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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Ultrafast conformational dynamics of Rydberg-excited N -methyl piperidine

We have observed the ultrafast conformational dynamics of electronically excited N-methyl piperidine (NMP) using time-resolved Rydberg fingerprint spectroscopy. Optical excitation at various wavelengths ranging from 212 nm to 229 nm leads to the 3s or 3p Rydberg states and induces coherent oscillatory motions with periods of about 700 fs. Furthermore, these coherent motions survive the internal conversion from 3p to 3s but then dephase on a time scale of a few oscillations. Intramolecular vibrational energy redistribution on a picosecond time scale leads to an equilibrium between two conformeric structures that are separated in binding energy by 0.09 eV. Model calculations using the DFT-SIC method are in excellent agreement with the experiments and identify the conformers as the chair and twist structures of NMP. The analysis of the equilibrium parameters at long time delays as a function of excitation wavelength allows for the extraction of thermodynamic parameters for the conformeric transformation. We derive an enthalpy of the chair to twist reaction in the 3s excited state of 62 meV with an entropy of 19.70 J mol –1 K –1 . An activation energy of 276 meV is also obtained with a kinetic model.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Mid-infrared nonlinear optics in thin-film lithium niobate on sapphire

Periodically poled thin-film lithium niobate (TFLN) waveguides have emerged as a leading platform for highly efficient frequency conversion in the near-infrared. However, the commonly used silica bottom-cladding results in high absorption loss at wavelengths beyond 2.5 µm. In this work, we demonstrate efficient frequency conversion in a TFLN-on-sapphire platform, which features high transparency up to 4.5 µm. In particular, we report generating mid-infrared light up to 3.66 µm via difference-frequency generation of a fixed 1 µm source and a tunable telecom source, with normalized efficiencies up to 200 % <#comment/> / W c m 2 . These results show TFLN-on-sapphire to be a promising platform for integrated nonlinear nanophotonics in the mid-infrared.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Apparatuses and methods involving DC voltage conversion using photonic transformers

In certain examples, methods and semiconductor structures are directed to an apparatus including a photon emitter such as an LED which operates over an emission wavelength range and a photo-voltaic device arranged relative to the photon emitter to provide index-matched optical coupling between the photo-voltaic device and the photon emitter for an emission wavelength range of the photon emitter.

