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At least 361 records · Page 20

Reverse Polarizability of Rare Earth Ions (La 3+ , Gd 3+ , Lu 3+ , Y 3+ ) in Tellurite Glasses and Glass Ceramics for Optical Limiting

All-optical modulation using inherent third-order optical nonlinearity of a medium has garnered considerable interest in photonics and optoelectronics. Herein, nonlinear optical (NLO) properties of tellurite glasses and glass ceramics (GCs) containing four different rare earths (RE = La, Gd, Lu, and Y) have been deliberated in near-infrared regions under an ultrafast regime. The La-based glass exhibits ~10 times higher nonlinear refraction (n 2 ) and absorption (α 2 ) than reported NLO materials. The NLO susceptibility [χ (3) ] trend in the studied glasses is La > Gd > Lu > Y, matching with RE 3+ polarizability. Furthermore, Ln 2 Te 6 O 15 nanocrystallite-embedded transparent GCs exhibit a larger NLO coefficient due to the enhanced local field from oxygen vacancies in crystallites. Interestingly, the trend of χ (3) in GCs follows the sequence of Y > Lu > Gd > La, precisely opposite to the glasses. This observation challenges the general polarizability approach of RE 3+ ions, emphasizing that quadratic hyperpolarizability of RE 3+ is pivotal for NLO properties of GCs. Among the studied matrices, Y-containing GCs showed the lowest optical limiting (OL) threshold (5.4 mJ/cm 2 at 800 nm), much lower than those of the reported NLO materials, suggesting its potential as a femtosecond NIR-laser safety material. A combination of large α 2 and n 2 from the studied matrices indicates their advantage for harmonic generation, potentially aiding in the design of ultrafast signal processing devices.

36 MATERIALS SCIENCE↗

Adaptive noise canceling for transient absorption microscopy

Significance: Ultrafast fiber lasers are an attractive alternative to bulk lasers for nonlinear optical microscopy for their compactness and low cost. The high relative intensity noise (RIN) of these lasers poses a challenge for pump-probe measurements such as transient absorption and stimulated Raman scattering, along with modalities that provide label-free contrast from the vibrational and electronic structure of molecules. Aim: Digital adaptive filtering was applied to determine the applicability for canceling laser RIN in a transient absorption microscope with an ultrafast fiber laser source. Approach: Digitized signals from the transmitted probe and reference photodetectors were fed to an adaptive filter in MATLAB, running in a noise canceling configuration. This result was then fed to a software lock-in algorithm to demodulate the pump-probe signal. Images were built up one line scan at a time with a 3.5-kHz resonant scanner, with 100× averaging. The imaging target was Bi4Ge3O12, which exhibits nondegenerate two-photon absorption at the pump/probe wavelengths used (530-nm pump and 490-nm probe). Results: Without adaptive noise cancellation, the lock-in output primarily passes the laser RIN within its detection bandwidth, resulting in images that closely follow the linear transmissivity and lack sensitivity to pump-probe time delay. With adaptive noise cancellation in front of the lock-in, the RIN rejection is enough to restore the z-sectioning and sensitivity to pump-probe delay, as expected for transient absorption. Results were limited primarily by noise from the photodetector and analog-to-digital converter. Conclusions: Digital adaptive noise cancellation, even when limited by electronics noise, can recover pump-probe signals by removal of laser RIN, under conditions where averaging alone fails.

42 ENGINEERING↗

Study of the rotational-level and temperature dependence of the quenching rate of OH fluorescence due to collisions with water molecules

