Optimized Source of Non-Gaussian States for Use in Hybrid Discrete/Continuous Variable Quantum Information Processing Schemes
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71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
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Interplay between Ultrafast Electronic and Librational Dynamics in Liquid Nitrobenzene Probed with Two-Color Four-Wave Mixing
Here, we present an experimental and theoretical study of the interplay between ultrafast electron dynamics and librational dynamics in liquid nitrobenzene. A femtosecond ultraviolet pulse and two femtosecond near-infrared pulses interact with nitrobenzene molecules, generating a four-wave mixing nonlinear signal measured in the Optical Kerr Effect geometry. The signal is measured to be nonzero only at negative time delays, corresponding to the near-infrared pulses arriving before the ultraviolet pulse. We perform time-dependent Quantum Master Equation calculations with classical libration to simulate the experiment. The simulations support the conclusion that the near-infrared pulses launch librational motion while creating electronic coherences resulting in a libration-modulated electronic nonlinear response. The analysis of the phase-matched four-wave mixing signals suggests a nonparametric process leaving the molecules in an excited electronic state, providing new insight into ultrafast nonlinear optical interactions in liquids and advancing toward probing ultrafast electronic coherences in complex molecular liquids.
Shivaram, Niranjan [Lawrence Berkeley National Lab↗
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↗
V‐Groove Si Nanopatterning for the Direct Epitaxy of Orientation‐Patterned III–V Nonlinear Optical Crystals
Orientation‐patterned (OP) III–V semiconductors—used as quasi‐phase‐matched crystals for nonlinear optics applications—are typically epitaxially grown on expensive III–V substrates using a complex process requiring three separate epitaxy steps. In this work, a method is demonstrated for growing orientation‐patterned III–V crystals on Si substrates through V‐groove nanopatterning and a single epitaxial growth. V‐groove Si allows for suppression of random antiphase domain formation that is typical of III–V growth on (001)‐oriented Si through the use of (111)‐faceted trenches patterned on (001)‐oriented Si substrates. By alternating the directions of the V‐groove trenches between [110] and [10], antiphase boundaries can be selectively induced at the boundaries between the two directions of trenches due to the difference in symmetry between the III–V material and Si. This approach allows for a greatly simplified process for growing OP‐III‐Vs and more broadly is a new, robust approach for precisely patterning antiphase boundaries of arbitrary shape and length scales down to 50 nm.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
Random quasi-phase-matching for pulse characterization from the near to the long wavelength infrared
Experiments requiring ultrafast laser pulses require a full characterization of the electric field to glean meaning from the experimental data. Such characterization typically requires a separate parametric optical process. As the central wavelength range of new sources continues to increase so too does the need for nonlinear crystals suited for characterizing these wavelengths. Here we report on the use of poly-crystalline zinc selenide as a universal nonlinear crystal in the frequency resolved optical gating characterization technique from the near to long-wavelength infrared. Due to its property of random quasi-phase-matching it’s capable of phase matching second-harmonic and sum-frequency generation of ultra-broadband pulses in the near and long wavelength infrared, while being crystal orientation independent. With the majority of ultra-fast laser sources being in this span of wavelengths, this work demonstrates a greatly simplified approach towards ultra-fast pulse characterization spanning from the near to the long-wavelength infrared. To our knowledge there is no single optical technique capable of such flexible capabilities.
Davis, Brandin (ORCID:0000000166964548)↗
Control of Nonlinear Compton Scattering in a Squeezed Vacuum
Electromagnetic radiation by accelerated charges is a fundamental process in physics. Here, we introduce a quantum-optical framework for controlling the emission of radiation of an electron in an intense laser field via squeezed vacuum states. By engineering the quantum fluctuations of the emission modes, we demonstrate that the probability of nonlinear Compton scattering can be significantly enhanced or suppressed through tunable squeezing amplitude and angle. We show numerically that our predictions are experimentally accessible with current squeezing technologies, establishing a new paradigm for quantum control in high-intensity light-matter interactions.
Light-matter interaction↗
Slot clock recovery in optical PPM communication systems with avalanche photodiode photodetectors
Slot timing recovery in a direct-detection optical PPM communication system can be achieved by processing the photodetector output waveform with a nonlinear device whose output forms the input to a phase-locked loop. The choice of a simple transition detector as the nonlinearity is shown to give satisfactory synchronization performance. The rms phase error of the recovered slot clock and the effect of slot timing jitter on the bit error probability were directly measured. The experimental system consisted of an AlGaAs laser diode (wavelength = 834 nm) and a silicon avalanche photodiode photodetector. The system used Q = 4 PPM signaling and operated at a source data rate of 25 Mbits/s. The mathematical model developed to compute the rms phase error of the recovered clock is shown to be in good agreement with results of actual measurements of phase errors. The use of the recovered slot clock in the receiver resulted in no significant degradation in receiver sensitivity compared to a system with perfect slot timing. The system achieved a bit error probability of 10 to the -6th at a received optical signal energy of 55 detected photons per information bit.
