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At least 37 records · Page 2

Broadband sum-frequency generation of spectrally incoherent pulses

We study and demonstrate the nonlinear frequency conversion of broadband optical pulses from 1053 nm to 351 nm using sum-frequency generation with a narrowband pulse at 526.5 nm. The combination of angular dispersion and noncollinearity cancels out the wave-vector mismatch and its frequency derivative, yielding an order-of-magnitude increase in spectral acceptance compared to conventional tripling. This scheme can support the nonlinear frequency conversion of broadband spectrally incoherent nanosecond pulses generated by high-energy lasers and optical parametric amplifiers to mitigate laser−plasma instabilities occurring during interaction with a target. The experimental results obtained with KDP crystals are in excellent agreement with modeling, demonstrating the generation of spectrally incoherent pulses with a bandwidth larger than 10 THz at 351 nm.

47 OTHER INSTRUMENTATION↗

Femtosecond ultraviolet laser absorption spectroscopy for simultaneous measurements of temperature and OH concentration

This Letter reports a femtosecond ultraviolet laser absorption spectroscopy (fs-UV-LAS) for simultaneous in situ measurements of temperature and species. Here, this fs-UV-LAS technique was demonstrated based on X 2 Π-A 2 Σ + transitions of OH radicals near 308 nm generated in low temperature plasmas and flames. The fs-UV-LAS technique has revealed three major diagnostic benefits. First, a series of absorption features within a spectral bandwidth of ~3.2 nm near 308 nm were simultaneously measured and then enabled simultaneous multi-parameter measurements with enhanced accuracy. The results show that the temperature and OH concentration could be measured with accuracy enhanced by 29–88% and 58–91%, respectively, compared to those obtained with past two-narrow-line absorption methods. Second, an ultrafast time resolution of ~120 picoseconds was accomplished for the measurements. Third, due to the large OH X 2 Π-A 2 Σ + transitions in the UV range, a simple single-pass absorption with a 3-cm path length was allowed for measurements in plasmas with low OH number density down to ~2 × 10 13 cm –3 . Also due to the large OH UV transitions, single-shot fs absorption measurements were accomplished in flames, which was expected to offer more insights into chemically reactive flow dynamics.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Atomistically resolved hot exciton relaxation dynamics in CdSe quantum dots: Experiment and theory

Semiconductor quantum dots (QDs) are well known to give rise to a quantum confined structure of excitons. Because of this quantum confinement, new physics of hot exciton relaxation dynamics arises. Decades of work using transient absorption (TA) spectroscopy have yielded initial simple observations, such as estimates of the cooling rate from single pump photon energy experiments. More detailed TA experiments employed variable pump photon energies to measure excitonic state-resolved transition rates. These TA measurements, usually the simplest form, have been employed to characterize QDs and their relaxation dynamics to this day. Yet, these TA measurements are fundamentally lacking in their ability to measure energy-resolved hot exciton cooling, which requires observation of the full cooling history through the real excitonic manifold. Here, we employ coherent multi-dimensional spectroscopy (CMDS) to perform an atomistically directed study of hot exciton cooling in CdSe QDs, revealing energy resolved relaxation dynamics. CMDS experiments are compared with simulations and prior TA measurements and simpler theories. Our findings reveal a hot exciton relaxation dynamics landscape. This relaxation dynamics landscape is a linear or sub-linear function of excess energy for different structures of QDs, with a strong size dependence. Our model simulations parameterized by the empirical pseudopotential model reproduces the experimental functional form and the dependence upon QD diameter and shell.

Atomistic simulations↗

Nonlinear quantum behavior of ultrashort-pulse optical parametric oscillators

The quantum features of ultrashort-pulse optical parametric oscillators (OPOs) are investigated theoretically in the nonlinear regime near and above threshold. Viewing the pulsed OPO as a multimode open quantum system, we rigorously derive a general input-output model that features nonlinear coupling among many cavity (i.e., system) signal modes and a broadband single-pass (i.e., reservoir) pump field. Under appropriate assumptions, our model produces a Lindblad master equation with multimode nonlinear Lindblad operators describing two-photon dissipation and a multimode four-wave-mixing Hamiltonian describing a broadband, dispersive optical cascade, which we show is required to preserve causality. To simplify the multimode complexity of the model, we employ a supermode decomposition to perform numerical simulations in the regime where the pulsed supermodes experience strong single-photon nonlinearity. We find that the quantum nonlinear dynamics induces pump depletion as well as corrections to the below-threshold squeezing spectrum predicted by linearized models. We also observe the formation of non-Gaussian states with Wigner-function negativity and show that the multimode interactions with the pump, both dissipative and dispersive, can act as effective decoherence channels. Finally, we briefly discuss some experimental considerations for potentially observing such quantum nonlinear phenomena with ultrashort-pulse OPOs on nonlinear nanophotonic platforms.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

