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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records

Improved high-resolution mapping of phase-matching conditions in second-order nonlinear crystals via imaging

Large-aperture nonlinear crystals for frequency conversion and parametric amplification exhibit spatial variations in phase-matching conditions, which affect the performance of high-power laser systems. We demonstrate significant improvements in speed and resolution to a technique that spatially maps these phase-matching conditions using imaging of the beam resulting from detuned second-harmonic generation. The phase-matching conditions at the pyramidal sector boundary of partially deuterated potassium dihydrogen phosphate (DKDP) are mapped with sub-0.1-mm resolution. We examine the effect of further increases in scan rate on the precision of the technique and demonstrate a scan rate of 0.8 cm 2 per minute at the aforementioned resolution.

Wampler, R. [Univ. of Rochester, NY (United States↗

Efficient bidirectional quantum frequency conversion between telecom and visible bands using adaptively phase-matched III-V nanophotonic waveguides

Quantum frequency conversion (QFC) is essential for interfacing quantum systems operating at different wavelengths and for realizing scalable quantum networks. Despite extensive progress, achieving QFC with simultaneous high efficiency, low pump power, minimal noise, broad bandwidth, and pump-wavelength flexibility remains challenging. Here, we demonstrate efficient, low-noise, and bidirectional QFC between the telecom (1550-nm) and visible (780-nm) bands using unpoled indium gallium phosphide (InGaP) χ (2) nanophotonic waveguides, eliminating the need for a long-wavelength pump. Leveraging the large nonlinear susceptibility of InGaP together with adaptive phase-matching control, we obtain 27% (55%) internal efficiency in a 6-mm (2.5-mm)-long waveguide with a low pump power of 20 mW (50 mW) and a noise flux spectral density of 10 −4 counts per second per hertz at signal–pump detuning of 20 nm. These results mark a significant advance in integrated nonlinear photonics for high-performance QFC, facilitating the development of versatile and scalable quantum networks.

Hu, Jierui [Univ. of Illinois at Urbana-Champaign,↗

Third-harmonic generation in phase-matched Rb vapor.

The generation of 0.3547-micron radiation was performed by tripling 1.064-micron radiation in a phase-matched mixture of rubidium vapor and xenon. A third-harmonic nonlinear susceptibility in Rb vapor is confirmed. It is about 100,000 times greater than that of He. This large susceptibility is due to the large oscillator strengths and resonant enhancements resulting from Rb transitions in the near infrared, visible, and UV.

Young, J. F.↗

Third harmonic generation in phase-matched alkali metal vapors

We report improvements in conversion efficiency for third harmonic generation in sodium and rubidium vapor. 30-psec pulses of radiation at 1.064 micron have been converted to 0.3547 micron with an energy conversion efficiency of 10%. Factors limiting conversion efficiency are discussed.

Bloom, D. M.↗

Multi-Dimensional Spectroscopy with Intense Entangled Beams: Entanglement-Enabled Phase Matching in a Collinear Beam Geometry

The experimental realization of quantum molecular spectroscopy with entangled photons remains challenging owing to the low signal-to-noise ratio resulting from the use of low-flux entangled photons. High-flux entangled photons via intense entangled beams can be used to improve the signal-to-noise ratio, but the presence of unentangled photons contaminates the quantum signal stemming from entangled photons. Here, we demonstrate how intense entangled beams can be used in multi-dimensional spectroscopy while retaining the advantage of photon entanglement. Our approach is broadly applicable to odd-ordered nonlinear spectroscopies, and it generates purely quantum spectroscopic signals. The proposed approach allows the recording of desired phase-matched signals even in a collinear beam geometry, which lifts the requirement of complicated beam geometry setups for phase matching in multi-dimensional spectroscopies.

Absorption spectroscopy↗

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↗

Circularly Polarized Attosecond Pulses Enabled by an Azimuthal Phase and Polarization Grating

High-harmonic generation (HHG) is an extreme nonlinear optical process that can map the properties of an infrared driving laser beam onto short wavelength attosecond pulse trains. However, current techniques for generating circularly polarized high harmonics for probing magnetic materials and chiral systems have limitations: two-color collinear counter-rotating driving lasers result in a low cutoff photon energy, while single-color non-collinear counter-rotating schemes suffer from low conversion efficiency. In this work, we generate circularly polarized attosecond pulse trains by using a structured laser driver which has a rotating polarization and phase grating along the azimuthal coordinate. Furthermore, our experimental and numerical results demonstrate the production of left and right circularly polarized harmonics, which naturally separate upon propagation. Our approach uses a single laser color in a collinear geometry, that can be scaled for high efficiency. Simulations show this scheme can extend into the soft x-ray region when driven by mid-infrared driving lasers, while preserving the same high phase-matching cutoff photon energy as for linearly-polarized high harmonics.

