Limited Spectral Resolution Research Articles

Performance Limits of THz Dispersive Spectroscopes Employing Super-Resolution Imaging

The performance of terahertz (THz) dispersive spectroscopes is limited in spectral resolution and frequency accuracy due to a finite pixel count. This article demonstrates that increasing the synthetic effective pixel count by exploiting super-resolution (SR) imaging results in improved performance. To this end, we investigated the performance of a CMOS camera-based THz dispersive spectroscope using SR imaging. From 0.75–0.9 THz, average spectral resolution improved from 76 GHz to 34.2 GHz (about a factor of two), while the average frequency accuracy enhanced from 30 GHz to 1.65 GHz. Further to providing enhanced spectral resolution and frequency accuracy, our results provide an insight into the fundamental performance limits. For low-resolution (LR) imaging, the finite pixel count sets the spectral resolution limit, and for SR imaging, the camera angular resolution defines the limiting factor. For this reason, SR imaging generally improves the spectral resolution at least by a factor of two. Pixel count and noise fluctuation limit the frequency accuracy using LR and SR imaging, respectively.

Urban Vegetation Mapping from Aerial Imagery Using Explainable AI (XAI).

Urban vegetation mapping is critical in many applications, i.e., preserving biodiversity, maintaining ecological balance, and minimizing the urban heat island effect. It is still challenging to extract accurate vegetation covers from aerial imagery using traditional classification approaches, because urban vegetation categories have complex spatial structures and similar spectral properties. Deep neural networks (DNNs) have shown a significant improvement in remote sensing image classification outcomes during the last few years. These methods are promising in this domain, yet unreliable for various reasons, such as the use of irrelevant descriptor features in the building of the models and lack of quality in the labeled image. Explainable AI (XAI) can help us gain insight into these limits and, as a result, adjust the training dataset and model as needed. Thus, in this work, we explain how an explanation model called Shapley additive explanations (SHAP) can be utilized for interpreting the output of the DNN model that is designed for classifying vegetation covers. We want to not only produce high-quality vegetation maps, but also rank the input parameters and select appropriate features for classification. Therefore, we test our method on vegetation mapping from aerial imagery based on spectral and textural features. Texture features can help overcome the limitations of poor spectral resolution in aerial imagery for vegetation mapping. The model was capable of obtaining an overall accuracy (OA) of 94.44% for vegetation cover mapping. The conclusions derived from SHAP plots demonstrate the high contribution of features, such as Hue, Brightness, GLCM_Dissimilarity, GLCM_Homogeneity, and GLCM_Mean to the output of the proposed model for vegetation mapping. Therefore, the study indicates that existing vegetation mapping strategies based only on spectral characteristics are insufficient to appropriately classify vegetation covers.

Versatile non-luminescent color palette based on guest exchange dynamics in paramagnetic cavitands

Multicolor luminescent portrayal of complexed arrays is indispensable for many aspects of science and technology. Nevertheless, challenges such as inaccessible readouts from opaque objects, a limited visible-light spectrum and restricted spectral resolution call for alternative approaches for multicolor representation. Here, we present a strategy for spatial COlor Display by Exploiting Host-guest Dynamics (CODE-HD), comprising a paramagnetic cavitand library and various guests. First, a set of lanthanide-cradled α-cyclodextrins (Ln-CDs) is designed to induce pseudo-contact shifts in the 19F-NMR spectrum of Ln-CD-bound guest. Then, capitalizing on reversible host-guest binding dynamics and using magnetization-transfer 19F-MRI, pseudo-colored maps of complexed arrays are acquired and applied in molecular-steganography scenarios, showing CODE-HD’s ability to generate versatile outputs for information encoding. By exploiting the widely shifted resonances induced by Ln-CDs, the guest versatility and supramolecular systems' reversibility, CODE-HD provides a switchable, polychromatic palette, as an advanced strategy for light-free, multicolor-mapping.

