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DOE OSTI2024

High repetition-rate pulse shaping of a spectrally broadened Yb femtosecond laser

We demonstrate compression and shaping of few cycle pulses from a high average power ytterbium laser system. The pulses from a commercial 20 W, 100 kHz Yb laser system are spectrally broadened in two-stages using cascaded, gas-filled, stretched hollow-core fibers and then compressed and shaped in an acousto-optic modulator-based pulse-shaper. The pulse-shaper allows for compression, characterization, and shaping all in one system, producing ∼10 fs pulses with 30 μ J of energy.

Codere, Julia↗

DOE OSTI2023

Flexible tape-drive target system for secondary high-intensity laser-driven sources

Here, we present the development of a flexible tape-drive target system to generate and control secondary high-intensity laser-plasma sources. Its adjustable design permits the generation of relativistic MeV particles and x rays at high-intensity (i.e., ≥1 × 10 18 W cm —2 ) laser facilities, at high repetition rates (>1 Hz). The compact and robust structure shows good mechanical stability and a high target placement accuracy (<4 μm RMS). Its compact and flexible design allows for mounting in both the horizontal and vertical planes, which makes it practical for use in cluttered laser-plasma experimental setups. The design permits ~170° of access on the laser-driver side and 120° of diagnostic access at the rear. A range of adapted apertures have been designed and tested to be easily implemented to the targetry system. The design and performance testing of the tape-drive system in the context of two experiments performed at the COMET laser facility at the Lawrence Livermore National Laboratory and at the Advanced Lasers and Extreme Photonics (ALEPH) facility at Colorado State University are discussed. Experimental data showing that the designed prototype is also able to both generate and focus high-intensity laser-driven protons at high repetition rates are also presented.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2025

Advancing X-ray quantum imaging through Monte-Carlo simulations

Imaging with X-rays poses fundamental limits due to radiation damage of the highly energetic photons. This becomes problematic for sensitive biological systems such as subcellular structures. Lowering the radiation dose, without sacrificing the signal-to-noise ratio, would be desirable for any kind of imaging modalities involving X-rays. To achieve this goal, quantum imaging with entangled X-ray photons constitutes a promising route. Production of biphotons have been demonstrated in the X-ray regime by the process of Spontaneous Parametric Down-Conversion (SPDC). However, compared to SPDC in the regime of visible light, the production rate for X-ray biphotons is extremely low. With the introduction of new high average brightness X-ray sources, such as 4th generation synchrotrons and high repetition rate Free-Electron X-ray Lasers (XFEL), quantum imaging may become practical. We introduce a ray tracing approach using Monte-Carlo sampling, specifically designed for quantum imaging with entangled X-ray photons generated by SPDC. By simulation, the superior image quality of quantum over classical imaging methods is demonstrated using realistic experimental conditions available at high repetition rate XFELs. With these simulations, we can efficiently assist the design of future experiments at beam lines, which can substantially accelerate the advancement of X-ray quantum imaging and reduce costs.

Entangled Photons↗

NASA NTRSDate not supplied

TPSAS-NF1676L-11930-DND

Under the NASA Laser Risk Reduction Program (LRRP), funded by Earth Science Technology Office (ESTO), an efficient, injection seeded, high repetition rate Tm:fiber laser pumped Ho:YLF laser has been developed and operation between 100 Hz to 10 kHz has been demonstrated. The work is underway to develop an efficient, high-repetition-rate, pulsed, 2-micron, coherent Differential Absorption Lidar (DIAL) / Integrated Path Differential Absorption (IPDA) instrument for measuring the atmospheric CO2 profiles (DIAL) and column densities (IPDA) from an airborne platform. In DIAL mode, this instrument will provide the first ever range-resolved, high-precision, remote measurements of the CO2 content of the atmospheric boundary layer (ABL) and lower troposphere.