The importance of the OH radical as an intermediate in many combustion reactions and in atmospheric photochemistry has led many researchers to use it as a diagnostic tool in these processes. The amount of data that has been acquired over the years for this radical is quite considerable. However, the quenching rate of OH with water molecules as a function of temperature and the rotational level of the excited state is not very well understood. The motivation of the studies undertaken is to bridge the gap between the low temperature measurements and the high temperature ones reported in the literature. The technique generally employed in these diagnostics is laser-induced fluorescence (LIF), through which rotational state selective excitation of the radical is possible. Furthermore, in a combustion medium, water is produced in abundance so that knowledge of the quenching rate of OH due to water molecules plays a crucial role in interpreting the data. In general, the precursor to an understanding of the collisional quenching rates of OH involves a characterization of the mode in which the radical is produced; the resulting rotational and translational distribution, followed by a measurement of the OH temperature; and ultimately obtaining the rate constants from the pressure dependence of the fluorescence signal. The experimental implementation of these measurements therefore involved, as a first step, the production of the OH radicals in a microwave discharge cell using water vapor as the source, wherein a hydrogen atom is abstracted from H2O. The second step involved the absorption of photons from the frequency-doubled output of a pulsed amplified, single-frequency cw ring dye laser. By tuning the laser to the peak of the transition and observing the fluorescence decay after the laser pulse, the lifetime of the OH in a particular rotational electronic state was determined (tau = 1.4 microseconds for Q(sub 1)(3)). Knowledge of this parameter led to a determination of the quenching rate. By varying the water vapor pressure in the cell and measuring the lifetime as a function of pressure a linear plot of the quenching rate as a function of pressure was obtained. Using this plot, the quenching cross section was deduced. It has therefore been possible to measure the local translational temperature and the quenching cross section with one laser system.

Koker, Edmond B.↗

Wavelength Calibration of the Full-sun Ultraviolet Rocket SpecTrograph: (FURST)

The Sun has a well-known periodicity in sunspot number and magnetic field variation. The underlying cause of this 11-year cycle is not fully understood and has yet to be connected with those processes in other stellar objects. The Full-sun Ultraviolet Rocket SpecTrograph (FURST) is a sounding rocket payload being developed by Montana State University (MSU) alongside the Marshall Space Flight Center (MSFC) solar physics group. Scheduled to launch from White Sands Missile Range (WSMR) in 2022, this instrument is unique in that it will provide the connection between stellar observatories with measurements of our Sun. It will achieve this through extremely high-resolution full-disk spectroscopy in EUV. We aim to obtain a wavelength resolution R > 10,000 in the 115 - 181 nm range, on par with that of the Hubble (HST) Space Telescope Imaging Spectrograph (STIS). The Lyman Alpha line (121 nm) is known to oversaturate most CCD electronics and is of particular challenge for this spectral range. In addition, this resolution goal will allow us to study the 3 km/s motion (a Doppler-shift of about 0.01 Angstroms) of the relatively low-temperature plasma in the chromosphere and lower corona. This paper will present the results of our simulation of the diagnostic lamp signal to be used in this wavelength calibration. To test the viability of this precise of a device, we are building a collimator capable of calibrating the FURST instrument under these strict radiometric requirements. By way of a diagnostic lamp simulation, we will account for photon noise, CCD electronic readout noise, and statistical error. These will lead to the development of our pre- and post-launch calibration plan. Future work includes absolute radiometric and wavelength calibration with this new collimator. In addition, the ability of FURST to measure extremely small Doppler-shifts will provide capabilities for planetary atmospheric scientists. This impact is coupled with the diverse international partnership created by the closely-knit Sounding Rocket teams across the globe. These Sounding Rockets have an even broader impact, as they encourage future satellite missions under the prospect of long-term observations.

FURST↗

Quantum vacuum processes in the extremely intense light of relativistic plasma mirror sources

Abstract The advent of petawatt-class laser systems allows generating electromagnetic fields of unprecedented strength in a controlled environment, driving increasingly more efforts to probe yet unobserved processes through their interaction with the quantum vacuum. Still, the lowest intensity scale governing these effects lies orders of magnitude beyond foreseen capabilities, so that such endeavor is expected to remain extremely challenging. In recent years, however, plasma mirrors have emerged as a promising bridge across this gap, by enabling the conversion of intense infrared laser pulses into coherently focused Doppler harmonic beams lying in the X-UV range. In this work, we present predictions on the quantum vacuum signatures produced when such beams are focused to intensities between 10 24 and 10 28 W cm −2 , specifically photon–photon scattering and electron–positron pair creation. These signatures are computed via the stimulated vacuum formalism, combined with a model of perfectly focused beam built from PIC-generated harmonics spectra, and implemented on state-of-the-art massively parallel numerical tools. In view of identifying experimentally favorable configurations, we also consider the coupling of the focused harmonic beam with an auxiliary optical beam, and provide comparison with other established schemes. Our results show that a single coherently focused harmonic beam can produce as much scattered photons as two infrared pulses in head-on collision, and confirm that the coupling of the harmonic beam to an auxiliary beam gives rise to significant levels of inelastic scattering, and hence holds the potential to strongly improve the attainable signal to noise ratios in experiments.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Astronomical Spectroscopy with Skipper CCDs: First Results from a Skipper CCD Focal Plane Prototype at SIFS

