Laser frequency stabilization using a molecular beam Final report, 1 Feb. - 31 Dec. 1969
Iodine molecular beam absorption resonance as long-term frequency reference for argon ion laser stabilization
Ezekiel, S.↗
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Single-photon absorption and emission from a natural photosynthetic complex
Photosynthesis is generally assumed to be initiated by a single photon from the Sun, which, as a weak light source, delivers at most a few tens of photons per nanometre squared per second within a chlorophyll absorption band1. Yet much experimental and theoretical work over the past 40 years has explored the events during photosynthesis subsequent to absorption of light from intense, ultrashort laser pulses. Here, we use single photons to excite under ambient conditions the light-harvesting 2 (LH2) complex of the purple bacterium Rhodobacter sphaeroides, comprising B800 and B850 rings that contain 9 and 18 bacteriochlorophyll molecules, respectively. Excitation of the B800 ring leads to electronic energy transfer to the B850 ring in approximately 0.7 ps, followed by rapid B850-to-B850 energy transfer on an approximately 100-fs timescale and light emission at 850–875 nm. Using a heralded single photon source20,21 along with coincidence counting, we establish time correlation functions for B800 excitation and B850 fluorescence emission and demonstrate that both events involve single photons. We also find that the probability distribution of the number of heralds per detected fluorescence photon supports the view that a single photon can upon absorption drive the subsequent energy transfer and fluorescence emission and hence, by extension, the primary charge separation of photosynthesis. An analytical stochastic model and a Monte Carlo numerical model capture the data, further confirming that absorption of single photons is correlated with emission of single photons in a natural light-harvesting complex.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Vibrational response and temperature of shock-compressed Pt: In situ extended x-ray absorption fine structure measurements to 325 GPa
Single pulse (~100 ps duration) extended x-ray absorption fine structure (EXAFS) measurements were obtained in laser shocked Pt to examine atomic vibrational properties and to determine temperatures for shock pressures from 72-325 GPa. Pt x-ray absorption spectra were recorded while a planar shock wave was propagating through the Pt sample. The absorption spectrum corresponding to the shocked Pt was obtained by subtracting the ambient Pt contribution from the measured absorption spectrum. Fits to the shocked state EXAFS data provided Pt lattice parameters consistent with the known Pt Hugoniot and the mean squared relative displacements (MSRDs) for nearest neighbor Pt atoms. Pt temperatures in the shocked state, estimated from the MSRDs using the correlated Debye model and correlated Einstein models, were consistent with both the Hugoniot temperatures calculated by integration along the Hugoniot and with the Hugoniot temperatures from published first-principles calculations. However, the agreement between the Hugoniot temperatures from EXAFS measurements and the calculated Hugoniot temperatures is not as good above 200 GPa, likely due to anharmonic effects. Furthermore, the present results demonstrate that single-pulse synchrotron EXAFS measurements in laser-shocked solids are useful for quantitative temperature determination and for examination of vibrational properties, including anharmonicity, at extreme pressure-temperature conditions.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Remote measurements of ambient air pollutants with a bistatic laser system
The ambient air pollutants ozone, nitric oxide, and ethylene have been monitored in the Pasadena area with a bistatic IR laser apparatus. These pollutants were measured with a differential absorption technique, using selected wavelengths in the 9.5-, 5.2-, and 10.5-micron regions, respectively. The transmitted laser radiation was detected using both direct and heterodyne detection techniques. In the direct detection case, cube corner retroreflectors provided the return, and the heterodyne detection responded to scattered radiation from various rough surfaces, ranging from 400 m to 1.9 km in distance from the apparatus. Significant departures from ambient background concentration levels were noticed in the region near a local freeway during periods of moderate and heavy traffic.
Menzies, R. T.↗
Frequency Comb-Based Remote Methane Observation Network (Final Scientific/Technical Report)
ARPA-E investment in long-range, frequency comb-based methane detection has resulted in the first scalable, cost-effective continuous methane emissions system. At the onset of this ARPA-E MONITOR award, the dual-frequency comb spectrometer was a sprawling, expensive, laboratory-confined device which had only recently been demonstrated capable of measuring atmospheric trace gases over open-paths. Bringing the technology to the point of being able to monitor for and characterize methane emissions at oil and natural gas production facilities seemed an almost impossible task. Over the subsequent months and years, our team transitioned the Nobel-prize-winning frequency-comb-laser spectrometer technology to a field-deployed regional methane leak detection system. The spectrometer enables highly sensitive near-infrared absorption measurements of methane along kilometer-scale laser beam paths. The measurements are coupled with an atmospheric modeling and inversion framework to triangulate the location of emission sources and quantify the emission rates.
