Coherent Light Source Research Articles

Multi-frame, ultrafast, x-ray microscope for imaging shockwave dynamics.

Inertial confinement fusion (ICF) holds increasing promise as a potential source of abundant, clean energy, but has been impeded by defects such as micro-voids in the ablator layer of the fuel capsules. It is critical to understand how these micro-voids interact with the laser-driven shock waves that compress the fuel pellet. At the Matter in Extreme Conditions (MEC) instrument at the Linac Coherent Light Source (LCLS), we utilized an x-ray pulse train with ns separation, an x-ray microscope, and an ultrafast x-ray imaging (UXI) detector to image shock wave interactions with micro-voids. To minimize the high- and low-frequency variations of the captured images, we incorporated principal component analysis (PCA) and image alignment for flat-field correction. After applying these techniques we generated phase and attenuation maps from a 2D hydrodynamic radiation code (xRAGE), which were used to simulate XPCI images that we qualitatively compare with experimental images, providing a one-to-one comparison for benchmarking material performance. Moreover, we implement a transport-of-intensity (TIE) based method to obtain the average projected mass density (areal density) of our experimental images, yielding insight into how defect-bearing ablator materials alter microstructural feature evolution, material compression, and shock wave propagation on ICF-relevant time scales.

Generation of a higher-order Poincaré sphere beam array with spatial coherence engineering.

We propose a protocol to synthesize a class of vector beam array in the far field with periodic higher-order Poincaré sphere (HOPS) polarization states by engineering the second-order spatial coherence structure of a partially coherent light source. We show that the polarization state of a single HOPS beam at the source plane can be mapped into a beam array in the far field when the spatial coherence of the beam source is engineered to have a lattice-like distribution. We demonstrate that the degree of polarization of the generated HOPS beam array can be conveniently controlled by modulating the transverse spatial coherence width of the source. Our method provides an additional way to construct the structured beam array and may find applications, e.g., in multiparticle manipulations.

Electrically stimulated droplet injector for reduced sample consumption in serial crystallography

With advances in X-ray free-electron lasers (XFELs), serial femtosecond crystallography (SFX) has enabled the static and dynamic structure determination for challenging proteins such as membrane protein complexes. In SFX with XFELs, the crystals are typically destroyed after interacting with a single XFEL pulse. Therefore, thousands of new crystals must be sequentially introduced into the X-ray beam to collect full data sets. Because of the serial nature of any SFX experiment, up to 99% of the sample delivered to the X-ray beam during its “off-time” between X-ray pulses is wasted due to the intrinsic pulsed nature of all current XFELs. To solve this major problem of large and often limiting sample consumption, we report on improvements of a revolutionary sample-saving method that is compatible with all current XFELs. We previously reported 3D-printed injection devices coupled with gas dynamic virtual nozzles (GDVNs) capable of generating samples containing droplets segmented by an immiscible oil phase for jetting crystal-laden droplets into the path of an XFEL. Here, we have further improved the device design by including metal electrodes inducing electrowetting effects for improved control over droplet generation frequency to stimulate the droplet release to matching the XFEL repetition rate by employing an electrical feedback mechanism. We report the improvements in this electrically triggered segmented flow approach for sample conservation in comparison with a continuous GDVN injection using the microcrystals of lysozyme and 3-deoxy-D-manno-octulosonate 8-phosphate synthase and report the segmented flow approach for sample injection applied at the Macromolecular Femtosecond Crystallography instrument at the Linear Coherent Light Source for the first time.

Rational design of a ZnO nanowire laser on a surface plasmon polariton.

Plasmonic lasers, which use the strong confinement of surface plasmon polaritons, are key parts to realize ultracompact coherent light sources at deep subwavelength scales. We propose a plasmonic laser composed of a silicon substrate, ZnO nanowire, dielectric layer, metal layer, and electrode. In this structure, the superimposed coupling of the surface plasmon mode at the metal interface with the high refractive index gain nanowire mode makes the electric field in the spacer layer significantly enhanced. The ZnO nanowire is used as gain material to provide gain compensation. The optical and electrical properties are simulated with the geometric parameters and dielectric layer material. The results show that the structure has strong confinement of the optical field and can realize a deep subwavelength constraint at a lower threshold level. It provides theoretical support for realizing ultracompact coherent light sources.