49 W carrier-envelope-phase-stable few-cycle 2.1 µm OPCPA at 10 kHz

We demonstrate a mid-infrared optical parametric chirped pulse amplifier (OPCPA), delivering 2.1 µm center wavelength pulses with 20 fs duration and 4.9 mJ energy at 10 kHz repetition rate. This self-seeded system is based on a kW-class Yb:YAG thin-disk amplifier driving a CEP stable short-wavelength-infrared (SWIR) generation and three consecutive OPCPA stages. Our SWIR source achieves an average power of 49 W, while still maintaining excellent phase and average power stability with sub-100 mrad carrier-envelope-phase-noise and 0.8% average power fluctuations. These parameters enable the OPCPA setup to drive attosecond pump probe spectroscopy experiments with photon energies in the water window.

47 OTHER INSTRUMENTATION↗

Quantum Versus Classical Switching Dynamics of Driven Dissipative Kerr Resonators

Here, we report a first-principles study of the driven dissipative dynamics for Kerr oscillators in the mesoscopic regime. This regime is characterized by large Kerr nonlinearity, realized here using the nonlinear kinetic inductance of a large array of Josephson junctions. The experimentally measured nonlinear resonance lineshapes of the junction array modes show significant deviations from steady-state numerical predictions, and necessitate time-dependent numerical simulations indicative of strong measurement-induced dephasing in the system arising from the large cross-Kerr effect between array modes. Analytical and numerical calculations of switching rate corroborate this by showing the emergence of a slow time scale, which is much longer than the linear decay rate and is set by fluctuation-induced switching times in the bistable regime. Furthermore, our analysis shows that the usual quantum-activated escape treatment is inadequate for prediction of the switching rates at large frequency shifts caused by strong nonlinearities, necessitating a quantum treatment that utilizes the full system Liouvillian. Based on our analysis, we identify a universal crossover parameter that delineates the regimes of validity of semiclassical and quantum descriptions, respectively. Our work shows how dynamical switching effects in strongly nonlinear systems provide a platform to study quantum-to-classical transitions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Parametric amplification of spin-motion coupling in three-dimensional trapped-ion crystals

Three-dimensional (3D) crystals offer a route to scaling up trapped-ion systems for quantum sensing and quantum simulation applications; however, engineering coherent spin-motion couplings and effective spin-spin interactions in large crystals poses technical challenges associated with decoherence and prolonged timescales to generate appreciable entanglement. Here, we explore the possibility of speeding up these interactions in 3D crystals via parametric amplification. For this purpose, we derive a general Hamiltonian for the parametric amplification of spin-motion coupling that is broadly applicable to normal modes with motion transverse to or along the spatial extent of the crystal. Unlike in lower-dimensional crystals, we find that the ability to faithfully (uniformly) amplify the spin-spin interactions in 3D crystals depends on the physical implementation of the spin-motion coupling. We consider the light-shift gate, and the so-called phase-insensitive and phase-sensitive Mølmer-Sørensen (MS) gates, and we find that only the phase-sensitive MS gate can be faithfully amplified in general 3D crystals. We discuss a situation where nonuniform amplification can be advantageous. We also reconsider the effect of counter-rotating terms on parametric amplification and find that they are not as detrimental as previous studies suggest.

Optical parametric oscillators & amplifiers↗

Long-wavelength-infrared laser filamentation in solids in the near-single-cycle regime

We experimentally demonstrate long-wavelength-infrared (LWIR) femtosecond filamentation in solids. Systematic investigations of supercontinuum (SC) generation and self-compression of the LWIR pulses assisted by laser filamentation are performed in bulk KrS-5 and ZnSe, pumped by ∼ <#comment/> 145 f s , 9 µm, 10 µJ pulses from an optical parametric chirped-pulse amplifier operating at 10 kHz of repetition rate. Multi-octave SC spectra are demonstrated in both materials. While forming stable single filament, 1.5 cycle LWIR pulses with 4.5 µJ output pulse energy are produced via soliton-like self-compression in a 5 mm thick KrS-5. The experimental results quantitatively agree well with the numerical simulation based on the unidirectional pulse propagation equation. This work shows the experimental feasibility of high-energy, near-single-cycle LWIR light bullet generation in solids.