We present the first on-sky results from an ultra-low-readout-noise Skipper CCD focal plane prototype for the SOAR Integral Field Spectrograph (SIFS). The Skipper CCD focal plane consists of four 6k x 1k, 15 $\mu$m pixel, fully-depleted, p-channel devices that have been thinned to ~250 $\mu$m, backside processed, and treated with an anti-reflective coating. These Skipper CCDs were configured for astronomical spectroscopy, i.e., single-sample readout noise < 4.3 e- rms/pixel, the ability to achieve multi-sample readout noise $\ll$ 1 e- rms/pixel, full-well capacities ~40,000-65,000 e-, low dark current and charge transfer inefficiency (~2 x 10$^{-4}$ e-/pixel/s and 3.44 x 10$^{-7}$, respectively), and an absolute quantum efficiency of $\gtrsim$ 80% between 450 nm and 980 nm ($\gtrsim$ 90% between 600 nm and 900 nm). We optimized the readout sequence timing to achieve sub-electron noise (~0.5 e- rms/pixel) in a region of 2k x 4k pixels and photon-counting noise (~0.22 e- rms/pixel) in a region of 220 x 4k pixels, each with a readout time of $\lesssim$ 17 min. We observed two quasars (HB89 1159+123 and QSO J1621-0042) at redshift z ~ 3.5, two high-redshift galaxy clusters (CL J1001+0220 and SPT-CL J2040-4451), an emission line galaxy at z = 0.3239, a candidate member star of the Bo\"{o}tes II ultra-faint dwarf galaxy, and five CALSPEC spectrophotometric standard stars (HD074000, HD60753, HD106252, HD101452, HD200654). We present charge-quantized, photon-counting observations of the quasar HB89 1159+123 and show the detector sensitivity increase for faint spectral features. We demonstrate signal-to-noise performance improvements for SIFS observations in the low-background, readout-noise-dominated regime. We outline scientific studies that will leverage the SIFS-Skipper CCD data and new detector architectures that utilize the Skipper floating gate amplifier with faster readout times.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Prospects of Detecting Nonthermal Protons in Solar Flares via Lyman Line Spectroscopy: Revisiting the Orrall-Zirker Effect

Solar flares are efficient particle accelerators, with a substantial fraction of the energy released manifesting as nonthermal particles. While the role that nonthermal electrons play in transporting flare energy is well studied, the properties and importance of nonthermal protons are rather less well understood. This is in large part due to the paucity of diagnostics, particularly at the lower-energy (deka-keV) range of nonthermal proton distributions in flares. One means to identify the presence of deka-keV protons is by an effect originally described by Orrall & Zirker. In the Orrall–Zirker effect, nonthermal protons interact with ambient neutral hydrogen, and via charge exchange produce a population of energetic neutral atoms (ENAs) in the chromosphere. These ENAs subsequently produce an extremely redshifted photon in the red wings of hydrogen spectral lines. We revisit predictions of the strength of this effect using modern interaction cross sections, and numerical models capable of self-consistently simulating the flaring nonequilibrium ionization stratification, and the nonthermal proton distribution (and, crucially, their feedback on each other). We synthesize both the thermal and nonthermal emission from Ly α and Ly β, the most promising lines that may exhibit a detectable signal. These new predictions are weaker and more transient than prior estimates, but the effects should be detectable in fortuitous circumstances. We degrade the Ly β emission to the resolution of the Spectral Imaging of the Coronal Environment (SPICE) instrument on board Solar Orbiter, demonstrating that though likely difficult, it should be possible to detect the presence of nonthermal protons in flares observed by SPICE.

Solar flares↗

The PCM is Dead! Long Live O-PCM!

