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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
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Probing autoionization decay lifetimes of the 4d−16ℓ core-excited states in xenon using attosecond noncollinear four-wave-mixing spectroscopy

The decay of core-excited states is a sensitive probe of autoionization dynamics and correlation effects in many-electron systems, occurring on ultrafast timescales. Xenon, with its dense manifold of autoionizing resonances that can be coupled with near-infrared light, provides a platform to investigate these processes. In this work, the autoionization decay lifetimes of 4d-16ℓ (ℓ = s, p, d, …) core-excited states in xenon atoms are probed with extreme ultraviolet (XUV) attosecond noncollinear four-wave-mixing (FWM) spectroscopy. The 4d{5/2,3/2}-16p XUV-bright states (optically dipole-allowed) exhibit decay lifetimes of ∼6 fs, which is consistent with spectator-type decay. In contrast, the 4d{5/2,3/2}-16s and 4d{5/2,3/2}-16d XUV-dark states (optically dipole forbidden) show longer decay lifetimes of ∼20 fs. Photoionization calculations confirm that all core-hole states with 4d character should decay via spectator channels in ≤6 fs, suggesting that the apparently longer dark-state decay times arise from an alternative mechanism. A few-level simulation of the FWM process shows that the inclusion of a nearby, longer-lived dark state can mimic the experimental FWM signal, suggesting population cycling with a second electronic state with non-4d character. Ab initio calculations support the presence of such multielectron excited states in the 60-70 eV range. These results demonstrate that FWM signals can encode coupled-state dynamics when probing complex systems, highlighting the importance of combining theoretical and experimental approaches to disentangle accurate core-level decay pathways and lifetimes.

Puskar, Nicolette G↗
DOE OSTI2022

State-selective probing of CO 2 autoionizing inner valence Rydberg states with attosecond extreme ultraviolet four-wave-mixing spectroscopy

Nonlinear spectroscopies can disentangle spectra that are congested due to inhomogeneous broadening. Here, in conjunction with theoretical calculations, attosecond extreme ultraviolet (XUV) four-wave-mixing (FWM) spectroscopy is utilized to probe the dynamics of autoionizing inner valence excited Rydberg states of the polyatomic molecule, CO 2 . This tabletop nonlinear technique employs a short attosecond XUV pulse train and two noncollinear, few-cycle near-infrared pulses to generate background-free XUV wave-mixing signals. FWM emission is observed from the n=5-7 states of the Henning sharp ndσ g Rydberg series that converges to the ionic $\widetilde{B}$ 2 Σ$^{+}_{u}$ state. However, these transient emission signals decay with lifetimes of 33 ± 6, 53 ± 2, and 94 ± 2 fs, respectively, which calculations show are consistent with the lifetimes of the short-lived n=6-8 members of the nsσ g character Henning diffuse Rydberg series. The oscillator strengths of transitions between states involved in all possible resonant FWM processes are calculated, verifying that the nonlinear spectra are dominated by pathways described by an initial excitation to the diffuse nsσ g Rydberg series and emission from the sharp ndσ g Rydberg series. The results substantiate not only that attosecond XUV FWM spectroscopy produces rigorous and meaningful measurements of ultrafast dynamics in polyatomic systems, but also that nonlinear spectroscopic techniques are versatile tools to selectively probe dynamics that are otherwise difficult to access.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Measuring autoionization decay lifetimes of optically forbidden inner valence excited states in neon atoms with attosecond noncollinear four-wave-mixing spectroscopy

Attosecond noncollinear four-wave-mixing spectroscopy with one attosecond extreme ultraviolet (XUV) pulse and two few-cycle near-infrared (NIR) pulses was used to measure the autoionization decay lifetimes of inner valence electronic excitations in neon atoms. After a 43-48-eV XUV photon excites a 2s electron into the 2s2p 6 (np) Rydberg series, broadband NIR pulses couple the 2s2p 6 3p XUV-bright state to neighboring 2s2p 6 3s and 2s2p 6 3d XUV-dark states. Controllable delays of one or both NIR pulses with respect to the attosecond XUV pulse reveal the temporal evolution of either the dark or bright states, respectively. Experimental lifetimes for the 3s, 3p, and 3d states are measured to be 7±2, 48±8, and 427±40 fs, respectively, with 95% confidence. Accompanying calculations with two independent ab initio theoretical methods, newstock and astra, verify the findings. The results support the expected trend that the autoionization lifetime should be longer for states that have a smaller penetration in the radial region of the 2s core hole, which in this case is for the higher angular momentum Rydberg orbitals. In conclusion, the underlying theory thus links the lifetime results to electron correlation and provides an assessment of the direct and exchange terms in the autoionization process.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Extracting doubly excited state lifetimes in helium directly in the time domain with attosecond noncollinear four-wave-mixing spectroscopy