Dispersive mirror characterization and application for mid-infrared post-compression

This paper presents a second harmonic assisted spectrally resolved interferometric technique that can overcome the limited spectral resolution of commercially available spectrometers in the mid-infrared. The discussed scheme was validated by measuring the group delay of several well-known and frequently used materials. Our main motivation was to characterize the spectral phase shift of newly designed and manufactured dispersive mirrors to be used for mid-infrared (MIR) post-compression. These mirrors were successfully implemented in the post-compression stage of our MIR laser system, where pulse duration was shortened below two optical cycles and the pulse peak power increased by 30.3% compared to the original output.

EEG-Based Auditory Attention Detection and Its Possible Future Applications for Passive BCI

The ability to discriminate and attend one specific sound source in a complex auditory environment is a fundamental skill for efficient communication. Indeed, it allows us to follow a family conversation or discuss with a friend in a bar. This ability is challenged in hearing-impaired individuals and more precisely in those with a cochlear implant (CI). Indeed, due to the limited spectral resolution of the implant, auditory perception remains quite poor in a noisy environment or in presence of simultaneous auditory sources. Recent methodological advances allow now to detect, on the basis of neural signals, which auditory stream within a set of multiple concurrent streams an individual is attending to. This approach, called EEG-based auditory attention detection (AAD), is based on fundamental research findings demonstrating that, in a multi speech scenario, cortical tracking of the envelope of the attended speech is enhanced compared to the unattended speech. Following these findings, other studies showed that it is possible to use EEG/MEG (Electroencephalography/Magnetoencephalography) to explore auditory attention during speech listening in a Cocktail-party-like scenario. Overall, these findings make it possible to conceive next-generation hearing aids combining customary technology and AAD. Importantly, AAD has also a great potential in the context of passive BCI, in the educational context as well as in the context of interactive music performances. In this mini review, we firstly present the different approaches of AAD and the main limitations of the global concept. We then expose its potential applications in the world of non-clinical passive BCI.

Frequency comb-based multidimensional coherent spectroscopy bridges the gap between fundamental science and cutting-edge technology.

Optical multidimensional coherent spectroscopy (MDCS) has become a powerful and routine technique for studying optical properties of a wide range of materials. However, current implementations of MDCS have spectral resolution and acquisition speed limitations. In this Perspective, I describe how frequency comb technology can be used to overcome the limitations and also show the recent progress that has been made in this field.

Simulation for measurement of lightning channel temperature using a dual-band high-precision lightning imaging spectrometer.

A dual-band high-precision lightning imaging spectrometer (DHLIS) is designed to capture the fine spectrum of transient lightning. DHLIS improves the theoretical spectral resolution limit to 10-3nm and broadens the spectral range to 30-40 nm by employing double echelle gratings in the arms of a spatial heterodyne spectrometer. Four strong and three fine spectral lines are selected to retrieve the temperature of the lightning channel using the Boltzmann plot method. The experimental results indicate that the inversion accuracy of the temperature obtained by inserting fine spectral lines is higher than that by implementation of four strong spectral lines.

3D Heteronuclear Magnetization Transfers for the Establishment of Secondary Structures in SARS-CoV-2-Derived RNAs.

Multidimensional NOESY experiments targeting correlations between exchangeable imino and amino protons provide valuable information about base pairing in nucleic acids. It has been recently shown that the sensitivity of homonuclear correlations involving RNA’s labile imino protons can be significantly enhanced, by exploiting the repolarization brought about by solvent exchanges. Homonuclear correlations, however, are of limited spectral resolution, and usually incapable of tackling relatively large homopolymers with repeating structures like RNAs. This study presents a heteronuclear-resolved version of those NOESY experiments, in which magnetization transfers between the aqueous solvent and the nucleic acid protons are controlled by selecting specific chemical shift combinations of a coupled 1H–15N spin pair. This selective control effectively leads to a pseudo-3D version of HSQC-NOESY, but with cross-peaks enhanced by ∼2–5× as compared with conventional 2D NOESY counterparts. The enhanced signal sensitivity as well as access to both 15N–1H and 1H–1H NOESY dimensions can greatly facilitate RNA assignments and secondary structure determinations, as demonstrated here with the analysis of genome fragments derived from the SARS-CoV-2 virus.

