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At least 415 records · Page 23

Quantum-amplified global-phase spectroscopy on an optical clock transition

Optical lattice clocks are at the forefront of precision metrology, operating near a standard quantum limit set by quantum noise. Harnessing quantum entanglement offers a promising route to surpass this limit; however, there are practical difficulties in terms of scalability and measurement resolution requirements. Here we adapt the holonomic quantum gate concept to develop a new Rabi-type ‘global-phase spectroscopy’ that uses the detuning-sensitive global Aharonov–Anandan phase19. With this approach, we can demonstrate quantum-amplified time-reversal spectroscopy on an optical clock transition that achieves directly measured 2.4(7) dB metrological gain and 4.0(8) dB improvement in laser noise sensitivity beyond the standard quantum limit. To this end, we introduce rotary echo to protect the dynamics from inhomogeneities in light–atom coupling and implement a laser-noise-cancelling differential measurement through symmetric phase encoding in two nuclear spin states. Our technique is not limited by measurement resolution, scales easily because of the global nature of entangling interaction and exhibits high resilience to typical experimental imperfections. As a result, we expect it to be broadly applicable to next-generation atomic clocks and other quantum sensors approaching the fundamental quantum precision limits.

Zaporski, Leon [Massachusetts Institute of Technol↗

Scaling and merging time-resolved pink-beam diffraction with variational inference

Time-resolved x-ray crystallography (TR-X) at synchrotrons and free electron lasers is a promising technique for recording dynamics of molecules at atomic resolution. While experimental methods for TR-X have proliferated and matured, data analysis is often difficult. Extracting small, time-dependent changes in signal is frequently a bottleneck for practitioners. Recent work demonstrated this challenge can be addressed when merging redundant observations by a statistical technique known as variational inference (VI). However, the variational approach to time-resolved data analysis requires identification of successful hyperparameters in order to optimally extract signal. In this case study, we present a successful application of VI to time-resolved changes in an enzyme, DJ-1, upon mixing with a substrate molecule, methylglyoxal. We present a strategy to extract high signal-to-noise changes in electron density from these data. Furthermore, we conduct an ablation study, in which we systematically remove one hyperparameter at a time to demonstrate the impact of each hyperparameter choice on the success of our model. We expect this case study will serve as a practical example for how others may deploy VI in order to analyze their time-resolved diffraction data.

47 OTHER INSTRUMENTATION↗

A laser powder bed fusion system for operando synchrotron x-ray imaging and correlative diagnostic experiments at the Stanford Synchrotron Radiation Lightsource

Laser powder bed fusion (LPBF) is a highly dynamic multi-physics process used for the additive manufacturing (AM) of metal components. Improving process understanding and validating predictive computational models require high-fidelity diagnostics capable of capturing data in challenging environments. Synchrotron x-ray techniques play a vital role in the validation process as they are the only in situ diagnostic capable of imaging sub-surface melt pool dynamics and microstructure evolution during LPBF-AM. In this article, a laboratory scale system designed to mimic LPBF process conditions while operating at a synchrotron facility is described. The system is implemented with process accurate atmospheric conditions, including an air knife for active vapor plume removal. Significantly, the chamber also incorporates a diagnostic sensor suite that monitors emitted optical, acoustic, and electronic signals during laser processing with coincident x-ray imaging. The addition of the sensor suite enables validation of these industrially compatible single point sensors by detecting pore formation and spatter events and directly correlating the events with changes in the detected signal. Experiments in the Ti–6Al–4V alloy performed at the Stanford Synchrotron Radiation Lightsource using the system are detailed with sufficient sampling rates to probe melt pool dynamics. X-ray imaging captures melt pool dynamics at frame rates of 20 kHz with a 2 µm pixel resolution, and the coincident diagnostic sensor data are recorded at 470 kHz. Furthermore, this work shows that the current system enables the in situ detection of defects during the LPBF process and permits direct correlation of diagnostic signatures at the exact time of defect formation.