The helium atom, with one nucleus and two electrons, is a prototypical system to study quantum many-body dynamics. Doubly excited states, or quantum states in which both electrons are excited by one photon, showcase electronic-correlation mediated effects. In this paper, the natural lifetimes of the doubly excited 1 P o 2 s n p Rydberg series and the 1 S e 2 p 2 dark state in helium in the 60–65 eV region are measured directly in the time domain with extreme-ultraviolet/near-infrared noncollinear attosecond four-wave-mixing (FWM) spectroscopy. The measured lifetimes agree with lifetimes deduced from spectral linewidths and theoretical predictions, and the roles of specific decay mechanisms are considered. While complex spectral line shapes in the form of Fano resonances are common in absorption spectroscopy of autoionizing states, the background-free and thus homodyned character of noncollinear FWM results exclusively in Lorentzian spectral features in the absence of strong-field effects. The onset of strong-field effects that would affect the extraction of accurate natural lifetimes in helium by FWM is determined to be approximately 0.3 Rabi cycles. This study provides a systematic understanding of the FWM parameters necessary to enable accurate lifetime extractions, which can be utilized in more complex quantum systems in the future. Published by the American Physical Society 2024

Rupprecht, Patrick (ORCID:000000026491793X)↗
DOE OSTI2025

Probing coherent electronic superpositions of singly and doubly excited states of krypton with extreme-ultraviolet four-wave-mixing spectroscopy

Radiative nonlinear four-wave mixing can monitor the evolution of electronic wave packets, providing access to lifetimes and quantifying the light-induced couplings between excited states. In this article, we report the observation of quantum beats in an autoionizing electronic wave packet in krypton, probed using this technique. Analysis of the signal reveals that these beats originate from the contribution of previously unassigned, doubly excited states interacting with singly excited ones. We introduce a minimal theoretical model, based on multichannel quantum-defect theory, which quantitatively reproduces both the wave-packet dynamics and the static spectrum. This work combines a versatile, noncommensurate XUV-IR-based experimental scheme with a tractable model, establishing a powerful approach for the metrology and control of complex, correlated electronic states.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Nonresonant coherent amplitude transfer in attosecond four-wave-mixing spectroscopy

Attosecond four-wave mixing (FWM) spectroscopy using an extreme ultraviolet (XUV) pulse and two noncollinear near-infrared (NIR) pulses is employed to measure Rydberg wave packet dynamics resulting from XUV excitation of a 3s electron in atomic argon into a series of autoionizing 3s –1 np Rydberg states ~29 eV. The emitted signals from individual Rydberg states exhibit oscillatory structure and persist well beyond the expected lifetimes of the emitting Rydberg states. These results reflect substantial contributions of longer-lived Rydberg states to the FWM emission signals of each individually detected state. A wave packet decomposition analysis reveals that coherent amplitude transfer occurs predominantly from photoexcited 3s –1 (n + 1) p states to the observed 3s –1 np Rydberg states. The experimental observations are reproduced by time-dependent Schrödinger equation simulations using electronic structure and transition moment calculations. Finally, the theory highlights that coherent amplitude transfer is driven nonresonantly to the 3s –1 np states by the NIR light through 3s –1 (n + 1)s and 3s –1 (n – 1)d dark states during the FWM process.

74 ATOMIC AND MOLECULAR PHYSICS↗
NASA NTRS2009

Distinguishing non-resonant four-wave-mixing noise in coherent stokes and anti-stokes Raman scattering

A method of examining a sample comprises exposing the sample to a pump pulse of electromagnetic radiation for a first period of time, exposing the sample to a stimulant pulse of electromagnetic radiation for a second period of time which overlaps in time with at least a portion of the first exposing, to produce a signal pulse of electromagnetic radiation for a third period of time, and interfering the signal pulse with a reference pulse of electromagnetic radiation, to determine which portions of the signal pulse were produced during the exposing of the sample to the stimulant pulse. The first and third periods of time are each greater than the second period of time.

Marks, Daniel L.↗
DOE OSTI2025

Tracing Long-Lived Atomic Coherences Generated via Molecular Conical Intersections

Accessing coherences is key to fully understand and control ultrafast dynamics of complex quantum systems like molecules. Most photochemical processes are mediated by conical intersections, which generate coherences between electronic states in molecules. We show with accurate calculations performed on gas-phase methyl iodide that electronic coherences of spin-orbit-split states persist in atomic iodine after dissociation. Our simulation predicts a maximum magnitude of vibronic coherence in the molecular regime of 0.75% of the initially photoexcited state population. Upon dissociation, one-third of this coherence magnitude is transferred to a long-lived atomic coherence where vibrational decoherence can no longer occur. To trace these dynamics, we propose a tabletop experimental approach—heterodyned attosecond four-wave-mixing spectroscopy. This technique can temporally resolve small electronic coherence magnitudes and reconstruct the full complex coherence function via phase cycling. Hence, heterodyned attosecond four-wave-mixing spectroscopy leads the way to a complete understanding and optimal control of spin-orbit-coupled electronic states in photochemistry.