03 NATURAL GAS↗
Lateral expansion of a laser-supported detonation wave in a gas.
A model satisfying the conditions in the burnt (ionized) and ambient undisturbed gases is presented for the two-dimensional case of the absorption wave resulting from the interaction of a laser beam with the plasma it generates in the gas through which the beam propagates. The flowfield of the rarefaction wave resulting from the laser-supported detonation is discussed, along with the computed shock and flow deflection angles.
Howe, J. T.↗
Measurement of polycyclic aromatic hydrocarbon (PAHs) in interplanetary dust particles
We report here the first definitive measurements of specific organic molecules (polycyclic aromatic hydrocarbons (PAH's)) in interplanetary dust particles (IDP's). An improved version of the microbeam-two-step laser mass spectrometer was used for the analysis. Two IDP's gave similar mass spectra showing an abundance of PAH's. Control samples, including particles of probable terrestrial origin from the same stratospheric collector, gave either null results or quite different spectra. We conclude that the PAH's are probably indigenous to the IDP's and are not terrestrial contaminants. The instrument used to study the particles is a two-step laser mass spectrometer. Constituent neutral molecules of the sample are first desorbed with a pulsed infrared laser beam focussed to 40 micrometers. In the second step, PAH's in the desorbed plume are preferentially ionized by a pulsed UV laser beam. Resulting ions produced by resonant absorption are extracted into a reflectron time-of-flight mass spectrometer. This instrument has high spatial resolution, high ion transmission, unlimited mass range, and multichannel detection of all ion masses from a single laser shot.
Clemett, S. J.↗
Effect of differential spectral reflectance on DIAL measurements using topographic targets
Differential absorption lidar (DIAL) measurements of atmospheric gases and temperature made using topographic targets to provide the backscattered signal are subject to errors from the differential spectral reflectance of the target materials. The magnitude of this effect is estimated for a number of DIAL measurements reported in the literature. Calculations are presented for several topographic targets. In general the effect on a DIAL measurement increases directly with increasing wavelength and laser line separation, and inversely with differential absorption coefficient and distance to the target. The effect can be minimized by using tunable or isotope lasers to reduce the laser line separation or by using additional reference wavelengths to determine the surface differential spectral reflectance.
Grant, W. B.↗
Differential absorption lidar signal averaging
This paper presents experimental results using an atmospheric backscatter dual CO2 laser DIAL. It is shown that DIAL signals can be averaged to obtain an N exp -1/2 dependence decrease in the standard deviation of the ratio of backscattered returns from two lasers, where N is the number of DIAL signals averaged, and that such a lidar system can make measurements of gas concentrations with a precision of 0.7 percent in absorptance over 75 m in a short measurement time when the signal strength is high. Factors that eventually limit the rate of improvement in the SNR, such as changes in the ratio of the absorption and/or backscatter at the two laser frequencies and background noise, are discussed. In addition, it is noted that DIAL measurements made using hard-target backscatter often show departures from N exp -1/2 dependence improvement in the standard deviation because they are further limited by the combined effects of atmospheric turbulence and speckle (since the relative reproducibility of the speckle pattern on the receiver gives rise to correlations of the lidar signals).
Grant, William B.↗
Laser‐Sintered Silver Metallization for Silicon Heterojunction Photovoltaic Cells
Herein, a novel metallization technique is reported for crystalline silicon heterojunction (SHJ) solar cells in which silver (Ag) fingers are printed on the SHJ substrates by dispensing Ag nanoparticle‐based inks through a needle and then sintered with a continuous‐wave carbon dioxide (CO 2 ) laser. The impact of the Ag ink viscosity on the line quality and the line resistance is investigated on three Ag inks with different viscosities. Increasing ink viscosity yields higher Ag contact heights, larger aspect ratios, and lower line resistance values. The Ag line height increases from less than a micrometer to ≈18.62 ± 3.48 μm with the increasing viscosity. Photoluminescence imaging shows that the low‐resistance Ag metal contacts obtained do not result in any passivation damage of the SHJ substrate. This is because the wavelength of light emitted from the CO 2 laser (i.e., 10.6 μm) leads to optical absorption in the Ag, but this light is effectively transparent to the transparent conductive oxide film, amorphous silicon films, and crystalline silicon substrate. Bulk resistivity values as low as 6.5 μΩ cm are obtained for the laser‐sintered Ag contact and printed using the Ag ink with the highest viscosity in this work.