Fan, Shanhui↗
DOE OSTI2023

A New Plasma Radar Concept for Simultaneous Magnetic and Density Measurements

An innovative, compact 288GHz interferometer has been fabricated, tested, installed and successfully demonstrated on the LAPD-U magnetized plasma at UCLA. The system takes advantage of frequency modulated (FM) radar techniques to deliver a compact heterodyne system. In addition, the reflected power from the source is taken advantage of to eliminate the need for additional quasi-optical components. Electron density in LAPD-U plasma has recently been increased substantially thereby requiring a higher frequency/shorter wavelength interferometer to avoid deleterious refractive effects. This system satisfies those needs. The system uses a 96GHz varactor tuned Gunn oscillator which passes to a passive tripler. This tripler has ~3% conversion efficiency. The 288GHz radiation is then coupled to free space using a so-called dual-mode or Pickett horn. The output 288GHz beam is then coupled to an aspheric lens manufactured from low-loss, high-density polyethylene. This lens is employed to collimate the emerging beam. Small axial adjustment of the lens position can also be used to create a slowly focusing beam so as to optimize the measured signal. In addition, up-down or side-to-side adjustment of the lens can be utilized to steer the beam vertically or horizontally – again to optimize alignment. The propagating beam passes through a beam splitter and then through a water-free, bubble-free fused quartz window into the LAPD-U vacuum vessel. The beam-splitter is a thin sheet of G10 which reflects a small fraction of the incident power (~5 %) towards a zero-bias detector optimized for the frequency range from 220 to 300GHz. Note that waveguides at this frequency have dimensions of ~0.9mm x 0.45mm and so have very large conductive losses. This drives the use of quasi-optical propagation. The detector requires no DC bias and is very responsive (> 1V/mW into 1MΩ). Radiation is coupled to the detector via a similar lens-horn arrangement used for the launch. This reflected beam acts as the local oscillator or reference millimeter-wave beam for the detector. The remainder of the launched source beam then enters the LAPD-U vacuum vessel and passes through the plasma at the mid-plane until reaching the opposing port which is closed off with an aluminum flange. This flange is used as a mirror to retroreflect the incident 288GHz beam back along its path. The retroreflected beam exits the input port but does NOT couple directly into the zero-bias detector. Instead, the majority of the return power continues towards the 288GHz source. As mentioned above the transmitted beam enters the source a second time. This would appear undesirable. However, at these frequencies multipliers are highly non-linear elements which results in a significant portion of the return beam (~20%) re-emerging from the multiplier and horn and then coupling via the G10 beam-splitter to the zero-bias detector. This approach eliminated the need for a second quasi-optical beam-splitter. The system is extremely compact measuring approximately 28 inches x 20 inches. The above did not explain how heterodyne operation was achieved. As mentioned above the Gunn oscillator is able to be varactor tuned. This allows a low voltage to be applied to control the operating frequency of the Gunn oscillator. During heterodyne operation a sawtooth shaped voltage is applied to the varactor at 750kHz using an 80MHz Arbitrary Waveform Generator (AWG). This voltage changes the Gunn frequency linearly during the up-sweep which is then reset abruptly at the sawtooth crash to be immediately followed by another linear sweep. Passage through the 288GHz multiplier triples the frequency change experienced by the electromagnetic wave. These frequency changes are small – tens of megahertz. This FM radar approach results in the launched electromagnetic wave frequencies at the detector for the reference and plasma wave to be different. The approximately 10 ns delay propagation delay for the plasma beam results in the local oscillator and plasma beams NOT having an identical frequency – there is in fact a fixed difference frequency. The frequency tuning level of the Gunn oscillator is then adjusted so that there is ONE cycle of this difference frequency during each linear ramp. During the sawtooth crash or downward re-sweep this one cycle replays in reverse but on a very fast timescale. The process then repeats. Low-pass filtering eliminates the fast re-sweep to leave a pure sine wave heterodyne signal. When the plasma is present it introduces a phase delay in the sine wave (caused by the extremely small Doppler shift resulting from the optical path length change). Of course, to measure this phase change we need a reference. This is simply obtained from an arbitrary waveform generator which provides a synchronized output pulse train which again is low pass filtered to obtain a 750kHz sinusoidal voltage reference for the interferometer. The interferometer was installed on LAPD-U where it has worked reliably and has established that electron densities exceeding 1x10 13 cm -3 are routinely achieved. In addition, the system sensitivity was able to easily observe density fluctuation at frequencies up to 50kHz. FM Radar techniques have enabled a full demonstration of a compact, sensitive, high frequency (288GHz/1mm) heterodyne interferometer.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Extremely Thin Perfect Absorber by Generalized Multipole Bianisotropic Effect

Symmetry breaking plays a crucial role in understanding the fundamental physics underlying numerous physical phenomena, including the electromagnetic response in resonators, giving rise to intriguing effects such as directional light scattering, supercavity lasing, and topologically protected states. Here, this work demonstrates that adding a small fraction of lossy metal (as low as 1 × 10 −6 in volume) to a lossless dielectric resonator breaks inversion symmetry (IS), thereby lifting its degeneracy, leading to a strong bianisotropic response. In the case of the metasurface composed of such resonators, this effect leads to unidirectional perfect absorption while maintaining nearly perfect reflection from the opposite direction. It has developed more general Onsager‐Casimir relations for the polarizabilities of particle arrays, taking into account the contributions of quadrupoles, which shows that bianisotropy is not solely due to dipoles, but also involves high‐order multipoles. The experimental validation demonstrates an extremely thin terahertz‐perfect absorber with a wavelength‐to‐thickness ratio of up to 25,000, where the material thickness is only 2% of the theoretical minimum thickness dictated by the fundamental limit. The findings can pave a new route to design devices for applications involving optical‐to‐heat conversion processes.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Time-varying gradient metasurface with applications in all-optical beam steering