Upendra N Singh↗

DOE OSTI2025

The Impact of Carotenoid Energy Levels on the Exciton Dynamics and Singlet–Triplet Annihilation in Isolated Bacterial Light-Harvesting 2 Complexes

The light-harvesting 2 (LH2) complex of purple phototrophic bacteria plays a critical role in absorbing solar energy and distributing the excitation energy. Exciton dynamics within LH2 complexes are controlled by the structural arrangement and energy levels of the bacteriochlorophyll (BChl) and carotenoid (Car) pigments. However, there is still debate over the competing light-harvesting versus energy-dissipation pathways. In this work, we compared five variants of the LH2 complex from genetically modified strains of Rhodobacter sphaeroides, all containing the same BChls but different Cars with increasing conjugation: zeta-carotene (N = 7; LH2 Zeta ), neurosporene (N = 9; LH2 Neu ), spheroidene (N = 10; LH2 Spher ), lycopene (N = 11; LH2 Lyco ), and spirilloxanthin (N = 13; LH2 Spir ). Absorption measurements confirmed that the Car excited-state energy decreased with increasing conjugation. Similarly, fluorescence spectra showed that the B850 BChl emission peak had an increasing red shift from LH2 Zeta →(LH2 Neu /LH2 Spher )→LH2 Lyco →LH2 Spir . In contrast, time-resolved fluorescence and ultrafast transient absorption (fs-TA) revealed similar excited-state lifetimes (∼1 ns) for all complexes except LH2 Spir (∼0.7 ns). From fs-TA analysis, an additional ∼7 ps nonradiative dissipation step from B850 BChl was observed for LH2 Zeta . Further, singlet− singlet and singlet−triplet annihilation studies showed a ∼50% average fluorescence lifetime reduction in LH2Zeta at high laser power and high repetition rate, compared to ∼10−15% reductions in LH2 Neu /LH2 Spher /LH2 Lyco and minimal lifetime change in LH2 Spir . In LH2 Zeta , the fastest decay component (<50 ps) became prominent at high repetition rates, consistent with strong singlet−triplet annihilation. Nanosecond TA measurements revealed long-lived (>40 μs) BChl triplet states in LH2 Zeta and signs of damage caused by singlet oxygen, whereas other LH2s showed faster triplet quenching (∼18 ns) by Cars. These findings highlight a key design principle of LH2 complexes: the Car triplet energy must be significantly lower than the BChl triplet energy to efficiently quench BChl triplets that otherwise act as potent “trap states,” causing exciton annihilation in laser-based experiments or photodamage in native membranes.

Absorption↗

DOE OSTI2024

Compact, ultrastable, high repetition-rate 2 μm and 3 μm fiber laser for seeding mid-IR OPCPA

We report a compact and reliable ultrafast fiber laser system optimized for seeding a high energy, 2 μ m pumped, 3 μ m wavelength optical parametric chirped pulse amplification to drive soft X-ray high harmonics. The system delivers 100 MHz narrowband 2 μ m pulses with >1 nJ energy, synchronized with ultra-broadband optical pulses with a ∼1 μ m FWHM spectrum centered at 3 μ m with 39 pJ pulse energy. The 2 μ m and 3 μ m pulses are derived from a single 1.5 μ m fiber oscillator, fully fiber integrated with free-space downconversion for the 3 μ m. The system operates hands-off with power instabilities <0.2% over extended periods of time.

Optics↗

DOE OSTI2024

Laboratory Study of Magnetic Reconnection in Lunar-relevant Mini-magnetospheres

Abstract Mini-magnetospheres are small ion-scale structures that are well suited to studying kinetic-scale physics of collisionless space plasmas. Such ion-scale magnetospheres can be found on local regions of the Moon, associated with the lunar crustal magnetic field. In this paper, we report on the laboratory experimental study of magnetic reconnection in laser-driven, lunar-like ion-scale magnetospheres on the Large Plasma Device at the University of California, Los Angeles. In the experiment, a high-repetition rate (1 Hz), nanosecond laser is used to drive a fast-moving, collisionless plasma that expands into the field generated by a pulsed magnetic dipole embedded into a background plasma and magnetic field. The high-repetition rate enables the acquisition of time-resolved volumetric data of the magnetic and electric fields to characterize magnetic reconnection and calculate the reconnection rate. We notably observe the formation of Hall fields associated with reconnection. Particle-in-cell simulations reproducing the experimental results were performed to study the microphysics of the interaction. By analyzing the generalized Ohm’s law terms, we find that the electron-only reconnection is driven by kinetic effects through the electron pressure anisotropy. These results are compared to recent satellite measurements that found evidence of magnetic reconnection near the lunar surface.