36 MATERIALS SCIENCE↗

Ultrafast formation of a transient two-dimensional diamondlike structure in twisted bilayer graphene

Due to the absence of matching carbon atoms at honeycomb centers with carbon atoms in adjacent graphene sheets, theorists predicted that a sliding process is needed to form AA, AB', or ABC stacking when directly converting graphite into sp 3 bonded diamond. Here, using twisted bilayer graphene, which naturally provides AA and AB' stacking configurations, we report the ultrafast formation of a transient two-dimensional diamondlike structure (which is not observed in aligned graphene) under femtosecond laser irradiation. This photoinduced phase transition is evidenced by the appearance of bond lengths of 1.94 and 3.14 Å in the time-dependent differential pair distribution function using MeV ultrafast electron diffraction. Molecular dynamics and first-principles calculation indicate that sp 3 bonds nucleate at AA and AB' stacked areas in a moiré pattern. This work sheds light on the direct graphite-to-diamond transformation mechanism, which has not been fully understood for more than 60 years.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Photoinduced Melting of V 4 O 7 Correlated State

The compound V 4 O 7 is one of the Magnéli phase (V n O 2n - 1 , n = 3, 4, …, 9) correlated vanadium oxides with distinct intriguing electronic and structural properties. The possibility to manipulate the phase state of V 4 O 7 on an ultrafast time scale by light makes this material promising for potential applications in photonics, optoelectronics, quantum, and neuromorphic circuit design. In this work, the ultrafast spectroscopy of V 4 O 7 reveals the second-order nature of the photoinduced insulator-to-metal transition, emphasizing electronic and lattice contributions. The findings reveal the influence of the laser excitation level and temperature on these dynamics, providing a comprehensive understanding of V 4 O 7 structural changes and response to external stimuli. The phenomenological model based on the Landau–Ginzburg formalism provides a robust framework for explaining the photoinduced transition dynamics, showing a detailed picture of the light interaction with the electronic and lattice subsystems. This integrated approach significantly enhances the understanding of V 4 O 7 complex behavior upon photoexcitation, opening new possibilities for developing new optoelectronic devices and noninvasive optical control of the phase transition pathways in vanadates.

36 MATERIALS SCIENCE↗

Unsupervised anomaly detection in MeV ultrafast electron diffraction

MeV ultrafast electron diffraction (MUED) is a pump-probe technique used to study the dynamic structural evolution of materials. An ultrashort laser pulse triggers structural changes, which are then probed by an ultrashort relativistic electron beam. To overcome low signal-to-noise ratios, diffraction patterns are averaged over thousands of shots. However, shot-to-shot instabilities in the electron beam can distort individual patterns, introducing uncertainty. Improving MUED accuracy requires detecting and removing these anomalous patterns from large datasets. In this work, we developed a fully unsupervised methodology for the detection of anomalous diffraction patterns. Using a convolutional autoencoder, we calculate the reconstruction mean squared error of the diffraction patterns. Based on the statistical analysis of this error, we provide the user an estimation of the probability that the pattern is normal, which also allows a posterior visual inspection of the images that are difficult to classify. This method has been trained with only 100 diffraction patterns and tested on 1521 patterns, resulting in a false positive rate between 0.2% and 0.4%, with a training time of 10 s per image and a test time of about 1 s per image. Here, the proposed methodology can also be applied to other diffraction techniques in which large datasets are collected that include faulty images due to instrumental instabilities.

