particular, reactive solute transport through fractured media is studied using a 2-D model, that considers advection and diffusion, to explore the coupled effects of kinetic and equilibrium chemical processes. The effects of water velocity in the fracture, matrix porosity and diffusion on solute transport are investigated and discussed. Some illustrative modelled results are presented to demonstrate the use of the model to examine the effects of media degradation on solute transport, under the influences of hydrogeological (diffusion dominant) and microbially mediated chemical processes. The challenges facing the prediction of long term degradation such as cracks evolution, interaction and coalescence are highlighted. The potential of a novel microstructure informed modelling approach to account for these effects is discussed, particularly with respect to investigating multiple phenomena impact on material performance. The GRM code is used to examine the effects of media degradation for a geological waste disposal package, under the combined hydrogeological (diffusion dominant) and chemical effects in low groundwater flow conditions that are typical of deep geological disposal systems. An illustrative reactive transport modelling application demonstrates the use of the code to examine the interplay of kinetic controlled biogeochemical reactive processes with advective and diffusive transport, under the influence of media degradation. The initial model results are encouraging which show the disposal system to evolve in a physically realistic manner. In the example presented the reactive-transport coupling develops chemically reducing zones, which limit the transport of uranium. This illustrates the potential significance of media degradation and chemical effect on the transport of radionuclides which would need to be taken into account when examining the long-term behaviour and containment properties of the geological disposal system. Microstructure-informed modelling and its potential linkage with continuum flow modelling is a subject of ongoing studies. The approach of microstructure-informed modelling is discussed to provide insight and a mechanistic understanding of macroscopic parameters and their evolution. The proposed theoretical and methodological basis for microstructure-informed modelling of porous quasi-brittle media has the potential to develop into an explanatory and predictive tool for deriving mechanism-based, as opposed to phenomenological, evolution laws for macroscopic properties. These concepts in micro-scale modelling are likely to be applicable to the diffusion process, in addition to advective transport illustrated here for porous media. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Collaborative Research: Advancing Arctic Climate Projection Capability at Seasonal to Decadal Scales (Final Technical Report)