Chemical Physics↗
DOE OSTI2025

N -way parametric frequency beamsplitter for quantum photonics

Optical networks are the leading platform for the transfer of information due to their low loss and ability to scale to many information channels using optical frequency modes. To fully leverage the quantum properties of light in this platform, it is desired to manipulate higher-dimensional superpositions by orchestrating linear, beamsplitter-type interactions between several channels simultaneously. We propose a method of achieving simultaneous, all-to-all coupling between N optical frequency modes via N -way Bragg-scattering four-wave mixing. By exploiting the frequency degree of freedom, additional modes can be multiplexed in an interaction medium of fixed volume and loss while avoiding the introduction of excess noise. We generalize the theory of the frequency-encoded two-mode interaction to N modes under this four-wave-mixing approach, finding that arbitrary unitary transformations are possible through successive four-wave-mixing pump configurations. We experimentally verify the quantum nature of this scheme by demonstrating three-way multiphoton interference. Two input photons are shared among three frequency modes and display interference differing from that of two classical (coherent-state) inputs. These results show the potential of our approach for the scalability of photonic quantum information processing to general N -mode systems in the frequency domain. Published by the American Physical Society 2025

Oliver, Richard (ORCID:0000000207760657)↗
NASA NTRS1993

Self-pumped phase conjugation and four-wave mixing in 0- and 45-deg-cut n-type BaTiO3:Co

Relatively fast self-pumped phase-conjugate and four-wave-mixing rise times are reported in n-type cobalt-doped barium titanate. With the crystal oriented in a 45-deg cut as compared with the same crystal in a 0-deg cut we find a factor of 3 decrease in the 0-90-percent rise time to 800 ms with 25-mW input power at 514.5 nm. Also, the self-pumped phase-conjugate reflectivity increases from 20 to 40 percent. We deduce that the phase conjugation is from internally seeded stimulated photorefractive backscattering. The four-wave-mixing rise time of the 45-deg-cut crystal is 4 ms with a reflectivity of 48 percent when the pumping beams are derived from self-pumped phase conjugation that has an input power of 25 mW.

Garrett, M. H.↗
DOE OSTI2024

Protocols for x-ray transient grating pump/optical probe experiments at x-ray free electron lasers

Abstract Transient grating spectroscopy is a specialized application of the four-wave-mixing methodology and constitutes a versatile technique for investigating the dynamics of vibrational, magnetic and electronic degrees of freedom of matter in a background-free fashion. Recent developments in free-electron laser sources have enabled the extension of this technique into the extreme ultraviolet range. Ongoing efforts to expand transient grating spectroscopy into the x-ray regime promise numerous advantages: (1) substantial penetration depths that allow for probing bulk material properties, (2) element specificity via specific core-excited states, and (3) short wavelengths that allow for excitation gratings with higher momentum transfer and improved spatial resolution. In this study, we comprehensively outline the procedures for conducting x-ray transient grating pump/optical probe experiment. The process encompasses the design and alignment of the experimental setup, as well as the subsequent steps involved in data acquisition and analysis. This paper is intended as a comprehensive guide for researchers interested in implementing x-ray transient grating spectroscopy, providing valuable insights into the intricacies of the experimental workflow required for this novel technique. Furthermore, we discuss the potential for extending this methodology to an x-ray pump/x-ray probe scheme, envisioning a future direction that holds promise for enhancing the capabilities and scope of x-ray transient grating spectroscopy, opening new opportunities for studying ultrafast processes with unprecedented temporal and spatial resolutions.

Optics↗
DOE OSTI2024

Multidimensional coherent spectroscopy of light-driven states and their collective modes in multiband superconductors

