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At least 163 records · Page 9

Laser-Induced Enhancement of Acoustic Mode Quality Factor Revealed by Correlated Single-Particle Optical and Electron Microscopy

Acoustic modes in plasmonic nanostructures provide fundamental insights into their optomechanical behavior at the nanoscale, enabling emerging applications in plasmon-enhanced optomechanics, ultrasensitive sensing, and nanoscale energy transduction. Here we explore the modulation of acoustic phonon dynamics in lithographically fabricated gold nanodisks via laser-induced photothermal annealing. Using a correlated approach that utilizes both single-particle transient extinction spectroscopy and advanced electron microscopy, we directly link nanoscale structural transformations to changes in mechanical properties as probed through the coherence of the excited acoustic modes. Specifically, ultrafast pump–probe microscopy reveals an enhancement in the acoustic mode quality factor of annealed gold nanodisks, indicative of reduced damping and improved vibrational coherence. Structural characterization via scanning electron microscopy and electron backscatter diffraction confirms that photoinduced annealing results in smoother surface morphology and overall enhanced crystallinity. The improved crystalline order reduces defect and crystal boundary scattering, which we suggest as the reason underlying the lower quality factor before annealing. Furthermore, these findings demonstrate that targeted structural engineering at the nanoscale offers a powerful strategy for optimizing the optomechanical performance of plasmonic nanostructures, with broad implications for the design of next-generation nanophotonic and optomechanical systems.

Annealing (metallurgy)↗

An intense, few-cycle source in the long-wave infrared

For the last several decades, the wavelength range accessible for strong-field, few-cycle studies has remained limited to the visible, near infrared and mid-wave infrared regimes. In particular, sources in the long-wave infrared have been lacking. We report the development of a 1 kHz, few-cycle laser source with up to a 9 μm central wavelength and gigawatt peak powers. When focused, this source can ionize gas targets, which we demonstrate here through the ionization of atomic xenon at wavelengths ranging from 5 μm to 9 μm. This opens up new opportunities for fundamental atomic and molecular physics, enabling experimental tests of strong-field ionization theories in the extreme long-wavelength, few-cycle limit and the direct excitation of vibrational transitions in organic molecules.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Sub-cycle Oscillations in Virtual States Brought to Light

Understanding and controlling the dynamic evolution of electrons in matter is among the most fundamental goals of attosecond science. While the most exotic behaviors can be found in complex systems, fast electron dynamics can be studied at the fundamental level in atomic systems, using moderately intense (≲10 13 W/cm 2 ) lasers to control the electronic structure in proof-of-principle experiments. Here, we probe the transient changes in the absorption of an isolated attosecond extreme ultraviolet (XUV) pulse by helium atoms in the presence of a delayed, few-cycle near infrared (NIR) laser pulse, which uncovers absorption structures corresponding to laser-induced “virtual” intermediate states in the two-color two-photon (XUV+NIR) and three-photon (XUV+NIR+NIR) absorption process. These previously unobserved absorption structures are modulated on half-cycle (~1.3 fs ) and quarter-cycle (~0.6 fs ) timescales, resulting from quantum optical interference in the laser-driven atom.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Monte Carlo study for optimal conditions in single-shot imaging with femtosecond x-ray laser pulses

Intense x-ray pulses from x-ray free electron lasers (XFELs) enable the unveiling of atomic structure in material and biological specimens via ultrafast single-shot exposures. As the radiation is intense enough to destroy the sample, a new sample must be provided for each x-ray pulse. These single-particle delivery schemes require careful optimization, though systematic study to find such optimal conditions is still lacking. We have investigated two major single-particle delivery methods: particle injection as flying objects and membrane-mount as fixed targets. The optimal experimental parameters were searched for via Monte Carlo simulations to discover that the maximum single-particle hit rate achievable is close to 40%.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Large-scale atomistic calculations of clusters in intense x-ray pulses

Here, we present the methodology of our recently developed Monte-Carlo/ Molecular-Dynamics method for studying the fundamental ultrafast dynamics induced by high-fluence, high-intensity x-ray free electron laser (XFEL) pulses in clusters. The quantum nature of the initiating ionization process is accounted for by a Monte Carlo method to calculate probabilities of electronic transitions, including photo absorption, inner-shell relaxation, photon scattering, electron collision and recombination dynamics, and thus track the transient electronic configurations explicitly. The freed electrons and ions are followed by classical particle trajectories using a molecular dynamics algorithm. These calculations reveal the surprising role of electron-ion recombination processes that lead to the development of nonuniform spatial charge density profiles in x-ray excited clusters over femtosecond timescales. In the high-intensity limit, it is important to include the recombination dynamics in the calculated scattering response even for a 2- fs pulse. We also demonstrate that our numerical codes and algorithms can make e!cient use of the computational power of massively parallel supercomputers to investigate the intense-field dynamics in systems with increasing complexity and size at the ultrafast timescale and in non-linear x-ray interaction regimes. In particular, picosecond trajectories of XFEL clusters with attosecond time resolution containing millions of particles can be e!ciently computed on upwards of 262,144 processes.