The Regional Arctic System Model (RASM) at process resolving configurations has been used to (i) advance understanding of physical processes and feedbacks involved in Arctic amplification and (ii) understand and potentially reduce uncertainty in prediction of arctic climate change at seasonal to decadal scales. RASM consists the atmosphere (Weather and Research Forecasting model, WRF), ocean (Parallel Ocean Program, POP), sea ice (CICE), land hydrology (Variable Infiltration Capacity model, VIC), river routing scheme (RVIC), marine biogeochemistry components and the coupling framework (CPL7). Its domain is pan-Arctic, with the atmosphere and land components configured on a 50-km or 25-km grid and four configurations of the ocean and sea ice components: 1/12°(~9.3km) or 1/48°(~2.4km) and 45 or 60 vertical layers. These RASM configurations have been motivated by the emerging exascale capability for high performance computing to improve model fidelity. The dynamical downscaling of reanalysis allows comparison of RASM results with observations in place and time to: (i) advance system level understanding of physical processes and coupling involved in an event, (ii) optimize model parameter space, (iii) diagnose and reduce model biases and (iv) produce realistic and consistent across all the components initial conditions for predictions and predictability studies, which are all unique capabilities not available in global Earth System Models (ESMs). An evaluation of RASM 1.0 (Cassano et al. 2017) revealed that it had a cold bias over the oceans and a warm bias over land areas due largely to cloud and radiation biases in the model, with too little cloud cover simulated over land and too much cloud cover simulated over sub-polar oceans. This study has motivated an upgrade to WRF version 3.7.1 in RASM and allowed for the inclusion of the radiative impact of convective clouds. A variety of atmospheric physics parameterizations were evaluated against observations (e.g. data from the Arctic Clouds in Summer Experiment (ACSE); Sedlar et al. 2020) to identify an optimal suite of WRF physics options in RASM. The RASM with the optimized WRF physics were used to study the impact of strong mesoscale winds over the ocean around the southern tip of Greenland (DuVivier and Cassano 2016) and their impact on oceanic convection (DuVivier et al. 2017a). Data from the PolarWinds field campaign were used to evaluate WRF boundary layer physics and resolution impacts on the simulation of a Greenland barrier wind event (DuVivier et al. 2017b). The RVIC streamflow routing model has been implemented in RASM to realistically represent high-resolution streamflow processes (Hamman et al. 2017) and to couple the land buoyancy fluxes to the ocean. The RASM-RVIC high-resolution data set of all coastal freshwater fluxes for the Arctic drainage basin and surrounding areas for 1979-2014 was published as a separate product (https://doi.org/10.5281/zenodo.293037). The fidelity of atmospheric momentum transfer to and the response of polar marine Ekman layer in RASM and Community Earth System Model (CESM) was investigated by Roberts et al. (2015). The increased frequency of oceanic flux exchange in CESM, following the RASM guidance, caused a considerable increase in the median inertial ice speed across the Southern Ocean and parts of the Arctic. A comprehensive evaluation of the RASM1.0 atmosphere-ocean-sea ice-land interface was completed by Brunke et al. (2018). RASM was also demonstrated for its capability to simulate extreme events in agreement with observations in space and time (Lee et al. submitted). In particular, the development of three open water events, known as polynyas, have been simulated north of Greenland in February of 2011, 2017 and 2018, in agreement with satellite observations for the past four decades. The optimized RASM sea ice results have been favorably evaluated against satellite observations and a subset of eleven CMIP6 models (Watts et al. submitted). In a complementary project, Jin et al. (2018) have shown that RASM with higher-resolution and new sea-ice processes contributed to lower model errors in sea-ice conditions, concentrations of nutrients and ice algae, in comparison to results from the coarse-resolution (1°) CESM. In two other complementary studies, RASM results were used (i) to explain areas of concentrated use by bowhead whales, the seasonal progression in the use, and the physical environment within those areas (Citta et al. 2015) and (ii) for a synthesis of fall bowhead whales distribution and migration in the Bering-Chukchi-Beaufort (BCB) Sea to investigate whale movements and feeding to the local ocean hydrography and currents (Citta et al. 2018). However, the multi-decadal output from the CESM Large Ensemble yielded unrealistic forcing. Instead, the shorter NCEP CFSv2 9-month forecasts were successfully tested and afforded an increased ensemble size (~30) to demonstrate gains of dynamical downscaling at sub-seasonal to intra-annual time scales. The improved model physics and coupling among RASM model components have yielded more realistic representation of the sea ice cover and consistent across all model components initial conditions. Consequently, RASM demonstrates significant gains compared to simulation of sea ice in the NCEP reanalysis. In addition, RASM 6-month ensemble forecasts yield very realistic sea ice distribution, which demonstrates both significant gains of dynamical downscaling and the continued impact of the initial conditions on forecasts out to 6 months (https://nps.edu/web/rasm/predictions). A follow up study using RASM for dynamical downscaling of the more realistic CESM initialized Decadal Prediction Large Ensemble output is currently ongoing as part of the DOE RGMA HiLAT-RASM project.

54 ENVIRONMENTAL SCIENCES↗

Understanding the distinctively skewed and heavy tailed character of atmospheric and oceanic probability distributions

The probability distributions of large-scale atmospheric and oceanic variables are generally skewed and heavy-tailed. We argue that their distinctive departures from Gaussianity arise fundamentally from the fact that in a quadratically nonlinear system with a quadratic invariant, the coupling coefficients between system components are not constant but depend linearly on the system state in a distinctive way. In particular, the skewness arises from a tendency of the system trajectory to linger near states of weak coupling. We show that the salient features of the observed non-Gaussianity can be captured in the simplest such nonlinear 2-component system. If the system is stochastically forced and linearly damped, with one component damped much more strongly than the other, then the strongly damped fast component becomes effectively decoupled from the weakly damped slow component, and its impact on the slow component can be approximated as a stochastic noise forcing plus an augmented nonlinear damping. In the limit of large time-scale separation, the nonlinear augmentation of the damping becomes small, and the noise forcing can be approximated as an additive noise plus a correlated additive and multiplicative noise (CAM noise) forcing. Much of the diversity of observed large-scale atmospheric and oceanic probability distributions can be interpreted in this minimal framework.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Lifetime of inner-shell hole states of Ar (2p) and Kr (3d) using equation-of-motion coupled cluster method