Astronomy & Astrophysics↗

DOE OSTI2021

Bandwidth extension and conversion efficiency improvements beyond phase matching limitations using cavity-enhanced OPCPA

The conversion efficiency and phase matching bandwidth of ultrafast optical parametric amplification (OPA) are constrained by the dispersion and nonlinear coefficient of the employed crystal as well as pulse shaping effects. In our work we show that an enhancement cavity resonant with the pump seeded at the full repetition rate of the pump laser can automatically reshape the small-signal gain in optical parametric chirped-pulse amplification (OPCPA) to achieve close-to-optimal operation. This new method termed cavity-enhanced OPCPA or C-OPCPA significantly increases both the gain bandwidth and the conversion efficiency, in addition to boosting gain for high-repetition-rate amplification. The goal in C-OPCPA is to arrive at a condition of impedance matching at all temporal coordinates, such that, in the absence of linear losses, all the incident pump power is dissipated in the nonlinear loss element, i.e., converted to signal and idler. The use of a low finesse enhancement cavity resonant with a low average power (<1W) and a high repetition rate (78MHz) pump source is shown to achieve more than 50% conversion efficiency into signal and idler from the coupled pump in an optical parametric process, whereas an equivalent amount of pump power in a single-pass configuration leads to negligible conversion. Additionally, the gain bandwidth is extended by a factor of 3-4 beyond the phase-matching limit. Our empirical observations are corroborated by a numerical analysis of depletion optimizing the single-pass case, which assesses the underlying impedance matching that is responsible for the observed performance improvements.

47 OTHER INSTRUMENTATION↗

DOE OSTI2022

Use of diamond sensors for a high-flux, high-rate X-ray pass-through diagnostic

X-ray free-electron lasers (XFELs) deliver pulses of coherent X-rays on the femtosecond time scale, with potentially high repetition rates. While XFELs provide high peak intensities, both the intensity and the centroid of the beam fluctuate strongly on a pulse-to-pulse basis, motivating high-rate beam diagnostics that operate over a large dynamic range. The fast drift velocity, low X-ray absorption and high radiation tolerance properties of chemical vapour deposition diamonds make these crystals a promising candidate material for developing a fast (multi-GHz) pass-through diagnostic for the next generation of XFELs. A new approach to the design of a diamond sensor signal path is presented, along with associated characterization studies performed in the XPP endstation of the LINAC Coherent Light Source (LCLS) at SLAC. Qualitative charge collection profiles (collected charge versus time) are presented and compared with those from a commercially available detector. Quantitative results on the charge collection efficiency and signal collection times are presented over a range of approximately four orders of magnitude in the generated electron–hole plasma density.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

NASA NTRSDate not supplied

Time-Resolved OH-PLIF Assessment of Deflagrations Levels in a CH4-O2 Rotating Detonation Rocket Combustor

The parasitic loss incurred by deflagrative pre-burning is considered to be one of the key challenges to the effective implementation of rotating detonation engine (RDE) systems. Thus far, there have been relatively limited high fidelity, spatio-temporally resolved measurements of the pre-burning process as a function of the reactant conditions and composition within an RDE. In this work, simultaneous high-repetition-rate broadband OH* chemiluminescence and OH planar laser-induced fluorescence (PLIF) imaging are employed to investigate deflagrative burning dynamics in a fully optically accessible CH4-O2 RDE as compared to a H2-air systems under the same conditions. A custom-built optical parametric oscillator (OPO) is coupled with a high-repetition-rate burst-mode laser to generate the 284 nm source for the excitation of the Q1(9) transition of the OH radical. Significant deflagrative burning is observed throughout the chamber as a consequence of the oxygen-rich environment. Trailing wave systems that consume unburned reactants in the region immediately following the primary detonation wave are observed. The formation of a product gas recirculation zone that entrains and combusts incoming reactants is observed, and quantitative analysis is performed to gain valuable insight into deflagration characteristics. At an oxidizer mass flux of Gox ≈ 350kg/m2/s, it is found that the levels of pre-wave burning in CH4-O2 are a factor of ∼2-3 times higher than in H2-air in the region directly ahead of the detonation wave at a global equivalence ratio Φ ≈ 1.0. This study highlights the key roles of ignition delay and turbulent mixing of the combustion product and reactant fields on the levels of pre-burning and establishes a methodology for further investigation, such as for the effects of various RDE inlet configurations.