attosecond science↗

Geometric control of hyperbolic exciton-polariton condensate dimers

Coupled many-body quantum systems exhibit rich emergent physics with diverse stationary and dynamical behaviours. By engineering platforms with tunable and distinct coupling mechanisms, new insights emerge into the collective behaviour of coupled many body systems. Particles can be exchanged via evanescent or ballistic coupling: the former, based on proximity, yields large spectral splitting, while the latter requires strict phase-matching, analogous to phase-coupled harmonic oscillators and has a smaller impact on the energy landscape. We demonstrate an all-optically tunable quantum fluid dimer based on exciton-polariton condensates in a photonic crystal waveguide with hyperbolic (saddle-like) dispersion. Varying the dimer’s angle relative to the grating tunes the coupling from evanescent to ballistic. We directly observe spectral features and mass flow shaped by the saddle dispersion. This work highlights photonic crystals as powerful platforms to explore condensed matter phenomena lying at the interface between delay-coupled nonlinear oscillators and tight binding physics.

Georgakilas, Ioannis [IBM Research-Zurich, Rüschli↗

Observation and origin of multi-THz quantum beats in superfluorescent emission from argon

We report observation of multi-THz quantum beats in the amplitude of superfluorescence in pure argon gas, using a time delayed 780-nm probe beam that interrogates the relevant population densities. The superfluorescence is induced by three-photon absorption of an ultrashort 260.5-nm laser pulse that creates coherent and coupled populations in multiple closely spaced 3⁢d and 5⁢s Ar levels. Argon pressure and pump laser focusing parameters are seen to modify the frequency of the quantum beats, which is attributed to the absorption of the self-generated, nonresonant third harmonic of the pump from Ar near the zero of the real part of the overlapping linear susceptibilities of the closely spaced 3⁢d and 5⁢s excited states. The self-absorption of the phase-matched THG photons creates a coherent population of atoms which acts like an atomic excited state (3⁢ω-induced state). Furthermore, we have also observed a new two-step superfluorescent cascade that results from the population redistribution enabled by the 780-nm probe pulse between the 3⁢d'[5/2] 3 and the 3⁢ω-induced state and gives rise to a previously unknown transition that emits on 1587 nm.

74 ATOMIC AND MOLECULAR PHYSICS↗

Enhancement of Rydberg Blockade via Microwave Dressing

Experimental control over the strength and angular dependence of interactions between atoms is a key capability for advancing quantum technologies. Here, in this work, we use microwave dressing to manipulate and enhance Rydberg-Rydberg interactions in an atomic ensemble. By varying the cloud length relative to the blockade radius and measuring the statistics of the light retrieved from the ensemble, we demonstrate a clear enhancement of the interaction strength due to microwave dressing. These results are successfully captured by a theoretical model that accounts for the excitation dynamics, atomic density distribution, and phase-matched retrieval efficiency. Our approach offers a versatile platform for further engineering interactions by exploiting additional features of the microwave fields, such as polarization and detuning, opening pathways for new quantum control strategies.

collective effects in quantum optics↗

Parametric amplification of angularly multiplexed waves for application to beam smoothing

The parametric amplification of angularly multiplexed waves is studied via modeling and experiments. The phase-matching properties of the amplification process with a single pump, including parasitic interactions of pairs of signal/idler, are investigated. An experimental demonstration with up to six signal waves is presented, with a quantification of the output properties, including stability relative to the input pump and seeds. A proof-of-concept study of beam smoothing induced by combining up to 12 speckle fields generated from six signal waves and six idler waves is shown.

Dorrer, C. [University of Rochester, NY (United St↗

Femtosecond two-photon-resonant parametric four-wave mixing detection of atomic hydrogen

Here, we demonstrate an ultrafast parametric four-wave mixing method for the collisional-quenching-free detection of atomic hydrogen. Two photons of 243 nm light resonantly excite the n = 1 to n = 2 transition of atomic hydrogen, and a third probe photon scatters from the electronic coherence to generate the parametric emission of a degenerate signal photon. Laser-induced photofragmentation fluorescence from water, also excited with the same 243 nm pulses, is used as a convenient method to visualize beam overlap in space and time. The femtosecond time resolution enables the suppression of unwanted nonresonant contributions to the signal and separation from resonant mixing in water molecules because of the significantly different coherence lifetimes. A folded BOXCARS phase-matching configuration yields a spatially isolated, laser-like, signal beam, amenable to measurements in highly luminous backgrounds. Measurements in an H 2 /CH 4 /air flame demonstrate quantitative agreement with simulated H-atom concentration profiles. A coherence decay time constant of 42 ps is recorded in the atmospheric pressure flame.

