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At least 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Substituent effect on napthodithiophene-fused porphyrins: Understanding the unusual trend of fluorescence quantum yield quenching

A series of π-extended porphyrins containing thiophene units was prepared to investigate an unusual trend observed in the fluorescence quantum yield of naphtho[2,1-b:3,4-b']dithiophene-fused porphyrins. Monobenzoporphyrins carrying 2-thiophenyl (vinyl thiophene porphyrin) groups (2VTP, 2VTBr and Br2VTP) (numbering 2 and 3 refers to the position of sulfur on the thiophene ring) were synthesized through a Heck-based cascade reaction followed by a newly developed bromination method. These were converted to naphtho[2,1-b:3,4-b']dithiophene-fused porphyrin derivatives (FBr2VTP and F2VTBr) via ring closure with an intramolecular Scholl reaction. Increasingly larger Stokes shifts with a higher number of bromo groups were observed in the unfused π-extended molecular systems, reflecting the heavy atom effect. Fluorescence spectroscopy further confirmed the unusual trend seen in the previous work: structural rigidification in naphtho[2,1-b:3,4-b']dithiophene-fused porphyrins leads to longer fluorescence lifetimes but unexpectedly lowers the quantum yield. Adding one bromo group to the naphtho[2,1-b:3,4-b']dithiophene unit does not change this trend. Furthermore, the presence of two bromo groups prevents the quantum yield from dropping. DFT, TDDFT, and NICS analyses suggest a drastic change in aromaticity in the pyrrole ring where the naphtho[2,1-b:3,4-b']dithiophene is fused in FBr2VTP, which might contribute to the quantum yield reductions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Deep learning-based temporal deconvolution for photon time-of-flight distribution retrieval

The acquisition of the time of flight (ToF) of photons has found numerous applications in the biomedical field. Over the last decades, a few strategies have been proposed to deconvolve the temporal instrument response function (IRF) that distorts the experimental time-resolved data. However, these methods require burdensome computational strategies and regularization terms to mitigate noise contributions. Herein, we propose a deep learning model specifically to perform the deconvolution task in fluorescence lifetime imaging (FLI). The model is trained and validated with representative simulated FLI data with the goal of retrieving the true photon ToF distribution. Its performance and robustness are validated with well-controlled in vitro experiments using three time-resolved imaging modalities with markedly different temporal IRFs. The model aptitude is further established with in vivo preclinical investigation. Overall, these in vitro and in vivo validations demonstrate the flexibility and accuracy of deep learning model-based deconvolution in time-resolved FLI and diffuse optical imaging.

Pandey, Vikas (ORCID:0000000154771095)↗
DOE OSTI2020

Ultrafast quantum photonics enabled by coupling plasmonic nanocavities to strongly radiative antennas

Quantum emitters coupled to plasmonic nanostructures can act as exceptionally bright sources of single photons, operating at room temperature. Plasmonic mode volumes supported by these nanostructures can be several orders of magnitude smaller than the cubic wavelength, which leads to dramatically enhanced light–matter interactions and drastically increased photon production rates. However, when increasing the light localization further, these deeply subwavelength modes may in turn hinder the fast outcoupling of photons into free space. Plasmonic hybrid nanostructures combining a highly confined cavity mode and a larger antenna mode circumvent this issue. We establish the fundamental limits for quantum emission enhancement in such systems and find that the best performance is achieved when the cavity and antenna modes differ significantly in size. We experimentally support this idea by photomodifying a nanopatch antenna deterministically assembled around a nanodiamond known to contain a single nitrogen–vacancy (NV) center. As a result, the cavity mode shrinks, further shortening the NV fluorescence lifetime and increasing the single-photon brightness. Our analytical and numerical simulation results provide intuitive insight into the operation of these emitter–cavity–antenna systems and show that this approach could lead to single-photon sources with emission rates up to hundreds of THz and efficiencies close to unity.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Anomalous Purcell decay of strongly driven inhomogeneous emitters coupled to a cavity

We perform resonant fluorescence lifetime measurements on a nanocavity-coupled erbium ensemble as a function of cavity-laser detuning and pump power. Our measurements reveal an anomalous three-fold suppression of the ensemble Purcell factor at zero cavity detuning and high pump fluence. We capture qualitative aspects of this decay rate suppression using a Tavis–Cummings model of non-interacting spins coupled to a common cavity.