Integrating the large, subpicosecond nonlinear optical response of epsilon-near-zero (ENZ) materials with the broad design freedoms of plasmonic metasurfaces shows potential for creating rapidly modulated optical devices with possible applications in telecommunications, sensing, and reactive beam steering. In this work, we experimentally investigate a metasurface consisting of a plasmonic gradient array on a thin layer of indium tin oxide (ITO), characterize how incident probe pulses diffract from a system as it is being dynamically modulated by a pump pulse at wavelengths near the ENZ region. Angular shifts in the diffraction orders are observed and can be principally attributed to the adiabatic wavelength conversion of the probe as it witnesses the temporal change of index induced by the pump. Of note, the asymmetric gradient metasurface, considered to be a blazed diffraction grating, shows significantly different dynamic responses for different diffraction orders. The free-space wavelength shift to +1 and -1 diffraction orders is 6 and 12 nm, resulting in steering angle changes of 0.65 and 1.5°, respectively.

42 ENGINEERING↗
DOE OSTI2022

Near–Band–Edge Enhancement in Perovskite Solar Cells via Tunable Surface Plasmons

Plasmonic perovskite solar cells (PSCs) using core-shell type plasmonic particles are designed, which possess the plasmon resonance in the near-infrared range. This can selectively strengthen the interaction of the perovskite layer with low-energy photons. The mesoporous PSCs employing the plasmonic particles have delivered a 10%-15% enhancement of external quantum efficiency in the plasmonic resonance range. This surface-plasmonic effect has been analyzed using complementary techniques, including selective wavelength excitation and time-dependent photoluminescence. Here it is shown that the metal-based core-shell-type plasmonic structures in PSCs optimize the scattering and absorption of incident light and the dynamics of photogenerated carriers. Furthermore, both optical and electronic effects increase the power conversion efficiency of PSCs from 17.49% to 19.88%, paving a way toward controlling the thickness of the photoactive layer for advanced devices such as tandem solar cells.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Optomechanical Tuning of Second Harmonic Generation Anisotropy in Janus MoSSe/MoS 2 Heterostructures

Symmetry breaking in van der Waals materials enables the realization of quantum states and advanced device functionalities. Janus transition-metal dichalcogenides (TMDs) exhibit distinctive nonlinear optical properties due to their broken out-of-plane mirror symmetry. However, the dynamic control of second harmonic generation (SHG) anisotropy and resonance behavior via optical excitation remains elusive. Here, in this work, we investigate the SHG response of Janus MoSSe/MoS 2 heterostructures with 2H and 3R stackings. We can tune the SHG response by varying the incident photon wavelength from 800 to 1000 nm, which shows a resonance-dependent enhancement in intensity and a deviation from 6-fold symmetry, indicating wavelength-dependent anisotropy. The ratio between maximum and minimum intensity in the armchair directions, associated with the SHG anisotropy, reaches a value of 1.73 at the excitation wavelength of 1000 nm. Group theory analysis and first-principles calculations reveal that the observed anisotropy arises from optically induced strain. Our findings highlight the role of symmetry breaking and optical resonance contributing to the optomechanical tuning of SHG anisotropy, offering opportunities for developing Janus TMD-based photonic devices for frequency conversion, light generation, and optical switching.

Janus transition metal dichalcogenides↗
DOE OSTI2024

Multicolor Inks of Black Phosphorus for Midwave‐Infrared Optoelectronics

Abstract Black phosphorus (bP) based ink with a bulk bandgap of 0.33 eV ( λ = 3.7 µm) has recently been shown to be promising for large‐area, high performance mid‐wave infrared (MWIR) optoelectronics. However, the development of multicolor bP inks expanding across the MWIR wavelength range has been challenging. Here a multicolor ink process based on bP with spectral emission tuned from 0.28 eV ( λ = 4.4 µm) to 0.8 eV ( λ = 1.5 µm) is demonstrated. Specifically, through the reduction of bP particle size distribution (i.e., lateral dimension and thickness), the optical bandgap systematically blueshifts, reaching up to 0.8 eV. Conversely, alloying bP with arsenic (bP 1− x As x ) induces a redshift in the bandgap to 0.28 eV. The ink processed films are passivated with an infrared‐transparent epoxy for stable infrared emission in ambient air. Utilizing these multicolor bP‐based inks as an infrared light source, a gas sensing system is demonstrated that selectively detects gases, such as CO 2 and CH 4 whose absorption band varies around 4.3 and 3.3 µm, respectively. The presented ink formulation sets the stage for the advancement of multiplex MWIR optoelectronics, including spectrometers and spectral imaging using a low‐cost material processing platform.

