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Results for “RESONANCE FLUORESCENCE”

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
NASA NTRS1980

Zeeman degeneracy effects in collisional intense-field resonance fluorescence

Resonance fluorescence due to intense laser fields from a Zeeman degenerate atom being perturbed by collisional interactions is calculated in the impact regime by using the quantum-fluctuation-regression theorem. Various interesting effects are found. For example, the scattered intensity spectrum for a J = 0 to J = 1 transition for polarization parallel to the laser polarization is essentially an asymmetric triplet, whereas for a perpendicular polarization due to collisions the spectrum is essentially a doublet (whose frequencies do not correspond with any of those of the triplet). Further, the width of the fluorescent component (whose frequency is close to the unperturbed frequency) actually decreases with increasing laser power.

Cooper, J.↗
DOE OSTI2018

High-accuracy Geant4 simulation and semi-analytical modeling of nuclear resonance fluorescence

Nuclear resonance fluorescence (NRF) is a photonuclear interaction that enables highly isotope-specific measurements in both pure and applied physics scenarios. High-accuracy design and analysis of NRF measurements in complex geometries is aided by Monte Carlo simulations of photon physics and transport, motivating Jordan and Warren (2007) to develop the G4NRF codebase for NRF simulation in Geant4. In this work, we enhance the physics accuracy of the G4NRF code and perform improved benchmarking simulations. The NRF cross section calculation in G4NRF, previously a Gaussian approximation, has been replaced with a full numerical integration for improved accuracy in thick-target scenarios. A high-accuracy semi-analytical model of expected NRF count rates in a typical NRF measurement is then constructed and compared against G4NRF simulations for both simple homogeneous and more complex heterogeneous geometries. Furthermore, agreement between rates predicted by the semi-analytical model and G4NRF simulation is found at a level of ~1% in simple test cases and ~3% in more realistic scenarios, improving upon the ~20% level of the initial benchmarking study and establishing a highly-accurate NRF framework for Geant4.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
NASA NTRS1993

Squeezing in phase-conjugated resonance fluorescence

Emission of resonance fluorescence by an atom near the surface of a four-wave mixing phase conjugator is considered. The dipole radiation field, regarded as a Heisenberg-operator field, is decomposed into plane waves with the aid of Weyl's representation of the Green's function for the wave equation. Each plane-wave component which is incident on the surface of the nonlinear medium, is reflected as its phase-conjugate image. Summation of all reflected plane waves then yields the phase conjugate replica of the incident dipole radiation. This field adds to the radiation which is emitted by the atom into the direction away from the medium. The condition under which squeezing occurs in the emitted resonance fluorescence is investigated.

Arnoldus, Henk F.↗
NASA NTRS1984

Spectrum of squeezing in resonance fluorescence

A spectral analysis of the squeezing in resonance fluorescence is accomplished via a study of a phase sensitive correlation function. In the case of resonance fluorescence from a two-level system, the initial state is a coherent state for the laser mode, a vacuum for the other states of the radiation field, and the atoms in the lower level. Maximum squeezing for resonance excitation is obtained for near resonant frequencies of the fluorescent light. Possible experimental configurations are discussed in order to detect spectral squeezing.

Collett, M. J.↗
DOE OSTI2013

A dark-field microscope for background-free detection of resonance fluorescence from single semiconductor quantum dots operating in a set-and-forget mode

Optically active quantum dots, for instance self-assembled InGaAs quantum dots, are potentially excellent single photon sources. The fidelity of the single photons is much improved using resonant rather than non-resonant excitation. With resonant excitation, the challenge is to distinguish between resonance fluorescence and scattered laser light. We have met this challenge by creating a polarization-based dark-field microscope to measure the resonance fluorescence from a single quantum dot at low temperature. We achieve a suppression of the scattered laser exceeding a factor of 10{sup 7} and background-free detection of resonance fluorescence. The same optical setup operates over the entire quantum dot emission range (920–980 nm) and also in high magnetic fields. The major development is the outstanding long-term stability: once the dark-field point has been established, the microscope operates for days without alignment. The mechanical and optical designs of the microscope are presented, as well as exemplary resonance fluorescence spectroscopy results on individual quantum dots to underline the microscope's excellent performance.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
NASA NTRS1994

Correlated quadratures of resonance fluorescence and the generalized uncertainty relation

Resonance fluorescence from a two-state atom has been predicted to exhibit quadrature squeezing below the Heisenberg uncertainty limit, provided that the optical parameters (Rabi frequency, detuning, laser linewidth, etc.) are chosen carefully. When the correlation between two quadratures of the radiation field does not vanish, however, the Heisenberg limit for quantum fluctuations might be an unrealistic lower bound. A generalized uncertainty relation, due to Schroedinger, takes into account the possible correlation between the quadrature components of the radiation, and it suggests a modified definition of squeezing. We show that the coherence between the two levels of a laser-driven atom is responsible for the correlation between the quadrature components of the emitted fluorescence, and that the Schrodinger uncertainty limit increases monotonically with the coherence. On the other hand, the fluctuations in the quadrature field diminish with an increasing coherence, and can disappear completely when the coherence reaches 1/2, provided that certain phase relations hold.