36 MATERIALS SCIENCE↗
NASA NTRS1979

The LASL program in nuclear pumped liquid lasers

The development of nuclear-pumped, liquid-based lanthanide ion lasers is discussed. Early investigations of lanthanide ion lasers have lead to solid-state and gaseous neodymium lasers, and a demonstration of lasing in the liquid state. Solvents containing organic chelating agents have been employed in liquid Eu(+3) and Tb(+3) lasers to extend fluorescence lifetimes, however aprotic solvents have been found to enable the development of large-scale liquid lasers. The advantages to be gained from high-power nuclear-pumped lasers based on lanthanide solutions include the high density of fissile materials possible, and a nuclear pumping cell which can operate in either a nuclear or optical pumping mode is being fabricated at the Los Alamos Scientific Laboratory to investigate the nuclear pumping of liquid lanthanide ion lasers. Areas that need exploration before specific laser design features can be considered include energy channeling within the liquid upon excitation, radiation damage due to solvent dissociation, and reactor technology for the development of a self-critical liquid reactor.

Mansfield, C. R.↗
NASA NTRS1985

Analysis of vibronic transitions in titanium doped sapphire using the temperature of the fluorescence spectra

An analysis of the fluorescence spectra of titanium-doped sapphire crystals for temperatures ranging from 13 to 578 K is made. Zero- and multiphoton assisted electronic transitions are observed at temperatures below 125 K. Zero-phonon transition energies agree with previously reported measured and predicted values. Photon-assisted transitions suggest that two principle modes of lattice vibrations with energies of 220 and 260/cm are coupled to the electronic 2T2g state. A single phonon energy of 173/cm is observed to couple to the 2Eg electronic state. Crossover energy is estimated to be about 11,800/cm using a simple harmonic approximation. Lineshape analysis is performed. The fluorescence lifetime as measured to be a constant 3.9 microsec below 150 k decreasing to 2.9 microsec at 300 K.

Byvik, C. E.↗
NASA NTRS1986

Spectroscopic and laser characteristics of Ti:Al2O3

Spectroscopic measurements and laser performance of T:Al2O3 are discussed in detail. Data on absorption and fluorescence spectra and fluorescence lifetime as a function of temperature are presented. Laser characteristics observed with pulsed-dye-laser, frequency-doubled Nd:YAG-laser, and argon-ion-laser pumping are covered and show that nearly quantum-limited conversion of pump radiation cna be achieved, along with tuning over the wavelength range 660-986 nm.

Moulton, P. F.↗
NASA NTRS1992

Time and wavelength domain algorithms for chemical analysis by laser radar

Laser-induced fluorescence (LIF) is a promising technique for laser radar applications. Laser radar using LIF has already been applied to algae blooms and oil slicks. Laser radar using LIF has great potential for remote chemical analysis because LIF spectra are extremely sensitive to chemical composition. However, most samples in the real world contain mixtures of fluorescing components, not merely individual components. Multicomponent analysis of laser radar returns from mixtures is often difficult because LIF spectra from solids and liquids are very broad and devoid of line structure. Therefore, algorithms for interpreting LIF spectra from laser radar returns must be able to analyze spectra that overlap in multicomponent systems. This paper analyzes the possibility of using factor analysis-rank annihilation (FARA) to analyze emission-time matrices (ETM) from laser radar returns instead of excitation-emission matrices (EEM). The authors here define ETM as matrices where the rows (or columns) are emission spectra at fixed times and the columns (or rows) are temporal profiles for fixed emission wavelengths. Laser radar usually uses pulsed lasers for ranging purposes, which are suitable for measuring temporal profiles. Laser radar targets are hard instead of diffuse; that is, a definite surface emits the fluorescence instead of an extended volume. A hard target would not broaden the temporal profiles as would a diffuse target. Both fluorescence lifetimes and emission spectra are sensitive to chemical composition. Therefore, temporal profiles can be used instead of excitation spectra in FARA analysis of laser radar returns. The resulting laser radar returns would be ETM instead of EEM.

