Controlling the longitudinal phase space of high-brightness relativistic electron beams is crucial for advancing a broad spectrum of charged-particle-based instrumentation and scientific frontiers. A generalized method for achieving this control involves manipulating the photoemission laser's temporal distribution at the picosecond level, a long-standing technical challenge. Recent developments in laser shaping have enabled the creation of high-power, picosecond-scale symmetrical and asymmetrical temporal profiles, capable of fine-tuning complex space-charge dynamics and external field effects in relativistic charged-particle beams. Here, we demonstrate that rather than deviations from theorized, idealized laser distributions, a controlled asymmetry can be harnessed to counteract accelerator-induced distortions. By implementing spatiotemporal shaping of the ultraviolet photocathode laser at the LCLS-II superconducting injector, we achieve deterministic control over the longitudinal phase space without downstream corrections. We find that this optical asymmetry induces a self-linearizing effect across both low (40 pC) and high (80 pC) charge regimes, effectively suppressing nonlinear compression and energy chirp. Consequently, this approach is expected to preserve a low emittance comparable to that of ideal flattop or regular Gaussian profiles, while delivering superior current uniformity and shot-to-shot stability. These results establish spatiotemporal laser shaping as a compact, generalizable tool for directly optimizing beam brightness at the source.

The complex refractive index of a material governs its light-matter interactions, with intense light fields enabling tailored nonlinear optical responses. In the X-ray regime, rapid photoionization limits the potential of nonlinear techniques by inducing irreversible electronic damage. Here we demonstrate that intense, sub-femtosecond X-ray pulses, shorter than typical Auger decay times, can partially reverse photoexcitation via stimulated emission near atomic resonances. By analyzing thousands of coherent diffraction patterns and ion spectra from neon nanoparticles exposed to sub-fs and 15-fs pulses, we observe enhanced X-ray diffraction alongside reduced energy absorption for sub-fs pulses. Theoretical modeling attributes this to dynamics akin to Rabi flopping that prolong the lifetime of resonant states and suppress electronic bleaching. These findings suggest that ultrashort, intense X-ray pulses enable active control of X-ray refractive index and damage pathways, opening avenues for improved high-resolution imaging and nonlinear spectroscopy in complex nanoscale systems.

We demonstrate adaptable X-ray pulse tailoring at the LCLS-II XFEL using programmable elements in the photoinjector laser, establishing a future control knob for high-rate XFEL tuning and optimization.

We investigate spatiotemporal laser pulse shaping using dispersion-managed nonlinear processes, aiming to achieve high-power, high-brightness, and programmable generation and manipulation of electron and X-ray beams for future attosecond applications.

We investigate the control of laser fields in space and time using dispersion-managed nonlinear techniques, enabling the tailored, high-brightness, high-power production and manipulation of electron and X-ray pulses.

We demonstrate the production of mutually phase-stable attosecond X-ray pulse pairs with tunable relative time delays and phases in a cascaded X-ray free-electron laser. We showcase the method in an experiment at the LCLS-II, in which a shaped electron beam is used in a split undulator configuration to generate the two attosecond pulses. We achieve mutual phase stability by reusing microbunching generated in the first undulator in order to seed the FEL process in the second at a detuned frequency. We measure controllable temporal delays between the two pulses directly in the time domain using angular streaking of photoelectrons, with a step size of 250 attoseconds. We then show that the behavior of the X-ray spectrum is consistent with phase stability between the two pulses, with a relative phase that can be easily tuned using inter-undulator phase shifters. This method is particularly well-suited to few to ten eV energy separations and sub to few femtosecond time delays, which are ideal for experiments in the soft X-ray regime for pushing the limits of our models for molecular dynamics and exerting direct coherent control over quantum systems.