Arnoldus, Henk F.↗
DOE OSTI2016

Photoelectron generation and capture in the resonance fluorescence of a quantum dot

Time-resolved resonance fluorescence on a single self-assembled quantum dot (QD) is used to analyze the generation and capture of photoinduced free charge carriers. We directly observe the capture of electrons into the QD as an intensity reduction of the exciton transition. The exciton transition is quenched until the captured electron tunnels out of the dot again in the order of milliseconds. Our results demonstrate that even under resonant excitation, excited free electrons are generated and can negatively influence the optical properties of a QD.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Multicolor Three-Dimensional Tracking for Single-Molecule Fluorescence Resonance Energy Transfer Measurements

Single-molecule fluorescence resonance energy transfer (smFRET) remains a widely utilized and powerful tool for quantifying heterogeneous interactions and conformational dynamics of biomolecules. However, traditional smFRET experiments either are limited to short observation times (typically less than 1 ms) in the case of “burst” confocal measurements or require surface immobilization which usually has a temporal resolution limited by the camera framing rate. We developed a smFRET 3D tracking microscope that is capable of observing single particles for extended periods of time with high temporal resolution. The confocal tracking microscope utilizes closed-loop feedback to follow the particle in solution by recentering it within two overlapping tetrahedral detection elements, corresponding to donor and acceptor channels. We demonstrated the microscope’s multicolor tracking capability via random walk simulations and experimental tracking of 200 nm fluorescent beads in water with a range of apparent smFRET efficiency values, 0.45-0.69. We also demonstrated the microscope’s capability to track and quantify double-stranded DNA undergoing intramolecular smFRET in a viscous glycerol solution. In future experiments, the smFRET 3D tracking system will be used to study protein conformational dynamics while diffusing in solution and native biological environments with high temporal resolution.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1980

A laser flash photolysis-resonance fluorescence kinetics study of the reaction Cl/2P/ + CH4 yields CH3 + HCl

The technique of laser flash photolysis-resonance fluorescence is employed to study the kinetics of the reaction Cl(2P) + CH4 yields CH3 + HCl over the temperature range 221-375 K. At temperatures less than or equal to 241 K the apparent bimolecular rate constant is found to be dependent upon the identity of the chemically inert gases in the reaction mixture. For Cl2/CH4/He reaction mixtures (total pressure = 50 torr) different bimolecular rate constants are measured at low and high methane concentrations. For Cl2/CH4/CCl/He and Cl2/CH4/Ar reaction mixtures, the bimolecular rate constant is independent of methane concentration, being approximately equal to the rate constant measured at low methane concentrations for Cl2/CH4/He mixtures. These rate constants are in good agreement with previous results obtained using the discharge flow-resonance fluorescence and competitive chlorination techniques. At 298 K the measured bimolecular rate constant is independent of the identity of the chemically inert gases in the reaction mixture and in good agreement with all previous investigations. The low-temperature results obtained in this investigation and all previous investigations can be rationalized in terms of a model which assumes that the Cl(2P 1/2) state reacts with CH4 much faster than the Cl(2P 3/2) state. Extrapolation of this model to higher temperatures, however, is not straightforward.

Ravishankara, A. R.↗
DOE OSTI2015

Contemporary research with nuclear resonance fluorescence at the S-DALINAC

In the last decades many nuclear resonance fluorescence experiments aiming for low-lying dipole excitations were performed at the Darmstadt High Intensity Photon Setup at S-DALINAC facility. On the electric dipole side, quadrupole-octupole coupled states and the Pygmy Dipole Resonance are of particular interest. On the magnetic dipole side, the so-called scissors mode is in the focus of interest. Furthermore, using the method of resonant self absorption, the decay behavior of J{sup π} = 1{sup −} states was investigated in {sup 140}Ce.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS1980

Velocity measurements by laser resonance fluorescence

The photonburst correlation method was used to detect single atoms in a buffer gas. Real time flow velocity measurements with laser induced resonance fluorescence from single or multiple atoms was demonstrated and this method was investigated as a tool for wind tunnel flow measurement. Investigations show that single atoms and their real time diffusional motion on a buffer gas can be measured by resonance fluorescence. By averaging over many atoms, flow velocities up to 88 m/s were measured in a time of 0.5 sec. It is expected that higher flow speeds can be measured and that the measurement time can be reduced by a factor of 10 or more by careful experimental design. The method is clearly not ready for incorporation in high speed wind tunnels because it is not yet known whether the stray light level will be higher or lower, and it is not known what detection efficiency can be obtained in a wind tunnel situation.

