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Results for “Frequency modulation spectroscopy”

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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Computational expressions for signals in frequency-modulation spectroscopy

In this study, general expressions for the signals in frequency-modulation spectroscopy (FMS) appear in the literature but are often reduced to simple analytical equations following the assumption of a weak modulation index. This is little help to the experimentalist who wants to predict signals for modulation depths of the order of unity or greater, where strong FMS signals reside. Here, we develop general formulas for FMS signals in the case of an absorber with a Voigt line shape and then link these expressions to an example and existing numerical code for the line shape. The resulting computational recipe is easy to implement and exercised here to show where the larger FMS signals are found over the coordinates of modulation index and modulation frequency. One can also estimate from provided curves the in-phase FMS signal over a wide range of modulation parameters at either the Lorentzian-broadening or Doppler-broadening limit, or anywhere in between by interpolation.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Multiplexing of frequency-modulation spectroscopy by spread-spectrum codes, demonstrated in continuous-wave LIDAR

Frequency-modulation spectroscopy (FMS) is generally suited to code-division multiplexing, and we demonstrate that capacity in a form of continuous-wave LIDAR, utilizing a sharp CO 2 absorption transition at 1.6 µm in simple ranging setups. The approach retains the advantages of FMS, including coherent detection and good rejection of broad absorption backgrounds. Extensions of this multiplexed approach to the continuous, simultaneous detection of several transitions would come by transmitting an encoded combination of frequency-modulated carriers, each tuned to detect a unique absorption transition. Signal analysis at the receiver involves a simple process of de-multiplexing that, in a general application, reveals targets at various distances and the absorption-related FMS signals in between.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2015

Time-Resolved, NIR Two-Tone Frequency Modulation Spectroscopy for Quantitative Measurement of HO 2 Radical in Fuel Oxidation Reactions

Time-resolved two-tone frequency modulation (TTFM) absorption spectroscopy has been used to measure, in situ and quantitatively, hydroperoxy (HO 2 ) radical in fuel oxidation reactions at the first overtone transitions (2v 1 ) of HO 2 near 1509nm. Typical HO 2 detection limit is on the order of 10 11 molecule cm -3 , which corresponds to a relative absorption of 10 -5 . TTFM method successfully removes low frequency thermal lensing noise in measured HO 2 kinetic time traces, which is a general noise source in fuel oxidation absorption experiments. Compared with previous works, we have upgraded the TTFM experiment with a NIR distributed feedback (DFB) diode laser, a fiber-coupled broadband phase modulator, and a two-channel wave generator, which have improve the performance of our experiment substantially.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Determination of the sign of the population difference in a two-level system by frequency-modulation spectroscopy

Population inversions can occur in two-level systems as a result of chemical kinetic processes that involve pulsed excitation of a system with a large amount of excess energy, for example, multi-photon dissociation. In this work, we report the use of frequency-modulation (FM) spectroscopy to determine, from the phase of the FM signal, the sign of the population difference in a two-level system – specifically, whether the two-level system is inverted. Here, as a proof of principle demonstration of this technique, we show that FM signals from an inverted I 2 B 3 Π 0+u – X 1 $Σ$ $^+$$_g$ transition, prepared by a pulsed laser, have opposite phase with respect to signals from a non-inverted system, the Rb D 1 -line absorption transition.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

One-colour (~220 nm) resonance-enhanced (S 1 –S 0 ) multi-photon dissociation of acetylene: probe of the C 2 A 1 Π u – X 1 Σ + g band by frequency-modulation spectroscopy

In a recent paper, we demonstrated that one-colour (~220 nm), resonance-enhanced (S 1 –S 0 ), photodissociation of acetylene generates strong $C_2$ Swan band ($d^3Π_g–a^3Π_u$) and $C_2$ Deslandres-d'Azambuja band ($C^1Π_g–A^1Π_u$) fluorescence, and long-lived (>3 µs) fluorescence from an electronically-excited $C_2$H * species. It was not known whether the $C_2A^1Π_u$ and $X^1Σ^+_g$ states are also directly populated in this process. In this paper, multiple vibration-rotation transitions between the $C_2A$-state v = 2 and the X-state v = 0 level are examined by time-resolved frequency-modulation (FM) spectroscopy. The photolysis laser wavelength is tuned into resonance at the one-photon level with S 1 –S 0 transitions that populate individual rotational levels of the S 1 $_{trans}$-conformer $3^2,3^3,$ and $3^4$ vibrational states. By comparing the phase of the FM signals from the $C_2A–X$ transitions with that from the Rb D 1 -line absorption transition, we determine that, for all of the probed A–X transitions, the X-state level is more populated than the A-state level. We propose that the acetylene S 1 level is excited by the second photon to an acetylene dissociation precursor state, which undergoes sequential C-H bond-breaking to produce the $C_2X$ state. The dissociation precursor is assigned as the $1^1B_g(trans-bent)/1^1B_1(cis-bent)$ valence state, which correlates to a doubly-excited configuration, $(1π_u)^2(1π_g)^2$, at linear geometry. Based on the rotational distributions of the $C_2X$-state fragments, we believe that at least one of the transition states involved in the photolysis via S 1 $3^4$ has a larger CC-H bend-angle for the departing H-atom than that involved in the S 1 $3^2$ and $3^3$ photolysis.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2012