Mousumi, Jannatul Ferdous↗
Planar laser induced fluorescence mapping of a carbon laser produced plasma
We present measurements of ion velocity distribution profiles obtained by laser induced fluorescence (LIF) on an explosive laser produced plasma. The spatiotemporal evolution of the resulting carbon ion velocity distribution was mapped by scanning through the Doppler-shifted absorption wavelengths using a tunable, diode-pumped laser. The acquisition of these data was facilitated by the high repetition rate capability of the ablation laser (1 Hz), which allowed for the accumulation of thousands of laser shots in short experimental times. By varying the intensity of the LIF beam, we were able to explore the effects of fluorescence power against the laser irradiance in the context of evaluating the saturation vs the non-saturation regime. The small size of the LIF beam led to high spatial resolution of the measurement compared to other ion velocity distribution measurement techniques, while the fast-gate operation mode of the camera detector enabled the measurement of the relevant electron transitions.
Instruments & Instrumentation↗
XeF lidar measurements of density and temperature in the middle atmosphere
In recent years, it has been widely recognized that vertically propagating internal gravity waves in the middle atmosphere play an important role in determining the large scale wind field by their momentum transport and deposition. However, very little is known about them in the upper stratosphere and lower mesosphere because of the lack of adequate techinques to observe small scale motions. A XeF excimer laser was used for the Rayleigh lidar observation. The characteristics of the XeF lidar system are given. The wavelength of the XeF laser is in the region that is ozone absorption free, and the Rayleigh scattering cross section is 5 times larger than in 532 nm. The advantages of using the XeF laser as against the YAG laser have been discussed in detail. The density and temperature profiles between the altitude range of 30 and 70 km measured with this lidar system are illustrated. The accuracy is less than + or - 3% and 10k at 60 km for an observation time of 15 min. The results on the gravity waves by the observation through about one year since Apr. 1985 is presented.
Shibata, T.↗
LASE validation experiment: preliminary processing of relative humidity from LASE derived water vapor in the middle to upper troposphere
Lidar Atmospheric Sensing Experiment (LASE) is the first fully engineered, autonomous airborne DIAL (Differentials Absorption Lidar) system to measure water vapor, aerosols, and clouds throughout the troposphere. This system uses a double-pulsed Ti:sapphire laser, which is pumped by a frequency-doubled flashlamp-pumped Nd: YAG laser, to transmit light in the 815 mn absorption band of water vapor. LASE operates by locking to a strong water vapor line and electronically tuning to any spectral position on the absorption line to choose the suitable absorption cross-section for optimum measurements over a range of concentrations in the atmosphere. During the LASE Validation Experiment, which was conducted over Wallops Island during September, 1995, LASE operated on either the strong water line for measurements in middle to upper troposphere, or on the weak water line for measurements made in the middle to lower troposphere including the boundary layer. Comparisons with water vapor measurements made by airborne dew point and frost point hygrometers, NASA/GSFC (Goddard Space Flight Center) Raman Lidar, and radiosondes showed the LASE water vapor mixing ratio measurements to have an accuracy of better than 6% or 0.01 g/kg, whichever is larger, throughout the troposphere. In addition to measuring water vapor mixing ratio profiles, LASE simultaneously measures aerosol backscattering profiles at the off-line wavelength near 815 nm from which atmospheric scattering ratio (ASR) profiles are calculated. ASR is defined as the ratio of total (aerosol + molecular) atmospheric scattering to molecular scattering. Assuming a region with very low aerosol loading can be identified, such as that typically found just below the tropopause, then the ASR can be determined. The ASR profiles are calculated by normalizing the scattering in the region containing enhanced aerosols to the expected scattering by the "clean" atmosphere at that altitude. Images of the total ASR clearly depict cloud regions, including multiple cloud layers, thin upper level cirrus, etc., throughout the troposphere. New data products that are being derived from the LASE aerosol and water measurements include: 1) aerosol extinction coefficient, 2) aerosol optical thickness, 3) precipitable water vapor, and 4) relative humidity (RH). These products can be compared with airborne in-situ, and ground and satellite remote sensing measurements,. This paper presents a preliminary examination of RH profiles in the middle to upper troposphere that are generated from LASE measured water vapor mixing ratio profiles coupled with rawinsonde profiles of temperature and pressure.