Auger decay is an efficient ultrafast relaxation process of core-shell or inner-shell excited atom or molecule. Generally, it occurs in femto-second or even atto-second time domain. Direct measurement of lifetimes of Auger process of single ionized and double ionized inner-shell state of an atom or molecule is an extremely difficult task. In this paper, we have applied the highly correlated complex absorbing potential-equation-of-motion coupled cluster (CAP-EOMCC) approach which is a combination of CAP and EOMCC approach to calculate the lifetime of the states arising from 2p inner-shell ionization of an Ar atom and 3d inner-shell ionization of Kr atom. We have also calculated the lifetime of Ar{sup 2+}(2p{sup −1}3p{sup −1}) {sup 1}D, Ar{sup 2+}(2p{sup −1}3p{sup −1}) {sup 1}S, and Ar{sup 2+}(2p{sup −1}3s{sup −1}) {sup 1}P double ionized states. The predicted results are compared with the other theoretical results as well as experimental results available in the literature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Green Factor

Los Alamos is designing a screening platform coupled to our biosensor to customize production processes in cell-free environments that offer biomanufacturers higher titers and yields, better resource utilization and cost-effective bioprocess. Our technology aims at enabling cell-free biosynthetic systems by providing enzyme variants generated by coupling with our biosensor technology, that can utilize cheap raw material cofactor analogues. This will enable bioprocesses based on cell free synthetic biology for a sustainable bioeconomy.

42 ENGINEERING↗

Understanding the changes in ductility and Poisson's ratio of metallic glasses during annealing from microscopic dynamics

In the paper K. L. Ngai et al., [J. Chem. 140, 044511 (2014)], the empirical correlation of ductility with the Poisson's ratio, ν{sub Poisson}, found in metallic glasses was theoretically explained by microscopic dynamic processes which link on the one hand ductility, and on the other hand the Poisson's ratio. Specifically, the dynamic processes are the primitive relaxation in the Coupling Model which is the precursor of the Johari–Goldstein β-relaxation, and the caged atoms dynamics characterized by the effective Debye–Waller factor f{sub 0} or equivalently the nearly constant loss (NCL) in susceptibility. All these processes and the parameters characterizing them are accessible experimentally except f{sub 0} or the NCL of caged atoms; thus, so far, the experimental verification of the explanation of the correlation between ductility and Poisson's ratio is incomplete. In the experimental part of this paper, we report dynamic mechanical measurement of the NCL of the metallic glass La{sub 60}Ni{sub 15}Al{sub 25} as-cast, and the changes by annealing at temperature below T{sub g}. The observed monotonic decrease of the NCL with aging time, reflecting the corresponding increase of f{sub 0}, correlates with the decrease of ν{sub Poisson}. This is important observation because such measurements, not made before, provide the missing link in confirming by experiment the explanation of the correlation of ductility with ν{sub Poisson}. On aging the metallic glass, also observed in the isochronal loss spectra is the shift of the β-relaxation to higher temperatures and reduction of the relaxation strength. These concomitant changes of the β-relaxation and NCL are the root cause of embrittlement by aging the metallic glass. The NCL of caged atoms is terminated by the onset of the primitive relaxation in the Coupling Model, which is generally supported by experiments. From this relation, the monotonic decrease of the NCL with aging time is caused by the slowing down of the primitive relaxation and β-relaxation on annealing, and vice versa.

36 MATERIALS SCIENCE↗

Technoeconomic Analysis of a Solar Thermochemical Fuel Production Process Using a Packed-Bed Redox Reactor

The production of sustainable liquid fuels is paramount in decarbonization of difficult to abate sectors such as the aviation and maritime sectors. Solar thermochemical fuel production is a promising pathway to produce such fuels using concentrated solar thermal (CST) power driving high-temperature redox reactions, coupled with a gas-to-liquid process. In this work we present a preliminary technoeconomic analysis of a solar fuels plant, utilizing a new fixed-bed countercurrent redox reactor and combining both CST and photovoltaic arrays to supply the required energy.