Davidson, Frederic M.↗
Optical communication with semiconductor laser diodes
Slot timing recovery in a direct detection optical PPM communication system can be achieved by processing the photodetector waveform with a nonlinear device whose output forms the input to a phase lock group. The choice of a simple transition detector as the nonlinearity is shown to give satisfactory synchronization performance. The rms phase error of the recovered slot clock and the effect of slot timing jitter on the bit error probability were directly measured. The experimental system consisted of an AlGaAs laser diode (lambda = 834 nm) and a silicon avalanche photodiode (APD) photodetector and used Q=4 PPM signaling operated at a source data rate of 25 megabits/second. The mathematical model developed to characterize system performance is shown to be in good agreement with actual performance measurements. The use of the recovered slot clock in the receiver resulted in no degradation in receiver sensitivity compared to a system with perfect slot timing. The system achieved a bit error probability of 10 to the minus 6 power at received signal energies corresponding to an average of less than 60 detected photons per information bit.
Davidson, F.↗
Frequency-domain computing using nonlinear acoustic-wave device on lithium niobate
Abstract Multiply-accumulation are crucial computing operations in signal processing, numerical simulations, and machine learning. In recent years, optical analog approaches have demonstrated higher computing performance and better power efficiency than their digital counterparts. However, analog computing chips usually need large areas and complex structures for parallel computing, as a single device element only executes one computing operation at a single time. Here, we demonstrate frequency-domain computing using the nonlinear acoustic-wave devices on lithium niobate, featuring a normalized external second-harmonic generation conversion efficiency of ~ 5.7 × 10-4 W-1. The second-order sum-frequency nonlinear process of lithium niobate enables multiplication of inputs encoded in the frequency domain. Compared to the analog schemes, our device features a notably simpler design, and nanofabrication requires only one lift-off. Using a single acoustic-wave device within an area of 0.03 mm2, we can simultaneously conduct over 130,000 multiply-accumulation operations. Our acoustic-wave device shows applications in real and complex vector convolutions and image processing. This demonstration sets the stage for experimental realizations into frequency-domain integrated nonlinear acoustic computing systems, potentially shaping future developments in acoustic neural networks and quantum computing.
chai, mingzhao (ORCID:0009000466226341)↗
Inverting Image Data For Optical Testing And Alignment
Data from images produced by slightly incorrectly figured concave primary mirror in telescope processed into estimate of spherical aberration of mirror, by use of algorithm finding nonlinear least-squares best fit between actual images and synthetic images produced by multiparameter mathematical model of telescope optical system. Estimated spherical aberration, in turn, converted into estimate of deviation of reflector surface from nominal precise shape. Algorithm devised as part of effort to determine error in surface figure of primary mirror of Hubble space telescope, so corrective lens designed. Modified versions of algorithm also used to find optical errors in other components of telescope or of other optical systems, for purposes of testing, alignment, and/or correction.
Shao, Michael↗
Nonlinear Loss Engineering in Near‐Zero‐Index Bulk Materials
Transparent conducting oxides (TCOs) show unprecedented optical nonlinearities in the near infrared wavelength range, where the real part of their linear refractive index approaches zero. More specifically, the Kerr nonlinearities of these materials have sparked widespread attention due to their magnitude and speed. However, due to the absorptive nature of these nonlinear processes, it is of fundamental interest to further investigate the imaginary component of the nonlinear index. The present work studies the nonlinear optical absorption properties of aluminium‐doped zinc oxide (AZO) thin films in their near‐zero‐index (NZI) spectral window. It is found that the imaginary part of the refractive index is reduced under optical excitation such that the field penetration depth more than doubles. An optically induced shift of the NZI bandwidth of ≈120 nm for a pump intensity of 1.3 TW cm −2 is also demonstrated. Looking into the optically induced spectral redistribution of the probe signal, local net gain is recorded, which is ascribed to a nonlinear adiabatic energy transfer. The present study adds key information about the fundamental interplay between real and imaginary nonlinear indices in NZI media, while advancing parametric amplification as viable direction for loss compensation.