43 PARTICLE ACCELERATORS↗

Time-resolved x-ray absorption spectroscopy probe in ultrafast surface chemistry

To celebrate the scientific achievement of Jo Stöhr, I present here a personal account of the use of x-ray absorption spectroscopy to probe dynamics on surfaces using x-ray lasers. In particular, I will review the investigation of ultrafast processes in adsorbates on surfaces using an optical pump and an x-ray absorption spectroscopy probe. Here, it is shown that it is possible to gain insight into the effects of electronic excitations in metals on adsorbates as well as laser-induced vibrational motions. Furthermore, the ultrafast optical pump allows the detection of the CO precursor state in the desorption channel, species close to the transition state in CO oxidation, and the transient HCO intermediate during CO hydrogenation on Ru(0001).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Comparing the shock sensitivity of insensitive energetic materials

We present a tabletop method to study the shock sensitivity of plastic-bonded explosives that are considered shock insensitive using high dynamic range optical emission spectroscopy with laser-launched km/s flyer plate impacts (2, 3, and 4 km/s), which measures the spectral radiance (the emission spectrum vs a calibrated intensity standard) every 0.8 ns in the nanosecond and microsecond regimes. The explosives were TATB (1,3,5 trinitro, 2,4,6 triamino benzene), FOX-7 (1,1-diamino-2,2-dinitroethylene), LLM-105 (2,6-diamino-3,5-dinitropyrazine-1-oxide), and NTO (nitrotriazolone), all with 20% Sylgard 182 binder. Time resolving emission from shocked explosives produces a unique fingerprint at each shock pressure, and the emission temporal profile can be used to understand each material's shock response and the underlying mechanisms within the framework of the well-known shock ignition and growth models. Ignition was characterized by the emission intensity during nanosecond hot spot ignition. The growth process, which occurs after the shock has unloaded, was characterized by the time derivative of microsecond emission intensity. Singular-value decomposition was used to determine a characteristic spectral radiance over the entire time range, and this radiance was fit to a graybody model to determine a characteristic temperature Tc. Even though these insensitive explosives have similar shock sensitivities, our method can clearly distinguish their shock response. FOX-7 and NTO were the most sensitive, with FOX-7 having the greatest shock ignition sensitivity, growth rate, and Tc. LLM-105 was much less sensitive than FOX-7 and NTO, and TATB consistently showed the lowest sensitivity by any measure.

Akhtar, Meysam (ORCID:0000000243897837)↗

Coherent diffractive imaging with twisted X-rays: Principles, applications, and outlook

Recent technological breakthroughs in synchrotron and x-ray free electron laser facilities have revolutionized nanoscale structural and dynamic analyses in condensed matter systems. This review provides a comprehensive overview of the advancements in coherent scattering and diffractive imaging techniques, which are now at the forefront of exploring materials science complexities. These techniques, notably Bragg coherent diffractive imaging and x-ray photon correlation spectroscopy, x-ray magnetic dichroism, and x-ray correlation analysis leverage beam coherence to achieve volumetric three-dimensional imaging at unprecedented sub-nanometer resolutions and explore dynamic phenomena within sub-millisecond timeframes. Such capabilities are critical in understanding and developing advanced materials and technologies. Simultaneously, the emergence of chiral crystals—characterized by their unique absence of standard inversion, mirror, or other roto-inversion symmetries—presents both challenges and opportunities. These materials exhibit distinctive interactions with light, leading to phenomena such as molecular optical activity, chiral photonic waveguides, and valley-specific light emissions, which are pivotal in the burgeoning fields of photonic and spintronic devices. This review elucidates how novel x-ray probes can be leveraged to unravel these properties and their implications for future technological applications. A significant focus of this review is the exploration of new avenues in research, particularly the shift from conventional methods to more innovative approaches in studying these chiral materials. Inspired by structured optical beams, the potential of coherent scattering techniques utilizing twisted x-ray beams is examined. This promising direction not only offers higher spatial resolution but also opens the door to previously unattainable insights in materials science. By contextualizing these advancements within the broader scientific landscape and highlighting their practical applications, this review aims to chart a course for future research in this rapidly evolving field.

Physics↗

Dual-wavelength channel GHz repetition rate mode-locked VECSEL cavities sourced from a common gain medium

Mode-locked vertical external cavity semiconductor lasers are a unique class of nonlinear dynamical systems driven far from equilibrium. We present a novel, to the best of our knowledge, experimental result, supported by rigorous microscopic simulations, of two coexisting mode-locked V-cavity configurations sourced by a common gain medium and operating as independent channels at angle controlled separated wavelengths. Microscopic simulations support pulses coincident on the common gain chip extracting photons from a nearby pair of coexisting kinetic holes burned in the carrier distributions.

