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Results for “two-photon absorption”

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 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Interactions of a Microdischarge with a Premixed Flame (Final Technical Report)

In this project we introduced an experimental platform that facilitates the study of the two-way interaction of plasma and flame, and the exploration of the impact of the spatial location of the discharge on its kinetics, in a controlled environment. The experimental platform is a mesoscale CH4/air premixed flame burner that also acts as a dielectric barrier discharge (DBD) operated by nanosecond pulsed voltage. A unique feature of this setup is that the DBD utilizes transparent electrodes, made of Indium Tin Oxide (ITO), to unlock optical access along the line-of-sight parallel to the dominant electric field. This platform is suitable to study both the forward problem (impact of plasma-on-flame), which manifests itself as a modified flame speed as well as flame wrinkling; and the backward problem (impact of flame-on-plasma), which includes plasma regime transitions, between microdischarges and uniform modes, driven by the flame passage. Prior work at MIT has focused on electrical measurements and direct imaging studies of the plasma-flame interaction through the ITO electrode. This project, which was awarded experimental runtime at the Low-temperature Plasma Research Facility (PRF) at Sandia National Laboratories, quantifies the flame-plasma interaction through temporally resolved measurement of key radicals (oxygen atom, O) produced by the nanosecond repetitively pused discharge (NRPD) in an individual microdischarge, using two-photon absorption laser-induced fluorescence (TALIF).

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
NASA NTRS1977

Formation of integrated optics components by multiphoton photorefractive processes

Phase holograms have been formed in pure outdiffused LiNbO3 waveguides using the photorefractive effect initiated by two-photon absorption. Efficient holograms were recorded with two guided waves, of less than 100 W peak power, and less than 10 microJ optical energy. This technique automatically compensates for wave front perturbations in the guide and allows the formation of various integrated components such as wavelength multiplexers and optical switches.

Verber, C. M.↗
NASA NTRS1980

Na + Xe collisions in the presence of two nonresonant lasers

Na+Xe collisions in the presence of two distinct laser fields (rhodamine 110 and Nd:glass) are investigated with reference to the response to nonresonant radiation of alkali metals collisionally perturbed by a buffer gas. It is found that the excited Na-asterisk (4s)+Xe state is produced with a measurable cross section due to two-photon absorption with field intensities as low as 10 MW/sq cm.

De Vries, P. L.↗
NASA NTRS1984

Absolute two-photon excitation cross-sections in NO

A technique has been developed which allows the determination of a two-photon absorption cross-section to be made relative to the Raman scattering cross-section in nitrogen. Spatial and temporal effects associated with the lasers are ratioed out to give a result independent of laser parameters. The necessary theory to extract a cross-section from the measured ratio of a Coherent Anti-Stokes Raman Scattering (CARS) signal in N2 to a four-wave mixing signal in NO has been developed. The technique has been demonstrated on the R(22) + S(12) (J-double-prime = 9 1/2) line in NO and a cross-section of (2.9 + or - 1.8) x 10 to the -49th (cm to the 4th power)-s was determined. This technique appears to be applicable to a number of other diatomic molecules.

Burris, J.↗
NASA NTRS1985

Time-resolved laser-induced fluorescence of selected even-parity 7p states of Xe I

Lifetimes and self-quenching rates have been measured for excited states of Xe I that were populated using simultaneous two-photon absorption. Lifetimes measured in this study are somewhat shorter than those measured using the broadband-excitation technique. Lifetimes reported here are all faster than 100 nsec. Deactivation rates are approximately 2 x 10 to the -10th cu cm/sec per mol.

