Bacteriorhodopsin: Structural Insights Revealed Using X-Ray Lasers and Synchrotron Radiation.

Directional transport of protons across an energy transducing membrane-proton pumping-is ubiquitous in biology. Bacteriorhodopsin (bR) is a light-driven proton pump that is activated by a buried all-trans retinal chromophore being photoisomerized to a 13-cis conformation. The mechanism by which photoisomerization initiates directional proton transport against a proton concentration gradient has been studied by a myriad of biochemical, biophysical, and structural techniques. X-ray free electron lasers (XFELs) have created new opportunities to probe the structural dynamics of bR at room temperature on timescales from femtoseconds to milliseconds using time-resolved serial femtosecond crystallography (TR-SFX). Wereview these recent developments and highlight where XFEL studies reveal new details concerning the structural mechanism of retinal photoisomerization and proton pumping. We also discuss the extent to which these insights were anticipated by earlier intermediate trapping studies using synchrotron radiation. TR-SFX will open up the field for dynamical studies of other proteins that are not naturally light-sensitive.

Light emission by free electrons in photonic time-crystals.

Photonic time-crystals (PTCs) are spatially homogeneous media whose electromagnetic susceptibility varies periodically in time, causing temporal reflections and refractions for any wave propagating within the medium. The time-reflected and time-refracted waves interfere, giving rise to Floquet modes with momentum bands separated by momentum gaps (rather than energy bands and energy gaps, as in photonic crystals). Here, we present a study on the emission of radiation by free electrons in PTCs. We show that a free electron moving in a PTC spontaneously emits radiation, and when associated with momentum-gap modes, the electron emission process is exponentially amplified by the modulation of the refractive index. Moreover, under strong electron-photon coupling, the quantum formulation reveals that the spontaneous emission into the PTC bandgap experiences destructive quantum interference with the emission of the electron into the PTC band modes, leading to suppression of the interdependent emission. Free-electron physics in PTCs offers a platform for studying a plethora of exciting phenomena, such as radiating dipoles moving at relativistic speeds and highly efficient quantum interactions with free electrons.

A perfect X-ray beam splitter and its applications to time-domain interferometry and quantum optics exploiting free-electron lasers.

X-ray free-electron lasers (FELs) deliver ultrabright X-ray pulses, but not the sequences of phase-coherent pulses required for time-domain interferometry and control of quantum states. For conventional split-and-delay schemes to produce such sequences, the challenge stems from extreme stability requirements when splitting Ångstrom wavelength beams, where the tiniest path-length differences introduce phase jitter. We describe an FEL mode based on selective electron-bunch degradation and transverse beam shaping in the accelerator, combined with a self-seeded photon emission scheme. Instead of splitting the photon pulses after their generation by the FEL, we split the electron bunch in the accelerator, prior to photon generation, to obtain phase-locked X-ray pulses with subfemtosecond duration. Time-domain interferometry becomes possible, enabling the concomitant program of classical and quantum optics experiments with X-rays. The scheme leads to scientific benefits of cutting-edge FELs with attosecond and/or high-repetition rate capabilities, ranging from the X-ray analog of Fourier transform infrared spectroscopy to damage-free measurements.

Generalized Optical Binding for Multiple Assemblies of Nanoparticles under Multiple Laser Beams.

Optical forces enable noncontact manipulation of micro- and nanoscale objects, offering diverse applications. When a laser beam irradiates multiple nanoparticles in a solvent, it induces the formation of an ordered array with a finite distance between particles due to optical binding, which results from the optical force exerted by scattered light. This scattered light extends beyond the irradiation area, facilitating interactions between spatially separated nanoparticle assemblies under multiple laser beams. However, the extension of optical binding in this context remains underexplored. In this study, we propose a concept of generalized optical binding between particle assemblies using two focal laser beams. Under carefully designed conditions, the scattered light between assemblies leads the particles to stable positions and impedes rotational dynamics driven by the circular polarization of the lasers. We demonstrate the fusion and reordering of two hexagonal assemblies, offering a blueprint for creating on-demand particle arrays through laser beam manipulation.

A Gold Needle Tip Array Ultrafast Electron Source with High Beam Quality.