The ability to reconfigure the optical behavior of a device enables free-space applications ranging from imaging to sensing and signal control. Such optical devices can be compacted via meta-surfaces, patterned structures with feature sizes below the incident wavelength. Leveraging geometry in addition to material properties and CMOS fabrication techniques has allowed meta-surfaces for lenses, holograms, beam steerers and more. To incorporate multiple optical functions into one device, various methods of device control have been implemented, such as stretching of flexible substrates, tuning the refractive index of the comprising meta-atoms via the electro-optic or the thermo-optic effects, phase transition materials such as VO2 and more. Chalcogenide glasses used as optical phase change materials, such as Ge¬2Sb2Te5 (GST), have gained increased traction in the optics community for potential use in the near infrared (NIR) and mid infrared (MIR) bands, including the telecom bands. Various chalcogenides such as Sb2Se3, Sb2S3, Ge2Sb¬2Se5 and Ge2Sb2Se4Te (GSST) have been investigated due to their broad NIR or MIR transparency window and large changes in refractive index. In their amorphous phase, these materials usually display a lower refractive index and low absorption when compared to their crystalline state which display a higher refractive index and typically larger extinction coefficients. The amorphous-crystalline reversible switching can be done via fast melt-quenching thermal processes triggered by laser or electrical impulses, relying on a substrate as a heat sink. The potential of PCMs in photonic devices can be limited by intrinsic material limitations as well as by device fabrication issues. To explore the cyclability of GSST, a PCM with large refractive index contrast and on-chip electrothermal switching on a silicon-on-insulator platform has been done to analyze potential failure mechanisms from both a material and device perspective. A brief outline of the instrumentation and phase change contrast analysis is provided. Dewetting of the PCM, delamination of and damage in the PECVD SiNx protective layer, elemental migration in the PCM and optical contrast decay have been observed in cycled GSST devices. Guidelines for device performance improvement are proposed, and an improved design with larger endurance is shown in progress.

reconfigurable photonics↗

Joint Acceptance Attenuation Factor of Integrated Pressure with Unsteady Pressure-Sensitive Paint Measurements

The Unsteady Pressure-Sensitive Paint (uPSP) is widely used to measure the surface pressure of the scaled model in the wind tunnel tests. Compared to the conventional pressure transducers, uPSP has the advantage of high spatial resolution. With multiple high-speed cameras, the uPSP data collected with the camera pixels are mapped to the surface grid of the scaled model and converted to pressure. The shot noise, which is associated with the quantum processes both in the generation of the photons by the luminescent uPSP and in the conversion of the photons into electrons within the camera, is the dominant component of the noise in the uPSP measurement. The integrated pressure is usually computed as an area-weighted average of the uPSP measured pressures on the grid nodes of a user-defined patch. The effect of the shot noise is reduced in the integrated pressure; however, the measurement of the aerodynamic pressure is also attenuated. This paper discusses the Joint Acceptance Attenuation Factor (JAAF) of the integrated pressure with uPSP measurements. The JAAF is defined as the ratio of the auto or cross Power Spectral Density (PSD) of the integrated aerodynamic pressure on the patch to the average auto PSD of the aerodynamic pressure on the grid nodes of the patch. Under the assumption that the cross spectrum of the aerodynamic pressure can be described with the Corcos model, the closed-form formula of the JAAF is derived for the integrated pressure on rectangular patches via the summation of uPSP measurements on discrete grid nodes. The closed-form formula is verified via the integration of the pressure field of Corcos model over continuous areas. The properties of the JAAF with different parameters are presented and the applications in the comparison of the spectrum of the pressure transducers and uPSP measurements, which were collected in the NASA Space Launch System (SLS) tests with the 11-by-11-foot transonic wind tunnel at NASA Ames Research Center in December 2017 and September 2019 respectively, are also discussed. The work described in this paper is a part of NASA’s development of a new state-of-the-art uPSP capability in production wind tunnels. Funding was provided by the NASA Aerosciences Evaluation and Test Capabilities(AETC) Portfolio Office.