Rosen, David L.↗
NASA NTRS2001

Making Sense of Plant Health

Ciencia, Inc. created a new device, known as a Portable Photosynthesis Analyzer, or Phase Fluorometer, that provides real-time data about the photochemical efficiency of phytoplankton and other plant forms. The commercial version of this technology is used for photosynthesis research and offers major benefits to the field of life science. This new instrument is the first portable instrument of its kind. Through a license agreement with Ciencia, Oriel Instruments, of Stratford, Connecticut, manufactures and markets the commercial version of the instrument under the name LifeSense.TMLifeSense is a 70 MHz single-frequency fluorometer that offers unrivaled capabilities for fluorescence lifetime sensing and analysis. LifeSense provides information about all varieties of photosynthetic systems. Photosynthesis research contributes important health assessments about the plant, be it phytoplankton or a higher form of plant life. With its unique sensing capabilities, LifeSense furnishes data regarding the yield of a plant's photochemistry, as well as its levels of photosynthetic activity. The user can then gain an extremely accurate estimate of the plant's chlorophyll biomass, primary production rates, and a general overview of the plant's physiological condition.

Source record↗
NASA NTRS2003

Cellular Oxygen and Nutrient Sensing in Microgravity Using Time-Resolved Fluorescence Microscopy

Oxygen and nutrient sensing is fundamental to the understanding of cell growth and metabolism. This requires identification of optical probes and suitable detection technology without complex calibration procedures. Under this project Microcosm developed an experimental technique that allows for simultaneous imaging of intra- and inter-cellular events. The technique consists of frequency-domain Fluorescence Lifetime Imaging Microscopy (FLIM), a set of identified oxygen and pH probes, and methods for fabrication of microsensors. Specifications for electronic and optical components of FLIM instrumentation are provided. Hardware and software were developed for data acquisition and analysis. Principles, procedures, and representative images are demonstrated. Suitable lifetime sensitive oxygen, pH, and glucose probes for intra- and extra-cellular measurements of analyte concentrations have been identified and tested. Lifetime sensing and imaging have been performed using PBS buffer, culture media, and yeast cells as a model systems. Spectral specifications, calibration curves, and probes availability are also provided in the report.

Szmacinski, Henryk↗
NASA NTRS2004

Depth-Penetrating Measurements Developed for Thermal Barrier Coatings Incorporating Thermographic Phosphors

The insulating properties of thermal barrier coatings (TBCs) provide highly beneficial thermal protection to turbine engine components by reducing the temperature sustained by those components. Therefore, measuring the temperature beneath the TBC is critical for determining whether the TBC is performing its insulating function. Currently, noncontact temperature measurements are performed by infrared pyrometry, which unfortunately measures the TBC surface temperature rather than the temperature of the underlying component. To remedy this problem, the NASA Glenn Research Center, under the Information Rich Test Instrumentation Project, developed a technique to measure the temperature beneath the TBC by incorporating a thin phosphor layer beneath the TBC. By performing fluorescence decay-time measurements on light emission from this phosphor layer, Glenn successfully measured temperatures from the phosphor layer up to 1100 C. This is the first successful demonstration of temperature measurements that penetrate beneath the TBC. Thermographic phosphors have a history of providing noncontact surface temperature measurements. Conventionally, a thermographic phosphor is applied to the material surface and temperature measurements are performed by exciting the phosphor with ultraviolet light and then measuring the temperature-dependent decay time of the phosphor emission at a longer wavelength. The innovative feature of the new approach is to take advantage of the relative transparency of the TBC (composed of yttria-stabilized zirconia) in order to excite and measure the phosphor emission beneath the TBC. The primary obstacle to achieving depth-penetrating temperature measurements is that the TBCs are completely opaque to the ultraviolet light usually employed to excite the phosphor. The strategy that Glenn pursued was to select a thermographic phosphor that could be excited and emit at wavelengths that could be transmitted through the TBC. The phosphor that was selected was yttria doped with europia (Y2O3:Eu), which has a minor excitation peak at 532 nm (green) and an emission peak at 611 nm (red)--both are wavelengths that exhibit significant transmission through the TBC. The measurements were performed on specimens consisting of a 25- m-thick phosphor layer beneath a 100- m-thick TBC. The 532-nm (green) excitation light was provided by a frequency-doubled YAG:Nd (yttrium-aluminum-garnet:neodymium) laser, and the fluorescence decay time measurements were acquired with a modified Raman microscope. The preceding graph compares the intensity of the phosphor emission of the phosphor layer above the TBC versus that of the phosphor layer beneath the TBC. Although there was considerable attenuation of the phosphor signal (a factor of 30), the phosphor emission at the reduced intensity was more than sufficient to perform fluorescence decay time measurements. The following graph shows the fluorescence lifetime temperature dependency for the Y2O3:Eu phosphor layers both above and below the TBC. These curves show an excellent match and indicate that, despite the attenuation due to the overlying TBC, the phosphor layer beneath the TBC still functions as an effective temperature indicator.