Thermally tunable and efficient second-harmonic generation on thin-film lithium niobate with integrated micro-heater.

In this Letter, we report thermo-optic tunable and efficient second-harmonic generation (SHG) based on an X-cut periodically poled lithium niobate (PPLN) waveguide. By applying an on-chip heater with thermo-isolation trenches and combining a type-0 quasi-phase matching mechanism, we experimentally achieve a high on-chip SHG conversion efficiency of 2500-3000% W-1 cm-2 and a large tuning power efficiency of 94 pm/mW inside a single 5-mm-long straight PPLN waveguide. Our design is for energy-efficient, high-performance nonlinear applications, such as wavelength conversion, highly tunable coherent light sources, and photon-pair generation.

Phase coherent noise reduction in digital holographic microscopy based on adaptive non-convex sparse regularization

Digital holographic microscopy is a new type of quantitative phase measurement tool. When a coherent light source is used for illumination, the phase coherent noise seriously affects the imaging quality and measurement accuracy. A method of phase coherent noise reduction based on adaptive non-convex sparse regularization is proposed in this paper. This denoising problem is considered as a sparse regularization model, which uses a non-convex penalty called the generalized minimax-concave; the penalty can lead to a more accurate estimation of the phase image amplitude and reduce most of the noise. Meanwhile, the threshold of the algorithm to solve this problem is guided by the edge credibility map adaptively. In edge regions, the threshold value is small so that edge details are preserved; however, in other regions, the threshold value is big so that the phase coherent noise is removed. The experimental results confirmed the validity of the proposed method.

Self-probed ptychography from semiconductor high-harmonic generation.

We demonstrate a method to image an object using a self-probing approach based on semiconductor high-harmonic generation. On the one hand, ptychography enables high-resolution imaging from the coherent light diffracted by an object. On the other hand, high-harmonic generation from crystals is emerging as a new source of extreme-ultraviolet ultrafast coherent light. We combine these two techniques by performing ptychography measurements with nanopatterned crystals serving as the object as well as the generation medium of the harmonics. We demonstrate that this strong field in situ approach can provide structural information about an object. With the future developments of crystal high harmonics as a compact short-wavelength light source, our demonstration can be an innovative approach for nanoscale imaging of photonic and electronic devices in research and industry.

Scotch-Tape and Graphene-Oxide Photomobile Polymer Film

In this work, we report on the fabrication and photonic activation of a novel kind of photomobile polymer (PMP) film based mainly on a double layered asymmetric configuration. The PMP is cheap and extremely easy to make. It is made of PVC/isoprene tape with a layer of graphene-oxide (GO) attached. Under illumination at different intensities, and with coherent and incoherent light sources, the bending of the PMP film changes considerably. In particular, we noticed a more efficient bending effect when the film is directly exposed to high light intensities or to NIR radiation in the case of incoherent light sources. For the exposure times used in our experiments, the process is completely reversible when the light source is switched off. Additionally, if we paint the side of the PVC tape exposed to light black, the film is not able to return to its starting position and the bending results are permanent. This suggests that the presence of the GO-layer is responsible for the restoration of the position of the PMP film.

Direct counterfactual quantum-communication protocol beyond a single-photon source

The direct counterfactual quantum communication protocol involving double chained Mach-Zehnder interferometers requires a single photon input. Here, we show that even with multiphoton light sources, including a strong coherent light source as inputs, the counterfactual communication can be achieved with success probability approaching unity in the ideal asymptotic limit. The path evolution of multiple photons is non-locally controlled. Thus, information is transmitted without any photons, or any other auxiliary information carriers, appearing in the public transmission channel. The effect is quantum since quantum measurements are essential requirement for this protocol. Furthermore, a modified scheme is proposed in which number of interferometers is reduced.

