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At least 55 records · Page 3

Spectral Similarity Masks Structural Diversity at Hydrophobic Water Interfaces

The air-water and graphene-water interfaces represent quintessential examples of the liquid-gas and liquid-solid boundaries, respectively. While the sum-frequency generation (SFG) spectra of these interfaces show similarities, a consensus on their signals and interpretations has yet to be reached. Leveraging deep learning, we computed first-principles SFG spectra for both systems, addressing experimental discrepancies. Here, our findings reveal that similarities in SFG signals do not translate into comparable interfacial microscopic properties. Instead, graphene-water and air-water interfaces exhibit fundamental differences in SFG-active thicknesses, hydrogen-bonding networks, and surface dynamics. These distinctions underscore roughness suppression and electronic interactions present at the solid-liquid interface but absent at the gas-liquid interface.

Wang, Yong [Princeton Univ., NJ (United States)] (

Non-resonant picosecond three-wave mixing in the gas phase

We report on the experimental observation of non-resonant, second-order optical sum-frequency generation (SFG) in five different atomic and molecular gases. The measured signal is attributed to a SFG process by characterizing its intensity scaling and its polarization behavior. We show that the electric quadrupole mechanism cannot explain the observed trends and suggest a mechanism based on symmetry breaking along the incident beam path arising from laser-induced species ground state number density gradients. Our results demonstrate that the SFG is about four orders of magnitude stronger than the third-harmonic generation (THG) and independent from any externally applied electric fields. In conclusion, these features make this method suitable for gas number density measurements at the picosecond time scale in reactive flows and plasmas.

LaCombe, Grayson

Institute for Catalysis in Energy Processes (ICEP) (Final Report)

The Institute for Catalysis in Energy Processes (ICEP) was a multi-PI program located at the Northwestern University Center for Catalysis and Surface Science from 2006-2024. Over several renewal cycles and several organizing themes, ICEP addressed fundamental questions in catalysis science. In turn, the scientific questions addressed were directly relevant to the efficient use of the nation’s resources to produce fuels and commodity chemicals, harness alternate energy sources for chemical reactions such as light or electricity, reduce emissions and waste, and minimize the impact of our use of plastics. Selective oxidation, (oxidative) dehydrogenation, deNOx, CO 2 reduction, hydrogen release, polymer decomposition / depolymerization, and many other reactions of intense interest to the US Department of Energy were studied in the center. Major ICEP strengths were in catalyst synthesis, in measurements that elucidated catalyst properties, in reaction mechanisms and kinetics, and in predictive theory and modeling. ICEP researchers were often the inventors or developers of materials and methods that were brought to bear on the Institute’s catalytic systems. Key characterization tools advanced through this project included resonance Raman and related techniques, sum frequency generation, and X-ray standing wave spectroscopy. Center members relied extensively on computational tools such as density functional theory and microkinetic modeling to fully investigate catalyst structures and catalytic mechanisms. ICEP researchers were early developers of atomic layer deposition (ALD) for catalyst synthesis and were early pioneers of metal organic frameworks for catalysis. ICEP innovations are found in areas of intense research such as single-atom catalysts, catalytic deconstruction of plastics, and catalytic MOFs, to name a few. Research areas initiated by ICEP indirectly led to DOE EFRCs, startup companies, and other achievements. Over its 18 years of existence, ICEP involved two different PIs (Stair and Notestein) and 24 senior investigators across several academic disciplines at Northwestern University. There were tight collaborations with Argonne National Laboratory, including specialized equipment and experiments permanently located there. The center supported ~400 person-years of effort by graduate students and postdocs, either directly through DOE support or indirectly by leveraging independent support provided to the trainees, e.g. through the NSF GRFP or internal fellowships. The project resulted in 328 manuscripts and numerous conference presentations.

36 MATERIALS SCIENCE

Chemical and Optical Control of Spin Crossover: Ultrafast XUV Spectroscopy of Molecular Magnets in Native Solvation Environments

With support from the US Department of Energy Office of Science, we have developed and utilized extreme ultraviolet (XUV) spectroscopy and sum frequency generation vibrational spectroscopy as probes of charge, spin, and solvation structure and dynamics in molecules and at interfaces. This work is crucial to advancing fundamental understanding of the processes that control the efficiency and speed of energy conversion and information processing in molecules and at interfaces. Accordingly, it has important applications for developing next generation technologies for information storage and processing with increasing data storage density and processing rates as well as developing new methods for efficient energy conversion and storage.

74 ATOMIC AND MOLECULAR PHYSICS

A solid state tunable laser for resonance measurements of atmospheric sodium

The measurement of wave dynamics in the upper mesosphere using a solid-state laser to excite the resonance fluorescence line of sodium is examined. Two Nd:YAG lasers are employed to produce the sodium resonance line. The method involves mixing the 1064 nm radiation with that from a second Nd:YAG operating at 1319 nm in a nonlinear infrared crystal to directly produce 589 nm radiation by sum frequency generation. The use of the transmitter to measure the sodium layer from the Space Shuttle Platform is proposed. A diagram of the laser transmitter is presented.