47 OTHER INSTRUMENTATION↗

Defect-engineered GaN high electron mobility transistors for enhanced radiation tolerance

This study explores the radiation resilience of GaN high-electron-mobility transistors (HEMTs) under various preconditioning treatments—pristine, electro-pulsed, electrically overstressed, and 60 Co gamma-irradiated—with a focus on enhancing survivability in high-radiation environments. Key findings emphasize the gate region’s central role in radiation sensitivity, with increased defect concentrations leading to reduced sensitivity—as determined from reduced single-event transient intensities during pulsed-laser studies—and impacting charge-transport dynamics. Notably, the most sensitive region shifted as a function of bias state, with the drain side of the gate being most sensitive under negative gate bias and the source side under unbiased conditions due to two-dimensional electron gas disruptions. These insights clarify the mechanisms influencing radiation sensitivity in microelectronics and highlight the potential of defect and strain engineering to enhance the radiation hardness of GaN HEMTs across various operational states, providing valuable guidance for applications in space, defense, and other radiation-rich environments.

36 MATERIALS SCIENCE↗

Evaluation of a novel mid-infrared pyrometer for dynamic material experiments

Dynamic experiments create high-pressure shock waves on the microsecond time scale (or smaller), compressing materials to high pressures and temperatures and enabling the study of material properties at these conditions. Other dynamic studies use quasi-isentropic compression to produce similar high pressures at much lower temperatures. High pressure experiments performed on dynamic platforms such as gas-guns, laser, and pinch machines generate up to several hundred GPa in the sample pressure conditions12. Related static studies include diamond anvil cells, which obtain high pressures and have extremely high precision, but are most often conducted at room temperature or modest temperature increases (often <2000K). By combining these methods, material properties across a wide range of thermodynamic conditions can be probed, and a high quality equation of state (EOS) constructed.

36 MATERIALS SCIENCE↗

The right conditions for high-precision dynamic temperature and heat capacity measurement via pyrometry and conductivity

The pursuit of accurate bulk temperature T under extreme conditions has been a long-standing goal of the high pressure science community, complicated by a lack of data to inform models. To reach these extremely high-pressure, high-temperature (high P − T) conditions, a combination of dynamic and heated static experiments (e.g., diamond or gem anvil cel experiments) are used. For example, in a diamond anvil cell (DAC) experiment, a sample placed in the DAC is first pressurized. Following pressurization, the sample T is increased either by heating the entire DAC (usually using resistive heating, and limited to ∼1000K) or by applying intense laser power to the sample surfaces. In a dynamic experiment, the process of pressurizing the sample also heats it. In the case of shock physics experiments, such heating is substantial, easily reaching thousands of Kelvin; in our work we have seen T ∼17000K. Most methods of measuring temperature at ambient are not compatible with experiments under these high-pressure, high-temperature conditions: thermocouples break, melt, or have conductivity properties that differ from ambient where they are calibrated; thermometers would melt; both are too slow. As a result most methods are based on non-contact techniques such as x-ray diffraction broadening, neutron scattering, or optical methods. Of these, optical methods using the visible and near-infrared region of the spectrum are the most commonly used as the sources and detectors are readily available. In the case of optical methods the optical depth, and therefore the measurement location, is limited to the surface. When a window or anvil material is used, heat flows from the sample into the window/anvil. Likewise, if the sample undergoes a change in thermodynamic state, such as expansion upon release, different T may be expected. As a result, the surface or apparent temperature T app measurement will differ from the bulk or interior temperature that is desired. This surface measurement must be related to the bulk measurement using thermal transport models and material models. While it is tempting to conclude that one should just use x-ray methods that directly probe the interior, even these methods have been shown to depend on thermal transport and material models. Regardless of the method used to create the high P − T condition, therefore, we must understand the role of thermal transport and material models upon our interpretation of the T measurement, as well as the errors and uncertainties associated with the choice of models used in the analysis. This is a substantial area of research and this paper is by no means a complete survey of the relevant sources of uncertainty. For example, we have yet to begin to address alternate transport models in a detailed manner (e.g., Tan-Ahrens), or the many models that use additional layers to approximate melting, turbulence, or epitaxial phenomena). Likewise, we have not explored the impact upon uncertainty of thermal models that use temperature-dependent thermal transport coefficients, or the wide range of material models that can be applied. Instead, this paper focuses on using one simple model, the Urtiew-Grover model, to understand the sources of error in T measurement so that we may identify how best to focus future research efforts to return the best improvements and avoid working on over-optimizing a single type of measurement. To this end, we work through some of the best and worst case scenarios for T measurement.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Table-Top High Photon Energy Sources for Chemical Dynamics Investigations