Kim, Jae Ik↗
DOE OSTI2025

Flat nonlinear optics with intersubband polaritonic metasurfaces

Nonlinear intersubband polaritonic metasurfaces produce some of the strongest second- and third-order nonlinear optical responses reported for condensed matter systems at infrared frequencies. These metasurfaces are fabricated as two-dimensional arrays of nanoresonators from multi-quantum-well semiconductor heterostructures, designed to produce strong nonlinear responses associated with intersubband transitions. By optimally coupling the optical modes of the nanoresonators to vertically polarized intersubband transitions in semiconductor heterostructures, one can boost the nonlinear response associated with intersubband transitions, make intersubband transitions interact with free-space radiation at normal incidence, and hence produce optically thin flat nonlinear optical elements compatible with free-space optical setups. As a result of the strong nonlinear response in these systems, significant nonlinear conversion efficiencies (>0.1 %) can be attained in deeply subwavelength optical films using modest pumping intensities of only 10–100 kW/cm 2 . Subwavelength metasurface thickness relaxes phase-matching constraints limiting the operation of bulk nonlinear crystals. Furthermore, the amplitude and phase of the nonlinear optical response in intersubband polaritonic metasurfaces can be tailored for a specific pump wavelength and a nonlinear process of interest through the co-optimization of quantum engineering of electron states in semiconductor heterostructures and photonic engineering of the metasurface nanoresonators design. Additionally, an applied voltage can dynamically control the amplitude and phase of the nonlinear optical response at a nanoresonator level. Here, we review the current state of the art in this rapidly expanding field, focusing on nonlinear processes supporting second-harmonic generation, saturable absorption, and optical power limiting.

flat optics↗
DOE OSTI2022

Coherent terahertz radiation with 2.8-octave tunability through chip-scale photomixed microresonator optical parametric oscillation

High-spectral-purity frequency-agile room-temperature sources in the terahertz spectrum are foundational elements for imaging, sensing, metrology, and communications. Here we present a chip-scale optical parametric oscillator based on an integrated nonlinear microresonator that provides broadly tunable single-frequency and multi-frequency oscillators in the terahertz regime. Through optical-to-terahertz down-conversion using a plasmonic nanoantenna array, coherent terahertz radiation spanning 2.8-octaves is achieved from 330 GHz to 2.3 THz, with ≈20 GHz cavity-mode-limited frequency tuning step and ≈10 MHz intracavity-mode continuous frequency tuning range at each step. By controlling the microresonator intracavity power and pump-resonance detuning, tunable multi-frequency terahertz oscillators are also realized. Furthermore, by stabilizing the microresonator pump power and wavelength, sub-100 Hz linewidth of the terahertz radiation with 10 –15 residual frequency instability is demonstrated. The room-temperature generation of both single-frequency, frequency-agile terahertz radiation and multi-frequency terahertz oscillators in the chip-scale platform offers unique capabilities in metrology, sensing, imaging and communications.

42 ENGINEERING↗
DOE OSTI2024

Circularly Polarized Attosecond Pulses Enabled by an Azimuthal Phase and Polarization Grating

High-harmonic generation (HHG) is an extreme nonlinear optical process that can map the properties of an infrared driving laser beam onto short wavelength attosecond pulse trains. However, current techniques for generating circularly polarized high harmonics for probing magnetic materials and chiral systems have limitations: two-color collinear counter-rotating driving lasers result in a low cutoff photon energy, while single-color non-collinear counter-rotating schemes suffer from low conversion efficiency. In this work, we generate circularly polarized attosecond pulse trains by using a structured laser driver which has a rotating polarization and phase grating along the azimuthal coordinate. Furthermore, our experimental and numerical results demonstrate the production of left and right circularly polarized harmonics, which naturally separate upon propagation. Our approach uses a single laser color in a collinear geometry, that can be scaled for high efficiency. Simulations show this scheme can extend into the soft x-ray region when driven by mid-infrared driving lasers, while preserving the same high phase-matching cutoff photon energy as for linearly-polarized high harmonics.