Mcgee, T. J.↗
DOE OSTI2025

Nonresonant two-photon x-ray absorption in Cu

We present a real-space Green's function theory and calculations of two-photon x-ray absorption (TPA). Our focus is on nonresonant 𝐾-shell TPA in metallic Cu, which has been observed experimentally at intense x-ray free electron laser (XFEL) sources. The theory is based on an independent particle Green's function treatment of the Kramers-Heisenberg equation and an approximation for the sum over nonresonant intermediate states in terms of a static quadrupole transition operator. XFEL effects are modeled by a partially depleted 𝑑 band. This approach is shown to give results for 𝐾-shell TPA in quantitative agreement with XFEL experiment and with a Bethe-Salpeter equation approach. Furthermore, we also briefly discuss many-body corrections and TPA sum rules.

Approximation methods for many-body systems↗
NASA NTRS1979

Two-photon lidar technique for remote sensing of atomic oxygen

A technique is proposed for remote sensing of atomic oxygen by laser excitation of a two-photon transition. Excitation at 2256 A and subsequent fluorescence at 8447 A allow probing of the mesosphere and lower thermosphere without interference by absorption. The two-photon excitation rate is calculated, and its dependence on laser power, duration, and linewidth is discussed. Values are given for remote sensing from a spacecraft at 200 km ranging down to 80 km with 1-km range resolution. Accuracies of better than 10% are expected with a 1 J, a 20-psec excitation pulse and a 1-sq-m collecting telescope.

Mcllrath, T. J.↗
DOE OSTI2025

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↗
NASA NTRS1972

Experimental investigation of transient stimulated Raman scattering in a linearly dispersionless medium.

The results of numerical calculations of the transient stimulated Raman scattering reported previously have been verified experimentally under conditions where both linear dispersion and self-focusing effects were negligible. The existence of a delay between maxima of the laser and Stokes pulses is experimentally demonstrated for the first time, while the pulse shortening in time via Raman scattering is established more firmly than in previous work. The incident-laser-pulse duration, generated-Stokes-pulse duration, and delay between intensity maxima for the laser and Stokes pulses were measured with the two-photon absorption-fluorescence technique. The effective phonon-dephasing time is determined via spontaneous Raman scattering. By using these measured quantities, inferences are made as to the magnitude of the transient gain and the shape of the exciting picosecond laser pulse.

Carman, R. L.↗
NASA NTRS1974

Dual photon effects in nitrogen dioxide photolysis

A previous study demonstrated two-photon consecutive absorption as being the most probable mechanism for the photodissociation of NO2 using a pulsed ruby laser at 6943 A. Additional data discussed here confirmed this and also examined an associated phenomenon, that of multiphoton induced fluorescence. The dissociation of NO2 by ON-O bond cleavage requires 3.4 eV, while the laser energy corresponds to 1.785 eV. The pooling of the energy of two photons would give more than enough energy to dissociate the NO2 into NO + O. Several mechanisms including (1) simultaneous absorption of two photons; (2) reaction of two singly excited NO2; (3) reaction of a singly excited NO2 with a ground state NO2; and (4) consecutive absorption of two photons were examined.

Hakala, D.↗
NASA NTRS1982

The ultraviolet spectrum of Herbig-Haro object 2H

IUE spectra of Herbig-Haro object 2H are presented. The spectra show a strong 'excess' UV continuum and prominent emission lines of C, N, O, Si, Mg, and possibly Al. The continuum, F(lambda), exhibits a turnover shortward of about 1450 A, confirming for the first time the H0 two-photon nature of the emission source. A possible absorption feature near 1680 A, which could result from a new grain or molecular constituent in these protostellar objects is also noted. Recently computed models of steady shocks into partially ionized gas reproduce the two-photon spectral shape, but its observed intensity relative to H-beta and the Balmer continuum is anomalously high. It is suggested that a range of shock velocities, 70-100 km/s, or nonsteady, 'truncated' shocks may be responsible. Future high-sensitivity UV observations of HH objects may be used to probe grain extinction curves in star-forming regions.

