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At least 1,045 records · Page 58

Vibrational Sum-Frequency Generation Hyperspectral Microscopy for Molecular Self-Assembled Systems

In this review, we discuss the recent developments and applications of vibrational sum-frequency generation (VSFG) microscopy. This hyperspectral imaging technique can resolve systems without inversion symmetry, such as surfaces, interfaces and noncentrosymmetric self-assembled materials, in the spatial, temporal, and spectral domains. We discuss two common VSFG microscopy geometries: wide-field and confocal point-scanning. We then introduce the principle of VSFG and the relationships between hyperspectral imaging with traditional spectroscopy, microscopy, and time-resolved measurements. We further highlight crucial applications of VSFG microscopy in self-assembled monolayers, cellulose in plants, collagen fibers, and lattice self-assembled biomimetic materials. In these systems, VSFG microscopy reveals relationships between physical properties that would otherwise be hidden without being spectrally, spatially, and temporally resolved. Lastly, we discuss the recent development of ultrafast transient VSFG microscopy, which can spatially measure the ultrafast vibrational dynamics of self-assembled materials. The review ends with an outlook on the technical challenges of and scientific potential for VSFG microscopy.

Chemistry↗

Time-refraction near the critical angle and angular streaking with attosecond resolution [Invited]

We study the time-refraction of optical waves as they propagate through a time-varying slab and find the frequency shift associated with the abrupt change in the refractive index. We discover a geometrical mechanism responsible for an ultrafast blueshift followed by a redshift, occurring while the refractive index is increased monotonically. Furthermore, we find high sensitivity to incident angles near the traditional critical angle and unravel a new critical angle that varies in time. Finally, we introduce an innovative concept of a streak camera design that utilizes ultrafast nonlinearities in time-varying media and offers attosecond resolution capabilities.

Fruhling, Colton (ORCID:0000000282968802)↗

Ultra-intense femtosecond laser interactions with aligned nanostructures

The interaction of ultrafast laser pulses of relativistic intensity with high aspect ratio nanostructures can efficiently and volumetrically heat matter to an ultra-high-energy-density regime encountered in the center of stars and within the core of fusion capsules compressed by the world’s largest lasers. It also generates gigantic quasi-static electromagnetic fields that accelerate particles to very high energy. Here, we present an overview of the physics and applications of these dense relativistic plasmas that can be created with pulses of relatively modest energy from lasers that can operate at a high repetition rate. Recent nanowire array experiments produced near-solid density plasmas with an extreme degree of ionization (e.g., Au +72 ), converted ultrafast pulses of laser light into intense x-ray flashes with record efficiency, and accelerated ions to MeV energies, efficiently driving micro-scale fusion reactions that generate flashes of quasi-monoenergetic neutrons. These plasmas also serve as a platform for advancing the understanding of atomic processes in extreme environments and open a new pathway to laser-driven fusion energy. The irradiation of nanostructures at intensities of > 1 x 10 22 W cm –2 is predicted to lead to an extreme ultra-high energy density plasma regime characterized by terabar pressures that is virtually unexplored.

Optics↗

All-optical sampling of few-cycle infrared pulses using tunneling in a solid

Recent developments in ultrafast laser technology have resulted in novel few-cycle sources in the mid-infrared. Accurately characterizing the time-dependent intensities and electric field waveforms of such laser pulses is essential to their applications in strong-field physics and attosecond pulse generation, but this remains a challenge. Recently, it was shown that tunnel ionization can provide an ultrafast temporal “gate” for characterizing high-energy few-cycle laser waveforms capable of ionizing air. Here, we show that tunneling and multiphoton excitation in a dielectric solid can provide a means to measure lower-energy and longer-wavelength pulses, and we apply the technique to characterize microjoule-level near- and mid-infrared pulses. The method lends itself to both all-optical and on-chip detection of laser waveforms, as well as single-shot detection geometries.

