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At least 37 records · Page 2

Advances in the photon avalanche luminescence of inorganic lanthanide-doped nanomaterials

Photon avalanche (PA)—where the absorption of a single photon initiates a ‘chain reaction’ of additional absorption and energy transfer events within a material—is a highly nonlinear optical process that results in upconverted light emission with an exceptionally steep dependence on the illumination intensity. Over 40 years following the first demonstration of photon avalanche emission in lanthanide-doped bulk crystals, PA emission has been achieved in nanometer-scale colloidal particles. The scaling of PA to nanomaterials has resulted in significant and rapid advances, such as luminescence imaging beyond the diffraction limit of light, optical thermometry and force sensing with (sub)micron spatial resolution, and all-optical data storage and processing. In this review, we discuss the fundamental principles underpinning PA and survey the studies leading to the development of nanoscale PA. Finally, we offer a perspective on how this knowledge can be used for the development of next-generation PA nanomaterials optimized for a broad range of applications, including mid-IR imaging, luminescence thermometry, (bio)sensing, optical data processing and nanophotonics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Coupling to rotational manifolds to improve gas-phase pump–probe spectroscopic models

The physical picture of gas-phase optical transitions is normally presented as an isolated two-level system balanced by upward and downward processes. Isolated models assume a phenomenological treatment of collisional dephasing but do not strictly account for collisional population exchange with the rotational baths. While this assumption is valid under low-intensity conditions, where excitation is rate-limiting, isolated models can deviate from Beer’s Law at sufficient pressures and monochromatic intensities when both collisional broadening and power broadening are comparable to (or greater than) lifetime broadening, which are not uncommon conditions for cavity enhanced spectroscopies in the mid-IR spectral range. Although this problem has been addressed by rate-equation models for linear absorption measurements, a general treatment for multi-level quantum mechanical models suitable for non-linear absorption measurements (two-photon/two-color/pump–probe) is lacking. Isolated models require physical parameter inputs that disagree with expected values by at least an order of magnitude. These non-physical models undermine the ability to predict non-linear signal strengths under untested conditions and thereby limit the potential to optimize the sensitivity of non-linear spectroscopies and to expand their analytical applications (e.g., new analytes and/or buffer gases, changes in cavity free-spectral-range, changes in intracavity powers or wavelengths, and accurate investigation of physical phenomena). In this study, we derive bath-coupled models for gaseous pump–probe spectroscopy by application of the quantum Lindblad equation and detailed balance. Bath-coupled models are shown to fit data consistently across variations in intensity and agree with all physically expected values.

Cavity ring-down spectroscopy↗

Soft x-ray high-harmonic generation in an anti-resonant hollow core fiber driven by a 3 μ m ultrafast laser

High-harmonic upconversion driven by a mid-infrared femtosecond laser can generate coherent soft x-ray beams in a tabletop-scale setup. Here, we report on a compact ytterbium-pumped optical parametric chirped pulse amplifier (OPCPA) laser system seeded by an all-fiber front-end and employing periodically poled lithium niobate (PPLN) nonlinear media operated near the pulse fluence limits of current commercially available PPLN crystals. The OPCPA delivers 3 µm wavelength pulses with 775 µJ energy at 1 kHz repetition rate, with transform-limited 120 fs pulse duration, diffraction-limited beam quality, and ultrahigh 0.33% rms energy stability over >18 h. Using this laser, we generate soft x-ray high harmonics (HHG) in argon gas by focusing into a low-loss, high-pressure gas-filled anti-resonant hollow core fiber (ARHCF), generating coherent light at photon energies up to the argon L-edge (250 eV) and carbon K-edge (284 eV), with high beam quality and ∼1% rms energy stability. This work demonstrates soft x-ray HHG in a high-efficiency guided-wave phase matched geometry, overcoming the high losses inherent to mid-IR propagation in unstructured waveguides, or the short interaction lengths of gas cells or jets. The ARHCF can operate in the long term without damage and with the repetition rate, stability, and robustness required for demanding applications in spectromicroscopy and imaging. Finally, we discuss routes for further optimizing the soft x-ray HHG flux by driving He at higher laser intensities using either the signal (1.5 μm) or idler wavelengths (3 μm).