Electron sources are crucial elements in diverse applications such as electron microscopes, synchrotrons, and free-electron lasers. Nanometer-sharp needle tips are electron emitters with the highest beam quality, yet for a single needle the current is limited. Combining the emission of multiple needles promises large current yields while preserving the individual emitters' favorable properties. We present an ultrafast electron source consisting of a lithographically fabricated array of sharp gold tips illuminated with 25 fs laser pulses. The source provides up to 2000 electrons per pulse for moderate laser peak intensities of 1011 W/cm2 and a narrow energy width of 0.5 ± 0.05 eV at low current. The electron beam has a well-behaved Gaussian profile and is highly collimated, yielding a small normalized emittance on the order of nm·rad. These properties are well suited for applications requiring both high current and spatial resolution, such as free-electron light sources and chip-based particle accelerators.

Near-Infrared II Photobiomodulation Preconditioning Ameliorates Stroke Injury via Phosphorylation of eNOS.

BACKGROUND: The current management of patients with stroke with intravenous thrombolysis and endovascular thrombectomy is effective only when it is timely performed on an appropriately selected but minor fraction of patients. The development of novel adjunctive therapy is highly desired to reduce morbidity and mortality with stroke. Since endothelial dysfunction is implicated in the pathogenesis of stroke and is featured with suppressed endothelial nitric oxide synthase (eNOS) with concomitant nitric oxide deficiency, restoring endothelial nitric oxide represents a promising approach to treating stroke injury. METHODS: This is a preclinical proof-of-concept study to determine the therapeutic effect of transcranial treatment with a low-power near-infrared laser in a mouse model of ischemic stroke. The laser treatment was performed before the middle cerebral artery occlusion with a filament. To determine the involvement of eNOS phosphorylation, unphosphorylatable eNOS S1176A knock-in mice were used. Each measurement was analyzed by a 2-way ANOVA to assess the effect of the treatment on cerebral blood flow with laser Doppler flowmetry, eNOS phosphorylation by immunoblot analysis, and stroke outcomes by infarct volumes and neurological deficits. RESULTS: Pretreatment with a 1064-nm laser at an irradiance of 50 mW/cm2 improved cerebral blood flow, eNOS phosphorylation, and stroke outcomes. CONCLUSIONS: Near-infrared II photobiomodulation could offer a noninvasive and low-risk adjunctive therapy for stroke injury. This new modality using a physical parameter merits further consideration to develop innovative therapies to prevent and treat a wide array of cardiovascular diseases.

"Giant" Colloidal Quantum Well Heterostructures of CdSe@CdS Core@Shell Nanoplatelets from 9.5 to 17.5 Monolayers in Thickness Enabling Ultra-High Gain Lasing.

Semiconductor colloidal quantum wells (CQWs) have emerged as a promising class of gain materials to be used in colloidal lasers. Although low gain thresholds are achieved, the required high gain coefficient levels are barely met for the applications of electrically-driven lasers which entails a very thin gain matrix to avoid charge injection limitations. Here, "giant" CdSe@CdS colloidal quantum well heterostructures of 9.5 to 17.5 monolayers (ML) in total with corresponding vertical thickness from 3.0 to 5.8 nm that enable record optical gain is shown. These CQWs achieve ultra-high material gain coefficients up to ≈140 000 cm-1, obtained by systematic variable stripe length (VSL) measurements and independently validated by transient absorption (TA) measurements, owing to their high number of states. This exceptional gain capacity is an order of magnitude higher than the best levels reported for the colloidal quantum dots. From the dispersion of these quantum wells, low threshold amplified spontaneous emission in water providing an excellent platform for optofluidic lasers is demonstrated. Also, employing these giant quantum wells, whispering gallery mode (WGM) lasing with an ultra-low threshold of 8 µJ cm-2 is demonstrated. These findings indicate that giant CQWs offer an exceptional platform for colloidal thin-film lasers and in-solution lasing applications.

Harmonic Imaging of Stem Cells in Whole Blood at GHz Pixel Rate.