Unsteady Pressure-Sensitive Paint↗

Astronomical Spectroscopy with Skipper CCDs: First Results from a Skipper CCD Focal Plane Prototype at SIFS

We present the first on-sky results from an ultra-low-readout-noise Skipper CCD focal plane prototype for the SOAR Integral Field Spectrograph (SIFS). The Skipper CCD focal plane consists of four 6k $\times$ 1k, 15 $\mu$m pixel, fully-depleted, $p$-channel devices that have been thinned to $\sim$250 $\mu$m, backside processed, and treated with an anti-reflective coating. These Skipper CCDs were configured for astronomical spectroscopy, i.e., a single-sample readout noise $< 4.3$\,e$^-$\,rms/pixel, the ability to achieve multi-sample readout noise $\ll 1\,$e$^-$\,rms/pix, full-well capacities $\sim$40,000--65,000 e$^-$, low dark current and charge transfer inefficiency ($\sim 2$ $\times$ $10^{-4}$ e$^-$/pixel/s and 3.44 $\times$ $10^{-7}$, respectively), and an absolute quantum efficiency of $\gtrsim 80\%$ between 450\,nm and 980\,nm ($\gtrsim 90\%$ between 600\,nm and 900\,nm). We optimize the readout sequence timing to achieve sub-electron noise ($\sim 0.5$\,e$^-$\,rms/pix) and photon-counting ($\sim 0.22$\,e$^-$\,rms/pix) readout noise over an area of 2k $\times$ 4k and 110 $\times$ 4k pixels, respectively in a readout time of $\lesssim 17$min. We observed two Lyman-$\alpha$ emitting quasars (HB89\,1159$+$123 and QSO\,J1621$–$0042) at redshift $z \sim 3.5$, two moderate redshift galaxy clusters (CL\,J1001$+$0220 and SPT-CL\,J2040$-$4451), an emission line galaxy at $z = 0.3239$, a candidate member star of the Bo\"{o}tes~II ultra-faint dwarf galaxy, and five CALSPEC spectrophotometric standard stars (HD074000, HD60753, HD106252, HD101452, HD200654). We present charge-quantized, photon-counting observation of the quasar HB89\,1159$+$123 and show the detector sensitivity increase for faint spectral features. We demonstrate signal-to-noise performance improvement for SIFS for observations in the low-background, readout-noise-dominated regime. We outline preliminary scientific studies that will leverage the SIFS-Skipper CCD data to derive new cosmological measurements in the context of dark matter and galaxy evolution.

79 ASTRONOMY AND ASTROPHYSICS↗

Development of Low-Noise High Value Chromium Silicide Resistors for Cryogenic Detector Applications

Extremely high sensitivity detectors, such as silicon bolometers are required in many NASA missions for detection of photons from the x-ray to the far infrared regions. Typically, these detectors are cooled to well below the liquid helium (LHe) temperature (4.2 K) to achieve the maximum detection performance. As photoconductors, they are generally operated with a load resistor and a pre-set bias voltage, which is then coupled to the input gate of a source-follower Field Effect Transistor (FET) circuit. It is imperative that the detector system signal to noise performance be limited by the noise of the detector and not by the noise of the external components. The load resistor value is selected to optimize the detector performance. These two criteria tend to be contradictory in that these detectors require load resistors in the hundreds of megaohms, which leads to a higher Johnson noise. Additionally, the physical size of the resistor must be small for device integration as required by such missions as the NASA High Resolution Airborne Wide-Band Camera (HAWC) instrument and the Submillimeter High Angular Resolution Camera (SHARC) for the Caltech Submillimeter Observatory (CSO). We have designed, fabricated and characterized thin film resistors using a CrSi/TiW/Al metal system on optical quality quartz substrates. The resistor values range from 100 megaohms to over 650 megaohms and are Johnson noise limited at LHe temperatures. The resistor film is sputtered with a sheet resistance ranging from 300 ohms to 1600 ohms and the processing sequence developed for these devices allows for chemically fine tuning the sheet resistance in-situ. The wafer fabrication process was of sufficiently high yield (>80%) providing clusters of good resistors for integrated multiple detector channels, a very important feature in the assembly of these two instruments.