Qu, Shizhen↗

A versatile high-average-power ultrafast infrared driver tailored for high-harmonic generation and vibrational spectroscopy

We report on an ultrafast infrared optical parametric chirped-pulse amplifier (OPCPA), pumped by a 200-W thin-disk Yb-based regenerative amplifier at a repetition rate of 100 kHz. The OPCPA is tunable in the spectral range 1.4–3.9 μm, generating up to 23 W of < 100-fs signal and 13 W of < 200-fs idler pulses for infrared spectroscopy, with additional spectral filtering capabilities for Raman spectroscopy. The OPCPA can also yield 19 W of 49-fs 1.75- μm signal or 5 W of 62-fs 2.8- μm idler pulses with active carrier-to-envelope-phase (CEP) stabilisation for high-harmonic generation (HHG). We illustrate the versatility of the laser design, catering to various experimental requirements for probing ultrafast science.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Enhancement of Parametric Effects in Polariton Waveguides Induced by Dipolar Interactions

Exciton-polaritons are hybrid light-matter excitations arising from the nonperturbative coupling of a photonic mode and an excitonic resonance. Behaving as interacting photons, they show optical third-order nonlinearities providing effects such as optical parametric oscillation or amplification. It has been suggested that polariton-polariton interactions can be greatly enhanced by inducing aligned electric dipoles in their excitonic part. However, direct evidence of a true particle-particle interaction, such as superfluidity or parametric scattering, is still missing. In this Letter, we demonstrate that dipolar interactions can be used to enhance parametric effects such as self-phase modulation in waveguide polaritons. By quantifying these optical nonlinearities, we provide a reliable experimental measurement of the direct dipolar enhancement of polariton-polariton interactions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

A highly efficient, 10-J output signal amplifier for ultra-intense all-OPCPA systems

Optical parametric chirped-pulse amplification (OPCPA) using high-energy Nd:glass lasers has the potential to produce ultra-intense pulses (>10 23 W/cm 2 ). We report on the performance of the final high-efficiency amplifier in an OPCPA system based on large-aperture (63 x 63-mm 2 ) partially deuterated potassium dihydrogen phosphate (DKDP) crystals. Here, the seed beam (170 nm, 240 mJ) was provided by the preceding OPCPA stages. The maximum pump-to-signal conversion efficiency of 37% was achieved with a 52-mm-long DKDP crystal and 40-J pump energy at 527 nm due to the flattop super-Gaussian pump beam profile and flat-in-time pulse shape. The 11.8-J output signal was compressed to 19 fs.

42 ENGINEERING↗

Octave-spanning mid-infrared femtosecond OPA in a ZnGeP 2 pumped by a 2.4 μm Cr:ZnSe chirped-pulse amplifier

We report on the highly efficient, octave-spanning mid-infrared (mid-IR) optical parametric amplification (OPA) in a ZnGeP 2 (ZGP) crystal, pumped by a 1 kHz, 2.4 μm, 250 fs Cr:ZnSe chirped-pulse amplifier. The full spectral coverage of 3−10 μm with the amplified signal and idler beams is demonstrated. The signal beam in the range of ∼3 − 5 μm is produced by either white light generation (WLG) in YAG or optical parametric generation (OPG) in ZGP using the common 2.4 μm pump laser. We demonstrate the pump to signal and idler combined conversion efficiency of 23% and the pulse energy of up to 130 μJ with ∼2 μJ OPG seeding, while we obtain the efficiency of 10% and the pulse energy of 55 μJ with ∼0.2 μJ WLG seeding. The OPA output energy is limited by the available pump pulse energy (0.55 mJ at ZGP crystal) and therefore further energy scaling is feasible with multi-stage OPA and higher pump pulse energy. The autocorrelation measurements based on random quasi-phase matching show that the signal pulse durations are ∼318 fs and ∼330 fs with WLG and OPG seeding, respectively. In addition, we show the spectrally filtered 30 μJ OPA output at 4.15 μm suitable for seeding a Fe:ZnSe amplifier. Our ultrabroadband femtosecond mid-IR source is attractive for various applications, such as strong-field interactions, dielectric laser electron acceleration, molecular spectroscopy, and medical surgery.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Amplification of 10 μm picosecond pulses in a compact optically pumped multiatmosphere CO 2 laser