We present a comprehensive theory of light-controlled multiband superconductivity, and apply it to predict distinctive signatures of light-driven superconducting (SC) states in terahertz multidimensional coherent spectroscopy (THz-MDCS) experiments. We first derive gauge-invariant Maxwell-Bloch equations for multiband BCS superconductors with spatial fluctuations. We consider driving electromagnetic fields determined self-consistently by Maxwell's equations. By calculating the THz-MDCS spectra measured experimentally in the clean SC limit, we identify unique signatures of finite-momentum Cooper-pairing states that live longer than the laser pulse. They are controlled by a pair of THz laser pulses with well-defined relative phase (pulse pair). The pseudospin oscillators that describe the properties of these SC states are parametrically driven by both finite-momentum Cooper pairing and by time oscillations of the order-parameter relative phase. We show that such strong parametric driving leads to drastic changes in the THz-MDCS spectral shape from the predictions of third-order nonlinear susceptibility calculations. These spectral changes strongly depend on the interband-to-intraband interaction ratio and on the collective modes of the light-driven state. For negligible interband interaction, the spectra show a transition with increasing field, from traditional pump-probe, four-wave-mixing, and third-harmonic generation peaks determined by the laser frequency to sidebands determined by the excitations of the driven system. These sidebands emerge from difference-frequency Raman processes in the nonequilibrium SC state. For interband couplings weaker than the intraband pairing, we show that the Leggett phase collective mode leads to harmonic sidebands around the traditional pump-probe peaks. Additional Higgs collective mode peaks result from light-induced inversion-symmetry breaking in a thin-film geometry. For strong interband coupling, we find a transition from a nonequilibrium finite Cooper-pair momentum state characterized by hybrid-Higgs amplitude mode peaks in THz-MDCS spectra to a driven state identified experimentally by the emergence of Floquet-type sidebands at bi-Higgs frequencies. Those dominant bi-Higgs-frequency satellites are manifestations of a new order parameter relative phase collective mode that characterizes the nonequilibrium SC state. The predicted interaction- and field-dependent transitions in the spectral profile allow us to propose THz-MDCS experiments for quantum tomography of light-driven superconductivity.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Mitigating Scattering in a Quantum System Using Only an Integrating Sphere

Strong quantum correlated sources are essential but delicate resources for quantum information science and engineering protocols. Decoherence and loss are the two main disruptive processes that lead to the loss of nonclassical behavior in quantum correlations. In quantum systems, scattering can contribute to both decoherence and loss. In this work, we present an experimental scheme capable of significantly mitigating the adverse impact of scattering in quantum systems. Our quantum system is composed of a two-mode squeezed light generated with the four-wave-mixing process in hot rubidium vapor and a scatterer is introduced to one of the two modes. An integrating sphere is then placed after the scatterer to recollect the scattered photons. We use mutual information between the two modes as the measure of quantum correlations and demonstrate a 47.5% mutual information recovery from scattering, despite an enormous photon loss of greater than 85%. Our scheme is the very first step toward recovering quantum correlations from disruptive random processes and thus has the potential to bridge the gap between proof-of-principle demonstrations and practical real-world implementations of quantum protocols. Published by the American Physical Society 2024

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1987

Four-mode squeezing

The four-wave-mixing interactions produced by pumping at two well-separated frequencies can couple four different radiation modes to generate a new kind of squeezed state of light. A dual-frequency homodyne detection scheme is described and is used to observe this type of nonclassical correlation. Initial experimental results in an optical fiber show a noise level 20 percent below the vacuum noise level for the output of the dual-frequency detector, even though the noise at each individual detector remains above the vacuum level.

Schumaker, B. L.↗
NASA NTRS1989

Optical Processing With Photorefractive Semiconductors

Experimental phase-conjugate four-wave-mixing apparatus used to demonstrate capabilities of GaAs (and potentially of other photorefractive semiconductors like InP and CdTe) for optical processing of information. With modifications, performs any of three basic image-processing functions: transfer to different light beam, enhancement of edges, and autocorrelation. Includes crystal of GaAs of 5 by 9 by 9 mm with cubic crystalline axes. Advantages include high speed and compatibilty with other semiconductor devices.

Cheng, Li-Jen↗
NASA NTRS1989

Optical Stark effect in the four-wave mixing and stimulated Raman spectra of N2

The influence of the optical Stark effect on spectral line shapes in four-wave-mixing Raman spectroscopy (FWMRS) and stimulated Raman spectroscopy (SRS) is investigated experimentally and theoretically. Using an experimental setup capable of rapid alternation between the simultaneous measurement of coherent Stokes Raman spectroscopy and inverse Raman spectroscopy at low and high intensities, together with a sophisticated frequency reference scheme, it was possible to perform a rather direct comparison between Stark-broadened and non-Stark-broadened spectra of both classes of Raman spectroscopies. The results demonstrate that SRS spectra show more Stark shift and broadening than their FWMRS counterparts. A discrepancy with theoretical results is pointed out, and an attempt is made to explain it.

Moosmuller, H.↗
NASA NTRS2004

Hyper-Parametric Oscillations in a Whispering Gallery Mode Fluorite Resonator

This viewgraph presentation summarizes the hyper-parametric oscillations observations of the fluorite resonator. The reporters have observed various nonlinear effects in ultra-high Q crystalline whispering gallery mode (WGM) resonators. In particular, it was demonstrated a low threshold optical hyper-parametric oscillations in a high-Q (Q=1010) CaF2 WGM resonator. The oscillations result from the resonantly enhanced four-wave-mixing occurring due to Kerr nonlinearity of the material.

four wave mixing↗