Jhabvala, Murzy↗

Phonon-enhanced nonlinearities in hexagonal boron nitride

Abstract Polar crystals can be driven into collective oscillations by optical fields tuned to precise resonance frequencies. As the amplitude of the excited phonon modes increases, novel processes scaling non-linearly with the applied fields begin to contribute to the dynamics of the atomic system. Here we show two such optical nonlinearities that are induced and enhanced by the strong phonon resonance in the van der Waals crystal hexagonal boron nitride (hBN). We predict and observe large sub-picosecond duration signals due to four-wave mixing (FWM) during resonant excitation. The resulting FWM signal allows for time-resolved observation of the crystal motion. In addition, we observe enhancements of third-harmonic generation with resonant pumping at the hBN transverse optical phonon. Phonon-induced nonlinear enhancements are also predicted to yield large increases in high-harmonic efficiencies beyond the third.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Wavelength conversion for single-photon polarization qubits through continuous-variable quantum teleportation

A quantum internet connects remote quantum processors that need to interact and exchange quantum signals over a long distance through photonic channels. However, these quantum nodes operate at the wavelength ranges unsuitable for long-distance transmission. Therefore, quantum wavelength conversion to telecom bands is crucial for long-distance quantum networks based on optical fiber. Here, we propose wavelength conversion devices for single-photon polarization qubits using continuous-variable quantum teleportation that can efficiently convert qubits between near-infrared (780–795 nm suitable for interacting with atomic quantum nodes) and telecom wavelength (1300–1500 nm suitable for long-distance transmission). The teleportation uses entangled photon fields (i.e., nondegenerate two-mode squeezed state) that can be generated by four-wave mixing in a rubidium atomic gas using a diamond configuration of atomic transitions. The entangled fields can be emitted in two orthogonal polarizations with locked relative phase, making them especially suitable for interfacing with single- photon polarization qubits. Furthermore, our work may pave the way for the realization of long-distance quantum networks.

74 ATOMIC AND MOLECULAR PHYSICS↗

A fast and large bandwidth superconducting variable coupler

Variable microwave-frequency couplers are highly useful components in classical communication systems and likely will play an important role in quantum communication applications. Conventional semiconductor-based microwave couplers have been used with superconducting quantum circuits, enabling, for example, the in situ measurements of multiple devices via a common readout chain. However, the semiconducting elements are lossy and furthermore dissipate energy when switched, making them unsuitable for cryogenic applications requiring rapid, repeated switching. Superconducting Josephson junction-based couplers can be designed for dissipation-free operation with fast switching and are easily integrated with superconducting quantum circuits. These enable on-chip, quantum-coherent routing of microwave photons, providing an appealing alternative to semiconductor switches. Here, we present and characterize a chip-based broadband microwave variable coupler, tunable over 4-8GHz with over 1.5GHz instantaneous bandwidth, based on the superconducting quantum interference device with two parallel Josephson junctions. The coupler is dissipation-free and features large on-off ratios in excess of 40dB, and the coupling can be changed in about 10ns. The simple design presented here can be readily integrated with superconducting qubit circuits and can be easily generalized to realize a four- or more port device.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Design and Performance of a Miniature Lidar Wind Profiler (MLWP)

The directional velocity of the wind is one of the most critical components for understanding meteorological and other dynamic atmospheric processes. Altitude-resolved wind velocity measurements, also known as wind profiles or soundings, are especially necessary for providing data for meteorological forecasting and overall global circulation models (GCM's). Wind profiler data are also critical in identifying possible dangerous weather conditions for aviation. Furthermore, a system has yet to be developed for wind profiling from the surface of Mars which could also meet the stringent requirements on size, weight, and power of such a mission. Obviously, a novel wind profiling approach based on small and efficient technology is required to meet these needs. A lidar system based on small and highly efficient semiconductor lasers is now feasible due to recent developments in the laser and detector technologies. The recent development of high detection efficiency (50%), silicon-based photon-counting detectors when combined with high laser pulse repetition rates and long receiver integration times has allowed these transmitter energies to be reduced to the order of microjoules per pulse. Aerosol lidar systems using this technique have been demonstrated for both Q-switched, diode-pumped solid-state laser transmitters (lambda = 523 nm) and semiconductor diode lasers (lambda = 830 nm); however, a wind profiling lidar based on this technique has yet to be developed. We will present an investigation of a semiconductor-laser-based lidar system which uses the "edge-filter" direct detection technique to infer Doppler frequency shifts of signals backscattered from aerosols in the planetary boundary layer (PBL). Our investigation will incorporate a novel semiconductor laser design which mitigates the deleterious effects of frequency chirp in pulsed diode lasers, a problem which has limited their use in such systems in the past. Our miniature lidar could be used on a future Mars lander and perhaps find its own niche in terrestrial applications due to its potential low cost an small size.