Attosecond pulses from free-electron lasers have opened the doors to atomic site-specific studies of bound electronic dynamics on their natural, sub-femtosecond timescales. Key to their success has been electron beam shaping techniques enabling the generation of sub-femtosecond current spikes with peak currents on the order of 10 kA. We demonstrate in an RF linac the generation of current spikes with extreme chirps on the order of 350 MeV/micron, directly competitive with the chirps expected from beam-driven plasma wakefield accelerators. Leveraging chirp-taper compensation, we use these highly chirped beams to generate hard X-ray attosecond pulses with bandwidths exceeding 30 eV, a factor of two beyond previous demonstrations. We simultaneously present the first explicit experimental evidence of chirp-taper compensation in an attosecond XFEL, finding that optimal tapering improves the bandwidth and pulse energy by factors of two and five, respectively, for our conditions. In addition to the immediate utility of such broadband hard X-ray pulses, electron beams with such extreme chirps can be utilized for unique new experimental modalities by performing further compression after the undulators. Such post-lasing compression can enable subsequent superradiant light emission at longer wavelengths, or direct excitation of quantum systems with the beam's intense space-charge field for unique attosecond pump-probe possibilities.

Leveraging the full scientific capabilities of next-generation high-repetition-rate free-electron lasers requires programmable control over electron-beam properties at their source. The photoinjector drive laser defines the electron beam's initial six-dimensional phase-space distribution, yet has historically been limited to Gaussian or static flat-top profiles, with most manipulation occurring downstream. Here we demonstrate software-programmable ultraviolet pulse shaping at the LCLS-II photoinjector as a source-level actuator that complements traditional accelerator controls. Using a coupled architecture combining dispersion-controlled nonlinear frequency conversion with spatial-light-modulator spectral shaping, we generate user-defined temporal structures and observe their imprint on electron bunches through high-resolution time-domain diagnostics. Laser-imposed multi-peaked modulation persists through acceleration, magnetic compression, and undulator transport with shot-to-shot repeatability, producing clearly resolved current structure in the compressed beam. Variance-based reconstruction from transverse deflecting cavity measurements reveals structured X-ray emission profiles exhibiting temporal features consistent with the programmed laser waveform. By providing rapid, software-controlled reconfiguration of electron-beam initial conditions, this source-level control approach establishes a programmable upstream actuator for future adaptive optimization and autonomous facility operation at high-repetition-rate light sources.

One pathway to producing high brightness electron beams is to use a radio-frequency (rf) driven high field photogun to rapidly accelerate photoemitted electrons to the relativistic regime and pre- serve the brightness. However, the highest attainable field is limited by rf breakdowns of materials used in a photogun. Shortening rf pulse duration feeding into a photogun provides a viable path- way to achieve high field and prevent rf breakdowns. Here we propose and investigate Compressed Ultrashort Pulse Injector Demonstrator (CUPID), a nanosecond rf pulses driven photogun powered by a klystron and rf pulse compression system capable of achieving 300 MW at 20 ns duration, to produce bright electron beams with high electric field. We first introduce the design of the CUPID photogun and its expected rf performance at 500 MV/m driven by high power nanosecond rf pulses, followed by beam dynamics studies showing its capability for producing bright electron beams with 60 nm emittance when forming a photoinjector with a superconducting solenoid and downstream accelerating structures. Finally, we show a proof-of-concept start-to-end simulation of the CUPID photoinjector paired with the existing Linac Coherent Light Source (LCLS) copper accelerator free-electron laser (FEL) to demonstrate achievable mJ pulse energy very hard x-ray photons at 40 keV or higher.

SLAC’s LCLS-II is advancing towards MHz repetition rate attosecond X-ray pulses, creating opportunities to optimize X-ray generation through machine-driven controls and diagnostics via start-to-end simulation. Advanced laser shaping and upconversion techniques at the photoinjector, such as spatial light modulator-based pre-amplifier pulse shaping linked to nonlinear methods such as dispersion-controlled nonlinear synthesis or four-wave mixing, enable precise electron bunch control at the source. Downstream, diagnostics like the Multi-Resolution COokiebox (MRCO)—a 16-channel time-of-flight spectrometer—characterize X-ray pulse profiles, providing real-time feedback on attosecond X-ray pulses or attosecond X-ray substructure. We present developments towards a framework linking programmable photoinjector laser shaping to X-ray diagnostics, enabling data-driven optimization of the X-ray source. This approach combines machine learning, high-throughput feedback, and advanced control to align LCLS-II capabilities with experimental goals, laying the foundation for optimization of attosecond-scale precision in X-ray experiments.