Femtosecond lasers↗

Remote detection of radioactive material using a short-pulse CO 2 laser

Detection of radioactive material at distances greater than the radiated particle range is an important goal with applications in areas such as national defense and disaster response. Here, we demonstrate avalanche-breakdown-based remote detection of a 3.6 mCi α-particle source at a standoff distance of 10 m, using 70 ps, long-wave infrared (λ = 9.2 µm) CO 2 laser pulses. This is ∼10 times longer than our previous results using a mid-IR laser. The primary detection method is direct backscatter from microplasmas generated in the laser focal volume. The backscatter signal is amplified as it propagates back through the CO 2 laser chain, enhancing sensitivity by >100 times. Here we also characterize breakdown plasmas with fluorescence imaging, and present a simple model to estimate backscattered signals as a function of the seed density profile in the laser focal volume. All of this is achieved with a relatively long-drive laser focal geometry (f/200) that is readily scalable to >100 m.

43 PARTICLE ACCELERATORS↗

One-dimensional mapping of femtosecond laser filaments using coherent microwave scattering

Here, this paper reports on the use of coherent microwave scattering (CMS) for spatially resolved electron number density measurements of elongated plasma structures induced at mid-IR femtosecond filamentation in air. The presented studies comprise one-dimensional mapping of laser filaments induced via 3.9 µm, 127.3 fs laser pulses at output energies up to 15 mJ. The axial electron number density was measured to be invariant (about 2 × 10 15 c⁢m −3 ) along the entire filament length and for all tested laser pulse energies 5–15 mJ, and the corresponding laser intensity in the middle portion of the filament was estimated to be nearly constant for 5–15 mJ pulse energies (about 30−40 TW/c⁢m 2 ). These findings support that intensity clamping conditions were achieved in the experiments. The proposed approach enables capabilities that are currently unavailable to perform absolute and longitudinally resolved measurements of electron number density in laser filaments and to precisely characterize conditions associated with self-focusing and intensity clamping.

plasma diagnostic techniques↗

Amplification of 10 μm picosecond pulses in a compact optically pumped multiatmosphere CO 2 laser

Picosecond pulses, generated by a commercial mid-IR optical parametric source (∼0.5 ps, 1-5 μJ), have been regeneratively amplified to an energy of ≤2 mJ in a palm-size high-pressure CO 2 amplifier optically pumped by a Q-switched 2.8 μm Cr:Er:YSGG laser. The characteristics of the amplified pulses have been studied as a function of seed wavelength centered around 10.3 or 10.6 μm, and the pressure in the gain medium. The measured amplified pulse length is ∼5 ps. Numerical modeling suggests that pulses as short as ∼0.5 ps with multi-GW peak power can be generated in a mixture of CO 2 isotopes. Robustness of the output of a compact CO 2 regenerative amplifier to the seed and pump fluctuations measured at 3 Hz and a perfect Gaussian beam profile indicates the potential of such laser technology for producing high-power ultrashort long-wave infrared pulses at high repetition rates.

43 PARTICLE ACCELERATORS↗

Ultrafast optical modulation of vibrational strong coupling in ReCl(CO) 3 (2,2-bipyridine)