36 MATERIALS SCIENCE↗
The Effects of Ground and Space Processing on the Properties of Organic, Polymeric, and Colloidal Materials
In recent years, a great deal of interest has been directed toward the use of organic materials in the development of high-efficiency optoelectronic and phototonic devices. There is a myriad of possibilities among organic materials which allow flexibility in the design of unique structures with a variety of functional groups. The use of nonlinear optical (NLO) organic materials as thin film wave-guides allows full exploitation of their desirable qualifies by permitting long interaction lengths and large susceptibilities allowing modest power input. There are several methods in use to prepare thin films such as Langmuir-Blodgett (LB) and self-assembly techniques, vapor deposition, growth from sheared solution or melt, and melt growth between glass plates. Organic-based materials have many features that make them desirable for use in optical devices, such as high second-and third-order nonlinearity, flexibility of molecular design, and damage resistance to optical radiation. However, their use in devices has been hindered by processing difficulties for crystals and thin films. We discuss the potential role of microgravity processing of a few organic and polymeric materials. It is of interest to note how materials with second-and third-order NLO behavior may be improved in a diffusion-limited environment and ways in which convection may be detrimental to these materials. We focus our discussion on third-order materials for all-optical switching, and second-order materials for frequency conversion and electrooptics. The goal of minimizing optical loss obviously depends on processing methods. For solution-based processes, such as solution crystal growth and solution photopolymerization, it is well known that thermal and solutal density gradients can initiate buoyancy-driven convection. Resultant fluid flows can affect transport of material to and from growth interfaces and become manifest in the morphology and homogeneity of the growing film or crystal. Likewise, buoyancy-driven convection can hinder production of defect-free, high-quality crystals or films during crystal and film growth by vapor deposition.
Frazier, Donald O.↗
Role of dipole-forbidden autoionizing resonances in nonresonant one-color two-photon single ionization of N 2
We present an experimental and theoretical energy- and angle-resolved study on the photoionization dynamics of non-resonant one-color two-photon single valence ionization of neutral N$_2$ molecules. Using 9.3 eV photons produced via high harmonic generation and a 3-D momentum imaging spectrometer, we detect the photoelectrons and ions produced from one-color two-photon ionization in coincidence. Photoionization of N$_2$ populates the X $^2\Sigma^+_g$, A $^2\Pi_u$, and B $^2\Sigma^+_u$ ionic states of N$_2^+$, where the photoelectron angular distributions associated with the X $^2\Sigma^+_g$ and A $^2\Pi_u$ states both vary with changes in photoelectron kinetic energy of only a few hundred meV. We attribute the rapid evolution in the photoelectron angular distributions to the excitation and decay of dipole-forbidden autoionizing resonances that belong to series of different symmetries, all of which are members of the Hopfield series, and compete with the direct two-photon single ionization.
74 ATOMIC AND MOLECULAR PHYSICS↗
Stationary and non-stationary nonlinear optical spectroscopy on surface polaritons
A phenomenological theory is given for non-stationary electromagnetic surface waves propagating along the boundary plane between two homogeneous isotropic media. The description of nonlinear optical effects using shortened wave equations is demonstrated for spontaneous and simulated Raman scattering processes on surface polaritons.
Ponath, H. E.↗
Precomputing Process Noise Covariance for Onboard Sequential Filters
Process noise is often used in estimation filters to account for unmodeled and mismodeled accelerations in the dynamics. The process noise covariance acts to inflate the state covariance over propagation intervals, increasing the uncertainty in the state. In scenarios where the acceleration errors change significantly over time, the standard process noise covariance approach can fail to provide effective representation of the state and its uncertainty. Consider covariance analysis techniques provide a method to precompute a process noise covariance profile along a reference trajectory using known model parameter uncertainties. The process noise covariance profile allows significantly improved state estimation and uncertainty representation over the traditional formulation. As a result, estimation performance on par with the consider filter is achieved for trajectories near the reference trajectory without the additional computational cost of the consider filter. The new formulation also has the potential to significantly reduce the trial-and-error tuning currently required of navigation analysts. A linear estimation problem as described in several previous consider covariance analysis studies is used to demonstrate the effectiveness of the precomputed process noise covariance, as well as a nonlinear descent scenario at the asteroid Bennu with optical navigation.
onboard↗
Anomalous ellipticity dependence of the generation of near-threshold harmonics in noble gases
We measured the ellipticity dependence of the harmonic yield of He, Ne, Ar, Kr, and Xe. It is found that the harmonic yield in general decreases monotonically with increasing laser ellipticity but anomalous dependence does occur for each atom for some harmonic orders. Additionally, we found that the degree of anomaly is weakest in helium but is stronger for the heavier atoms. The anomaly also depends on laser intensity. To explain these features, we developed a quantum trajectory Monte Carlo (QTMC) model based on the quantum path integral theory to study high-order harmonic generation (HHG). The model includes the effect of Coulomb potential from the target ion, thus it is capable of calculating near-threshold harmonics quantitatively. This model reveals that the presence of Coulomb potential would generate orbiting trajectories which are responsible for the anomalous ellipticity dependence near the threshold.