The timescale for electrons to break interatomic bonds during photoinduced physical or biochemical processes such as vision or photosynthesis is femtoseconds or less. For this reason, electron dynamics in a chemical bond must be viewed with attosecond pulses, but until now, laboratory attosecond sources have been too slow or weak to capture this intrabond motion. Tunable, powerful, attosecond X-rays from free-electron lasers now fill this gap and enable the first studies of site-specific electron motion within molecules, to the best of our knowledge. Here we explain how these sources work and how to use them to explore the attosecond frontier of physics, chemistry, and biology. (c) 2025 Optica Publishing Group. All rights, including for text and data mining (TDM), Artificial Intelligence (AI) training, and similar technologies, are reserved.

In this Letter we report on the experimental generation of high energy (10 GeV), ultra-short (fs-duration), ultra-high current (0.1 MA), petawatt peak power electron beams in a particle accelerator. These extreme beams enable the exploration of a new frontier of high intensity beam-light and beam-matter interactions broadly relevant across fields ranging from laboratory astrophysics to strong field quantum electrodynamics and ultra-fast quantum chemistry. We demonstrate our ability to generate and control the properties of these electron beams by means of a laser-electron beam shaping technique. This experimental demonstration opens the door to on-the-fly customization of extreme beam current profiles for desired experiments and is poised to benefit a broad swathe of cross-cutting applications of relativistic electron beams.

We propose a scheme allowing coherent shaping, i.e., controlling both the amplitude and phase, of attosecond x-ray pulses at free-electron lasers. We show that by seeding a free-electron laser with a short coherent seed that overfills the amplification bandwidth, one can shape the Wigner function of the pulse by controlling the undulator taper profile. The examples of controllable pulse pairs and trains, as well as isolated spectrotemporally shaped pulses with very broad bandwidths are examined in detail. Existing attosecond x-ray free-electron lasers can achieve these experimental conditions in a two-stage cascade, in which the seed is generated by a short current spike in an electron bunch and shaped in an unspoiled region within the same bunch. We experimentally demonstrate the production and control of phase-stable pulse trains using this method at the Linac Coherent Light Source II.

This document outlines a community-driven Design Study for a 10 TeV pCM Wakefield Accelerator Collider. The 2020 ESPP Report emphasized the need for Advanced Accelerator R&D, and the 2023 P5 Report calls for the “delivery of an end-to-end design concept, including cost scales, with self-consistent parameters throughout." This Design Study leverages recent experimental and theoretical progress resulting from a global R&D program in order to deliver a unified, 10 TeV Wakefield Collider concept. Wakefield Accelerators provide ultra-high accelerating gradients which enables an upgrade path that will extend the reach of Linear Colliders beyond the electroweak scale. Here, we describe the organization of the Design Study including timeline and deliverables, and we detail the requirements and challenges on the path to a 10 TeV Wakefield Collider.

We present the first direct experimental confirmation of attosecond pulse generation in the hard X-ray regime with a free-electron laser. Our experiment is based on measurements of a nonlinear optical phenomenon known as amplified spontaneous emission (ASE) from 3d transition metals. By analyzing the yield of the collective X-ray fluorescence induced by ultrashort pulses at the Linac Coherent Light Source, we identify the generation of attosecond pulses and shot-to-shot fluctuations in their duration, ranging from 100 as to 400 as. The observed product of bandwidth and pulse duration for 100 as pulses is approximately 2 fs·eV, indicating the generation of nearly transform-limited pulses. Our results extend the photon energy reach of attosecond techniques by one order of magnitude, providing the ability to simultaneously probe matter on the time-scales of electronic phenomena and with atomic spatial resolution. Furthermore, attosecond hard X-ray pulses can outrun the fastest radiation damage processes, paving the way to single-shot damage-free X-ray measurements.