Polaritons – hybrid light-matter states formed from the strong coupling of a bright molecular transition with a confined photonic mode – may offer new opportunities for optical control of molecular behavior. Vibrational strong coupling (VSC) has been reported to impact ground-state chemical reactivity, but its influence on electronic excited-state dynamics remains unexplored. Here, we take a first step towards excited-state VSC by demonstrating optical modulation of the ReCl(CO) 3 (bpy), (bpy = 2,2-bipyridine) complex under VSC using femtosecond ultraviolet (UV)-pump/infrared (IR)-probe spectroscopy. We establish ground-state VSC of ReCl(CO) 3 (bpy) in a microfluidic Fabry-Pérot cavity equipped with indium tin oxide (ITO)-coated mirrors. ITO is effectively dichroic as it is reflective in the IR and transmissive in the UV-visible and therefore minimizes optical interference. Excitation with UV pump light drives ReCl(CO) 3 (bpy) into a manifold of electronic excited states that subsequently undergo non-radiative relaxation dynamics. We probe the transient response of the strongly-coupled system in the mid-IR, observing both Rabi contraction and cavity-filtered excited-state absorption signatures. We reconstruct the intrinsic response of intracavity molecules from the transient cavity transmission spectra to enable quantitative comparison with extracavity control experiments. We report no changes in the excited-state dynamics of ReCl(CO) 3 (bpy) under ground-state VSC. However, we do observe significant amplification of transient vibrational signals due to classical cavity-enhanced optical effects. This effort lays the groundwork to pursue direct excited-state VSC aimed at modulating photochemical reactivity.

cavity-enhanced spectroscopy↗

A Comparison of Three Neodymium Atomic Data Sets for Kilonova Modeling

We examine the impact of input neodymium (Nd) atomic data on the light curves and spectra of kilonovae (KNe), probing the sensitivity of kilonova observables to the atomic physics of this important lanthanide element. We use the SuperNu Monte Carlo radiative transfer code, simulating a simple semianalytic 1D kilonova (KN) with a pure Nd atmosphere, fixing the radiative transfer method while using input atomic data generated by three different codes: the LANL suite of atomic physics codes, HULLAC, and Autostructure. We see that the choice of atomic data significantly shapes the resulting light curves and spectra. Peak bolometric luminosities differ by a ratio of nearly 1.5 between HULLAC/Autostructure and LANL data sets. Moreover, we observe significant near- to mid-IR differences in the structure of the spectra. We specifically attribute these differences to the choice of atomic data for neutral Nd I. Many of the results here have been adapted from a presentation at “Radiative Transfer and Atomic Physics of Kilonovae” in Stockholm, 2023. We additionally present a LANL data set with energies calibrated to available values in the NIST Atomic Spectra Database, and demonstrate that this calibration also significantly affects IR spectral structure at late time. The substantial differences in KN observables that arise from tuning the atomic data of just one lanthanide element highlight the special attention that must be paid to atomic physics uncertainties when modeling KNe, from AT2017gfo to beyond.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

JWST Observations of Starbursts: Dust Processing in the M82 Superwind

We present JWST MIRI and NIRCam imaging of the inner ∼5 kpc of the M82 superwind at ~ $0''_{.}05 - 0''_{.}375$(∼0.9–6.5 pc) resolution. Targeted filters probe emission from polycyclic aromatic hydrocarbons (PAHs; F335M, F360M, F770W, F1130W) and continuum (F250M, F360M) The images reveal a network of cool wind filaments traced by PAHs. PAH surface brightness declines with the inverse square of distance to the midplane, suggesting that the incident radiation field from the starburst drives the observed PAH intensity out to ±2.5 kpc. The 3.3/11.3 and 3.3/7.7 μm band ratios show uniformity with distance from the starburst, though comparisons with mid-IR dust emission models indicate a modest shift toward larger PAHs. Outside the disk, 11.3/7.7 μm increases moderately, reflecting that PAHs become more neutral with distance from the starburst as they are exposed to a declining radiation field and ionization parameter. Overall, PAHs in the wind are consistent with standard-to-large sizes and standard-to-high ionization states. Including Spitzer and Herschel data, PAH abundance (q PAH ) is set at ∼1% in the starburst and remains unchanging out to ±5 kpc off the disk. This flat q PAH profile suggests that PAHs are shielded from the hot wind, perhaps residing in the surface layers of cool clouds, with possible replenishment from cloud interiors and enrichment of the halo from previous bursts. In this picture, clouds are not dense enough to promote PAH growth, and they likely undergo radiative cooling and mixing with the hot phase to survive the gauntlet for at least ∼20 Myr.