74 ATOMIC AND MOLECULAR PHYSICS↗

First High-Gradient Results of UED/UEM SRF Gun at Cryogenic Temperatures

Benefiting from the rapid progress on RF photogun technologies in the past two decades, the development of MeV range ultrafast electron diffraction/microscopy (UED and UEM) has been identified as an enabling instrumentation. UEM or UED use low power electron beams with modest energies of a few MeV to study ultrafast phenomena in a variety of novel and exotic materials. SRF photoguns become a promising candidate to produce highly stable electrons for UEM/UED applications because of the ultrahigh shot-to-shot stability compared to room temperature RF photoguns. SRF technology was prohibitively expensive for industrial use until two recent advancements: Nb₃Sn and conduction cooling. The use of Nb₃Sn allows to operate SRF cavities at higher temperatures (4K) with low power dissipation which is within the reach of commercially available closed-cycle cryocoolers. Euclid is developing a continuous wave (CW), 1.5-cell, MeV-scale SRF conduction cooled photogun operating at 1.3 GHz. In this paper, we present first high gradient results of the gun conducted in liquid helium.

43 PARTICLE ACCELERATORS↗

Soft X-ray measurements of transport and MHD activity in the core and edge NSTX plasma (Final Technical Report)

A comprehensive suite of innovative diagnostic instrumentation and techniques has been developed by the Johns Hopkins collaboration for measurements of transport and MHD activity in the core and edge of the National Spherical Torus Experiment (NSTX) at the Princeton Plasma Physics Laboratory (PPPL). These include ultrafast multi-energy poloidal soft X-ray arrays, high spatial resolution multi-energy tangential soft X-ray arrays, high spectral resolution transmission grating imaging VUV spectrometers and ultrafast bolometric arrays, which measure over a broad range of spatial, spectral, and temporal scales the emission from ohmic, RF, and beam driven NSTX plasmas. The instrumentation was designed to fulfill the specific measurement needs of the Spherical Torus (ST) magnetic fusion concept and is accompanied by a comprehensive set of numerical tools for data analysis and modeling, aimed at determining as many as possible plasma parameters and at extracting as much as possible physics information from NSTX experiments. The Johns Hopkins diagnostics have been and continue to be instrumental for essentially all the NSTX experiments. In addition, our own research and experiments using these diagnostics has led over the years to fundamental conclusions for the ST fusion physics, such as the establishment of near neoclassical impurity transport in the NSTX core and edge plasma, and the critical role of the Global Alfven Eigenmode (GAE) MHD activity for the ST core electron thermal transport. The Johns Hopkins Diagnostics continue to be operational on the upgraded NSTX-U and will provide key plasma information in its upcoming high field, current and power experimental campaigns. The present report summarizes the main technical characteristics and measurement capabilities of the diagnostic instrumentation and methods developed within our research and describes a key physics result achieved during this research. Success in our research was made possible also by the excellent support and cooperation of the NSTX research team and of PPPL researchers, who are warmly acknowledged here.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Using femtosecond pump-probe spectroscopy to shed new light on complex materials

We know a lot about events that have occurred during the earth’s history, on timescales of millions of years. We are much less familiar with events that occur on “ultra”-short timescales of less than a billionth of a second. Unlike in geology, we can actually do experiments at ultrashort timescales, so we should be able to understand the “ultrafast” world much better! Ultrafast optical spectroscopy is the only technique capable of measuring processes at the fundamental time scales of electron, lattice and nuclear motion.

36 MATERIALS SCIENCE↗

Organic Macromolecular materials for Efficient Transport Properties in Light-Energy Conversion Applications. Final Report

We are grateful for the Department of Energy for support of this research related to the improvement of power conversion efficiency of organic photovoltaic architectures over the years. As we noted at the beginning and now, the fundamental photophysical pathways that connect the absorption of light to the production of charge carriers remain elusive in spite of continuing experimental and theoretical efforts. Our investigations were directed toward gaining information about the mechanism of this ultrafast, long-range charge separation in photovoltaic systems with non-fullerene acceptors. This problem is still of high importance for the organic photovoltaics because solving this problem will allow us to minimize the contribution of the geminate recombination and trapping the charges in bound charge transfer states. Extremely low charge separation driving energy specific to non-fullerene acceptor systems reduces the energy loss in organic photovoltaic cells making them competitive with inorganic and perovskite photovoltaic systems. A major accomplishment of this study was to detail the long-range ballistic charge separation in donor-non-fullerene acceptor photovoltaic systems. We have successfully probed the spatial structure of ultrafast long-range (~40nm) ballistic charge separation in donor-non-fullerene acceptor photovoltaic system. We performed a systematic investigation of the delocalized states in their connection to the efficient long-range charge separation using the pulse pair interferometric near-field microscopy method. This method possesses unique capability of detecting coherent effects with spatial resolution of few tens of nanometers. These measurements allowed us the determination of delocalized excitations locally in a thin film photovoltaic system and to be connected to the long-range charge separation and the power conversion efficiency. We also investigated long-lived coupled triplet pairs in a singlet fission process for the possibility of concerted extraction of two electrons from triplet entangled states. New experimental and theoretical approaches of the concerted double electron extraction were carried out. The impact of this work is the development of important structure-property relationships to the design criteria of more efficient organic photovoltaic cells in accordance with the BES mission.