Time-resolved Hyperspectral Fluorescence Spectroscopy using Frequency Modulated Excitation

An intensity-modulated excitation light source is used together with a micro channel plate intensified CCD (ICCD) detector gated at a slightly different frequency to generate a beat frequency from a fluorescent sample. The addition of a spectrograph produces a hyperspectral time-resolved data product where the resulting beat frequency is detected with a low frame rate camera. Measuring the beat frequency of the spectrum as a function of time allows separation of the excited fluorescence from ambient constant light sources. The excitation and detector repetition rates are varied over a range of discrete frequencies, and the phase shift of the beat wave maps out the emission decay rate(s).

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2014

Frequency stabilization of a 1083 nm fiber laser to {sup 4}He transition lines with optical heterodyne saturation spectroscopies

Two kinds of optical heterodyne saturation spectroscopies, namely, frequency modulation spectroscopy (FMS) and modulation transfer spectroscopy (MTS), are demonstrated for locking a fiber laser to the transition lines of metastable {sup 4}He atoms around 1083 nm. The servo-loop error signals of FMS and MTS for stabilizing laser frequency are optimized by studying the dependence of the peak-to-peak amplitude and slope on the optical power of pump and probe beams. A comparison of the stabilization performances of FMS/MTS and polarization spectroscopy (PS) is presented, which shows that MTS exhibits relatively superior performance with the least laser frequency fluctuation due to its flat-background dispersive signal, originated from the four-wave mixing process. The Allan deviation of the stabilized laser frequency is 5.4 × 10{sup −12}@100 s with MTS for data acquired in 1000 s, which is sufficiently applicable for fields like laser cooling, optical pumping, and optical magnetometry.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2019

Kinetic Study of the OH + Ethylene Reaction using Frequency Modulated Laser Absorption Spectroscopy

The pressure dependence of the OH + C 2 H 4 addition reaction has been investigated using frequency modulated laser absorption spectroscopy to monitor OH kinetics. Bimolecular rate coefficients for the title reaction are reported in argon bath gas at room temperature and total pressures ranging from 2–361Torr. The pressure dependent rate coefficients measured here agree well with the majority of published kinetic studies under similar conditions. Previous high-level ab initio calculations have identified a pre-reaction complex on the OH + C 2 H 4 potential energy surface. In conclusion, the influence of this complex on the OH + C 2 H 4 kinetics has been investigated using one-dimensional master equation analyses of the current and previous experimental measurements

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Investigating the photodissociation of H 2 O 2 using frequency modulation laser absorption spectroscopy to monitor radical products

In this study, the photodissociation of H 2 O 2 dilute in argon at 193 nm has been investigated using near infrared frequency modulation laser absorption spectroscopy on selected rotational lines of the OH vibrational overtone bands between 6500 and 7100 cm -1 to detect the OH and HO 2 radical products with the same laser. Sequential OH and HO 2 time-dependent profiles have been measured at room temperature and total pressures ranging from 3 to 56 Torr. Kinetic analysis gives the product distribution following H 2 O 2 photolysis of (82±1) % OH and (18±1)% HO 2 under the present conditions, in excellent agreement with previously reported measurements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2011

A discharge with a magnetic X-point as a negative hydrogen ion source

The study presents first results from investigations of a novel low-pressure plasma source, intended for a negative hydrogen ion production. The source utilizes a dc magnetic field, shaped to form a cusp with a magnetic null-point (X-point). Beside the common role of filtering out the high energy electrons, this magnetic field configuration ensures in the present case also an interesting mechanism of coupling the RF power to the plasma. Investigations performed using radio frequency modulation spectroscopy (RFMOS) reveal that the main power coupling to the electrons is confined in the region on one side of the X-point. The modulation of the light intensity indicates also the presence of a strong dc drift close to the plane of the X-point. Several hypothesises for its explanation are raised: an azimuthal diamagnetic drift due to strong axial gradients of the electron energy, the excitation of a standing helicon wave, which couples to the radial magnetic field in the plane of the X-point, or a Trivelpiece-Gould wave which is resonantly absorbed near the plane of the X-point.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2017