Inelastic Electron Tunneling Spectroscopy at High-Temperatures.

Ion conducting materials are critical components of batteries, fuel cells, and devices such as memristive switches. Analytical tools are therefore sought that allow the behavior of ions in solids to be monitored and analyzed with high spatial resolution and in real time. In principle, inelastic tunneling spectroscopy offers these capabilities. However, as its spectral resolution is limited by thermal softening of the Fermi-Dirac distribution, tunneling spectroscopy is usually constrained to cryogenic temperatures. This constraint would seem to render tunneling spectroscopy useless for studying ions in motion. Here, the first inelastic tunneling spectroscopy studies above room temperature are reported. For these measurements, high-temperature-stable tunnel junctions that incorporate within the tunnel barrier ultrathin layers for efficient proton conduction are developed. By analyzing the vibrational modes of OH bonds in BaZrO3 -based heterostructures, the detection of protons with a spectral resolution of 20 meV at 400 K (full-width-at-half maximum) is demonstrated. Overturning the hitherto existing prediction for the spectral resolution limit of 186 meV (5.4 kB T ) at 400 K, this resolution enables high-temperature tunneling spectroscopy of ion conductors. With these advances, inelastic tunneling spectroscopy constitutes a novel, valuable analytical tool for solid-state ionics.

Advances in optical engineering for future telescopes

Significant optical engineering advances at the University of Arizona are being made for design, fabrication, and construction of next generation astronomical telescopes. This summary review paper focuses on the technological advances in three key areas. First is the optical fabrication technique used for constructing next-generation telescope mirrors. Advances in ground-based telescope control and instrumentation comprise the second area of development. This includes active alignment of the laser truss-based Large Binocular Telescope (LBT) prime focus camera, the new MOBIUS modular cross-dispersion spectroscopy unit used at the prime focal plane of the LBT, and topological pupil segment optimization. Lastly, future space telescope concepts and enabling technologies are discussed. Among these, the Nautilus space observatory requires challenging alignment of segmented multi-order diffractive elements. The OASIS terahertz space telescope presents unique challenges for characterizing the inflatable primary mirror, and the Hyperion space telescope pushes the limits of high spectral resolution, far-UV spectroscopy. The Coronagraphic Debris and Exoplanet Exploring Pioneer (CDEEP) is a Small Satellite (SmallSat) mission concept for high-contrast imaging of circumstellar disks and exoplanets using vector vortex coronagraph. These advances in optical engineering technologies will help mankind to probe, explore, and understand the scientific beauty of our universe.

Hyperspectral multiphoton microscopy for in vivo visualization of multiple, spectrally overlapped fluorescent labels.

The insensitivity of multiphoton microscopy to optical scattering enables high-resolution, high-contrast imaging deep into tissue, including in live animals. Scattering does, however, severely limit the use of spectral dispersion techniques to improve spectral resolution. In practice, this limited spectral resolution together with the need for multiple excitation wavelengths to excite different fluorophores limits multiphoton microscopy to imaging a few, spectrally-distinct fluorescent labels at a time, restricting the complexity of biological processes that can be studied. Here, we demonstrate a hyperspectral multiphoton microscope that utilizes three different wavelength excitation sources together with multiplexed fluorescence emission detection using angle-tuned bandpass filters. This microscope maintains scattering insensitivity, while providing high enough spectral resolution on the emitted fluorescence and capitalizing on the wavelength-dependent nonlinear excitation of fluorescent dyes to enable clean separation of multiple, spectrally overlapping labels, in vivo. We demonstrated the utility of this instrument for spectral separation of closely-overlapped fluorophores in samples containing ten different colors of fluorescent beads, live cells expressing up to seven different fluorescent protein fusion constructs, and in multiple in vivo preparations in mouse cortex and inflamed skin with up to eight different cell types or tissue structures distinguished.