The pre-clinical validation of cell therapies requires monitoring the biodistribution of transplanted cells in tissues of host organisms. Real-time detection of these cells in the circulatory system and identification of their aggregation state is a crucial piece of information, but necessitates deep penetration and fast imaging with high selectivity, subcellular resolution, and high throughput. In this study, multiphoton-based in-flow detection of human stem cells in whole, unfiltered blood is demonstrated in a microfluidic channel. The approach relies on a multiphoton microscope with diffractive scanning in the direction perpendicular to the flow via a rapidly wavelength-swept laser. Stem cells are labeled with metal oxide harmonic nanoparticles. Thanks to their strong and quasi-instantaneous second harmonic generation (SHG), an imaging rate in excess of 10 000 frames per second is achieved with pixel dwell times of 1 ns, a duration shorter than typical fluorescence lifetimes yet compatible with SHG. Through automated cell identification and segmentation, morphological features of each individual detected event are extracted and cell aggregates are distinguished from isolated cells. This combination of high-speed multiphoton microscopy and high-sensitivity SHG nanoparticle labeling in turbid media promises the detection of rare cells in the bloodstream for assessing novel cell-based therapies.

Exploring Carbon Dots: Green Nanomaterials for Unconventional Lasing.

In recent years, the progress toward lighting miniaturization is focused on luminescent nanomaterials. Among them, fluorescent carbon dots (CDs) are receiving increasing attention thanks to their astonishing optical properties complemented by their intrinsic biocompatibility and low toxicity. The CDs can be easily dispersed in water, organic solvents or incorporated in polymeric matrices, preserving their emission properties. However, the relationship between their structural and optical properties is still not fully elucidated, motivating a consistent research effort for the comprehension of their features. Nevertheless, CDs demonstrate to be efficient gain materials for lasing, thanks to their high quantum yield (QY), emission tunability in the visible and near infrared (NIR) range, short lifetimes, and high absorption cross section, even if the synthetic reproducibility, the low reaction yield and the spectral width of the emission may limit their effective exploitation. This review summarizes the latest advancements in the investigation of the characteristic properties of CDs that make laser action possible, illustrating optical geometries for lasing and random lasing, both in solution and solid state, and the few currently demonstrated breakthroughs. While the journey toward their effective application is still long, the potential of CD-based laser sources is promising in various technological fields and futuristic perspectives will be discussed.

Strong Laser Emission Modulation by Coherent Perfect Absorption Inside Complex-Coupled Distributed Feedback Laser Diodes.

The proof-of-concept of the exploitation of Coherent Perfect Absorption (CPA) in electrically-injected distributed-feedback laser sources is reported. Capitalizing on the essence of CPA as "light extinction by light", an integrated laser-modulator scheme emerges. The key ingredient compared to conventional single-frequency laser diodes is a careful periodic in-phase modulation of both real and imaginary parts of the complex grating index profile that enables both single-frequency operation and 40 dB line purity at the Bragg frequency. It is shown that this combination is most apt for the operation of CPA as a modulation mechanism that respects the laser spectral purity. The specific proof-of-concept is based on an ultra-short external cavity formed by a metallic micro-mirror, whose role is to generate the second beam of more conventional CPA interferometric approaches. The implemented complex-coupled grating is compatible with existing industrial technologies and promising for real-life laser source applications. Furthermore, the concept can be directly transferred to other material platforms and other wavelengths ranging from terahertz to ultraviolet.

Enhanced X-ray free-electron laser performance with optical klystron and helical undulators.

This article presents a demonstration of the improved performance of an X-ray free-electron laser (FEL) using the optical klystron mechanism and helical undulator configuration, in comparison with the common planar undulator configuration without optical klystron. The demonstration was carried out at Athos, the soft X-ray beamline of SwissFEL. Athos has variable-polarization undulators, and small magnetic chicanes placed between every two undulators to fully exploit the optical klystron. It was found that, for wavelengths of 1.24 nm and 3.10 nm, the required length to achieve FEL saturation is reduced by about 35% when using both the optical klystron and helical undulators, with each effect accounting for about half of the improvement. Moreover, it is shown that a helical undulator configuration provides a 20% to 50% higher pulse energy than planar undulators. This work represents an important step towards more compact and high-power FELs, rendering this key technology more efficient, affordable and accessible to the scientific community.