Eldridge, Jeffrey I.↗
NASA NTRS2005

Two-Photon Fluorescence Microscope for Microgravity Research

A two-photon fluorescence microscope has been developed for the study of biophysical phenomena. Two-photon microscopy is a novel form of laser-based scanning microscopy that enables three-dimensional imaging without many of the problems inherent in confocal microscopy. Unlike one-photon optical microscopy, two-photon microscopy utilizes the simultaneous nonlinear absorption of two near-infrared photons. However, the efficiency of two-photon absorption is much lower than that of one-photon absorption, so an ultra-fast pulsed laser source is typically employed. On the other hand, the critical energy threshold for two-photon absorption leads to fluorophore excitation that is intrinsically localized to the focal volume. Consequently, two-photon microscopy enables optical sectioning and confocal performance without the need for a signal-limiting pinhole. In addition, there is a reduction (relative to one-photon optical microscopy) in photon-induced damage because of the longer excitation wavelength. This reduction is especially advantageous for in vivo studies. Relative to confocal microscopy, there is also a reduction in background fluorescence, and, because of a reduction in Rayleigh scattering, there is a 4 increase of penetration depth. The prohibitive cost of a commercial two-photon fluorescence-microscope system, as well as a need for modularity, has led to the construction of a custom-built system (see Figure 1). This system includes a coherent mode-locked titanium: sapphire laser emitting 120-fs-duration pulses at a repetition rate of 80 MHz. The pulsed laser has an average output power of 800 mW and a wavelength tuning range of 700 to 980 nm, enabling the excitation of a variety of targeted fluorophores. The output from the laser is attenuated, spatially filtered, and then directed into a confocal scanning head that has been modified to provide for side entry of the laser beam. The laser output coupler has been replaced with a dichroic filter that reflects the longer-wavelength excitation light and passes the shorter-wavelength fluorescence light. Also, the confocal pinhole has been removed to increase the signal strength. The laser beam is scanned by a twoperpendicular- axis pair of galvanometer mirrors through a pupil transfer lens into the side port of an inverted microscope. Finally, the beam is focused by a 63-magnification, 1.3-numerical- aperture oil-immersion objective lens onto a specimen. The pupil transfer lens serves to match the intermediate image planes of the scanning head and the microscope, and its location is critical. In order to maximize the quality of the image, (that is, the point spread function of the objective lens for all scan positions), the entire system was modeled in optical-design software, and the various free design parameters (the parameters of the spatial-filter components as well as the separations of all of the system components) were determined through an iterative optimization process. A modular design was chosen to facilitate access to the optical train for future fluorescence correlation spectroscopy and fluorescence-lifetime experiments.

Fischer, David G.↗
NASA NTRS2004

NASA Tech Briefs, April 2004

Topics covered include: Analysis of SSEM Sensor Data Using BEAM; Hairlike Percutaneous Photochemical Sensors; Video Guidance Sensors Using Remotely Activated Targets; Simulating Remote Sensing Systems; EHW Approach to Temperature Compensation of Electronics; Polymorphic Electronic Circuits; Micro-Tubular Fuel Cells; Whispering-Gallery-Mode Tunable Narrow-Band-Pass Filter; PVM Wrapper; Simulation of Hyperspectral Images; Algorithm for Controlling a Centrifugal Compressor; Hybrid Inflatable Pressure Vessel; Double-Acting, Locking Carabiners; Position Sensor Integral with a Linear Actuator; Improved Electromagnetic Brake; Flow Straightener for a Rotating-Drum Liquid Separator; Sensory-Feedback Exoskeletal Arm Controller; Active Suppression of Instabilities in Engine Combustors; Fabrication of Robust, Flat, Thinned, UV-Imaging CCDs; Chemical Thinning Process for Fabricating UV-Imaging CCDs; Pseudoslit Spectrometer; Waste-Heat-Driven Cooling Using Complex Compound Sorbents; Improved Refractometer for Measuring Temperatures of Drops; Semiconductor Lasers Containing Quantum Wells in Junctions; Phytoplankton-Fluorescence-Lifetime Vertical Profiler; Hexagonal Pixels and Indexing Scheme for Binary Images; Finding Minimum-Power Broadcast Trees for Wireless Networks; and Automation of Design Engineering Processes.