Encoding Higher-Order Polarization States into Robust Partially Coherent Optical Beams

Optical vector beams with a higher-order polarization state, represented by a point on a higher-order Poincar\'e sphere, have recently found advantages in various applications. However, the considered beams are usually spatially fully coherent (monochromatic), which makes them susceptible to complex environments. In this work, we introduce a coherence-engineering protocol to generate partially coherent vectorial secondary light sources in which a higher-order polarization state is encoded into the structure of electromagnetic spatial coherence. The encoded complex polarization state is well reconstructed in the far field whose global degree of polarization can be controlled with the transverse coherence length of the source. In particular, the produced partially coherent beams are highly robust against obstructions, which is demonstrated theoretically and experimentally by inserting a static obstacle against the source or introducing strong atmospheric turbulence into the transmission link. The results of this work can find useful applications in the transfer of complicated polarization-encoded information in harsh environments.

Ultrafast Suppression of the Ferroelectric Instability in KTaO_{3}.

We use an x-ray free-electron laser to study the lattice dynamics following photoexcitation with ultrafast near-UV light (wavelength 266nm, 50fs pulse duration) of the incipient ferroelectric potassium tantalate, KTaO_{3}. By probing the lattice dynamics corresponding to multiple Brillouin zones through the x-ray diffuse scattering with pulses from the Linac Coherent Light Source (LCLS) (wavelength 1.3Å and <10 fs pulse duration), we observe changes in the diffuse intensity associated with a hardening of the transverse acoustic phonon branches along Γ to X and Γ to M. Using force constants from density functional theory, we fit the quasiequilibrium intensity and obtain the instantaneous lattice temperature and density of photoexcited charge carriers. The density functional theory calculations demonstrate that photoexcitation transfers charge from oxygen 2p derived π-bonding orbitals to Ta 5d derived antibonding orbitals, further suppressing the ferroelectric instability and increasing the stability of the cubic, paraelectric structure.

Calculation of high-order harmonic generation of atoms and molecules by combining time series prediction and neural networks.

High-order harmonic generation (HHG) from the interaction of ultra-intense laser pulses with atoms is an important tabletop short-wave coherent light source. Accurate quantum simulations of it present large computational difficulties due to multi-electron multidimensional effects. In this paper, the time-dependent response of hydrogen atoms is calculated using a time-series prediction scheme, the HHG spectrum is reconstructed very accurately. The accuracy of the forecasting is further improved by using a neural network scheme. This scheme is also applied to the simulation of the harmonic emission on multi-electron systems, and the applicability of the scheme is confirmed by the harmonic calculation of complex systems. This method is expected to simulate the nonlinear dynamic process of multi-electron atoms and molecules irradiated by intense laser pulses quickly and accurately.

An Approach to Developing Cyanines with Upconverted Photosensitive Efficiency Enhancement for Highly Efficient NIR Tumor Phototheranostics.

Upconverted reactive oxygen species (ROS) photosensitization with one-photon excitation mode is a promising tactic to elongate the excitation wavelengths of photosensitive dyes to near-infrared (NIR) light region without the requirement of coherent high-intensity light sources. However, the photosensitization efficiencies are still finite by the unilateral improvement of excited-state intersystem crossing (ISC) via heavy-atom-effect, since the upconverted efficiency also plays a decisive role in upconverted photosensitization. Herein, a NIR light initiated one-photon upconversion heavy-atom-free small molecule system is reported. The meso-rotatable anthracene in pentamethine cyanine (Cy5) is demonstrated to enrich the populations in high vibrational-rotational energy levels and subsequently improve the hot-band absorption (HBA) efficiency. Moreover, the spin-orbit charge transfer intersystem crossing (SOCT-ISC) caused by electron donated anthracene can further amplify the triplet yield. Benefiting from the above two aspects, the 1 O2 generation significantly increases with over 2-fold improved performance compared with heavy-atom-modified method under upconverted light excitation, which obtains efficient in vivo phototheranostic results and provides new opportunities for other applications such as photocatalysis and fine chemical synthesis.