She, C. Y.↗
DOE OSTI2015

Single-molecule-sensitive fluorescence resonance energy transfer in freely-diffusing attoliter droplets

Fluorescence resonance energy transfer (FRET) from individual, dye-labeled RNA molecules confined in freely-diffusing attoliter-volume aqueous droplets is carefully compared to FRET from unconfined RNA in solution. The use of freely-diffusing droplets is a remarkably simple and high-throughput technique that facilitates a substantial increase in signal-to-noise for single-molecular-pair FRET measurements. We show that there can be dramatic differences between FRET in solution and in droplets, which we attribute primarily to an altered pH in the confining environment. We also demonstrate that a sufficient concentration of a non-ionic surfactant mitigates this effect and restores FRET to its neutral-pH solution value. At low surfactant levels, even accounting for pH, we observe differences between the distribution of FRET values in solution and in droplets which remain unexplained. Our results will facilitate the use of nanoemulsion droplets as attoliter volume reactors for use in biophysical and biochemical assays, and also in applications such as protein crystallization or nanoparticle synthesis, where careful attention to the pH of the confined phase is required.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1974

A flash photolysis-resonance fluorescence study of the formation of O(D-1) in the photolysis of water and reaction of O(D-1) with H2, Ar and He

The relative importance of two primary processes in the photolyis of water: (1) H2O + h (nu) yields H + OH, and (2) H2O + h (nu) yields H2 + OD-1 were determined in a direct manner by time resolved detection (via resonance fluorescence) of H and O formed in processes 1 and 2 respectively. The initially formed OD-1 was deactivated to ground state OP-3 prior to detection via resonance fluorescence. The relative quantum yields for processes 1 and 2 are 0.89 and 0.11 for the wavelength interval 105 to 145nm and = to or greater than 0.99, and = to or less than 0.01 for the wavelength interval 145 to 185nm. Rate constants at 300 K for the reactions OD-1 + H2, + Ar, and + He are presented.

Stief, L. J.↗
DOE OSTI2016

Resonance fluorescence of strongly driven two-level system coupled to multiple dissipative reservoirs

We present a theoretical formalism for resonance fluorescence radiating from a two-level system (TLS) driven by any periodic driving and coupled to multiple reservoirs. The formalism is derived analytically based on the combination of Floquet theory and Born–Markov master equation. The formalism allows us to calculate the spectrum when the Floquet states and quasienergies are analytically or numerically solved for simple or complicated driving fields. We can systematically explore the spectral features by implementing the present formalism. To exemplify this theory, we apply the unified formalism to comprehensively study a generic model that a harmonically driven TLS is simultaneously coupled to a radiative reservoir and a dephasing reservoir. We demonstrate that the significant features of the fluorescence spectra, the driving-induced asymmetry and the dephasing-induced asymmetry, can be attributed to the violation of detailed balance condition, and explained in terms of the driving-related transition quantities between Floquet-states and their steady populations. In addition, we find the distinguished features of the fluorescence spectra under the biharmonic and multiharmonic driving fields in contrast with that of the harmonic driving case. In the case of the biharmonic driving, we find that the spectra are significantly different from the result of the RWA under the multiple resonance conditions. By the three concrete applications, we illustrate that the present formalism provides a routine tool for comprehensively exploring the fluorescence spectrum of periodically strongly driven TLSs.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1978

In situ measurement of reactive neutral constituents in the thermosphere by atomic and molecular resonance fluorescence

The Tethered Satellite System in combination with in situ atomic and molecular resonance fluorescence techniques can treat the problem of simultaneously determining the absolute density of atomic and molecular species known to control the photochemical structure of the upper atmosphere. Two familities of reactants which can be treated by these techniques are the nitrogen oxygen family and the hydrogen oxygen family.

Anderson, J. G.↗
NASA NTRS1972

Upper atmospheric probing by resonance fluorescence excited by tunable laser radiation.

Consideration of the application of the measurement of resonance fluorescence radiation excited by tunable laser radiation to the detection of atomic, molecular, and ionic species in the upper atmosphere. The species considered are N2, N2(+), NO, NO(+), O2(+), CO, CO(+), CH, Na, K, and Ca. Calculations of the resonance scattering cross sections, photon returns, and signal-to-noise ratios are given for these species for a range of conditions. Based on a probing altitude of 100 km, the detections of N2, NO, CO, CH, O2, and the trace metals appear feasible with state-of-the-art systems and within the concentration range present in the atmosphere.

Saunders, A. R.↗