Source record↗
NASA NTRS1992

Radiative lifetimes in B I using ultraviolet and vacuum-ultraviolet laser-induced fluorescence

Radiative lifetimes of the eight lowest even parity levels in the doublet system of B I are measured using time-resolved laser-induced fluorescence in the UV and VUV on an atomic beam of boron. The accurate lifetimes provide a base for improved determination of absolute transition probabilities in B I. The techniques described are broadly applicable to measurement of lifetimes of levels with transitions in the visible, UV, and VUV in almost any element.

O'Brian, T. R.↗
DOE OSTI2025

Generation of a fluorescent short-lifetime oxygen nanosensor by coupling of an exciplex forming dye pair

Typical oxygen-sensitive dyes have lifetimes in the μs-ms regime for sensitive oxygen detection based on molecular quenching. Due to the long triplet-state lifetimes and poor quenching efficiency of these probes, it has been difficult to develop short lifetime probes. We have developed oxygen sensors using a short-lifetime dye (∼30–60 ns) that forms an anthracene-aniline exciplex, which is quenched by molecular oxygen through an excited-state charge transfer mechanism. To achieve measurements in aqueous systems, we have tethered the dyes together via a C3 alkyl linker to facilitate greater exciplex formation at low dye concentration (20 μg mL −1 ) and encapsulated the resulting compound into polymeric nanoparticles to form an aqueous-dispersible short-lifetime oxygen nanosensor. The sensors emit at 420 nm (unfolded dye) and 500 nm (exciplex), and the ratiometric Stern-Volmer Constant is 1.52 ± 0.02 L mol −1 , showing good sensitivity from 0 % to 40 % dissolved oxygen without the tradeoff of a long lifetime needed for direct molecular quenching. In this paper, we characterize this sensor for both lifetime-based measurements using time-correlated single-photon counting and ratiometric intensity-based measurements using the unfolded dye emission as an internal reference peak.

Biological and medical sciences↗
NASA NTRS2005

Improved Charge-Transfer Fluorescent Dyes

Improved charge-transfer fluorescent dyes have been developed for use as molecular probes. These dyes are based on benzofuran nuclei with attached phenyl groups substituted with, variously, electron donors, electron acceptors, or combinations of donors and acceptors. Optionally, these dyes could be incorporated as parts of polymer backbones or as pendant groups or attached to certain surfaces via self-assembly-based methods. These dyes exhibit high fluorescence quantum yields -- ranging from 0.2 to 0.98, depending upon solvents and chemical structures. The wavelengths, quantum yields, intensities, and lifetimes of the fluorescence emitted by these dyes vary with (and, hence, can be used as indicators of) the polarities of solvents in which they are dissolved: In solvents of increasing polarity, fluorescence spectra shift to longer wavelengths, fluorescence quantum yields decrease, and fluorescence lifetimes increase. The wavelengths, quantum yields, intensities, and lifetimes are also expected to be sensitive to viscosities and/or glass-transition temperatures. Some chemical species -- especially amines, amino acids, and metal ions -- quench the fluorescence of these dyes, with consequent reductions in intensities, quantum yields, and lifetimes. As a result, the dyes can be used to detect these species. Another useful characteristic of these dyes is a capability for both two-photon and one-photon absorption. Typically, these dyes absorb single photons in the ultraviolet region of the spectrum (wavelengths < 400 nm) and emit photons in the long-wavelength ultraviolet, visible, and, when dissolved in some solvents, near-infrared regions. In addition, these dyes can be excited by two-photon absorption at near-infrared wavelengths (600 to 800 nm) to produce fluorescence spectra identical to those obtained in response to excitation by single photons at half the corresponding wavelengths (300 to 400 nm). While many prior fluorescent dyes exhibit high quantum yields, solvent-polarity- dependent fluorescence behavior, susceptibility to quenching by certain chemical species, and/or two-photon fluorescence, none of them has the combination of all of these attributes. Because the present dyes do have all of these attributes, they have potential utility as molecular probes in a variety of applications. Examples include (1) monitoring curing and deterioration of polymers; (2) monitoring protein expression; (3) high-throughput screening of drugs; (4) monitoring such chemical species as glucose, amines, amino acids, and metal ions; and (5) photodynamic therapy of cancers and other diseases.

Meador, Michael↗