14 SOLAR ENERGY↗

Spatio-temporally shaped deep UV laser source for ultrabright photocathodes using novel upconversion techniques (Final Report)

The goal of this project was to take a VUV laser system designed by Kapteyn-Murnane Labs (KMLabs)—the Hyperion VUV, and increase its functionality, efficiency, and applicability by further probing the fundamental physics taking place in the system and optimizing the system performance. More specifically, DOE accelerator applications—particularly for XFELs that require low-emittance electron beams, require precisely controlled ultrashort pulses in the deep-UV at 250-260 nm to drive the photocathode electron source. This is conventionally done using an ultrafast infrared laser, with subsequent stages of nonlinear upconversion in solid-state nonlinear-optical crystal media (principally BBO, which is commonly used for UV upconversion). However, maintaining high spatial mode beam quality, as well as precisely controlled temporal profile, has proven a persistent challenge. As a possible alternative to this approach, KMLabs has demonstrated a system that generates vacuum ultraviolet light (VUV) by upconverting pulses from an infrared ultrafast laser in a gas-filled hollow waveguide, driving a process of highly cascaded harmonic generation (HCHG). Because HCHG upconversion is done in a gas, rather than a solid, at high intensity in a guided-wave geometry, it retains an excellent beam spatial profile as well as a large spectral bandwidth that allows for control over the temperal structure of the pulse. A challenge, however, is in energy scaling of this HCHG technique to the ~1-20 μJ pulses required for photocathode applications. To-date, the pulse energies used in published HCHG work are sub-10-nJ. This project proposed to explore ways to generate higher-energy pulses using HCHG, as well as to investigate spectral and temporal shaping of the deep UV pulses by pulse shaping the infrared laser used to seed the process. Although we showed that our approach works for generating light at 259 nm, the total pulse energy achieved seems limited to approximately the same value as past work. However, the techniques we investigated may well have benefits for extending this source to much shorter wavelength output.

43 PARTICLE ACCELERATORS↗

Nanoscale X-ray Imaging and Dynamics of Electronic and Magnetic Materials

This project supported cutting-edge nanoscale characterization developments including X-ray Imaging by utilizing the power of Coherent X-ray Diffractive Imaging (CXDI). This research pioneered new directions in studies of nanoscale dynamics using X-ray Photon Correlation Spectroscopy (XPCS) and Ultrafast X-ray Scattering (UXS), extending our understanding of science and technology at the limits of ultrasmall (atomic/nanoscale) and ultrafast (from seconds to femtosecond dynamics). The research funded by this award spans a wide range of condensed matter and materials physics systems, from correlated oxides and nanomaterials to energy-related materials, and quantum materials for neuromorphic computing.

25 ENERGY STORAGE↗

Probing coherence in nanoscale energy transport with high spatial-temporal resolution. Final Technical Report for DOE Award Number DE-SC0019244

The overarching goal of this project is to understand how the phase coherence of phonons and the interaction of phonons with other microscopic degrees of freedom in nanomaterials, such as 2D materials, can affect the energy transport properties and eventually lead to control of energy transport by manipulating phonon interference and phonon scatterings. On the computational side, we are developing and applying first-principles methods to study emerging phonon properties in nanomaterials, including coherent phonons, resonant bonding and gate-tunable phonon-electron scatterings, which hold the promise of enabling significant tunability of energy transport processes with external fields for a wide range of applications. On the experimental side, we are developing ultrafast transient grating spectroscopy and scanning ultrafast electron microscopy (SUEM) to directly probe the coherent phonon transport and phonon-electron interaction processes in nanomaterials with high combined spatial-temporal resolutions. This program will not only provide new insights into the microscopic transport and interaction processes of fundamental energy carriers, but also open new venue towards energy-relevant applications such as thermal switches and coherent energy harvesters.