Correlation of refractive index based and THz streaking arrival time tools for a hard X-ray free-electron laser.

To fully exploit ultra-short X-ray pulse durations routinely available at X-ray free-electron lasers to follow out-of-equilibrium dynamics, inherent arrival time fluctuations of the X-ray pulse with an external perturbing laser pulse need to be measured. In this work, two methods of arrival time measurement were compared to measure the arrival time jitter of hard X-ray pulses. The methods were photoelectron streaking by a THz field and a transient refractive index change of a semiconductor. The methods were validated by shot-to-shot correction of a pump-probe transient reflectivity measurement. An ultimate shot-to-shot full width at half-maximum error between the devices of 19.2 ± 0.1 fs was measured.

Development of a portable and cost-effective femtosecond fibre laser synchronizable with synchrotron X-ray pulses.

This study introduces a compact, portable femtosecond fibre laser system designed for synchronization with SPring-8 synchrotron X-ray pulses in a uniform filling mode. Unlike traditional titanium-sapphire mode-locked lasers, which are fixed installations, our system utilizes fibre laser technology to provide a practical alternative for time-resolved spectroscopy, striking a balance between usability, portability and cost-efficiency. Comprehensive evaluations, including pulse characterization, timing jitter and frequency stability tests revealed a centre wavelength of 1600 nm, a pulse energy of 4.5 nJ, a pulse duration of 35 fs with a timing jitter of less than 9 ps, confirming the suitability of the system for time-resolved spectroscopic studies. This development enhances the feasibility of experiments that combine synchrotron X-rays and laser pulses, offering significant scientific contributions by enabling more flexible and diverse research applications.

Development and commissioning of a broadband online X-ray spectrometer for the SXFEL Facility.

A broadband online X-ray spectrometer has been designed and commissioned at the SUD beamline of the Shanghai Soft X-ray Free-Electron Laser Facility, which can deliver both SASE and seeded FEL pulses to user experiments, spanning the photon energy range of 50-620 eV. The resolving powers of the spectrometer calibrated via online measurement at 92 eV and 249 eV are ∼20000 and ∼15000, respectively, and the absolute photon energy is characterized by an electron time-of-flight spectrometer. The high energy resolution provided by the spectrometer can differentiate the fine structure in the FEL spectrum, to determine its pulse length.

Diamond sensors for hard X-ray energy and position resolving measurements at the European XFEL.

The diagnostics of X-ray beam properties has a critical importance at the European X-ray Free-Electron Laser facility. Besides existing diagnostic components, utilization of a diamond sensor was proposed to achieve radiation-hard, non-invasive beam position and pulse energy measurements for hard X-rays. In particular, with very hard X-rays, diamond-based sensors become a useful complement to gas-based devices which lose sensitivity due to significantly reduced gas cross-sections. The measurements presented in this work were performed with diamond sensors consisting of an electronic-grade single-crystal chemical-vapor-deposition diamond with position-sensitive resistive electrodes in a duo-lateral configuration. The results show that the diamond sensor delivers pulse-resolved X-ray beam position data at 2.25 MHz with an uncertainty of less than 1% of the beam size. To our knowledge this is the first demonstration of pulse-resolved position measurements at the MHz rate using a transmissive diamond sensor at a free-electron laser facility. It can therefore be a valuable tool for X-ray free-electron lasers, especially for high-repetition-rate machines, enabling applications such as beam-based alignment and intra-pulse-train position feedback.

Hard X-ray operation of X-ray gas monitors at the European XFEL.