Silicon Photoelectrode Thermodynamics and Hydrogen Evolution Kinetics Measured by Intensity-Modulated High-Frequency Resistivity Impedance Spectroscopy

Here, we present an impedance technique based on light intensity-modulated high-frequency resistivity (IMHFR) that provides a new way to elucidate both the thermodynamics and kinetics in complex semiconductor photoelectrodes. We apply IMHFR to probe electrode interfacial energetics on oxide-modified semiconductor surfaces frequently used to improve the stability and efficiency of photoelectrochemical water splitting systems. Combined with current density-voltage measurements, the technique quantifies the overpotential for proton reduction relative to its thermodynamic potential in Si photocathodes coated with three oxides (SiO x , TiO 2 , and Al 2 O 3 ) and a Pt catalyst. In pH 7 electrolyte, the flatband potentials of TiO 2 - and Al 2 O 3 -coated Si electrodes are negative relative to samples with native SiO x , indicating that SiO x is a better protective layer against oxidative electrochemical corrosion than ALD-deposited crystalline TiO 2 or Al 2 O 3 . Adding a Pt catalyst to SiO x /Si minimizes proton reduction overpotential losses but at the expense of a reduction in available energy characterized by a more negative flatband potential relative to catalyst-free SiO x /Si.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2019

Accuracy of tip-sample interaction measurements using dynamic atomic force microscopy techniques: Dependence on oscillation amplitude, interaction strength, and tip-sample distance

Atomic force microscopy (AFM) is a versatile surface characterization method that can map a sample’s topography with high spatial resolution while simultaneously interrogating its surface chemistry through the site-specific high-resolution quantification of the forces acting between the sample and the probe tip. Thanks to considerable advances in AFM measurement technology, such local measurements of chemical properties have gained much popularity in recent years. To this end, dynamic AFM methodologies are implemented where either the oscillation frequency or the oscillation amplitude and phase of the vibrating cantilever are recorded as a function of tip-sample distance and subsequently converted to reflect tip-sample forces or interaction potentials. Such conversion has, however, been shown to produce non-negligible errors when applying the most commonly used mathematical conversion procedures if oscillation amplitudes are of the order of the decay length of the interaction. Extending on these earlier findings, the computational study presented in this paper reveals that the degree of divergence from actual values may also critically depend on both the overall strength of tip-sample interaction and the distance at which the interaction is obtained. These systematic errors can, however, be effectively eliminated by using oscillation amplitudes that are sufficiently larger than the decay length of the interaction potential.

Electrical properties and parameters↗
DOE OSTI2012

Laser frequency stabilisation by the Pound - Drever - Hall method using an acousto-optic phase modulator operating in the pure Raman - Nath diffraction regime

Frequency stabilisation of diode laser radiation has been implemented by the Pound - Drever - Hall method using a new acousto-optic phase modulator, operating in the pure Raman - Nath diffraction regime. It is experimentally shown that, as in the case of saturated-absorption spectroscopy in atomic vapour, the spatial divergence of the frequency-modulated output spectrum of this modulator does not interfere with obtaining error signals by means of heterodyne frequency-modulation spectroscopy with a frequency discriminator based on a high-Q Fabry - Perot cavity with finesse of several tens of thousands.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Near-MHz temperature and H 2 O measurements in post-detonation fireballs of 25 g hemispherical explosives using scanned-wavelength-modulation spectroscopy

A laser absorption spectroscopy diagnostic integrated within a hardened optical probe was used to measure temperature and water mole fraction at 500 kHz in post-detonation fireballs of explosives. In the experiments, an exploding-bridgewire detonator initiated a 25 g hemisphere of explosive (N5 or PETN). This produced a hemispherical fireball that traveled radially towards a hardened measurement probe. The probe contained a pressure transducer and optical equipment to pitch fiber-coupled laser light across a 12.6 cm gap onto a detector. Tunable diode lasers emitting near 7185.6 and 6806 c m − <#comment/> 1 were used to measure the absorbance spectrum of H 2 O utilizing peak-picking scanned-wavelength-modulation spectroscopy with a scan frequency of 500 kHz and modulation frequencies of 35 and 45.5 MHz, respectively. This enabled measurements of temperature and X H 2 O in the shock-heated air and trailing fireball at 500 kHz. Time histories of pressure, temperature, and H 2 O mole fraction were acquired at different standoff distances to quantify how the fireball evolved in space and time as well as to compare measured quantities between PETN and N5 fireballs. The standard deviation of temperature and X H 2 O during one representative test were found to be 17 K (1.3%) and 0.011 (5%), respectively. These measurements demonstrate this diagnostic’s ability to provide rapid and reliable measurements in harsh, highly transient post-detonation environments produced by solid explosives.