ENERGY STORAGE,HYDROGEN,SOLAR ENERGY↗

Ultrafast carrier dynamics in polycrystalline bismuth telluride nanofilm

In this study, the dynamics of energy carriers in polycrystalline bismuth telluride nanofilm are investigated by the ultrafast pump-probe method. The energy relaxation processes are quantitatively analyzed by using the numerical fitting models. The extracted hot carrier relaxation times of photon excitation, thermalization, and diffusion are around sub-picosecond. The initial reflectivity recovery is found to be dominantly determined by the carrier diffusion, electron-phonon coupling, and photo-generated carriers trapping processes. High-frequency and low-frequency oscillations are both observed and attributed to coherent optical phonons and coherent acoustic phonons, respectively.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Coupled geomechanical investigation of depletion-induced fault reactivation

Fault reactivation during subsurface fluid production pose significant challenges to safe and sustainable resource extraction. Here, this study presents a three-dimensional coupled geomechanical framework to investigate the processes driving fault reactivation, capturing the interactions between reservoir dynamics and geomechanical responses. Verification against theoretical estimations based on linear poroelasticity confirms the model's capacity in representing reservoir background stress responses. However, the study reveals that relying solely on background stress states can underestimate or overestimate fault reactivation potential, emphasizing the importance of including localized stress perturbations such as differential compaction and stress redistribution. Applied to a fault (M1) inspired by the geological characteristics of the Groningen field, the model shows slip initiation at 2965 m depth with 16.0 MPa depletion, aligning with field observations where seismicity occurred at approximately 3 km depth after 15.8 MPa depletion. Parametric studies reveal: (1) inelastic reservoir compaction delays fault reactivation and mitigates fault slip by reducing stress concentration, (2) higher intermediate in-situ stress magnitudes decrease the Coulomb Failure Stress (CFS) increase rate and reduce fault slip, (3) larger fault offsets amplify shear stress near the offset zone, promoting earlier reactivation and longer rupture propagation, and (4) fault permeability significantly influences pressure diffusion, with low-permeability faults leading to sharper stress changes and earlier fault destabilization. These insights highlight the critical role of geological and mechanical parameters in fault reactivation and provide a predictive framework for mitigating induced seismicity risks.

Coupled geomechanical modeling↗

Methyl-Driven Overhauser Dynamic Nuclear Polarization

The Overhauser effect is unique among DNP mechanisms in that it requires the modulation of the electron-nuclear hyperfine interactions. While it dominates DNP in liquids and metals, where unpaired electrons are highly mobile, Overhauser DNP is possible in insulating solids if rapid structural modulations are linked to a modulation in hyperfine coupling. In this study, we report that Overhauser DNP can be triggered by the strategic addition of a methyl group, demonstrated here in a Blatter’s radical. The rotation of the methyl group leads to a modulation of the hyperfine coupling to its protons, which in turn facilitates electron-nuclear cross-relaxation. Removal of the methyl protons, through deuteration, quenches the process, as does the reduction of the hyperfine coupling strength. This result suggests the possibility for the design of tailor-made Overhauser DNP polarizing agents for high-field MAS-DNP.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Redirecting data to improve page locality in a scalable data fabric

A data processing system includes a host processor, a local memory coupled to the host processor, a plurality of remote memory media, and a scalable data fabric coupled to the host processor and to the plurality of remote memory media. The scalable data fabric includes a filter for storing information indicating a location of data that is stored by the data processing system. The host processor includes a hardware sequencer coupled to the filter for selectively moving data stored by the filter to the local memory.

97 MATHEMATICS AND COMPUTING↗

Capturing Coupled Structural and Electronic Motions During Excited-State Intramolecular Proton Transfer via Computational Multiedge Resonant Inelastic X-ray Scattering

Proton-transfer processes build the foundation of many chemical processes. In Excited State Intramolecular Proton Transfer (ESIPT) processes the proton transfer process is impulsively started through light. Here, in this study, we explore the changes in coupled atomic and electronic motions during and following ESIPT through computational time-resolved Resonant Inelastic X-ray Scattering (trRIXS). Excited-state Ab Initio Molecular Dynamics (AIMD) simulations combined with Time-Dependent Density Functional Theory (TDDFT) calculations were performed for 10-hydroxybenzo[h]quinoline to obtain trRIXS signatures. RIXS at both the nitrogen and oxygen K-edges were computed to resolve the dynamics electronic structure from both the proton donor and acceptor perspective. The results show how RIXS can reveal the local electronic structure, the coupling between different electronic states and how electronic structure and coupling change during the proton transfer process. Additionally, we observe a strong correlation between spectral changes and structural changes during ESIPT.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