74 ATOMIC AND MOLECULAR PHYSICS↗

State-resolved ultrafast charge and spin dynamics in [Co/Pd] multilayers

We use transient absorption spectroscopy with circularly polarized x rays to detect laser-excited hole states below the Fermi level and compare their dynamics with that of unoccupied states above the Fermi level in ferromagnetic [Co/Pd] multilayers. While below the Fermi level, an instantaneous and significantly stronger demagnetization is observed, above the Fermi level, the demagnetization is delayed by 35 ± 10 fs. This provides a direct visualization of how ultrafast demagnetization proceeds via initial spin-flip scattering of laser-excited holes to the subsequent formation of spin waves.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Manipulating and Probing Ultrafast Atomic and Molecular Dynamics (Final Report)

This program has focused on the exploration and control of dynamics in atoms, small molecules, clusters, and micro- or nano-structures following ultrafast excitation and/or driven by strong oscillating fields. In our principal experiments, gas phase atoms and molecules were exposed to short pulses of electromagnetic radiation with frequencies ranging from THz into the XUV spectral regions, and with durations from picoseconds to attoseconds. The pulses coherently induce and/or probe dynamics in the electronic, vibrational, and rotational degrees of freedom of the targets. The overarching goal of the various projects has been to exploit strong-field processes and/or implement novel ultrafast techniques for manipulating and probing coherent electronic and nuclear motion. Typically, the relevant system evolution occurs over attosecond to picosecond timescales. In doing so, we have gained a more complete picture of correlated multi-particle dynamics in atoms, molecules, and other complex systems and expanded the toolbox of useful techniques for manipulating and probing those dynamics. Grant funds were primarily used to: (i) pay salaries and fringe benefits for the PI and postdocs and stipends, tuition, and health care costs for graduate students; (ii) cover travel expenses for the PI, postdocs, and students to attend and participate in professional meetings, conferences, and workshops; and (iii) purchase research materials, supplies, and equipment required for experiments. The research resulted in the publication of 24 peer reviewed articles (including 1 in Nature Physics, 2 in Nature Communications, 7 in Physical Review Letters, and 12 in Physical Review A), and 4 PhD dissertations. The specific results from different funding periods are summarized separately in the main report.

74 ATOMIC AND MOLECULAR PHYSICS↗

Measuring the scintillation decay time for different energy deposited by γ-rays and neutrons in a Cs 2 LiYCl 6 :Ce 3+ detector

In nuclear safeguards and homeland security applications, it is greatly beneficial to simultaneously detect γ-rays, thermal neutrons, and fast neutrons using a single detector with reasonable pulse shape discrimination capability, energy resolution comparable with or even better than NaI(Tl) detectors, and high detection efficiency. Cs 2 LiYCl 6 :Ce 3+ detector (CLYC) scintillation detectors have been proven to be one promising candidate to meet these requirements. In this work, the decay time and fraction of each scintillation component for different energy deposition and incident particle type (γ-ray, thermal neutron, and fast neutron) were investigated based on fitting the PMT anode output with exponential functions. For γ-rays, four components were determined with ultrafast decay time of less than one nanosecond and slow time in the order of magnitude of microsecond. It was found that the dependence on the energy deposited by γ-rays of the fraction as well as the decay time of the three slow components was small. However, significant dependence was observed for the ultrafast component. Two or three components were determined for thermal neutrons and fast neutrons without observing a component with fast decay time. To verify the approach used it was first applied to scintillation pulses induced by γ-rays in a NaI(Tl) detector. We found the results were consistent with well-known data already published in the literature.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Time delay measurement in the frequency domain

Pump–probe studies at synchrotrons using X-ray and laser pulses require accurate determination of the time delay between pulses. This becomes especially important when observing ultrafast responses with lifetimes approaching or even less than the X-ray pulse duration (~100 ps). The standard approach of inspecting the time response of a detector sensitive to both types of pulses can have limitations due to dissimilar pulse profiles and other experimental factors. Here, a simple alternative is presented, where the frequency response of the detector is monitored versus time delay. Measurements readily demonstrate a time resolution of ~1 ps. Improved precision is possible by simply extending the data acquisition time.