Schwartz, Charles J.↗
DOE OSTI2012

Multiplexed gas spectroscopy using tunable VCSELs

Detection and identification of gas species using tunable laser diode laser absorption spectroscopy has been performed using vertical cavity surface emitting lasers (VCSEL). Two detection methods are compared: direct absorbance and wavelength modulation spectroscopy (WMS). In the first, the output of a DC-based laser is directly monitored to detect for any quench at the targeted specie wavelength. In the latter, the emission wavelength of the laser is modulated by applying a sinusoidal component on the drive current of frequency {omega}, and measuring the harmonics component (2{omega}) of the photo-detected current. This method shows a better sensitivity measured as signal to noise ratio, and is less susceptible to interference effects such as scattering or fouling. Gas detection was initially performed at room temperature and atmospheric conditions using VCSELs of emission wavelength 763 nm for oxygen and 1392 nm for water, scanning over a range of approximately 10 nm, sufficient to cover 5-10 gas specific absorption lines that enable identification and quantization of gas composition. The amplitude and frequency modulation parameters were optimized for each detected gas species, by performing two dimensional sweeps for both tuning current and either amplitude or frequency, respectively. We found that the highest detected signal is observed for a wavelength modulation amplitude equal to the width of the gas absorbance lines, in good agreement with theoretical calculations, and for modulation frequencies below the time response of the lasers (<50KHz). In conclusion, we will discuss limit of detection studies and further implementation and packaging of VCSELs in diode arrays for continuous and simultaneous monitoring of multiple species in gaseous mixtures.

42 ENGINEERING↗
DOE OSTI2023

THz Plasmonics and Topological Optics of Weyl Semimetals

THz magneto-optical properties of 3D topological Weyl semimetals were investigated with both THz spectroscopy and THz pump-probe measurements. The unique THz effects predicted in these materials may have important applications in THz technology. The electronic band structure was characterized spectroscopically through THz zero-field reflectance and/or cyclotron resonance measurements. The studies included the dynamic chiral pumping and the study of the predicted novel magneto-electric effects arising from the underlying Berry curvature and magneto plasmonic-like effects in the absence of an applied magnetic field. Chiral pumping in the extreme quantum limit was studied on Weyl semimetals to directly probe the chiral N=0 Landau level. Non-linear pump-probe measurements were used to measure the chiral pumping lifetime. Solids with topologically robust electronic states exhibit unusual electronic and optical transport properties that do not exist in other materials. A particularly interesting example is chiral charge pumping, the so-called chiral anomaly, in recently discovered topological Weyl and Dirac semimetals, where simultaneous application of parallel DC electric and magnetic fields creates an imbalance in the number of carriers of opposite topological charge (chirality). In an earlier study we investigated the Weyl metals Na 3 Bi and Cd 3 As 2 . In this grant we followed up with magneto-optical studies of TaAs, another Weyl semimetal. More recently, we have also characterized other Weyl and Dirac systems that have come on line. The Physics community is still looking for the “hydrogen atom” of the Weyl semimetal. CoSi is one promising new system which features Weyl node spacing comparable to the Brillouin zone size. This system may be suitable for study of the predicted chiral plasmons that arise from the Berry curvature in Weyl materials. In other experiments gates can be applied to the samples in order to study the Fermi arc surface states by modulation reflectance spectroscopy at THz frequencies.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Rotational Spectra in 29 Vibrationally Excited States of Interstellar Aminoacetonitrile

We report a detailed spectroscopic investigation of the interstellar aminoacetonitrile, a possible precursor molecule of glycine. Using a combination of Stark and frequency-modulation microwave and millimeter wave spectroscopies, we observed and analyzed the room-temperature rotational spectra of 29 excited states with energies up to 1000 cm{sup −1}. We also observed the {sup 13}C isotopologues in the ground vibrational state in natural abundance (1.1%). The extensive data set of more than 2000 new rotational transitions will support further identifications of aminoacetonitrile in the interstellar medium.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