Propulsion↗

NASA NTRS1983

The development, performance, and potential application of the copper halide laser

The copper halide laser (CHL) is an efficient gas discharge laser that emits short pulses at two discrete wavelengths in the yellow and green spectral region. The laser pulse results from transitions in excited copper atoms. The CHL has produced pulses of up to 10 mJ in a double-pulsed mode at low repetition rates and has been operated at very high repetition rates (8 to over 35 kHz) in a continuously pulsed mode with a maximum average-power of 15 watts. In this paper, the development of the copper halide laser is reviewed along with a brief description of the copper laser operating principles. In the final section, a number of applications of the CHL are identified.

Pivirotto, T. J.↗

DOE OSTI2024

Toward electron temperature profiles in hot-dense plasmas from x-ray spectral ensembles

High repetition rate laser systems enable new strategies for diagnosing plasma behavior with large datasets. Here, we define an ensemble technique that relies on randomized targeting of x-ray tracer micro-stripes. On each shot, a high-intensity laser pulse is focused on a solid target with Ti tracer stripes embedded in an Al foil, randomly targeting a micro-stripe, a portion of a stripe, or a gap between stripes. High-resolution, time-integrated x-ray spectrometers capture line emission from the portion of the micro-stripe that is heated to sufficiently high electron temperatures. Accumulation of many such cases is used to construct ensemble distributions of x-ray line intensities that encompass all relative offsets of the laser focus to the micro-stripe centers. Synthetic intensity distributions are likewise generated using collisional-radiative modeling. Bayesian fitting of modeled to measured intensity distributions establishes the most likely radial temperature profiles, enabling comparison to hydrodynamic models and calling into question the cylindrical symmetry of these micro-stripe-embedded systems. Ensemble techniques have significant potential for high-energy-density plasma diagnostics, especially with the advent of high repetition rate experiments.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2020

High resolution time- and angle-resolved photoemission spectroscopy with 11 eV laser pulses

Performing time- and angle-resolved photoemission (tr-ARPES) spectroscopy at high momenta necessitates extreme ultraviolet laser pulses, which are typically produced via high harmonic generation (HHG). Despite current advances, HHG-based setups still require large pulse energies (from hundreds of μ J to mJ) and their energy resolution is limited to tens of meV. Here, we present a novel 11 eV tr-ARPES setup that generates a flux of 5 × 10 10 photons/s and achieves an unprecedented energy resolution of 16 meV. It can be operated at high repetition rates (up to 250 kHz) while using input pulse energies down to 3 µ J. We demonstrate these unique capabilities by simultaneously capturing the energy and momentum resolved dynamics in two well-separated momentum space regions of a charge density wave material ErTe 3 . This novel setup provides the opportunity to study the non-equilibrium band structure of solids with exceptional energy and time resolutions at high repetition rates.

47 OTHER INSTRUMENTATION↗

DOE OSTI2026

Collisionless Larmor coupling and blob formation in a laser-plasma expanding into a magnetized ambient plasma

Collisionless Larmor coupling is a fundamental process in space and astrophysical plasmas that enables momentum transfer between an expanding plasma and a magnetized ambient medium. Here, in this paper, we report on the laboratory experimental study of Larmor coupling leading to the formation of a plasma blob associated with a laser-driven, super-Alfvénic plasma flow on the Large Plasma Device at the University of California, Los Angeles. The high-repetition rate enables systematic spatial and temporal scans of the plasma evolution using Doppler spectroscopy, as well as measurements of the magnetic field, electrostatic field, and self-emission of both debris and ambient ions using filtered imaging. We observe the self-focusing of the laser-produced plasma and the formation of a secondary diamagnetic cavity associated with a blob composed of background ions. Doppler spectroscopy reveals the transverse velocity distribution of the background ions, providing direct evidence of ion energization via Larmor coupling. The systematic spatial and temporal scans enabled by the high-repetition-rate experiment allow for a detailed characterization of the ion dynamics. These experimental observations are supported by numerical simulations that provide more insight into the kinetic-scale physics associated with blob formation as well as the role of the ambient plasma density.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Low Repetition-Rate, High-Resolution Femtosecond Transmission Electron Microscopy