attosecond science↗
DOE OSTI2020

Engineering of Lead Selenide Quantum Dot Based Devices and Core/Shell Heterostructures

Near infrared (NIR) emitting colloidal quantum dots (QDs) such as PbSe are interesting materials for implementation in various optoelectronic devices such as solar cells, photodetectors, and radiation detectors. Material properties like size tunable emission wavelengths, facile solution processability, the possibility of carrier multiplication and Auger assisted up-conversion, and high Z number provide PbSe QDs with unique advantages over many currently available commercial materials used in these devices. In this dissertation, after an introduction to QDs in general, we first focus on synthesis of PbSe-based heterostructured QDs for study via optical spectroscopy. PbSe/CdSe QDs synthesized via cation exchange reaction were used as seeds to study the proper conditions for further CdSe or CdS shell growth. Optical spectroscopy studies show that growth of thicker CdSe shells leads to tunable visible emission, while growth of thick CdS shells can greatly increase the photoluminescence quantum yield (PLQY) observed from the intermediate CdSe shell. NIR PL lifetimes can be greatly enhanced by the growth of CdS shells, due to strong delocalization of the hole wavefunction within the PbSe core, while the electron is delocalized throughout the QD including in the CdS shell, resulting in radiative lifetimes in the tens of microseconds. Two pulse delay measurements show that Auger assisted up conversion is also taking place in these engineered QD dot heterostructures. In the sections that follow, we look at QD devices, first with a focus on novel devices fabricated from PbSe QDs, using an amine synthesis method that allows for facile in-solution ligand exchange. QD film mobilities are measured for PbSe QDs capped with various short ionic ligands. Carrier densities in PbSe QD films are calculated from C-V measurements, showing for the first time that carrier densities can be modulated by simply changing the capping ligand. vii Radiation detectors utilizing PbSe QDs capped with KI and NH4I ligands show tangible response to incident alpha radiation. Current output response to alpha radiation is dependent on strength of radiation source and amount of bias voltage applied. In the final section a critical review of hybrid layered 2D-QD photodetectors is presented. In a typical example, PbSe and PbS QDs act as the absorbing layer in phototransistor devices which utilize layered 2D materials such as graphene and transition metal dichalcogenides as transport layers. Resulting devices display high gains and improved directivities compared to QD only and 2D only devices.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Neuromorphic Information Processing by Optical Media

Classification of features in a scene typically requires conversion of the incoming photonic field int the electronic domain. Recently, an alternative approach has emerged whereby passive structured materials can perform classification tasks by directly using free-space propagation and diffraction of light. In this manuscript, we present a theoretical and computational study of such systems and establish the basic features that govern their performance. We show that system architecture, material structure, and input light field are intertwined and need to be co-designed to maximize classification accuracy. Our simulations show that a single layer metasurface can achieve classification accuracy better than conventional linear classifiers, with an order of magnitude fewer diffractive features than previously reported. For a wavelength λ, single layer metasurfaces of size 100λ x 100λ with aperture density λ -2 achieve ~96% testing accuracy on the MNIST dataset, for an optimized distance ~100λ to the output plane. This is enabled by an intrinsic nonlinearity in photodetection, despite the use of linear optical metamaterials. Furthermore, we find that once the system is optimized, the number of diffractive features is the main determinant of classification performance. The slow asymptotic scaling with the number of apertures suggests a reason why such systems may benefit from multiple layer designs. Finally, we show a trade-off between the number of apertures and fabrication noise.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Cascaded Optical Nonlinearities in Dielectric Metasurfaces