Brugel, E. W.↗
DOE OSTI2026

Proposed framework for applying squeezed light to multi-photon absorption plasma diagnostics

We propose a quantum-enhanced plasma diagnostic based on squeezed states of light. Squeezed light can exhibit super-Poissonian photon statistics, leading to enhanced multiphoton absorption cross-sections compared to classical light. This effect enables improved sensitivity for two-photon excitation of high-energy atomic transitions such as ground-state excitation, and results in increased absorbed power and fluorescence in a plasma. We consider two methods of generating squeezed states and evaluate their advantages and limitations in the context of plasma absorption diagnostics. By comparing with and extending previous theoretical work, we predict an enhancement of the absorption signal by up to seven orders of magnitude at low intensities (10 1 W/m 2 ), with diminishing enhancement persisting up to high intensities (10 10 W/m 2 ). These results suggest that squeezed-light sources offer a viable pathway toward quantum-enhanced plasma diagnostics.

imaging↗
NASA NTRS1986

Resonance ionization mass spectrometry for isotopic abundance measurements

Resonance ionization mass spectrometry (RIMS) is a relatively new laser-based technique for the determination of isotopic abundances. The resonance ionization process depends upon the stepwise absorption of photons from the laser, promoting atoms of the element of interest through progressively higher electronic states until an ion is formed. Sensitivity arises from the efficiency of the resonant absorption process when coupled with the power available from commercial laser sources. Selectivity derives naturally from the distinct electronic structure of different elements. This isobaric discrimination has provided the major impetus for development of the technique. Resonance ionization mass spectrometry was used for analysis of the isotopic abundances of the rare earth lutetium. Isobaric interferences from ytterbium severely effect the ability to measure small amounts of the neutron-deficient Lu isotopes by conventional mass spectrometric techniques. Resonance ionization for lutetium is performed using a continuous-wave laser operating at 452 nm, through a sequential two-photon process, with one photon exciting the intermediate resonance and the second photon causing ionization. Ion yields for microgram-sized quantities of lutetium lie between 10(6) and 10(7) ions per second, at overall ionization efficiencies approaching 10(-4). Discrimination factors against ytterbium greater than 10(6) have been measured. Resonance ionization for technetium is also being explored, again in response to an isobaric interference, molybdenum. Because of the relatively high ionization potential for Tc, three-photon, two-color RIMS processes are being developed.

Miller, C. M.↗
DOE OSTI2024

Exploring direct photodetachment and photodissociation–photodetachment dynamics of platinum iodide anions (PtI n - , n = 2–5) using cryogenic photoelectron spectroscopy

The direct photodetachment and two-photon photodissociation–photodetachment processes of a series of PtI n - (n = 2–5) anions were systematically studied using cryogenic anion photoelectron spectroscopy and first-principles electronic structure calculations. The adiabatic/vertical detachment energies (ADEs/VDEs) of these anions were determined from their 193 nm photoelectron (PE) spectra, i.e., 3.54/3.63, 4.04/4.09, 4.33/4.36, and 4.37/4.41 eV for n = 2–5, respectively, and well reproduced by B3LYP-D3(BJ)/aug-cc-pVTZ-pp calculations. As the coordination number increases, the electron affinity (EA) of PtI n • (n = 2–5) neutrals (equivalent to the corresponding anion’s ADE) gradually increases, exceeding the EA of Cl at n = 3 and exhibiting superhalogen characteristics for n ≥ 3. Meanwhile, the ground state transition contributed from detaching electrons in the highest occupied molecular orbital gradually evolves from the central metal Pt to the iodine ligands. For the PtI 3 - anion, besides one-photon direct detachment, four distinct two-photon photodissociation–photodetachment channels were identified, and the competition between them was discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Photoionization of seeded combustion products as a method of enhancing the efficiency of magnetohydrodynamic power generators

