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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 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Molecular bond stabilization in the strong-field dissociation of O 2 +

We theoretically examine the rotational and vibrational dynamics of O 2 + molecular ions exposed to intense, short laser pulses for conditions realized in contemporary pump-probe experiments. We solve the time-dependent Schrödinger equation within the Born-Oppenheimer approximation for an initial distribution of randomly aligned molecular ions. For fixed peak intensities, our numerical results show that total, angle-integrated O 2 + → O( 3 P) + O + ( 4 S 0 ) dissociation yields do not monotonically increase with increasing infrared-probe pulse duration. We find this pulse-duration-dependent stabilization to be consistent with the transient trapping of nuclear probability density in a light-induced (bond-hardening) potential-energy surface and robust against rotational excitation. We analyze this stabilization effect and its underlying bond-hardening mechanism (i) in the time domain, by following the evolution of partial nuclear probability densities associated with the dipole-coupled O 2 + (a 4 Π u ) and O 2 + (f 4 Π g ) cationic states, and (ii) in the frequency domain, by examining rovibrational quantum-beat spectra for the evolution of the partial nuclear probability densities associated with these states. In this work, our analysis reveals the characteristic timescale for the bond-hardening mechanism in O 2 + and explains the onset of bond stabilization for sufficiently long pulse durations.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Vibrational Cooper minima used to verify the dissociation pathway induced by a short intense laser pulse

Vibrational Cooper minima due to weak dipole coupling were previously observed in strong-field dissociation of H 2⁡ + as minima in the kinetic-energy-release (KER) spectrum [McKenna et al., Phys. Rev. Lett. 103, 103006 (2009)]. We demonstrate in two independent experiments that these vibrational Cooper minima occur more generally and can be used as “fingerprints” to identify the final electronic state in the dissociation pathway. In the first experiment, we show the wavelength dependence of the vibrational Cooper minima observed in the KER spectrum of O 2⁢ + dissociation induced by 396- and 264-nm photons. These minima appear at the locations predicted by our first-order perturbation-theory calculations. In the second experiment, a delay-dependent KER spectrum is obtained from O 2 using an ionizing pump and a dissociating probe, then Fourier-transformed to generate a spin-rotation quantum beat spectrum of O 2 ⁢+ . As a result, this spectrum shows vibrational Cooper minima at the expected locations, confirming their presence in another observable. In this case, these minima are used to identify the dissociation pathway.

Molecular dissociation↗
DOE OSTI2023

Effects of Autoionizing Resonances on Wave-Packet Dynamics Studied by Time-Resolved Photoelectron Spectroscopy

Here, we report a combined experimental and theoretical study on the effect of autoionizing resonances in time-resolved photoelectron spectroscopy. The coherent excitation of N 2 by ~14.15 eV extreme-ultraviolet photons prepares a superposition of three dominant adjacent vibrational levels (v'=14–16) in the valence b' 1 $Σ^+_u$ state, which are probed by the absorption of two or three near-infrared photons (800 nm). The superposition manifests itself as coherent oscillations in the measured photoelectron spectra. A quantum-mechanical simulation confirms that two autoionizing Rydberg states converging to the excited A 2 Π u and B 2 $Σ^+_u$ $N^+_2$ cores are accessed by the resonant absorption of near-infrared photons. We show that these resonances apply different filters to the observation of the vibrational wave packet, which results in different phases and amplitudes of the oscillating photoelectron signal depending on the nature of the autoionizing resonance. This work clarifies the importance of resonances in time-resolved photoelectron spectroscopy and particularly reveals the phase of vibrational quantum beats as a powerful observable for characterizing the properties of such resonances.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Coherent Transfer of Lattice Entropy via Extreme Nonlinear Phononics in Metal Halide Perovskites