Since the discovery of the laser, optical nonlinearities have been at the core of efficient light conversion sources. Typically, thick transparent crystals or quasi-phase matched waveguides are utilized in conjunction with phase-matching techniques to select a single parametric process. In recent years, due to the rapid developments in artificially structured materials, optical frequency mixing has been achieved at the nanoscale in subwavelength resonators arrayed as metasurfaces. Phase matching becomes relaxed for these wavelength-scale structures, and all allowed nonlinear processes can, in principle, occur on an equal footing. This could promote harmonic generation via a cascaded (consisting of several frequency mixing steps) process. However, so far, all reported work on dielectric metasurfaces have assumed frequency mixing from a direct (single step) nonlinear process. In this work, we prove the existence of cascaded second-order optical nonlinearities by analyzing the second- and third-wave mixing from a highly nonlinear metasurface in conjunction with polarization selection rules and crystal symmetries. We find that the third-wave mixing signal from a cascaded process can be of comparable strength to that from conventional third-harmonic generation and that surface nonlinearities are the dominant mechanism that contributes to cascaded second-order nonlinearities in our metasurface.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Semiconductor quantum dots: Technological progress and future challenges

In quantum-confined semiconductor nanostructures, electrons exhibit distinctive behavior compared with that in bulk solids. This enables the design of materials with tunable chemical, physical, electrical, and optical properties. Zero-dimensional semiconductor quantum dots (QDs) offer strong light absorption and bright narrowband emission across the visible and infrared wavelengths and have been engineered to exhibit optical gain and lasing. These properties are of interest for imaging, solar energy harvesting, displays, and communications. Here, we offer an overview of advances in the synthesis and understanding of QD nanomaterials, with a focus on colloidal QDs, and discuss their prospects in technologies such as displays and lighting, lasers, sensing, electronics, solar energy conversion, photocatalysis, and quantum information.

García de Arquer, F. Pelayo↗
DOE OSTI2021

Spectroscopy of GR1 centers in synthetic diamonds

We report on the spectroscopic characterization, absorption saturation, and excited-state dynamics of GR1 centers in synthetic diamonds. The non-linear optical measurements reveal an efficient bleaching of the GR1 center’s ground level under ns-pulsed 633 nm excitation. The maxima of absorption and emission cross sections were estimated to be 4.5 × 10 −17 cm 2 and 9 × 10 −17 cm 2 at 630 nm and 780 nm, respectively. The radiative lifetime of the excited level was estimated to be 8.5 ns. The 658 nm probe kinetics uncovered relaxation of 1 T 2 excited level going predominantly to a metastable state with a lifetime of 220 μs. An induced absorption detected with the use of a highly concentrated diamond sample could be due to up-conversion and photoionization processes in additional impurity-vacancy center with absorption at the short-wavelength tail of GR1. The results presented here indicate that synthetic diamonds with GR1 centers could serve as near infrared gain media or passive Q-switchers for laser cavities over the 633–750 nm spectral range. Optimization of the center concentration and the crystal parameters are required to minimize the induced absorption at the lasing wavelengths.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Co-Design of Free-Space Metasurface Optical Neuromorphic Classifiers for High Performance

Classification of features in a scene typically requires conversion of the incoming photonic field into the electronic domain. Recently, an alternative approach has emerged whereby passive structured materials can perform classification tasks by directly using free-space propagation and diffraction of light. In this manuscript, we present a theoretical and computational study of such systems and establish the basic features that govern their performance. We show that system architecture, material structure, and input light field are intertwined and need to be co-designed to maximize classification accuracy. Our simulations show that a single layer metasurface can achieve classification accuracy better than conventional linear classifiers, with an order of magnitude fewer diffractive features than previously reported. For a wavelength λ, single layer metasurfaces of size 100λ × 100λ with an aperture density λ –2 achieve ~96% testing accuracy on the MNIST data set, for an optimized distance ~100λ to the output plane. This is enabled by an intrinsic nonlinearity in photodetection, despite the use of linear optical metamaterials. Furthermore, we find that once the system is optimized, the number of diffractive features is the main determinant of classification performance. The slow asymptotic scaling with the number of apertures suggests a reason why such systems may benefit from multiple layer designs. Finally, we show a trade-off between the number of apertures and fabrication noise.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