X-ray gas monitors (XGMs) are operated at the European XFEL for non-invasive single-shot pulse energy measurements and average beam-position monitoring. The underlying measurement principle is the photo-ionization of rare gas atoms at low gas pressures and the detection of the photo-ions and photo-electrons created. These are essential for tuning and sustaining self-amplified spontaneous emission (SASE) operation, machine radiation safety, and sorting single-shot experimental data according to pulse energy. In this paper, the first results from XGM operation at photon energies up to 30 keV are presented, which are far beyond the original specification of this device. Here, the Huge Aperture MultiPlier (HAMP) is used for single-shot pulse energy measurements since the standard X-ray gas monitor detectors (XGMDs) do not provide a sufficient signal-to-noise ratio, even at the highest operating gas pressures. A single-shot correlation coefficient of 0.98 is measured between consecutive XGMs operated with HAMP, which is as good as measuring with the standard XGMD detectors. An intra-train non-linearity of the HAMP signal is discovered, and operation parameters to mitigate this effect are studied. The upper repetition rate limit of HAMP operation at 2.25 MHz is also determined. Finally, the possibilities and limits for future XGM operation at photon energies up to 50 keV are discussed.

X-ray optics for the cavity-based X-ray free-electron laser.

A cavity-based X-ray free-electron laser (CBXFEL) is a possible future direction in the development of fully coherent X-ray sources. CBXFELs consist of a low-emittance electron source, a magnet system with several undulators and chicanes, and an X-ray cavity. The X-ray cavity stores and circulates X-ray pulses for repeated FEL interactions with electron pulses until the FEL reaches saturation. CBXFEL cavities require low-loss wavefront-preserving optical components: near-100%-reflectivity X-ray diamond Bragg-reflecting crystals, outcoupling devices such as thin diamond membranes or X-ray gratings, and aberration-free focusing elements. In the framework of the collaborative CBXFEL research and development project of Argonne National Laboratory, SLAC National Accelerator Laboratory and SPring-8, we report here the design, manufacturing and characterization of X-ray optical components for the CBXFEL cavity, which include high-reflectivity diamond crystal mirrors, a diamond drumhead crystal with thin membranes, beryllium refractive lenses and channel-cut Si monochromators. All the designed optical components have been fully characterized at the Advanced Photon Source to demonstrate their suitability for the CBXFEL cavity application.

X-ray beam diagnostics at the MID instrument of the European X-ray Free-Electron Laser Facility.

The Materials Imaging and Dynamics (MID) instrument at the European X-ray Free-Electron Laser Facility (EuXFEL) is equipped with a multipurpose diagnostic end-station (DES) at the end of the instrument. The imager unit in DES is a key tool for aligning the beam to a standard trajectory and for adjusting optical elements such as focusing lenses or the split-and-delay line. Furthermore, the DES features a bent-diamond-crystal spectrometer to disperse the spectrum of the direct beam to a line detector. This enables pulse-resolved characterization of the EuXFEL spectrum to provide X-ray energy calibration, and the spectrometer is particularly useful in commissioning special modes of the accelerator. Together with diamond-based intensity monitors, the imager and spectrometer form the DES unit which also contains a heavy-duty beamstop at the end of the MID instrument. Here, we describe the setup in detail and provide exemplary beam diagnostic results.

A 1D imaging soft X-ray spectrometer for the small quantum systems instrument at the European XFEL.

A 1D imaging soft X-ray spectrometer installed on the small quantum systems (SQS) scientific instrument of the European XFEL is described. It uses movable cylindrical constant-line-spacing gratings in the Rowland configuration for energy dispersion in the vertical plane, and Wolter optics for simultaneous 1D imaging of the source in the horizontal plane. The soft X-ray fluorescence spectro-imaging capability will be exploited in pump-probe measurements and in investigations of propagation effects and other nonlinear phenomena.

The development and application of matrix assisted laser desorption electrospray ionization: The teenage years.

In the past 15 years, ambient ionization techniques have witnessed a significant incursion into the field of mass spectrometry imaging, demonstrating their ability to provide complementary information to matrix-assisted laser desorption ionization. Matrix-assisted laser desorption electrospray ionization is one such technique that has evolved since its first demonstrations with ultraviolet lasers coupled to Fourier transform-ion cyclotron resonance mass spectrometers to extensive use with infrared lasers coupled to orbitrap-based mass spectrometers. Concurrently, there have been transformative developments of this imaging platform due to the high level of control the principal group has retained over the laser technology, data acquisition software (RastirX), instrument communication, and image processing software (MSiReader). This review will discuss the developments of MALDESI since its first laboratory demonstration in 2005 to the most recent advances in 2021.