On obtaining high spectral resolution in extreme ultraviolet/soft X-ray monochromators operating off-plane diffraction in a divergent incident beam.

When the trajectory of an incident beam is oriented parallel to the grooves of a periodic grating structure the radiation beam is diffracted off-plane orthogonal to the plane of incidence. The diffraction efficiency in this condition is very high and in a grating with a sawtooth profile it can approach the reflection coefficient for a simple mirror, when the diffraction order of interest follows the direction for specular reflection at the flat part of the steps. When this concept is used in a plane grating in a monochromator for synchrotron radiation sources, the incident beam is almost always collimated in order to minimize any deterioration of the beam properties due to aberrations, which will be introduced in the diffraction process when an uncollimated beam is used. These aberrations are very severe when the groove density is constant. It will be shown that the effect of these aberrations can be corrected after the diffraction by the use of astigmatic focusing. The latter can be provided by a crossed mirror pair with different focal lengths in the corresponding orthogonal directions. Then a monochromator based on this concept can provide source size limited spectral resolution in an uncollimated incident beam. This is identical to the spectral resolution that can be provided by the same grating when operated at the same position in a collimated incident beam. The source size limited spectral resolution in this case corresponds to a high spectral resolving power of better than ΔE/E = 10 000 for photon energies around 300 eV in the soft X-ray range.

Effect of Spectral Contrast Enhancement on Speech-on-Speech Intelligibility and Voice Cue Sensitivity in Cochlear Implant Users.

Speech intelligibility in the presence of a competing talker (speech-on-speech; SoS) presents more difficulties for cochlear implant (CI) users compared with normal-hearing listeners. A recent study implied that these difficulties may be related to CI users' low sensitivity to two fundamental voice cues, namely, the fundamental frequency (F0) and the vocal tract length (VTL) of the speaker. Because of the limited spectral resolution in the implant, important spectral cues carrying F0 and VTL information are expected to be distorted. This study aims to address two questions: (1) whether spectral contrast enhancement (SCE), previously shown to enhance CI users' speech intelligibility in the presence of steady state background noise, could also improve CI users' SoS intelligibility, and (2) whether such improvements in SoS from SCE processing are due to enhancements in CI users' sensitivity to F0 and VTL differences between the competing talkers. The effect of SCE on SoS intelligibility and comprehension was measured in two separate tasks in a sample of 14 CI users with Cochlear devices. In the first task, the CI users were asked to repeat the sentence spoken by the target speaker in the presence of a single competing talker. The competing talker was the same target speaker whose F0 and VTL were parametrically manipulated to obtain the different experimental conditions. SoS intelligibility, in terms of the percentage of correctly repeated words from the target sentence, was assessed using the standard advanced combination encoder (ACE) strategy and SCE for each voice condition. In the second task, SoS comprehension accuracy and response times were measured using the same experimental setup as in the first task, but with a different corpus. In the final task, CI users' sensitivity to F0 and VTL differences were measured for the ACE and SCE strategies. The benefit in F0 and VTL discrimination from SCE processing was evaluated with respect to the improvement in SoS perception from SCE. While SCE demonstrated the potential of improving SoS intelligibility in CI users, this effect appeared to stem from SCE improving the overall signal to noise ratio in SoS rather than improving the sensitivity to the underlying F0 and VTL differences. A second key finding of this study was that, contrary to what has been observed in a previous study for childlike voice manipulations, F0 and VTL manipulations of a reference female speaker (target speaker) toward male-like voices provided a small but significant release from masking for the CI users tested. The present findings, together with those previously reported in the literature, indicate that SCE could serve as a possible background-noise-reduction strategy in commercial CI speech processors that could enhance speech intelligibility especially in the presence of background talkers that have longer VTLs compared with the target speaker.