Entropy transfer in metal halide perovskites, characterized by significant lattice anharmonicity and low stiffness, underlies the remarkable properties observed in their optoelectronic applications, ranging from solar cells to lasers. The conventional view of this transfer involves stochastic processes occurring within a thermal bath of phonons, where the lattice arrangement and energy flow from higher- to lower-frequency modes. Here, we unveil a comprehensive chronological sequence detailing a conceptually distinct coherent transfer of entropy in a prototypical perovskite CH 3 NH 3 Pbl 3 . The terahertz periodic modulation imposes vibrational coherence into electronic states, leading to the emergence of mixed (vibronic) quantum beat between approximately 3 and 0.3 THz. We highlight a well-structured bidirectional time-frequency transfer of these diverse phonon modes, each developing at different times and transitioning from high to low frequencies from 3 to 0.3 THz, before reversing direction and ascending to around 0.8 THz. First-principles molecular dynamics simulations disentangle a complex web of coherent-phononic coupling pathways and identify the salient roles of the initial modes in shaping entropy evolution at later stages. Capitalizing on coherent entropy transfer and dynamic anharmonicity presents a compelling opportunity to exceed the fundamental thermodynamic (Shockley-Queisser) limit of photoconversion efficiency and to pioneer novel optoelectronic functionalities. Published by the American Physical Society 2024

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Theoretical analysis of the role of complex transition dipole phase in XUV transient-absorption probing of charge migration

We theoretically investigate the role of complex dipole phase in the attosecond probing of charge migration. The iodobromoacetylene ion (ICCBr + ) is considered as an example, in which one can probe charge migration by accessing both the iodine and bromine ends of the molecule with different spectral windows of an extreme-ultraviolet (XUV) pulse. The analytical expression for transient absorption shows that the site-specific information of charge migration is encoded in the complex phase of cross dipole products for XUV transitions between the I-4 d and Br-3 d spectral windows. Ab-initio quantum chemistry calculations on ICCBr + reveal that there is a constant π phase difference between the I-4 d and Br-3 d transient-absorption spectral windows, irrespective of the fine-structure energy splittings. Transient absorption spectra are simulated with a multistate model including the complex dipole phase, and the results correctly reconstruct the charge-migration dynamics via the quantum beats in the two element spectral windows, exhibiting out-of-phase oscillations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Probing ultrafast excited-state dynamics using EUV-IR six-wave-mixing emission spectroscopy

Non-linear processes such as four-wave-mixing have become instrumental in attosecond EUV spectroscopy. Using EUV high harmonics in conjunction with collinear near-infrared and mid-infrared fields, we extended this approach to high-order-mixing between three colors. Specifically, we find that atomic resonances in neon exhibit a significant cross section for six-wave mixing. The MIR probe frequency tunability in our multicolor scheme is employed to access several optically dark resonances and probe the quantum beat of a coherent electronic wavepacket using background-free EUV emission as a diagnostic. This technique can be easily extended to other atomic and molecular systems, and opens the door to multi-dimensional non-linear spectroscopy.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2026

Time-domain terahertz emission spectroscopy on van der Waals materials

Time-domain terahertz (THz) emission spectroscopy provides a direct method to probe transient photo-currents by recording the emitted terahertz electric field. Although the basic principles of THz surface emission have been understood for more than 30 years, the constant progress in ultrafast laser science to ever shorter pulses, the development of new materials and enhanced sensitivity promote THz emission spectroscopy as a reliable method to gain insights into charge carrier dynamics with unprecedented precision. It provides a versatile tool to study ultrafast processes, such as plasmon-driven hot carriers, dynamics of Dirac fermions, interfacial charge transfer, coherent phonon emission and quantum beating, to name only a few. However, despite the rapidly growing body of research on van der Waals materials, especially in their low-dimensional limit, THz emission spectroscopy has only been applied to a limited extent in these material systems. In this prospective, we review time-domain THz emission spectroscopy as a complementary approach to probe ultrafast charge carrier dynamics and the material’s nonlinear response. After a description of the experimental method, we report on THz emission spectroscopy of bulk and 2D van der Waals materials with special focus on graphene and transition metal dichalcogenide layers.