Mid-infrared ultra-broadband optical Kerr frequency comb based on a CdTe ring microresonator: a theoretical investigation.

Microresonator Kerr frequency combs are coherent light sources that emit broadband spectrum of evenly spaced narrow lines in an optical microresonator, which provide breakthroughs in many technological areas, such as spectroscopy, metrology, optical telecommunications, and molecular sensing. The development of mid-infrared (MIR) optical frequency comb (OFC) based on microresonators could pave the way for high performance spectroscopy in the MIR "molecular fingerprint" region. However, the generation of microresonator MIR OFC, especially towards the long-wavelength MIR (>10 µm) region, is prohibited by the transmission window of the commonly used Kerr optical media such as Si and Si3N4, and low nonlinearity at long wavelengths. Here, we seek the possibility to realize an ultra-broadband frequency comb operating in the long-wavelength MIR region based on a cadmium telluride (CdTe) ring microresonator. CdTe features a broad transmission range covering the wavelengths of 1∼25 µm, a flat dispersion profile, and an extraordinary third-order nonlinear refractive index (∼1.4 × 10-17 m2W-1 at 7 µm) which is 2-order greater than that of Si3N4, making it a promising platform to realize MIR Kerr frequency comb. Based on the above excellent optical properties, we design a CdTe/cadmium sulfide (CdS)/Si heterojunction microring resonator to generate an ultra-broadband MIR OFC. Through the numerical simulation, the geometric parameters (width, height, and radius) of the microresonator, polarization, wavelength of the pump, and quality factor are investigated and optimized. As a result, a MIR OFC covering 3.5∼18 µm is numerically demonstrated by using the pump wavelength of 7 µm and a pump power of 500 mW. This is the first simulation demonstration of Kerr OFC with the spectral range extending beyond 10 µm, to the best of our knowledge. This work provides new opportunities for the realization of ultrabroad microresonator frequency combs based on novel Kerr optical medium, which can find important applications ranging from calibration of astronomical spectrographs to high-fidelity molecular spectroscopy.

Nonsequential two-photon absorption in solid Ge irradiated by an intense x-ray free-electron-laser pulse

We theoretically investigate the formation of highly charged ions in a germanium (Ge) solid driven by intense, ultrashort x-ray pulses and its effect on the cross sections for nonsequential two-photon absorption from the $K$ shell. Our investigation is related to an experiment conducted at the Linac Coherent Light Source, in which $K\ensuremath{\alpha}$ fluorescence was measured to identify nonsequential two-photon ionization. When a solid Ge target is irradiated by an intense x-ray free-electron-laser (XFEL) pulse, it undergoes severe ionization and turns into a plasma state. We employ a Monte Carlo molecular-dynamics approach to simulate the time evolution of Ge plasma formation, and the time-dependent configuration-interaction-singles method for cross-section calculations, taking into account various experimental x-ray beam parameters and Ge charge states created during the plasma formation dynamics. We find that under the given experimental condition at a photon energy of 7200 eV, charged ions are formed quickly (the average charge is $\ensuremath{\approx}+6$ at the peak of the pulse and $\ensuremath{\approx}+10$ at the end of the pulse). The cross sections of Ge for nonsequential two-photon absorption, however, turn out to be insensitive to different charge states, and the average value over all computed data is $(2.61\ifmmode\pm\else\textpm\fi{}0.05)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}59}\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{4}\phantom{\rule{0.16em}{0ex}}\mathrm{s}$. Our paper proposes a theoretical framework of photoabsorption cross-section calculations under the influence of plasma formation, when a solid target is employed in XFEL experiments.