Time-resolved spectroscopies using high-energy photons in the vacuum ultraviolet (VUV) to the X-ray region of the electromagnetic spectrum, have proven to be powerful probes of chemical dynamics. These high-energy photons can access valence and core orbitals of molecules and materials, providing key information on molecular and electronic structure and their time evolution. This report details the development of table-top sources of extreme ultraviolet (XUV) and VUV pulses at Sandia National Laboratories for use in studies of gas phase chemical dynamics. Femtosecond duration XUV pulses are produced using laser-driven high harmonic generation and their detected range span ~40-140 eV photon energies. These pulses are used in conjunction with ultraviolet pulses in a pump-probe scheme to study excited state dynamics of gas phase molecules. VUV pulses at 7.75 eV are generated using a four-wave-mixing scheme driven by 800 nm and 266 nm pulses in an argon-filled hollow-core fiber.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High-throughput quantification of quasistatic, dynamic and spall strength of materials across 10 orders of strain rates

Abstract The response of metals and their microstructures under extreme dynamic conditions can be markedly different from that under quasistatic conditions. Traditionally, high strain rates and shock stresses are achieved using cumbersome and expensive methods such as the Kolsky bar or large spall experiments. These methods are low throughput and do not facilitate high-fidelity microstructure–property linkages. In this work, we combine two powerful small-scale testing methods, custom nanoindentation, and laser-driven microflyer (LDMF) shock, to measure the dynamic and spall strength of metals. The nanoindentation system is configured to test samples from quasistatic to dynamic strain-rate regimes. The LDMF shock system can test samples through impact loading, triggering spall failure. The model material used for testing is magnesium alloys, which are lightweight, possess high-specific strengths, and have historically been challenging to design and strengthen due to their mechanical anisotropy. We adopt two distinct microstructures, solutionized (no precipitates) and peak-aged (with precipitates) to demonstrate interesting upticks in strain-rate sensitivity and evolution of dynamic strength. At high shock-loading rates, we unravel an interesting paradigm where the spall strength vs. strain rate of these materials converges, but the failure mechanisms are markedly different. Peak aging, considered to be a standard method to strengthen metallic alloys, causes catastrophic failure, faring much worse than solutionized alloys. Our high-throughput testing framework not only quantifies strength but also teases out unexplored failure mechanisms at extreme strain rates, providing valuable insights for the rapid design and improvement of materials for extreme environments.

Eswarappa Prameela, Suhas (ORCID:0000000334530184)↗

Density-matrix approach for sequential dissociative double ionization of molecules

Intense femtosecond infrared (IR) laser pulses have been used in recent years to study the breakup dynamics of molecules. However, observables such as kinetic energy release and branching ratios of molecular fragments are often difficult to predict by theory, making information of the molecular dynamics difficult to retrieve. In this work, we develop a simple model for sequential double ionization of molecules based on a density-matrix approach. The model describes tunneling ionization of the neutral and the ion as well as laser couplings between the ionic states simultaneously. Population of different doubly charged states can be obtained at a low computational cost. Furthermore, we applied our model to N 2 and obtained a good agreement on the kinetic energy release spectrum with a previous experiment. This theoretical development could open up the opportunities to use intense short IR laser pulses with coincidence measurement to probe molecular dynamics.