Spatial and energy resolutions of state-of-the-art transmission electron microscopes (TEMs) have surpassed 50 pm and 5 meV. However, with respect to the time domain, even the fastest detectors combined with the brightest sources may only be able to reach the microsecond timescale. Thus, conventional methods are incapable of resolving myriad fundamental ultrafast (i.e., attosecond to picosecond) atomic-scale dynamics. The successful demonstration of femtosecond (fs) laser-based (LB) ultrafast transmission electron microscopy (UEM) nearly 20 years ago provided a means to span this nearly 10-order-of-magnitude temporal gap. While nanometer-picosecond UEM studies of dynamics are now well established, ultrafast Å-scale imaging has gone largely unrealized. Further, while instrument development has rightly been an emphasis, and while new modalities and uses of pulsed-beam TEM continue to emerge, the overall chemical and materials application space has been only modestly explored to date. In this Perspectives article, we argue that these apparent shortfalls can be attributed to a simple lack of data and detail. We speculate that present work and continued growth of the field will ultimately lead to the realization that Å-scale fs dynamics can indeed be imaged with minimally modified UEM instrumentation and with repetition rates (f rep ) below - and perhaps even well below - 1 MHz. We further argue that use of low f rep , whether for LB UEM or for chopped/bunched beams, significantly expands the accessible application space. Furthermore, this calls for systematically establishing modality-specific limits so that especially promising technologies can be pursued, thus ultimately facilitating broader adoption as individual instrument capabilities expand.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2011

Multi-Wavelength, Multi-Beam, and Polarization-Sensitive Laser Transmitter for Surface Mapping

A multi-beam, multi-color, polarized laser transmitter has been developed for mapping applications. It uses commercial off-the-shelf components for a lowcost approach for a ruggedized laser suitable for field deployment. The laser transmitter design is capable of delivering dual wavelengths, multiple beams on each wavelength with equal (or variable) intensities per beam, and a welldefined state of polarization. This laser transmitter has been flown on several airborne campaigns for the Slope Imaging Multi-Polarization Photon Counting Lidar (SIMPL) instrument, and at the time of this reporting is at a technology readiness level of between 5 and 6. The laser is a 1,064-nm microchip high-repetition-rate laser emitting energy of about 8 microjoules per pulse. The beam was frequency-doubled to 532 nm using a KTP (KTiOPO4) nonlinear crystal [other nonlinear crystals such as LBO (LiB3O5) or periodically poled lithium niobiate can be used as well, depending on the conversion efficiency requirements], and the conversion efficiency was approximately 30 percent. The KTP was under temperature control using a thermoelectric cooler and a feedback monitoring thermistor. The dual-wavelength beams were then spectrally separated and each color went through its own optical path, which consisted of a beam-shaping lens, quarterwave plate (QWP), and a birefringent crystal (in this case, a calcite crystal, but others such as vanadate can be used). The QWP and calcite crystal set was used to convert the laser beams from a linearly polarized state to circularly polarized light, which when injected into a calcite crystal, will spatially separate the circularly polarized light into the two linear polarized components. The spatial separation of the two linearly polarized components is determined by the length of the crystal. A second set of QWP and calcite then further separated the two beams into four. Additional sets of QWP and calcite can be used to further split the beams into multiple orders of two. The spatially separated beams had alternating linearly polarization states; a half-wave plate (HWP) array was then made to rotate the alternating states of A multi-beam, multi-color, polarized laser transmitter has been developed for mapping applications. It uses commercial off-the-shelf components for a lowcost approach for a ruggedized laser suitable for field deployment. The laser transmitter design is capable of delivering dual wavelengths, multiple beams on each wavelength with equal (or variable) intensities per beam, and a welldefined state of polarization. This laser transmitter has been flown on several airborne campaigns for the Slope Imaging Multi-Polarization Photon Counting Lidar (SIMPL) instrument, and at the time of this reporting is at a technology readiness level of between 5 and 6. The laser is a 1,064-nm microchip high-repetition-rate laser emitting energy of about 8 microjoules per pulse. The beam was frequency-doubled to 532 nm using a KTP (KTiOPO4) nonlinear crystal [other nonlinear crystals such as LBO (LiB3O5) or periodically poled lithium niobiate can be used as well, depending on the conversion efficiency requirements], and the conversion efficiency was approximately 30 percent. The KTP was under temperature control using a thermoelectric cooler and a feedback monitoring thermistor. The dual-wavelength beams were then spectrally separated and each color went through its own optical path, which consisted of a beam-shaping lens, quarterwave plate (QWP), and a birefringent crystal (in this case, a calcite crystal, but others such as vanadate can be used). The QWP and calcite crystal set was used to convert the laser beams from a linearly polarized state to circularly polarized light, which when injected into a calcite crystal, will spatially separate the circularly polarized light into the two linear polarized components. The spatial separation of the two linearly polarized components is determined by the length of the crystal. A cond set of QWP and calcite then further separated the two beams into four. Additional sets of QWP and calcite can be used to further split the beams into multiple orders of two. The spatially separated beams had alternating linearly polarization states; a half-wave plate (HWP) array was then made to rotate the alternating states of