Picosecond pulses, generated by a commercial mid-IR optical parametric source (∼0.5 ps, 1-5 μJ), have been regeneratively amplified to an energy of ≤2 mJ in a palm-size high-pressure CO 2 amplifier optically pumped by a Q-switched 2.8 μm Cr:Er:YSGG laser. The characteristics of the amplified pulses have been studied as a function of seed wavelength centered around 10.3 or 10.6 μm, and the pressure in the gain medium. The measured amplified pulse length is ∼5 ps. Numerical modeling suggests that pulses as short as ∼0.5 ps with multi-GW peak power can be generated in a mixture of CO 2 isotopes. Robustness of the output of a compact CO 2 regenerative amplifier to the seed and pump fluctuations measured at 3 Hz and a perfect Gaussian beam profile indicates the potential of such laser technology for producing high-power ultrashort long-wave infrared pulses at high repetition rates.

43 PARTICLE ACCELERATORS↗

Final amplifier of an ultra-intense all-OPCPA system with 13-J output signal energy and 41% pump-to-signal conversion efficiency

Optical parametric chirped-pulse amplification (OPCPA) using high-energy Nd:glass lasers has the potential to produce ultra-intense pulses (>10 23 W/cm 2 ). We report on the performance of the final high-efficiency amplifier in an OPCPA system based on large-aperture (63 × 63-mm 2 ) partially deuterated potassium dihydrogen phosphate (DKDP) crystals. The seed beam (180-nm bandwidth, 110 mJ) was provided by the preceding OPCPA stages. A maximum pump-to-signal conversion efficiency of 41% and signal energy up to 13 J were achieved with a 52-mm-long DKDP crystal due to the flattop super-Gaussian pump beam profile and flat-in-time pulse shape.

47 OTHER INSTRUMENTATION↗

Ytterbium laser system for studying parametric amplification of femtosecond pulses with a centre wavelength of ∼2 μm

A laser system is developed with an optical synchronisation of a femtosecond signal with a pump channel. The signal of a driving ytterbium fibre laser with a 60 MHz repetition rate of stretched femtosecond pulses is amplified in energy from several nanojoules to 0.4 mJ at a pulse repetition rate of 3 kHz in a wideband amplifier and then is compressed in time to 250 fs. The obtained radiation is used for generating femtosecond laser pulses with a centre wavelength of ∼2 μm, pulse energy of above 20 μJ, duration of several field oscillations, and phase stabilisation between the electromagnetic field and envelope. The other pulse of the driving fibre laser provides optical synchronisation and a minimal time delay and is directed to a regenerative Yb : YAG disk amplifier for amplification to an energy of 4 mJ at a pulse repetition rate of 3 kHz and duration of 20 ps. A multipass disk amplifier is developed for further increasing the energy of pump chirped pulses to an energy of 70 mJ at a pulse repetition rate of 10 Hz and duration of 400 ps for studying parametric amplification under sub-nanosecond pumping. (paper)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Optical parametric amplification of spectrally incoherent pulses

The optical parametric amplification of spectrally incoherent signals is analyzed and simulated using a set of normalized equations describing phase-matched three-wave nonlinear mixing. Varying the amplifier’s properties and the seeding conditions reveals different amplification regimes. In particular, the relative temporal walk-off of the signal, idler, and pump has a strong impact on the temporal and spectral properties of the amplified signal. The amplification efficiency for spectrally incoherent signals is not significantly lower than that of a coherent monochromatic signal, provided that the phase-matching bandwidth is sufficient. Here, the results obtained with the normalized set of equations are in good agreement with simulations based on the full description of the crystals’ dispersion for high-gain LBO and BBO preamplifiers and a low-gain DKDP power amplifier.