Philbrick, C. R.

Program Predicts Performance of Optical Parametric Oscillators

A computer program predicts the performances of solid-state lasers that operate at wavelengths from ultraviolet through mid-infrared and that comprise various combinations of stable and unstable resonators, optical parametric oscillators (OPOs), and sum-frequency generators (SFGs), including second-harmonic generators (SHGs). The input to the program describes the signal, idler, and pump beams; the SFG and OPO crystals; and the laser geometry. The program calculates the electric fields of the idler, pump, and output beams at three locations (inside the laser resonator, just outside the input mirror, and just outside the output mirror) as functions of time for the duration of the pump beam. For each beam, the electric field is used to calculate the fluence at the output mirror, plus summary parameters that include the centroid location, the radius of curvature of the wavefront leaving through the output mirror, the location and size of the beam waist, and a quantity known, variously, as a propagation constant or beam-quality factor. The program provides a typical Windows interface for entering data and selecting files. The program can include as many as six plot windows, each containing four graphs.

Cross, Patricia L.

Sensitive Infrared Signal Detection by Upconversion Technique

We demonstrated upconversion assisted detection of a 2.05-micron signal by sum frequency generation to generate a 700-nm light using a bulk periodically poled lithium niobate crystal. The achieved 94% intrinsic upconversion efficiency and 22.58% overall detection efficiency at a pW level of 2.05 micron pave the path to detect extremely weak infrared (IR) signals for remote sensing applications.

Wong, Teh-Hwa

Linear and Nonlinear X-ray Spectra of Chiral Molecules: X-ray Circular Dichroism, Sum- and Difference-Frequency Generation of Fenchone and Cysteine

Recent advancements in X-ray light sources enable element-sensitive nonlinear spectroscopies for probing molecular chirality. We simulate X-ray absorption spectroscopy, X-ray circular dichroism (XCD), and nonlinear optical/X-ray SFG and DFG (OX SFG/DFG) signals for two prototypical chiral molecules, fenchone and cysteine. Furthermore, our multireference simulations reproduce experimental data and reveal how novel X-ray spectroscopies exploit the site- and element-sensitivity of X-rays to uncover molecular asymmetry. The XCD spectra show strong asymmetries at chiral centers, while distant atoms contribute weaker signals. The OX SFG/DFG signals, under fixed resonant optical excitation, strongly depend on the core and valence excitations. This allows us to introduce two-dimensional (2D) chirality-sensitive valence-core spectroscopy, which provides insight into the overlap between valence orbitals and local molecular asymmetry. Finally, our estimates using realistic laser and X-ray pulse parameters demonstrate that such nonlinear experiments are feasible at XFELs, offering a promising tool for investigating chiral molecules.

Circular dichroism spectroscopy

Twisted Nonlinear Optics in Monolayer van der Waals Crystals

In addition to a plethora of emergent phenomena, the spatial topology of optical vortices enables an array of applications in optical communications and quantum information science. Multibeam nonlinear optical processes, augmented by optical vortices, are essential in this context, providing robust access to an infinitely large set of quantum states associated with the orbital angular momentum of light. Here, we push the boundaries of vortex nonlinear optics to the ultimate limits of material dimensionality. By exploiting multipulse difference frequency, sum frequency, and four-wave mixing in monolayer quantum materials, we demonstrate their ability to independently control the orbital angular momentum and radial distribution of vortex light-fields in addition to their wavelength. Due to the atomically thin nature of the host crystal, this control spans a broad spectral bandwidth in a highly integrable platform that is unconstrained by the traditional limits of bulk nonlinear optical materials. Our work heralds an innovative path for ultracompact and scalable hybrid nanophotonic technologies empowered by twisted nonlinear light–matter interactions in van der Waals nanomaterials.

36 MATERIALS SCIENCE

Deep learning-assisted modeling for χ (2) nonlinear optics

Modeling second-order (χ(2)) nonlinear optical processes remains computationally expensive due to the need to resolve fast field oscillations and simulate wave propagation using methods such as the split-step Fourier method (SSFM). This can become a bottleneck in real-time applications, such as high-repetition-rate laser systems requiring rapid feedback and control. We present a long short-term memory-based surrogate model trained on SSFM simulations generated from a start-to-end model of the photocathode drive laser at SLAC National Accelerator Laboratory’s Linac Coherent Light Source II. The model achieves over 250× speedup while maintaining high fidelity, enabling future real-time optimization and laying the foundation for data-integrated modeling frameworks and digital twins of laser systems.

Accelerator Physics (physics.acc-ph)

Characterization of Artificial Guidestars Generated in the Mesospheric Sodium Layer

Using a 10 W average power sum-frequency laser, we have generated resonant fluorescence beacons in the mesospheric sodium layer and are currently evaluating them for use as an artificial guidestar for atmospheric compensation using adaptive optics. Two flashlamp pumped Nd:YAG lasers operating at 1.064 and 1.319 microns are mixed in a lithium triborate crystal to produce 589 nm light at 840 Hz. The laser emits 47.5 microsec mode-locked pulse trains at 11-14 mJ per pulse and is tuned to the sodium resonance transition with intracavity etalons.