74 ATOMIC AND MOLECULAR PHYSICS↗

Pre-Ionization Controlled Laser Plasma Formation for Ignition Applications (Final Scientific/Technical Report)

This report consists of three grand funded papers. Abstracts for each follow. 1) In this work, we present experimental and modeling studies of air pre-ionization using ultraviolet (UV) laser pulses and its effect on laser breakdown of an overlapped near-infrared (NIR) pulse. Experimental studies are conducted with a 266 nm beam (fourth harmonic of Nd:YAG) for UV pre-ionization and an overlapped 1064 nm NIR beam (fundamental of Nd:YAG), both having pulse duration of 10 ns. Results show that the UV beam produces a pre-ionized volume which assists in breakdown of the NIR beam, leading to reduction in NIR breakdown threshold by factor of >2. Numerical modeling is performed to examine the ionization and breakdown of both beams. The modeled breakdown threshold of the NIR, including assist by pre-ionization, is in reasonable agreement with the experimental results. 2) The present contribution compares the energy absorption, optical emission, temperature, and fluid dynamics of ultraviolet (UV) λ = 266 nm and near infrared (NIR) λ = 1064 nm nanosecond laser induced plasmas in ambient air. For UV pulses at the conditions studied, energy absorption by the plasmas increases relatively gradually with laser pulse energy starting at delivered energy of E~8 mJ. Corresponding measurements of plasma luminosity show that the absorption of UV radiation does not necessarily result in visible plasma emission. For the NIR induced plasmas, the energy absorption profile is far more abrupt and begins at ~55 mJ. In contrast with UV, the absorption of NIR radiation is always accompanied by intense optical emission. The temperatures of both types of plasma have been measured with Rayleigh scattering thermometry (at times after the Thomson signal sufficiently diminishes). The UV plasmas can attain a wider range of temperatures, including lower temperatures, depending on the pulse energy (e.g., T ~400–2000K for E ~7–35 mJ at Δt = 10 μs after the pulse) while the NIR plasmas show only hotter temperatures (e.g., T ~ 12 000 K for E = 75 mJ at Δt = 10 μs after the pulse) as is consistent with the literature. Differences in the fluid dynamics for UV versus NIR pulses are shown with Schlieren imaging. In this work, the contrast in the UV and NIR plasma threshold behavior is attributed to differing roles of avalanche ionization and multiphoton ionization as is also illustrated by a simple numerical model. 3) The present contribution examines the impact of plasma dynamics and plasma-driven fluid dynamics on the flame growth of laser ignited mixtures and shows that a new dual-pulse scheme can be used to control the kernel formation process in ways that extend the lean ignition limit. We perform a comparative study between (conventional) single-pulse laser ignition (λ = 1064 nm) and a novel dual-pulse method based on combining an ultraviolet (UV) pre-ionization pulse (λ = 266 nm) with an overlapped near-infrared (NIR) energy addition pulse (λ = 1064 nm). We employ OH* chemiluminescence to visualize the evolution of the early flame kernel. For single-pulse laser ignition at lean conditions, the flame kernel separates through third lobe detachment, corresponding to high strain rates that extinguish the flame. In this work, we investigate the capabilities of the dual-pulse to control the plasma-driven fluid dynamics by adjusting the axial offset of the two focal points. In particular, we find there exists a beam waist offset whereby the resulting vorticity suppresses formation of the third lobe, consequently reducing flame stretch. With this approach, we demonstrate that the dual-pulse method enables reduced flame speeds (at early times), an extended lean limit, increased combustion efficiency, and decreased laser energy requirements.

Mechanical engineering↗