Rapid adaptation to non-native speech is impaired in cochlear implant users.

To examine difficulties experienced by cochlear implant (CI) users when perceiving non-native speech, intelligibility of non-native speech was compared in conditions with single and multiple alternating talkers. Compared to listeners with normal hearing, no rapid talker-dependent adaptation was observed and performance was approximately 40% lower for CI users following increased exposure in both talker conditions. Results suggest that lower performance for CI users may stem from combined effects of limited spectral resolution, which diminishes perceptible differences across accents, and limited access to talker-specific acoustic features of speech, which reduces the ability to adapt to non-native speech in a talker-dependent manner.

Multicolor Time‐Resolved Upconversion Imaging by Adiabatic Sum Frequency Conversion

AbstractUpconversion imaging, where mid‐infrared (IR) photons are converted to visible and near‐IR photons via a nonlinear crystal and detected on cheap and high‐performance silicon detectors, is an appealing method to address the limitations of thermal sensors that are expensive, often require cooling, and suffer from both limited spectral response and limited spatial resolution as well as poor sensitivity. However, phase matching severely limits the spectral bandwidth of this technique, therefore requiring serial acquisitions in order to cover a large spectrum. Here, a novel upconversion imaging scheme covering the mid‐IR based on adiabatic frequency conversion is introduced. The study presents mid‐IR multicolor imaging and demonstrates simultaneous imaging on a complementary metal–oxide–semiconductor (CMOS) camera of radiation spanning a spectrum from 2 to 4 µm. This approach being coherent and ultrafast in essence, spectrally resolved spatiotemporal imaging is further demonstrated that allows spatially distinguishing the temporal evolution of spectral components.

Phase-sensitive nuclear target spectroscopy

M\"ossbauer nuclei feature exceptionally narrow resonances at hard x-ray energies, which render them ideal probes for structure and dynamics in condensed-matter systems, and a promising platform for x-ray quantum optics and fundamental tests. However, a direct spectroscopy at modern x-ray sources such as synchrotrons or x-ray free electron lasers is challenging, because of the broad spectral bandwidth of the delivered x-ray pulses, and because of a limited spectral resolution offered by x-ray optics and detectors. To overcome these challenges, here, we propose a spectroscopy technique based on a spectrally narrow reference absorber that is rapidly oscillating along the propagation direction of the x-ray light. The motion induces sidebands to the response of the absorber, which we scan across the spectrum of the unknown target to gain spectral information. The oscillation further introduces a dependence of the detected light on the motional phase at the time of x-ray excitation as an additional controllable degree of freedom. We show how a Fourier analysis with respect to this phase enables one to selectively extract parts of the recorded intensity after the actual experiment, throughout the data analysis. This allows one to improve the spectral recovery by removing unwanted signal contributions. Our method is capable of gaining spectral information from the entire measured intensity, and not only from the intensity at late times after the excitation, such that a significantly higher part of the signal photons can be used. Furthermore, it not only enables one to measure the amplitude of the spectral response, but also its phase.

Microsecond Resolved Infrared Spectroelectrochemistry Using Dual Frequency Comb IR Lasers.

A dual infrared frequency comb spectrometer with heterodyne detection has been used to perform time-resolved electrochemical attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS). The measurement of the potential dependent desorption of a monolayer of a pyridine derivative (4-dimethylaminopyridine, DMAP) with time resolution as high as 4 μs was achieved without the use of step-scan interferometry. An analysis of the detection limit of the method as a function of both time resolution and measurement coadditions is provided and compared to step-scan experiments of an equivalent system. Dual frequency comb spectroscopy is shown to be highly amenable to time-resolved ATR-SEIRAS. Microsecond resolved spectra can be obtained with high spectral resolution and fractional monolayer detection limits in a total experimental duration that is 2 orders of magnitude less than the equivalent step-scan experiment.