Kliewer, Christopher Jesse [Sandia National Labora↗

Three-beam hybrid fs/ps coherent anti-Stokes Raman scattering of rotation–vibration non-equilibrium

In this work, we demonstrate time-resolved rotational and vibrational temperature measurements to probe plasma non-equilibrium through a simple three-beam hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps CARS) system. A single pump/Stokes pair is employed to generate both the pure-rotational and ro-vibrational Raman coherence. A novel phase-matching scheme, to our knowledge, is employed to spatially overlap the two CARS signals, simplifying the optical design and allowing signal selection by tuning a single spectrometer grating. Measurements were performed near the electrodes in a N 2 DC glow discharge. Both the rotational temperature and the vibrational populations up to $v$ = 8 were calculated from the separately measured single-shot pure-rotational and ro-vibrational CARS spectra. Strong rotation–vibration non-equilibrium was observed at both electrodes, with the cathode showing higher vibrational and rotational temperatures. In addition, non-Boltzmann behaviors were observed at both electrodes. This simplified approach enables measurements of rotational and vibrational temperatures with high spatial resolution in non-equilibrium flows.

42 ENGINEERING↗

Flat nonlinear optics with intersubband polaritonic metasurfaces

Nonlinear intersubband polaritonic metasurfaces produce some of the strongest second- and third-order nonlinear optical responses reported for condensed matter systems at infrared frequencies. These metasurfaces are fabricated as two-dimensional arrays of nanoresonators from multi-quantum-well semiconductor heterostructures, designed to produce strong nonlinear responses associated with intersubband transitions. By optimally coupling the optical modes of the nanoresonators to vertically polarized intersubband transitions in semiconductor heterostructures, one can boost the nonlinear response associated with intersubband transitions, make intersubband transitions interact with free-space radiation at normal incidence, and hence produce optically thin flat nonlinear optical elements compatible with free-space optical setups. As a result of the strong nonlinear response in these systems, significant nonlinear conversion efficiencies (>0.1 %) can be attained in deeply subwavelength optical films using modest pumping intensities of only 10–100 kW/cm 2 . Subwavelength metasurface thickness relaxes phase-matching constraints limiting the operation of bulk nonlinear crystals. Furthermore, the amplitude and phase of the nonlinear optical response in intersubband polaritonic metasurfaces can be tailored for a specific pump wavelength and a nonlinear process of interest through the co-optimization of quantum engineering of electron states in semiconductor heterostructures and photonic engineering of the metasurface nanoresonators design. Additionally, an applied voltage can dynamically control the amplitude and phase of the nonlinear optical response at a nanoresonator level. Here, we review the current state of the art in this rapidly expanding field, focusing on nonlinear processes supporting second-harmonic generation, saturable absorption, and optical power limiting.

flat optics↗

Second-order microscopic nonlinear susceptibility in a centrosymmetric material: application to imaging valence electron motion

We report measurements of phase-matched nonlinear x-ray and optical sum-frequency generation from single-crystal silicon using sub-resonant 0.95 eV laser pulses and 9.5 keV hard x-ray pulses from the LCLS free-electron laser. The sum-frequency signal appears as energy and momentum sidebands to the elastic Bragg peak. It is proportional to the magnitude squared of the relevant temporal and spatial Fourier components of the optically induced microscopic charges/currents. We measure the first- and second-order sideband to the 220 Bragg peak and find that the efficiency is maximized when the applied field is along the reciprocal lattice vector. For an optical intensity of $\sim10^{12} \text{W}/\text{cm}^2$, we measure peak efficiencies of $3\times 10^{-7}$ and $3\times 10^{-10}$ for the first and second-order sideband respectively (relative to the elastic Bragg peak). The first-order sideband is consistent with induced microscopic currents along the applied electric field (consistent with an isotropic response). The second-order sideband depends nontrivially on the optical field orientation and is consistent with an anisotropic response originating from induced charges along the bonds with C$_{3v}$ site symmetry. The results agree well with first-principles Bloch-Floquet calculations.

FOS: Physical sciences↗

High-quantum-efficiency infrared up-conversion.

Experimental study in which 100% conversion of infrared photons into visible photons was achieved through three wave interactions in a nonlinear medium. The first experimental evidence of overconversion is presented, and the classical theory of up-conversion in the high-conversion-efficiency region is confirmed. A laser pump light feedback technique is described that promises to make the process practical with modestly powerful pump lasers and less than perfect nonlinear crystals. The nonlinear medium used was a LiIO3 crystal that cannot be 90-deg phase-matched. The 'walk off' that resulted helped make possible the attainment of 100% conversion efficiency.

Gurski, T. R.↗