Attosecond photoemission or photoionization delays are a unique probe of the structure and the electronic dynamics of matter. However, the spectral congestion of valence photoelectron spectra sets fundamental limits to the complexity of systems that can be studied, and the delocalization of valence electron wave functions blurs the spatial origin of the photoelectron wave packet. Using attosecond x-ray pulses from LCLS, we demonstrate the key advantages of measuring core-level delays: The photoelectron spectra remain atomlike, the measurements become element specific, and the observed scattering dynamics originate from a pointlike source when multicenter interference effects are negligible. We exploit these unique features to reveal the effects of changing functional groups (C-H vs N) and symmetry on attosecond scattering dynamics by measuring and calculating the photoionization delays between N-1s and C-1s core shells of a series of aromatic azabenzene molecules. Remarkably, the delays increase with the number of nitrogen atoms in the molecule and reveal multiple resonances. We identify two previously unknown mechanisms regulating the associated attosecond dynamics, namely the enhanced confinement of the trapped wave function with the replacement of C-H groups by N atoms and the decrease of the coupling strength among the photoemitted partial waves with increasing symmetry. This study demonstrates the unique opportunities opened by measurements of core-level photoionization delays for unraveling attosecond electron dynamics in complex matter.

Attosecond hard x-ray pulses from the LCLS are focused to nanometer-sized spots using an advanced Kirkpatrick-Baez mirror system. Peak intensity at the focal point exceeds 1019 W/cm2, enabling a suite of damage-free nonlinear x-ray spectroscopy. (c) 2025 Optica Publishing Group under the terms of the Optica Open Access Publishing Agreement

The advent of isolated and intense sub-femtosecond X-ray pulses enables tracking of quantummechanical motion of electrons in molecules and solids. The combination of X-ray spectroscopy and diffraction imaging is a powerful approach to visualize non-equilibrium dynamics in systems beyond few atoms. However, extreme x-ray intensities introduce significant electronic damage, limiting material contrast and spatial resolution. Here we show that newly available intense subfemtosecond (sub-fs) x-ray FEL pulses can outrun most ionization cascades and partially reverse x-ray damage through stimulated x-ray emission in the vicinity of a resonance. In our experiment, we compared thousands of coherent x-ray diffraction patterns and simultaneously recorded ion spectra from individual Ne nanoparticles injected into the FEL focus. Our experimental results and theoretical modeling reveal that x-ray diffraction increases and the average charge state decreases in particles exposed to sub-fs pulses compared to those illuminated with 15-femtosecond pulses. Sub-fs exposures outrun most Auger decays and impact ionization processes, and enhance nonlinear effects such as stimulated emission, which cycle bound electrons between different states. These findings demonstrate that intense sub-fs x-ray FEL pulses are transformative for advancing high-resolution imaging and spectroscopy in chemical and material sciences, and open the possibilities of coherent control of the interaction between x-rays and complex specimen beyond few atoms.

Attosecond hard x-ray pulses from the LCLS are focused to nanometer-sized spots using an advanced Kirkpatrick-Baez mirror system. Peak intensity at the focal point exceeds 1019W/cm2, enabling a suite of damage-free nonlinear x-ray spectroscopy.

The detailed understanding of electronic coherence in quantum systems requires measurements on the attosecond timescale. Attosecond x-ray pulses enable the study of electronic coherence in core-excited molecular systems. Here we report on the coherent motion of electrons in the 1,1-difluoroethylene ion following ionization of the K shell of the two nonequivalent carbon sites with a subfemtosecond x-ray pulse. Using the angular streaking technique to track the Auger-Meitner decay, we observe temporal modulations of the emission, indicating the electronic coherence of the core-excited ionic states, and extract a 6.5±0.8 fs average lifetime of the core-level vacancies. A quantum-mechanical model is employed to interpret the measurement, and we find the observed temporal modulations are independent of charge density oscillations. This work opens a new regime of coherent electronic motion, beyond charge migration, where electronic coherence manifests in the nonlocal quantum correlation between atomic sites while charge density oscillation is absent. Our results broaden the landscape of electronic coherence in molecular systems. Published by the American Physical Society 2025