Cronin, Serena A. [University of Maryland, College↗

The role of earth-based observations of asteroids during the next decade

Present reconnaissance studies of asteroids shift ground based programs to more specialized, intensive studies of selected individual bodies and special classes. Two powerful techniques--radar and mid-IR spectroscopy--have yet to be widely applied to asteroids; high priority should be given to: (1) search programs with a large Schmidt telescope (especially for Mars- and Earth-approaching bodies); (2) a moderate resolution visible and near-IR spectrophotometric survey of at least half the asteroids; (3) high resolution spectrophotometry and radiometry of unusual objects; (4) radar studies of representative main belt asteroids; and (5) application of the full complement of astrophysical techniques to objects of high scientific interest and to potential space mission targets. The infrared astronomical satellite also has high potential for contributing to asteroid science.

Chapman, C. R.↗

Infrared and optical measurements of the ionized gas in K3-50

Results are reported for optical, near-IR, and mid-IR spectrophotometry of the compact H II region K3-50A. The emission-line observations imply an electron density of about 100,000 per cu cm; the consistency of density measurements in the optical, IR, and radio sources suggests that the optical counterpart of K3-50A is a reflection nebula. Previous measurements of the anomalous extinction law in K3-50A are confirmed, this law is extended out to B-alpha at 4 microns, and a 9-micron optical depth of about 2.5 is obtained. Elemental abundances are derived from measurements of emission lines of several dominant ions of the same element and found to be in close agreement (50%) with mean cosmic abundances. Individual ionic ratios are compared with model H II region calculations to determine the nature of the ionizing radiation. It is concluded that if nongray UV dust absorption does not modify the spectrum appreciably, the radiation temperature can be associated with a stellar surface temperature of about 37,000 K, corresponding to an O6 supergiant.

Lester, D. F.↗

Integrated band intensities of gaseous N/2/O/5/

Values for mid-IR integrated band intensities of gaseous N2O5 were determined at room temperature. The absorptions studied were at 1720, 1246, 743, and 557/cm. The integrated intensities were 2204, 581, 685, and 699/atm cm, respectively. Implications of these results for the stratospheric detection of N(2)O(5) are discussed.

Lovejoy, R. W.↗

Thematic Mapper Data Quality and Performance Assessment in Renewable Resources/agriculture Remote Sensing

It is believed that the increased spatial resolution will provide solutions to proportion estimation error due to mixed pixels, and the increased spectral resolution will provide for the identification of important agricultural features such as crop stage, and condition. The results of analyses conducted relative to these hypothesis from sample segments extracted from the 4-band Detroit scene and the 7-band Mississippi County, Arkansas engineering test scene are described. Several studies were conducted to evaluate the geometric and radiometric performance of the TM to determine data viability for the more pertinent investigations of TM utility. In most cases this requirement was more than sufficiently satisfied. This allowed the opportunity to take advantage of detailed ground observations for several of the sample segments to assess class separability and detection of other important features with TM. The results presented regarding these TM characteristics show that not only is the increased definition of the within scene variance captured by the increased spatial and spectral resolution, but that the mid-IR bands (5 and 7) are necessary for optimum crop type classification. Both qualitative and quantitative results are presented that describe the improvements gained with the TM both relative to the MSS and on its own merit.

Bizzell, R. M.↗

Integration and compaction of optical systems in the mid-infrared

Problems in the design of optical systems for use with mid-IR (MIR; 10.6-micron) lasers are reviewed. The cryogenically operated lead-chalcogenide tunable diode lasers currently used as sources emit complex far-field patterns and require sophisticated beam collection, shaping, and guide optics. Since conventional optics using large mirrors and Ge lenses are often awkward to use and sensitive to vibration, and since optical fibers for the MIR have not been perfected, current research concentrates on hollow flexible rectangular metallic pipes. These pipes are shown to provide transmission of 95 percent or better over a 1-m length, with beam shaping and polarization control. The low transmission losses and wideband IR transmission of single-crystal alkali halides suggest the feasibility of their use in MIR optical fibers and waveguides.