Here, in this study, we performed an experimental and computational investigation into the feasibility of utilizing photoionization to enhance the electrical conductivity of seeded oxy-fuel combustion products and improve the performance of magnetohydrodynamic (MHD) power generators. We applied a variety of optical and microwave diagnostics to study the ionization and recombination processes of potassium excited by an excimer laser in a high-velocity oxy-fuel free jet. Computational fluid dynamic (CFD) simulations were performed to model the thermophysical properties and species densities of the free jet. The CFD results were validated with position-dependent potassium concentration measurements. Electron recombination exponential lifetimes were measured through time-resolved microwave transmission. The experimental electron lifetimes were compared with lifetimes calculated from CFD-predicted species densities and literature recombination rates. It was determined that K + or O 2 are the most likely recombination partners for photoionized electrons. Time-resolved fluorescence measurements provided evidence of an ionization pathway involving a two-photon ionization of KOH . Finally, a zero-dimensional chemical kinetic model was developed to assess the fundamental viability of inducing a non-equilibrium electron population to provide a net energy return in combustion-driven MHD power generators. We determined that a high energy return is feasible for targeting electrode boundary layers with ultraviolet photoionization. We also found that photoionization could potentially lower the required temperature of the bulk gas flow.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2026

Spectroscopy and dynamics of the v = 1 levels derived from the OH(D) stretching modes in the I‾∙HDO complex using CW and time-resolved, resonant two-photon infrared excitation of the cryogenically cooled ions

The vibrational energy levels of the two isotopomers adopted by the I‾∙HDO ion-molecule complex occur such that the OH(D) stretching fundamentals span its dissociation energy, thus enabling a spectroscopic investigation of the dynamics displayed by a system prepared in the vicinity of the dissociation threshold. This regime is explored using infrared photoexcitation of the mass-selected complexes cooled in a cryogenic radiofrequency (Paul) ion trap. Survey spectra are obtained at modest resolution using two-color, IR-IR photodissociation with nanosecond lasers to establish the level structure and unimolecular decay dynamics of the v = 1 and 2 levels of the bound OH(D) oscillator. The v = 1 levels are prepared by fixed frequency excitation in the trap and the absorption spectra arising from this excited state are probed by photofragmentation of the complex with a second pulsed IR laser after a variable delay time (0 to 20 ms). The transitions to levels above the dissociation threshold for I‾ + HDO formation are observed to be sharp (~5 cm -1 FWHM). At low pressure, the bound OD (v = 1) population relaxes very slowly (~3 ms), consistent with resonant fluorescence in the IR. The collisional quenching rate constants of this level by the He buffer gas were estimated to be on the order 3 x 10 -12 cm 3 /s based on a crude Stern-Volmer analysis. Here, the rotational fine structure and linewidths (≲0.01 cm -1 FWHM) arising from transitions of the non-bonded OH stretch fundamental of the OD-bound isotopomer that lies just above the dissociation energy are determined using single photon photodissociation by excitation of the 10 K ions with a single-frequency, CW IR laser in the ion trap.

Cryogenic ion infrared spectroscopy↗
DOE OSTI2025

Structural dynamics of laser-ionized cis-stilbene studied by ultrafast electron diffraction

Stilbene has been a model system for studying photoisomerization upon absorption of a UV photon. Although the dynamics of the first excited state have been investigated in great detail, the structural dynamics of cationic states remains largely experimentally unexplored. In this study, the dynamics following ionization via absorption of two UV photons was captured using ultrafast electron diffraction. cis-stilbene (CS) was optically pumped with 267 nm ultraviolet light with two different pump fluences and probed with 3.7 MeV electrons. We compare our experimental results to ab-initio multiple spawning simulations for single-photon excitation and molecular dynamics simulations for ionization in order to separate the contributions from the two channels. We found that with a fluence of 170 mJ cm −2 both the single and two-photon channels are present, while with higher fluence of 280 mJ cm −2 the two-photon channel dominates. We did not observe isomerization of the CS cation and found the main structural motion a to be a vibration of the phenyl rings about the central C–C bond.

74 ATOMIC AND MOLECULAR PHYSICS↗