Cornwell, Donald M., Jr.↗

Spatial Mapping of Valence Excited-State Landscapes Using Time-Resolved Shake-Down Spectroscopy

Time-resolved X-ray photoelectron spectroscopy (XPS) is used to track the photodissociation dynamics of 2-iodothiophene following 262 nm excitation. The transient XPS features include both direct ionization of the initially populated excited states and pronounced satellite peaks arising from shake-down processes. While the direct ionization signals exhibit only minimal energy shifts during C−I bond cleavage, the shake-down transitions undergo a substantial, 5 eV, shift over the reaction coordinate. By correlating these shifts with simulated C−I bond lengths, a direct structural mapping is established that reveals the exceptional sensitivity of shake-down channels to molecular geometry. These results demonstrate that shake-down transitions provide a new and powerful probe of ultrafast structural dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Effect of Electronic Shot Noise on Dynamic Measurements using Optical Techniques: Examples from Rayleigh Scattering and Unsteady PSP

Electronic shot noise is an unavoidable reality in all optical techniques that depend on measuring light intensity. For steady-state, time-averaged measurements the impact of shot noise can be easily reduced by increasing the exposure time, or by averaging over multiple-exposures. That is not the case for unsteady measurements, where time histories of light intensity variations need to be created either by high-speed photography (unsteady PSP) or via photoelectron counting (spectrally resolved Rayleigh scattering) over short time durations using a photo-multiplier tube (PMT) and photon counting electronics. Electronic shot noise introduces a fixed amount of random error, which can overwhelm the light intensity variation caused by turbulent fluctuations. Spectrum computed from such time series shows a fixed noise floor that is independent of the number of data points in the time series. For a fixed optical system, where the collected power of the luminescent light (uPSP), or the scattered light (Rayleigh) is fixed, one needs to resort to special techniques to obtain enough signal-to noise ratio (SNR). For the uPSP application it is shown that averaging of the adjacent pixels improves SNR; although this may lead to a sacrifice of spatial resolution. A second means is to increase the exposure time, which leads to a lowering of the frequency range. For the Rayleigh application, improvements of SNR can be achieved via two different cross-correlation based approaches. The first involves measuring the light intensity using two PMTs using short, contiguous gates; thereby, creating two time-series of data. The second one involves collecting one long time-series of data using one set of measurement device, followed by an odd-even splitting into two time series. When the two time-series are cross-correlated, and a power spectrum is calculated, a significant reduction in the shot noise floor can be achieved. Examples from measurements of density and velocity fluctuations spectra from two different Rayleigh setup are presented to demonstrate the process.

uPSP↗

Continuum-electron interferometry for enhancement of photoelectron circular dichroism and measurement of bound, free, and mixed contributions to chiral response

We develop photoelectron interferometry based on laser-assisted extreme ultraviolet ionization for flexible and robust control of photoelectron circular dichroism in randomly oriented chiral molecules. A comb of XUV photons ionizes a sample of chiral molecules in the presence of a time-delayed infrared or visible laser pulse promoting interferences between components of the XUV-ionized photoelectron wave packet. In striking contrast to multicolor phase control schemes relying on pulse shaping techniques, the magnitude of the resulting chiral signal is here controlled by the time delay between the XUV and laser pulses. Furthermore, we show that the relative polarization configurations of the XUV and IR fields allow for disentangling the contributions of bound and continuum states to the chiral response. Our proposal provides a simple, robust, and versatile tool for the control of photoelectron circular dichroism and experimentally feasible protocol for probing the individual contributions of bound and continuum states to the photoelectron circular dichroism in a time-resolved manner.

atomic and molecular processes in external fields↗