Yu, Anthony W.↗

DOE OSTI2023

Multi-scale time-resolved electron diffraction: A case study in moiré materials

Ultrafast-optical-pump — structural-probe measurements, including ultrafast electron and x-ray scattering, provide direct experimental access to the fundamental timescales of atomic motion, and are thus foundational techniques for studying matter out of equilibrium. High-performance detectors are needed in scattering experiments to obtain maximum scientific value from every probe particle. Here we deploy a hybrid pixel array direct electron detector to perform ultrafast electron diffraction experiments on a WSe 2 /MoSe 2 2D heterobilayer, resolving the weak features of diffuse scattering and moiré superlattice structure without saturating the zero order peak. Enabled by the detector’s high frame rate, we show that a chopping technique provides diffraction difference images with signal-to-noise at the shot noise limit. Finally, we demonstrate that a fast detector frame rate coupled with a high repetition rate probe can provide continuous time resolution from femtoseconds to seconds, enabling us to perform a scanning ultrafast electron diffraction experiment that maps thermal transport in WSe 2 /MoSe 2 and resolves distinct diffusion mechanisms in space and time.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Foreword to special issue: Papers from the 63rd annual meeting of the APS Division of Plasma Physics, November 8–12, 2021

The 63rd annual meeting of the APS Division of Plasma Physics (DPP) was held on November 8–12, 2021 in Pittsburgh at the David Lawrence Convention Center with both a live (in person) component and a virtual component. Following guidance from an APS COVID task force, all in-person attendees were fully vaccinated and masked. More than 800 physicists attended, safely, in-person. With both virtual and on-site participants, discussions were lively, and the research presentations showed unmatched mastery in the modern observation, theory, simulation, and manipulation of plasma. The presentations included four invited review talks, 97 invited talks, four tutorials, and four presentations from this year's prize and award recipients. There were more than 1200 contributed poster presentations and 725 contributed oral presentations. Including both in-person and remote attendees, DPP 2021 had a record of 2232 participants. As a hybrid meeting, in-person presentations of all invited presentations were broadcast live and were accompanied by a Q&A discussion. Contributed oral and poster presentations were prerecorded along with options to schedule in-person discussions on demand. Five mini-conferences were held: “Gatekeeper Workshop: Creating a Diverse, Equitable, and Inclusive Pipeline,” “Collisionless Shocks in Laboratory and Space Plasmas,” “The High Repetition Rate Frontier in High-Energy-Density Physics,” “Measuring and Modeling Plasma Surface Interactions,” and “The Second Mini-Conference on Machine Learning, Data Science and Artificial Intelligence in Plasma Research.” Finally, on the day before the official start of the meeting, an afternoon “for students, by students” included lightning talks, plasma trivia, and an informal occasion to connect with other students, learn how to get the most from the DPP Annual Meeting, and share successful ways to connect with colleagues and advance their professional careers.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