47 OTHER INSTRUMENTATION↗

Tunable Laser-Plasma Amplifier (Final Report)

Exploration at the laser intensity frontier has always offered new avenues for physics and reaching beyond this frontier is a grand challenge. Present-day petawatt-class lasers provide focused intensities on target of 10 22 W/cm 2 , corresponding to electric fields of 200 TV/m, while laser-plasma amplification opens a route for focused intensities well above 10 23 W/cm 2 . Intensities in this range provide the ability to test quantum electrodynamics in the unexplored low-energy, strong-field regime where signatures for new physics may arise. The behavior of matter under such extraordinary conditions is a rich and fascinating subject, not only in its own right in fundamental plasma physics, but for the many potential applications that promise to enrich the natural sciences in the future, including compact electron-beam, ion-beam particle accelerators, and ultra-bright X-ray sources. Although laser systems are now under construction internationally to access intensities of 10 23 W/cm 2 , the current technologies used appear to be fundamentally limited to these intensities. The realization of intensities beyond 10 23 W/cm 2 using parametric amplification in plasmas promises a breakthrough in high-energy density physics. Parametric amplification using Raman scattering in a plasma could provide the enabling technology for the generation of ultra-high-power laser pulses, but a more complete understanding of the nonlinear optics of plasmas is required. There is a significant gap in well-diagnosed laser-plasma instability studies of nonlinear plasma-wave phenomena, which are critical to understand for future laser-plasma devices. To achieve an efficient laser-plasma amplifier, plasma waves must be driven to large amplitude where significant energy can be rapidly transferred from the pump to the seed over the pulse duration of the seed. Simulations suggest that this nonlinear pump depletion regime can be achieved in the “pi-pulse” amplification regime. While simulations show this optimal regime with efficient amplification, it has remained elusive in experiments and there is a growing consensus within the community that thermal effects and pump beam limitations prevent laser-plasma amplifiers from progressing through the linear regime into the nonlinear pump depletion regime. Previous experiments have been significantly limited by the laser power available at the necessary wavelengths for the seed laser; therefore, the amplification is required to start in the linear regime where it is sensitive to many deleterious effects. The enabling technology (currently unique to plasma-wave amplification in the world) at the University of Rochester is the ability to provide a seed pulse with sufficient power (4 mJ/100 fs seed) to immediately drive nonlinear plasma waves into the pi-pulse regime and to tune its wavelength to optimize the efficiency of energy transfer. This in combination with the state-of-the-art OMEGA heater beams providing multiple kilojoules in a nanosecond to sufficiently heat the plasma make this system distinct from previous studies. These heater beams will provide, for the first time in Raman amplification studies, a homogeneous electron temperature high enough to prevent pump beam propagation issues that have plagued previous experiments. These systems will provide a platform for driving electron-plasma waves into the nonlinear regime where pump depletion and pulse shortening are predicted to lead to high amplification efficiencies (>30%). The Team has made significant progress through prior support from DOE Fusion Energy Sciences [DOE Office of Science Award Number DE-SC0016253 (2016-2022)]. This includes twenty-two peer-reviewed manuscripts, one patent, ten contributed talks presented at international conferences, and research that was highlighted as invited talks at fifteen international conferences. The broader impacts of this research are evident in the support of early career scientists, two Ph.D. theses, four current graduate students, a Masters Project, two undergraduate researchers, and an underrepresented minority student hired through the California Alliance for Minority Participation who now works as a Research Engineer in the group. This research met all of the funded research objectives and the highlights from primary Raman amplification thrust of this work are discussed below and form the foundation for the proposed research.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Impact of the optical parametric amplification phase on laser pulse compression

Optical parametric chirped-pulse amplification (OPCPA) is an effective way to generate ultrashort pulses that has been used extensively for a variety of applications requiring high peak intensities. Precise control and measurement of a system’s spectral and spatial phases are required for Fourier transform–limited pulse compression and diffraction-limited focusing. Phase accumulated during optical parametric amplification (OPA) can degrade the compressibility and focusability of the pulse, reducing peak intensity. We used analytic and numerical analysis of OPA to study the influence of crystal parameters, wavefront of the pump and signal, and their relative optical alignment on the accumulated phase. Here, we show that the accumulated signal phase is largely independent of amplifier saturation and, with significant local wavefront gradients in the signal or pump beam, the quality of the compressed pulses can be degraded. We use first-order expressions for the pump- and signal-angle sensitivity to evaluate an OPCPA system consisting of a highly deuterated potassium dihydrogen phosphate (DKDP) amplifier designed to support bandwidth for 15 fs pulses centered at 920 nm.

47 OTHER INSTRUMENTATION↗