2D materials↗
DOE OSTI2025

Entanglement-enhanced ac magnetometry in the presence of Markovian noise

Entanglement is a resource to improve the sensitivity of quantum sensors. In an ideal case, using an entangled state as a probe to detect target fields, we can beat the standard quantum limit by which all classical sensors are bounded. However, since entanglement is fragile against decoherence, it is unclear whether entanglement-enhanced metrology is useful in a noisy environment. Its benefit is indeed limited when estimating the amplitude of dc magnetic fields under the effect of parallel Markovian decoherence, where the noise operator is parallel to the target field. In this paper, on the contrary, we show an advantage to using an entanglement over the classical strategy under the effect of parallel Markovian decoherence when we try to detect ac magnetic fields. We consider a scenario to induce a Rabi oscillation of the qubits with the target ac magnetic fields. Although we can, in principle, estimate the amplitude of the ac magnetic fields from the Rabi oscillation, the signal becomes weak if the qubit frequency is significantly detuned from the frequency of the ac magnetic field. We show that, by using the Greenberger-Horne-Zeilinger (GHZ) states, we can significantly enhance the signal of the detuned Rabi oscillation even under the effect of parallel Markovian decoherence. Further, our method is based on the fact that the interaction time between the GHZ states and ac magnetic fields scales as 1/L to mitigate the decoherence effect, where L is the number of qubits, which contributes to improving the bandwidth of the detectable frequencies of the ac magnetic fields. Our results pave the way for new applications of entanglement-enhanced ac magnetometry.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Dynamical quantum phase transitions in interacting atomic interferometers

Particle-wave duality has allowed physicists to establish atomic interferometers as celebrated complements to their optical counterparts in a broad range of quantum devices. In particular, interactions give rise to multiparticle correlations unavailable in linear interferometers. Here, we show that interactions lead to dynamical quantum phase transitions (DQPTs) between NOON states in an atomic interferometer. These transition points result from zeros of the Loschmidt echo, which approach the real axis of the complex time plane in the large-particle-number limit, and signify pair condensates, another type of exotic quantum states featured with prevailing two-body correlations. Such DQPTs thus provide us with a new angle to understand many-body states emergent from quantum nonequilibrium dynamics. Further, our work also suggests interacting atomic interferometers as a new tool for creating highly entangled states to beat the standard quantum limit.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

Comparison of quantum advantage experiments using random circuit sampling

Random circuit sampling, the task of sampling bit strings from a random unitary operator, has been implemented to demonstrate quantum advantage on the Sycamore quantum processor with 53 qubits and on the Zuchongzhi quantum processor with 56 and 61 qubits. Recently, it was claimed that classical computers using tensor network simulation could catch on to current noisy quantum processors for random circuit sampling. While the linear cross-entropy benchmark fidelity was used to certify all these claims, it may not capture statistical properties of outputs in detail. Here, we compare the bit strings sampled from classical computers using tensor network simulation by Pan et al. [F. Pan, K. Chen, and P. Zhang, Phys. Rev. Lett. 129, 090502 (2022)] and by Kalachev et al. [G. Kalachev, P. Panteleev, P. Zhou, and M.-H. Yung, arXiv:2112.15083] with the bit strings from the Sycamore quantum processor. It is shown that all of Kalachev et al.'s samples passed the NIST random number tests. The heat maps of bit strings show that Pan et al.'s and Kalachev et al.'s samples are quite different from the Sycamore or Zuchongzhi samples. The analysis with the Marchenko-Pastur distribution and the Wasssertein distances demonstrates that Kalachev et al.'s samples are statistically closer to the Sycamore samples than Pan et al.'s while the three datasets have similar values for the linear cross-entropy fidelity. In conclusion, our finding implies that further study is needed to certify or beat the claims of quantum advantage using random circuit sampling.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Real-time quantum error correction beyond break-even