Excitation–Emission Synchronization-Mediated Directional Fluorescence: Insight into Plasmon-Coupled Emission at Vibrational Resolution

Light-matter interactions have always been a fundamentally significant topic that has attracted much attention. It is important to reveal a fluorophore-plasmon interaction on the nanoscale. However, as a powerful investigative tool, fluorescence spectroscopy still suffers from a limited spectral resolution and the susceptibility to interfering substances. In this work, excitation-emission synchronization-mediated surface-plasmon-coupled emission (EES-SPCE) is proposed to break the bottleneck. By actively screening the energy transitions for observation, an improved spectral resolution has been achieved, which is advantageous to the investigation of the fluorophore-plasmon interactions under different coupling modes. The spectral information related to the plasmonic interactions through tuning vibrational energy levels is clearly distinguished at directional emission angles. EES-SPCE is demonstrated to selectively and efficiently extract the coupled emission from the vibrational resolution, which would open up the opportunity to improve the capability of spectral feature identification and signal collection for practical applications of plasmonic fluorescence spectroscopy.

COLMAR Lipids Web Server and Ultrahigh-Resolution Methods for Two-Dimensional Nuclear Magnetic Resonance- and Mass Spectrometry-Based Lipidomics

Accurate identification of lipids in biological samples is a key step in lipidomics studies. Multidimensional nuclear magnetic resonance (NMR) spectroscopy is a powerful analytical tool for this purpose as it provides comprehensive structural information on lipid composition at atomic resolution. However, the interpretation of NMR spectra of complex lipid mixtures is currently hampered by limited spectral resolution and the absence of a customized lipid NMR database along with user-friendly spectral analysis tools. We introduce a new two-dimensional (2D) NMR metabolite database "COLMAR Lipids" that was specifically curated for hydrophobic metabolites presently containing 501 compounds with accurate experimental 2D 13C-1H heteronuclear single quantum coherence (HSQC) chemical shift data measured in CDCl3. A new module in the public COLMAR suite of NMR web servers was developed for the (semi)automated analysis of complex lipidomics mixtures (http://spin.ccic.osu.edu/index.php/colmarm/index2). To obtain 2D HSQC spectra with the necessary high spectral resolution along both 13C and 1H dimensions, nonuniform sampling in combination with pure shift spectroscopy was applied allowing the extraction of an abundance of unique cross-peaks belonging to hydrophobic compounds in complex lipidomics mixtures. As shown here, this information is critical for the unambiguous identification of underlying lipid molecules by means of the new COLMAR Lipids web server, also in combination with mass spectrometry, as is demonstrated for Caco-2 cell and lung tissue cell extracts.

Nine Localized Deviations from Keplerian Rotation in the DSHARP Circumstellar Disks: Kinematic Evidence for Protoplanets Carving the Gaps

Abstract We present evidence for localized deviations from Keplerian rotation, i.e., velocity “kinks,” in 8 of the 18 circumstellar disks observed by the DSHARP program: DoAr 25, Elias 2–27, GW Lup, HD 143006, HD 163296, IM Lup, Sz 129, and WaOph 6. Most of the kinks are detected over a small range in both radial extent and velocity, suggesting a planetary origin, but for some of them foreground contamination prevents us from measuring their spatial and velocity extent. Because of the DSHARP limited spectral resolution and signal to noise in the 12CO J = 2−1 line, as well as cloud contamination, the kinks are usually detected in only one spectral channel, and will require confirmation. The strongest circumstantial evidence for protoplanets in the absence of higher spectral resolution data and additional tracers is that, upon deprojection, we find that all of the candidate planets lie within a gap and/or at the end of a spiral detected in dust continuum emission. This suggests that a significant fraction of the dust gaps and spirals observed by Atacama Large Millimeter/submillimeter Array in disks are caused by embedded protoplanets.