42 ENGINEERING↗

Radiation-Induced Late Actinides Redox Chemistry

The goal of this proposal was to understand how radiation alters actinide redox chemistry, especially via the generation of transient oxidation states that typically cannot be isolated in bulk and need to be measured on ultrafast timescales. While these studies are of fundamental importance, they also impact the recycling of used nuclear fuel because the radiation field not only alters the oxidation states of actinides, but also induces chemical transformations of the extractants, typically in a deleterious manner. The majority of actinide radiation chemistry knowledge is concentrated toward the beginning of the series especially for uranium and plutonium, for which radiation-induced reactions have been demonstrated to significantly impact the accessibility and lifetime of actinide oxidation states at both ultrafast (pico- to microseconds) and steady-state timescales. Furthermore, there is precedence for these radiation-induced actinide redox reactions altering the radiolytic integrity of their corresponding complexes, relative to the free ligand, through facilitation of inner- versus outer-sphere reaction pathways.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Particle Beam Acceleration Using 3 Petawatt Laser Pulses

The Zettawatt-Equivalent Ultrashort pulse laser System (ZEUS) is presently operational at the Gerard Mourou Center for Ultrafast Optical Science (CUOS) at the University of Michigan. ZEUS is a significant upgrade of the previous high power laser systems at CUOS and consists of two beamlines thatoperate in perfect synchronization. The 500 TW beamline became operational in 2023, 2 PW operation started in 2025 and full 3 PW power levels will be available in 2026. It is presently the highest power laser system in the US. In this grant the high field science group at CUOS has leveraged this unique high power laser facility to investigate laser wake field acceleration (LWFA) in ultra-high power laser plasma interactions and have shown how this can scale for future electron–positron colliders at high energy. The dual beam experimental configuration enables flexibility for many frontier experiments in laser-driven acceleration research, in particular, enabling extended channelling/acceleration experiments, positron generation/acceleration experiments and proof-of-principle transverse pumping “dephasingless” electron acceleration experiment and theory. LWFA may be able to miniaturize particle accelerators for high energy physics and also enable new sources of ultrafast, extreme brightness and precise x-rays for a wide variety of applications. In laser wake field acceleration, an electron bunch “surfs” on the electron plasma wave (the “wake field”) generated by the ponderomotive force of an intense laser. The plasma wave has a strong longitudinal electric field that stays in phase with the relativistic driver. A relativistic charged particle may, therefore, remain in phase with the accelerating field over long distances and gain ultra-relativistic energies. The accelerating electric field strength that the plasma wave can support can be many orders of magnitude higher than that of conventional accelerators, which makes laser wakefield acceleration an exciting prospect as an advanced accelerator concept. In this research project we have investigated the scaling of this mechanism to laser powers of 2 PW and have measured the x-ray emission and radio frequency emission resulting from the acceleration process. We have also performed theoretical investigation of mechanisms to scale laser driven accelerators to much higher energy using dephasingless acceleration processes.

43 PARTICLE ACCELERATORS↗

Controlling Interfacial Energetics and Charge Transfer Rates in 2D Semiconductors: Fundamental Studies en Route to Photoelectrochemical Energy Conversion Beyond the Shockley-Queisser Limit (Final Scientific/Technical Report)

Current photovoltaic and solar-to-fuel technologies do not fully utilize the energy of sunlight because excess photon energy above the semiconductor band gap is rapidly lost as heat through hot-carrier thermalization. Overcoming this loss mechanism is critical, as hot-carrier-based energy conversion systems are predicted to exceed the conventional efficiency limit of ~33%. This project advanced fundamental understanding of hot-carrier energy conversion in two-dimensional (2D) semiconductors, with a focus on monolayer MoS 2 . Using a combination of electrochemical microscopy and in situ ultrafast spectroscopic measurements, this research directly demonstrated hot-carrier extraction from monolayer MoS 2 photoelectrodes in proof-of-concept liquid junction solar cells. These measurements established that hot-carrier transfer can compete with ultrafast carrier cooling at solid–liquid interfaces, providing unambiguous experimental evidence that hot-carrier extraction is feasible in atomically thin semiconductors under operating photoelectrochemical conditions. Beyond demonstration, the project identified design rules for tuning hot-carrier extraction rates relative to cooling rates in 2D semiconductor photoelectrodes. The outcomes of this research provide foundational thermodynamic and kinetic insights for the rational design of next-generation hot-carrier-enabled solar energy conversion systems. These findings have broad implications for photoelectrochemical solar fuels production, electrocatalysis, and emerging energy conversion architectures that seek to harness nonequilibrium charge carriers for enhanced efficiency.