The ambition of harnessing the quantum for computation is at odds with the fundamental phenomenon of decoherence. The purpose of quantum error correction (QEC) is to counteract the natural tendency of a complex system to decohere. This cooperative process, which requires participation of multiple quantum and classical components, creates a special type of dissipation that removes the entropy caused by the errors faster than the rate at which these errors corrupt the stored quantum information. Previous experimental attempts to engineer such a process faced an excessive generation of errors that overwhelmed the error-correcting capability of the process itself. Whether it is practically possible to utilize QEC for extending quantum coherence thus remains an open question. We answer it by demonstrating a fully stabilized and error-corrected logical qubit whose quantum coherence is significantly longer than that of all the imperfect quantum components involved in the QEC process, beating the best of them with a coherence gain of G=2.27±0.07. Here we achieve this performance by combining innovations in several domains including the fabrication of superconducting quantum circuits and model-free reinforcement learning.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Quantum Super-resolution Bioimaging using Massively Entangled Multimode Squeezed Light

This report presents a new method for realizing a super-resolution quantum imaging using massively entangled multimode squeezed light (MEMSL). Each branch of the entangled multimode light interacts with the sample and bears the spatially varying optical phase delay. When imaging optics with finite pupil sizes are used, information is lost. Thanks to the analyticity in the Fourier plane, a noiseless measurement would recover the lost information and accomplish super resolution imaging beating the Rayleigh diffraction limit. I proved rigorously in a fully quantum formalism and presented that (1) such information recovery is possible and (2) the information recovery can be accomplished with much less resources when MEMSL is used than those needed in any non-entangled or non-squeezed classical imaging method. Furthermore, the action of the optical loss in the imaging system that degrades the imaging performance is also rigorously analyzed and presented. Several bioimaging applications that can benefit tremendously from the proposed quantum imaging scheme are also suggested.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

A Reference Implementation for a Quantum Message Passing Interface

Practical applications of quantum computing are currently limited by the number of qubits that can be set with reasonable fidelities for each system. Therefore, a distributed quantum computing system with multiple quantum computers coherently connected is highly demanding. To realize the internode communication of quantum information, the software interface, Quantum Message Passing Interface (QMPI), leveraging the framework built for classical MPI but taking advantage of quantum teleportation to communicate between different quantum nodes was proposed. In this project, we develop the QMPI with point-to-point and collective operations in Qiskit and characterize its performance by demonstrating the application implementations. Moreover, we developed a new technique for optimizing collective communication of the distributed quantum programs with Multi-Controlled Toffoli gates. This technique beats the state-of-the-art in terms of fidelity and the number of remote EPR pairs consumed in both simulations and experiments.

Shi, Yue↗
DOE OSTI2026

Phase-Dependent Squeezing in Dual-Comb Interferometry

Manipulating the quantum noise of continuous-wave lasers through squeezing has reshaped optical interferometry. However, progress in optical frequency comb interferometry with pulsed squeezed sources has been limited, despite the role of frequency combs in ultraprecise optical metrology. Here, we introduce a new time-domain approach to characterizing squeezed femtosecond light pulses using dual-comb interferometry. Time-domain interferograms are generated via multiheterodyne beating between the modes of a Kerr soliton-squeezed frequency comb and a coherent state comb. The interferogram noise reveals phase-dependent squeezing and antisqueezing, dipping as much as 3.8 ± 0.2 dB below the shot noise level at alternating zero crossings. We model this nonstationary quantum noise as a periodic optical displacement of the squeezed comb by the coherent comb. These results support a route toward quantum-enhanced dual-comb timing applications and high-speed quantum state tomography with dual-comb interferometers.

Herman, Daniel Issac [University of Colorado, Boul↗
DOE OSTI2022

Sensing ultrashort electronic coherent beating at conical intersections by single-electron pulses

In a theoretical study, we present an ultrafast technique for probing time-dependent molecular charge densities. An ultrafast optical pump first brings the molecule into an electronic nonstationary state. This is followed by coherent inelastic scattering of a broadband single-electron probe pulse with a variable delay T, which is detected spectrally. The technique is applied to reveal phase-sensitive background-free coherent electron beating in the conical intersection passage in uracil and reveals the otherwise elusive coherent beating of strongly coupled electrons and nuclei.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