Yu, C.↗

Evaluation of Landsat Thematic Mapper for vegetated alluvium soils information

Landsat Thematic Mapper data acquired over Mississippi County, Arkansas, on August 22, 1982, were evaluated whether TM provides information that could be used for soil association maps and if soil properties (variability within vegetated fields) can be detected with the new bands on TM. It was found that TM data - especially the mid-IR and thermal bands - show the capability for separating vegetated soil landscapes on a broad basis. Analysis at the field level with a crop growing indicates that TM, with its additional and narrower bands and improved spatial resolution is influenced by within-field variability due to soils.

Thompson, D. R.↗

Evidence for the interaction of the IRS 16 wind with the ionized and molecular gas at the Galactic center

We present a number of high-resolution radio images showing evidence for the dynamical interaction of the outflow arising from the IRS 16 complex with the ionized gas associated with the Northern Arm of Sgr A West, and with the northwestern segment of the circumnuclear molecular disk which engulfs the inner few parsecs of the Galactic center. We suggest that the wind disturbs the dynamics of the Northern Arm within 0.1 pc of the center, is responsible for the waviness of the arm at larger distances, and is collimated by Sgr A West and the circumnuclear disk. The waviness is discussed in terms of the Rayleigh-Taylor instability induced by the ram pressure of the wind incident on the surface of the Northern Arm. Another consequence of this interaction is the strong mid-IR polarization of the Northern Arm in the vicinity of the IRS 16 complex which is explained as a result of the ram pressure of the wind compressing the gas and the magnetic field.

Yusef-Zadeh, Farhad↗

Novel, Middle and Long Wave Infrared Laser Sources For Accelerator Applications

The main accomplishment during Years 2020-2024 of the DOE Accelerator Stewardship Program is proof-of-principle demonstration of amplification of an ultrashort 10 µm seed pulse in a multiatmosphere CO 2 laser optically pumped by nanosecond pulses of either a ~4.3 µm Fe:ZnSe laser or a 2.8 µm electro-optically (EO) Q-switched Er: Laser. This has been accomplished at the UCLA Neptune Laboratory by using about 100 mJ, ~100 ns long pulses generated by the pump laser built for this purpose by the UAB team. Implementation of EO Q-switching regime in the solid-state Er:laser system made possible nanosecond synchronization between the pump pulse and the 0.5 ps seed pulse produced by a commercial Ti:sapphire laser based mid-IR OPA/DFG. The injection mode-locking regime realized in a compact Mult atmosphere 3 Hz CO 2 -He regenerative amplifier enabled generation of a train of ultrashort pulses separated by the cavity round-trip time of ~3.2 ns. The measured gain lifetime of ~1 µs at a total pressure of ~12-15 atm indicates that lifetime of the upper laser level is a critical limiting factor in designing high-pressure CO 2 amplifiers. A single picosecond 10 mm pulse with an energy 0.1-0.2 mJ was extracted from the amplifier’s cavity using an ultrafast Ge semiconductor switch whose reflectivity was photo-induced by a femtosecond 800 nm pulse. For direct amplification regime, nonlinear absorption in Ge at 10 mm at GW/cm 2 intensities limited the extracted energy. Therefore, the generated energy could be further increased by minimizing losses in the switch and optimizing the cavity mode size. Based on the obtained data in collaboration with BNL colleagues, we have designed a high-pressure CO 2 amplifier to be used as a preamplifier for the future experiments at the ATF BNL. The latter work is the subject of funding availability.

60 APPLIED LIFE SCIENCES↗