74 ATOMIC AND MOLECULAR PHYSICS↗
Lidar Measurements of Methane and Applications for Aircraft and Spacecraft
Atmospheric methane levels have remained relatively constant over the last decade around 1.78 parts per million (ppm) but observations since 2007 show that levels may be increasing. This trend may be caused by increased fossil fuel production, rice farming, livestock and landfills, but the underlying causes are quite uncertain. One hypothesis is that reservoirs of carbon trapped in the permafrost regions of northern Canada, Europe, and Siberia thaw as global temperatures rise and are releasing increasing amounts of methane. Another hypothesis points to increased production of methane by microbes as the permafrost warms. Currently most observations of greenhouse gases are limited to in-situ (surface and tower sites) and limited airborne in-situ measurements. Space column density measurements are starting to become available from the GOSAT mission. Although methane survives for a shorter time in the atmosphere than CO2, its impact on climate change per molecule is about 23 times than that of CO2. Accurate global observations of several greenhouse gases, including methane, are urgently needed in order to better understand climate change processes and to reduce the uncertainty in the carbon budget. Differential absorption lidar is a well-established technique to measure atmospheric gases, and methane has optical absorption bands near 1.65,2.2,3.4 and 7.8 micron. The near infrared overtones lines of CH4 near 1650 nm are relatively free of interference from other species. There are absorption lines near 1651 nm which are both temperature insensitive and have line strengths well suited for lidar measurements. We have developed a laser and demonstrated lidar measurements of CH4 using lines in this band. Our laser uses a narrow linewidth 1064 nm laser pulse passing through a nonlinear crystal. We generate the tunable laser signals near 1651 nm by using the optical parametric amplification (OPA) process. Inside the crystal the 1064 nm beam overlaps with an injection seed laser near 1651 nm from a wavelength tunable diode laser. Incident photons from the pump laser pulse are converted into two photons, with one at the wavelength of the injection seeder. The wavelength of the OPA output is tuned via the wavelength of diode laser. Our laser is tunable, operates near 1651 nm and generates approximately 4 uJ/pulse at 6 KHz. We vary the emission wavelengths within this band by tuning the diode laser's wavelength. We have used this OPA transmitter to make measurements of CH4 at various pressures in a gas cell and over open outdoor horizontal paths. We have measured the lineshape of methane in a 6 cm long cell at various energy levels with this transmitter, with excellent agreement with the lineshape calculated by HITRAN. We have also measured the absorption lineshape of atmospheric methane in an open 3 km outdoor path. The agreement between the measurements and HITRAN, for 1746 ppb and 760 Torr was quite good. We have also made pulsed two wavelength lidar measurements of methane line absorption in the column to a tower at 1.5 km range. These used on- and off-line wavelengths of 1650.957 nm, and 1651.072 nm, and a 20 cm diameter receiver telescope with an infrared PMT detector. The absorption of the on-line photons was 30%. The methane column absorption was estimated via HITRAN, and was in good agreement with the expected methane absorption for a concentration of 1750 ppm. Finally we have calculated the measurement performance of an airborne methane lidar using this transmitter, as well as the energy and telescope scaling needed for a lidar for space. These results, and more details of our experiments will be described in the presentation.
Riris, Haris↗
Synthesis of Polymers Containing Covalently Bonded NLO Chromophores
Polymers containing covalently bonded nonlinear optical (NLO) chromophores are expected to possess special properties such as greater stability, better mechanical processing, and easier film formation than their non-polymeric equivalent. For the present work, polymethylmethacrylate (PMMA) was selected as the basic polymer unit on which to incorporate different NLO chromophores. The NLO components were variations of DIVA {[2-methoxyphenyl methylidene]-propanedinitrile} which we prepared from vanillin derivatives and malononitrile. These were esterified with methacrylic acid and polymerized either directly or with methyl methacrylate to form homopolymers or copolymers respectively. Characterization of the polymers and NLO property studies are underway.
Denga, Xiao-Hua↗