14 SOLAR ENERGY↗

Photon-In/Photon-Out X-ray Free-Electron Laser Studies of Radiolysis

Understanding the origin of reactive species following ionization in aqueous systems is an important aspect of radiation–matter interactions as the initial reactive species lead to production of radicals and subsequent long-term radiation damage. Tunable ultrafast X-ray free-electron pulses provide a new window to probe events occurring on the sub-picosecond timescale, supplementing other methodologies, such as pulse radiolysis, scavenger studies, and stop flow that capture longer timescale chemical phenomena. We review initial work capturing the fastest chemical processes in liquid water radiolysis using optical pump/X-ray probe spectroscopy in the water window and discuss how ultrafast X-ray pump/X-ray probe spectroscopies can examine ionization-induced processes more generally and with better time resolution. Ultimately, these methods will be applied to understanding radiation effects in complex aqueous solutions present in high-level nuclear waste.

47 OTHER INSTRUMENTATION↗

Harnessing Ultra-Intense Long-Wave Infrared Lasers: New Frontiers in Fundamental and Applied Research

This review explores two main topics: the state-of-the-art and emerging capabilities of high-peak-power, ultrafast (picosecond and femtosecond) long-wave infrared (LWIR) laser technology based on CO2 gas laser amplifiers, and the current and advanced scientific applications of this laser class. The discussion is grounded in expertise gained at the Accelerator Test Facility (ATF) of Brookhaven National Laboratory (BNL), a leading center for ultrafast, high-power CO2 laser development and a National User Facility with a strong track record in high-intensity physics experiments. We begin by reviewing the status of 9–10 μm CO2 laser technology and its applications, before exploring potential breakthroughs, including the realization of 100 terawatt femtosecond pulses. These advancements will drive ongoing research in electron and ion acceleration in plasma, along with applications in secondary radiation sources and atmospheric energy transport. Throughout the review, we highlight how wavelength scaling of physical effects enhances the capabilities of ultra-intense lasers in the LWIR spectrum, expanding the frontiers of both fundamental and applied science.

43 PARTICLE ACCELERATORS↗

Making and breaking terahertz waves with fluid plasmas

Vigorous research efforts during the past several decades have successfully closed the “terahertz gap” between microwaves and infrared light, offering new and increasingly efficient ways to produce, detect, and manipulate radiation fields in the terahertz (THz) frequency range. In our laboratory, THz time-domain spectroscopy (THz-TDS) and optical-pump THz-probe (OPTP) experiments have been routinely utilized as ultrafast spectroscopy tools to investigate a variety of emerging quantum materials and metamaterials. The ultrafast THz pulses are produced by femtosecond laser excitation of photoconductive antennas, semiconductor surfaces (InAs), and nonlinear crystals (ZnTe, GaSe, and LiNbO 3 ). Photoconductive antennas and nonlinear crystals also allow for the coherent detection of these pulses in the time domain, with amplitude and phase spectra obtained in the frequency domain via fast Fourier transform. Although such solid-state schemes are highly desirable in many aspects and thus also commonly utilized in many research laboratories and industrial applications, they typically suffer from limited bandwidths due to the absorption and frequency dispersion induced primarily by phonon resonances, limiting THz applications such as spectroscopy of emerging materials, imaging and detection, and biomedical characterization.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Dynamical Scaling Reveals Topological Defects and Anomalous Evolution of a Photoinduced Phase Transition

Nonequilibrium states of quantum materials can exhibit exotic properties and enable unprecedented functionality and applications. These transient states are inherently inhomogeneous, characterized by the formation of topologically protected structures, requiring nanometer spatial resolution on femtosecond timescales to resolve their evolution. Using ultrafast total x-ray scattering at a free electron laser and a sophisticated scaling analysis, we gain unique access to the dynamics on the relevant mesoscopic lengthscales. Our results provide direct evidence that ultrafast excitation of LaTe$_3$ leads to formation of topological vortex strings of the charge density wave. These dislocations of the charge density wave exhibit anomalous, subdiffusive dynamics, slowing the equilibration process, providing rare insight into the nonequilibrium mesoscopic response in a quantum material. Our findings establish a general framework to investigate properties of topological defects, which are expected to be ubiquitous in nonequilibrium phase transitions and may arrest equilibration and enhance competing orders.

FOS: Physical sciences↗