43 PARTICLE ACCELERATORS↗

Theory of time-resolved Raman scattering in correlated systems: Ultrafast engineering of spin dynamics and detection of thermalization

Ultrafast characterization and control of many-body interactions and elementary excitations are critical to understanding and manipulating emergent phenomena in strongly correlated systems. In particular, spin interaction plays an important role in unconventional superconductivity, but efficient tools for probing spin dynamics, especially out of equilibrium, are still lacking. To address this question, we develop a theory for nonresonant time-resolved Raman scattering, which can be a generic and powerful tool for nonequilibrium studies. We also use exact diagonalization to simulate the pump-probe dynamics of correlated electrons in the square-lattice single-band Hubbard model. Different ultrafast processes are shown to exist in the time-resolved Raman spectra and dominate under different pump conditions. For high-frequency and off-resonance pumps, we show that the Floquet theory works well in capturing the softening of bimagnon excitation. By comparing the Stokes and anti-Stokes spectra, we also show that effective heating dominates at small pump fluences, while a coherent many-body effect starts to take over at larger pump amplitudes and frequencies on resonance to the Mott gap. In conclusion, time-resolved Raman scattering thereby provides the platform to explore different ultrafast processes and design material properties out of equilibrium.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Low-Rate Cycling Regeneration Sustains NMC811–Graphite Battery Performance through Extreme Ultrafast Charging

Urban air mobility (UAM) systems, such as electric vertical takeoff and landing (eVTOL) aircraft, require batteries capable of extreme ultrafast charging to support high-frequency operations. Here, in this work, we evaluate the electrochemical stability of NMC811–graphite full cells using a complex mixed-modal protocol designed to simulate the aggressive turnaround demands of UAM missions. We demonstrate that incorporating a periodic low-rate (0.3C) “regeneration” cycle enables cells to maintain 96% capacity retention over 900 cycles, despite repeated exposure to ultrafast pulses. To validate the efficacy of this regeneration mechanism, we performed simplified control experiments comparing continuous 10C charging against a 10C–0.3C interleaved protocol. Advanced characterization reveals that while mechanical particle fracture is pervasive at these rates, the regeneration cycles decelerate the electrochemical degradation by resolving spatially heterogeneous Ni oxidation states and relaxing lithium-ion concentration gradients. These findings provide a vital mechanistic framework for battery operation, proving that restorative charging can effectively delay and mitigate failure in demanding UAM applications.

batteries↗

Attosecond x-ray free-electron lasers utilizing an optical undulator in a self-selection regime

Accelerator-based x-ray free-electron lasers (XFELs) are the latest addition to the revolutionary tools of discovery for the 21st century. The two major components of an XFEL are an accelerator-produced electron beam and a magnetic undulator, which tend to be kilometer-scale long and expensive. A proof-of-principle demonstration of free-electron lasing at 27 nm using beams from compact laser wakefield accelerators was shown recently by using a magnetic undulator. However, scaling these concepts to x-ray wavelengths is far from straightforward as the requirements on the beam quality and jitters become much more stringent. Here, we present an ultracompact scheme to produce tens of attosecond x-ray pulses with several GW peak power utilizing a novel aspect of the FEL instability using a highly chirped, prebunched, and ultrabright tens of MeV electron beam from a plasma-based accelerator interacting with an optical undulator. The FEL resonant relation between the prebunched period and the energy selects resonant electrons automatically from the highly chirped beam which leads to a stable generation of attosecond x-ray pulses. Furthermore, two-color attosecond pulses with subfemtosecond separation can be produced by adjusting the energy distribution of the electron beam so that multiple FEL resonances occur at different locations within the beam. Such a tunable coherent attosecond x-ray sources may open up a new area of attosecond science enabled by x-ray attosecond pump/probe techniques. Published by the American Physical Society 2024

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Opportunities in Intense Ultrafast Lasers: Reaching for the Brightest Light

The laser has revolutionized many areas of science and society, providing bright and versatile light sources that transform the ways we investigate science and enables trillions of dollars of commerce. Now a second laser revolution is underway with pulsed petawatt-class lasers (1 petawatt: 1 million billion watts) that deliver nearly 100 times the total world’s power concentrated into a pulse that lasts less than one-trillionth of a second. Such light sources create unique, extreme laboratory conditions that can accelerate and collide intense beams of elementary particles, drive nuclear reactions, heat matter to conditions found in stars, or even create matter out of the empty vacuum. These powerful lasers came largely from U.S. engineering, and the science and technology opportunities they enable were discussed in several previous National Academies’ reports. Based on these advances, the principal research funding agencies in Europe and Asia began in the last decade to invest heavily in new facilities that will employ these high-intensity lasers for fundamental and applied science. No similar programs exist in the United States. Opportunities in Intense Ultrafast Lasers assesses the opportunities and recommends a path forward for possible U.S. investments in this area of science.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