Jelonek, M. P.

Development of Mesospheric Sodium Laser Beacon for Atmospheric Adaptive Optics

A solid-state source of long pulse length, sodium-resonance radiation was developed for the purpose of generating an artificial star in the earth's mesospheric sodium layer. This radiation is generated by sum-frequency mixing the output of a 1.064 micron Nd:YAG laser with the output of a 1.319-micron Nd:YAG laser. By operating these lasers at wavelengths very close to the peak of their tuning curves, it is possible to match the wavelength of the sum-frequency radiation to that of the sodium D2 adsorption wavelength. Two pulsed laser systems were constructed, one producing as much as 0.6 J of sodium resonance radiation at a 10-Hz repetition rate and another producing as much as 24 mJ at a 840-Hz repetition rate. In both laser systems, the 1.06-micron and 1.32-micron Nd:YAG lasers are configured as mode-locked master oscillators followed by power amplifiers. Other aspects of this project are presented.

Jeys, T. H.

Exciton dressing by extreme nonlinear magnons in a layered semiconductor

Collective excitations presenting nonlinear dynamics are fundamental phenomena with broad applications. A prime example is nonlinear optics, where diverse frequency mixing processes are central to communication, sensing, wavelength conversion, and attosecond physics. Leveraging recent progress in van der Waals magnetic semiconductors, we demonstrate nonlinear opto-magnonic coupling by presenting exciton states dressed by up to 20 harmonics of magnons, resulting from their nonlinearities, in the layered antiferromagnetic semiconductor CrSBr. We also create tunable optical side bands from sum- and difference-frequency generation between two optically bright magnon modes under symmetry breaking magnetic fields. Moreover, the observed difference-frequency generation mode can be continuously tuned into resonance with one of the fundamental magnons, resulting in parametric amplification of magnons. These findings realize the modulation of the optical frequency exciton with the extreme nonlinearity of magnons at microwave frequencies, which could find applications in magnonics and hybrid quantum systems, and provide new avenues for implementing opto-magnonic devices.

Diederich, Geoffrey M.

Nonlinear ultrasonic scanning to detect material defects

A method and system are provided to detect defects in a material. Waves of known frequency(ies) are mixed at an interaction zone in the material. As a result, at least one of a difference wave and a sum wave are generated in the interaction zone. The difference wave occurs at a difference frequency and the sum wave occurs at a sum frequency. The amplitude of at least one nonlinear signal based on the sum and/or difference waves is then measured. The nonlinear signal is defined as the amplitude of one of the difference wave and sum wave relative to the product of the amplitude of the surface waves. The amplitude of the nonlinear signal is an indication of defects (e.g., dislocation dipole density) in the interaction zone.

Yost, William T.

Lunar and Solar Torques on the Oceanic Tides

Brosche and Seiler recently suggested that direct lunar and solar tidal torques on the oceanic tides play a significant role in the earth's short-period angular momentum balance ("short-period" here meaning daily and sub-daily). We reexamine that suggestion here, concentrating on axial torques and hence on variations in rotation rate. Only those spherical harmonic components of the ocean tide having the same degree and order as the tidal potential induce nonzero torques. Prograde components (those moving in the same direction as the tide-generating body) produce the familiar secular braking of the earth's rotation. Retrograde components, however, produce rapid variations in UTI at twice the tidal frequency. There also exist interaction torques between tidal constituents, e.g. solar torques on lunar tides. They generate UTI variations at frequencies equal to the sums and differences of the original tidal frequencies. We give estimates of the torques and angular momentum variations for each of the important regimes, secular to quarter-diurnal. For the M(sub 2) potential acting on the M(sub 2) ocean tide, we find an associated angular momentum variation of amplitude 3 x 10(exp 19) N m. This is 5 to 6 orders of magnitude smaller than the angular momentum variations associated with tidal currents. We conclude that these torques do not play a significant role in the short-period angular momentum balance.

Ray, Richard D.

Lunar and Solar Torques on the Oceanic Tides

A general framework for calculating lunar and solar torques on the oceanic tides is developed in terms of harmonic constituents. Axial torques and their associated angular momentum and earth-rotation variations are deduced from recent satellite-altimeter and satellite-tracking tide solutions. Torques on the prograde components of the tide produce the familiar secular braking of the rotation rate. The estimated secular acceleration is approximately -1300 sec/century(sup 2) (less 4% after including atmospheric tides); the implied rate of change in the length of day is 2.28 milliseconds/century. Torques on the retrograde components of the tide produce periodic rotation variations at twice the tidal frequency. Interaction torques, e.g. solar torques on lunar tides, generate a large suite of rotation-rate variations at sums and differences of the original tidal frequencies. These are estimated for periods from 18.6 years to quarter-diurnal. At subdaily periods the angular momentum variations are 5 to 6 orders of magnitude smaller than the variations caused by ocean tidal currents.

Ray, Richard D.

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)