Brackett, Vincent G.↗
X-ray free electron laser studies of electron and phonon dynamics of graphene adsorbed on copper
Here, we report optical pumping and x-ray absorption spectroscopy experiments at the Pohang Accelerator Laboratory free electron laser that probes the electron dynamics of a graphene monolayer adsorbed on copper in the femtosecond regime. By analyzing the results with ab initio theory we infer that the excitation of graphene is dominated by indirect excitation from hot electron-hole pairs created in the copper by the optical laser pulse. However, once the excitation is created in graphene, its decay follows a similar path as in many previous studies of graphene adsorbed on semiconductors, i.e., rapid excitation of strongly coupled optical phonons and eventual thermalization. It is likely that the lifetime of the hot electron-hole pairs in copper governs the lifetime of the electronic excitation of the graphene.
36 MATERIALS SCIENCE↗
Simulations of Attosecond Metallization in Quartz and Diamond Probed with Inner-Shell Transient Absorption Spectroscopy
When dielectrics are hit with intense infrared (IR) laser pulses, transient metalization can occur. The initial attosecond dynamics behind this metallization are not entirely understood. Therefore, simulations are needed to understand this process and to help interpret experimental observations of it, such as with attosecond transient absorption (ATA). In this paper, we present first-principles simulations of ATA based on bulk-mimicking clusters and real-time time-dependent density functional theory (RT-TDDFT), with Koopmans-tuned range-separated hybrid functionals and Gaussian basis sets. Our method gives good agreement with the experiment for the breakdown threshold in silica and diamond. This breakdown voltage corresponds to a Keldysh parameter of approximately one and thus involves a transition to a regime where the dynamics are driven by tunneling. Pumping at an amplitude just below this value causes a mixture of multiphoton and tunneling excitations across the band gap to occur. The computed extreme ultraviolet and X-ray attosecond transient spectra also agree well with the experiment and show a decrease in optical density due to the transient population of the conduction band from the IR field. First-principles approaches such as this are valuable for interpreting the complicated modulations in a spectrum and for guiding future attosecond experiments on solids.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Computer Processing Of Tunable-Diode-Laser Spectra
Tunable-diode-laser spectrometer measuring transmission spectrum of gas operates under control of computer, which also processes measurement data. Measurements in three channels processed into spectra. Computer controls current supplied to tunable diode laser, stepping it through small increments of wavelength while processing spectral measurements at each step. Program includes library of routines for general manipulation and plotting of spectra, least-squares fitting of direct-transmission and harmonic-absorption spectra, and deconvolution for determination of laser linewidth and for removal of instrumental broadening of spectral lines.
May, Randy D.↗
Lidar profiling of thermodynamic properties of the atmosphere
Principles and applications of pulsed laser methods for temperature, pressure, density, and humidity measurements in the altitude range 0-100 km are discussed. The differential absorption lidar (DIAL) method requires that at least one of the transmitted laser pulses be carefully tuned onto an absorption feature of the species, whereas Raman backscatter methods do not require tunability. OH and Na fluorescence require tuning of the excitation, and are the most suitable methods for high altitude where the atomic and molecular reemission is relatively unquenched by collisions.
Wilkerson, T. D.↗
Low Power Consumption Lasers for Miniature Optical Spectrometers for Trace Gas Analysis
The air quality of any manned spacecraft needs to be continuously monitored in order to safeguard the health of the crew. Air quality monitoring grows in importance as mission duration increases. Due to the small size, low power draw, and performance reliability, semiconductor laser-based instruments are viable candidates for this purpose. Achieving a minimum instrument size requires lasers with emission wavelength coinciding with the absorption of the fundamental absorption lines of the target gases, which are mostly in the 3.0-5.0 micron wavelength range. In this paper we report on our progress developing high wall plug efficiency type-I quantum-well GaSb-based diode lasers operating at room temperatures in the spectral region near 3.0-3.5 micron and quantum cascade (QC) lasers in the 4.0-5.0 micron range. These lasers will enable the development of miniature, low-power laser spectrometers for environmental monitoring of the spacecraft.
Distributed Feedback (DFB) Diode Lasers↗