New insights into the mechanism of ultrasonic atomization for the production of metal powders in additive manufacturing

Ultrasonic atomization is one of the promising technologies for producing metal powders for additive manufacturing, where precise control of particle size and morphology is essential. In this study, we coupled an ultrasonic transducer with a carbon fiber plate and atomized liquid droplets and films under different vibration amplitudes. Water, glycerol, and pure aluminum melt were used to study the atomization mechanism and the resulting droplet/powder characteristics, respectively. High-speed optical and ultrafast synchrotron X-ray imaging were used to study in situ the ultrasonic atomization dynamics, including pulsation and clustering of cavities inside the liquid layer/films, development of capillary waves, and formation of liquid droplets. For the first time, we observed and captured the occurrence of cavitation during the atomization of resting drops, films and impact droplets. The inertial cavitation events interfered with the capillary waves across the interphase boundary, puncturing and breaking the boundary to produce atomized mist. The in situ observation revealed the intricate dynamics of ultrasonic atomization and underscored the pivotal role of cavitation events throughout the entire atomization process. We also conducted experiments on ultrasonic atomization of liquid aluminum, producing particles of perfectly spherical shape. The particle size tended to decrease with reduced vibration amplitude Our work has demonstrated the important processing strategies on how to tailor the particle size while ensuring consistent particle shape and morphology, which is the key processing capability for producing high quality powders for additive manufacturing applications.

36 MATERIALS SCIENCE↗

Kinetics of Magnetic Skyrmion Crystal Formation from the Conical Phase

The particle-like magnetic skyrmion or skyrmion lattice (SkX) formation has promoted strong application and fundamental science interests. Despite extensive research, the kinetic of the SkX development is much less understood because of the ultrafast spin rotation and high sensitivity to external perturbations. In this work, using in situ Lorentz transmission electron microscopy, we successfully measured the dynamics of SkX formation from the conical phase with precise control of both the temperature and the magnetic field. We discovered that the Avrami equation can accurately describe the transition process with an initial Avrami constant around 1, suggesting that the rate-limiting step for the quasiparticle lattice formation is one-dimensional heterogeneous nucleation of individual skyrmions. A modified Arrhenius rate law is established, with an energy barrier that has a square-root dependence on temperature and a quadratic dependence on the magnetic field. This study paves the way toward precise and predictable manipulation of topological spin structures.

36 MATERIALS SCIENCE↗

350 ps Ultrafast room-temperature scintillation realized on CsPbBr 3 -based single crystals via Br 2 over-doping

Ultrafast scintillators are essential for next-generation radiation detection, positron emission tomography, and high-speed medical imaging. All-inorganic CsPbBr 3 perovskites are attractive candidates because of their high stopping power, and excellent optical quality, yet their long carrier lifetimes result in slow scintillation responses on the order of hundreds of nanoseconds. Here, we demonstrate that controlled over-doping with Br 2 produces CsPbBr 3.03 single crystals with sub-nanosecond scintillation at room temperature while preserving crystal quality. Single crystals grown by the Bridgman method exhibit high transparency and maintain the orthorhombic perovskite structure. Br 2 over-doping induces a slight lattice expansion (about 0.42% increase in unit-cell volume) while maintaining the orthorhombic perovskite phase and high optical transparency. Optical absorption reveals a slight redshift of the absorption edge after Br 2 introduction, indicating a modified defect landscape. Time-resolved photoluminescence and radioluminescence measurements show that Br 2 doping creates dense and efficient recombination centers that reduce the scintillation decay time from more than 100 ns in undoped crystals to 350 ps under 5.486 MeV α-particle excitation, and the scintillation decay time decreases by two orders of magnitude. The doped crystals also achieve a spatial resolution of 12 lp mm −1 in X-ray imaging. These results reveal a defect-engineering route for achieving ultrafast scintillation in halide perovskites and highlight the potential of Br 2 -modified CsPbBr 3 for fast timing applications.

Li, Zongxiao [Chinese Academy of Sciences (CAS), N↗

Third-order nonlinear optical response of colloidal gold nanoparticles prepared by sputtering deposition

The nonlinear optical responses of gold nanoparticles dispersed in castor oil produced by sputtering deposition were investigated, using the thermally managed Z-scan technique. Particles with spherical shape and 2.6 nm of average diameter were obtained and characterized by transmission electron microscopy and small angle X-ray scattering. This colloid was highly stable, without the presence of chemical impurities, neither stabilizers. It was observed that this system presents a large refractive third-order nonlinear response and a negligible nonlinear absorption. Moreover, the evaluation of the all-optical switching figures of merit demonstrated that the colloidal nanoparticles prepared by sputtering deposition have a good potential for the development of ultrafast photonic devices.

36 MATERIALS SCIENCE↗