Femtosecond diffraction studies of the sodium chloride phase diagram under laser shock compression

The phase diagram of sodium chloride (NaCl) under laser shock compression has been studied at Linac Coherent Light Source (LCLS) at the x-ray free-electron laser facility. Both solid–solid (B1 → B2) and solid–liquid (B2 → liquid) transitions have been observed along the Hugoniot over nanosecond time scales. By combining structural measurements through in situ x-ray diffraction, pressure determination through velocimetry, and a thermal equation-of-state, the shock-compressed data are used to constrain the phase diagram of NaCl. Transformation into the B2 phase is found to occur at 28(2) GPa, and B2–liquid coexistence is observed between 54(4) and 66(6) GPa, with near full melt at 66(6) GPa. Late-time pressure release from an initial shocked B2-state results in a B2 → B1 back transformation. Our results show agreement with previous static compression data, suggesting that the time scale for melting is very rapid and that equilibrium states in NaCl are being accessed over nanosecond time scales. A multiphase equation-of-state description of NaCl incorporated into a one-dimensional hydrocode is used to interpret pressure and temperature evolution over these rapid time scales.

Preserving High‐Q Lattice Plasmon Resonances for Poor Spatial Coherence of Light: Application in Enhanced Second Harmonic Generation

AbstractSurface lattice plasmon resonances (SLPR) in periodic arrays of metal nanostructures can feature a narrow spectral linewidth in case of the spectral overlap between the localized plasmons and Rayleigh anomalies. However, because of strong angular dispersion in experimental realizations, the excitation of SLPR requires collimated light, which has high spatial coherence. Here, excellent quality (Q)‐factor preservation in 1D all‐metallic nanograting metasurfaces due to the unique angular dispersion is reported. A high Q‐factor around 400 is obtained even when poor collimation, a numerical aperture (NA) objective with NA = 0.4, is employed for focusing the excitation light. With the advantages of highly focused excitation and high Q‐factor of the SLPR, a strong enhancement of second harmonic generation is realized from the proposed metasurface integrated with a few‐layers of GaSe flake. The results demonstrate that a 1D all‐metallic nanograting metasurface can overcome the demand for collimated light for the SLP resonances and manipulate focused light beams. The avenue of research proposed in this paper can open the door for the use of plasmonic metamaterials with SLPRs in many practical applications involving poorly coherent light sources, like the optoelectronic devices utilizing solar and daylight illuminations.

Camera-Derived Photoplethysmography (rPPG) and Speckle Plethysmography (rSPG): Comparing Reflective and Transmissive Mode at Various Integration Times Using LEDs and Lasers.

Background: Although both speckle plethysmography (SPG) and photoplethysmography (PPG) examine pulsatile changes in the vasculature using opto-electronics, PPG has a long history, whereas SPG is relatively new and less explored. The aim of this study was to compare the effects of integration time and light-source coherence on signal quality and waveform morphology for reflective and transmissive rSPG and rPPG. Methods: (A) Using time-domain multiplexing, we illuminated 10 human index fingers with pulsed lasers versus LEDs (both at 639 and 850 nm), in transmissive versus reflective mode. A synchronized camera (Basler acA2000-340 km, 25 cm distance, 200 fps) captured and demultiplexed four video channels (50 fps/channel) in four stages defined by illumination mode. From all video channels, we derived rPPG and rSPG, and applied a signal quality index (SQI, scale: Good > 0.95; Medium 0.95–0.85; Low 0.85–0.8; Negligible < 0.8); (B) For transmission videos only, we additionally calculated the intensity threshold area (ITA), as the area of the imaging exceeding a certain intensity value and used linear regression analysis to understand unexpected similarities between rPPG and rSPG. Results: All mean SQI-values. Reflective mode: Laser-rSPG > 0.965, LED-rSPG < 0.78, rPPG < 0.845. Transmissive mode: 0.853–0.989 for rSPG and rPPG at all illumination settings. Coherent mode: Reflective rSPG > 0.951, reflective rPPG < 0.740, transmissive rSPG and rPPG 0.990–0.898. Incoherent mode: Reflective all <0.798 and transmissive all 0.92–0.987. Linear regressions revealed similar R2 values of rPPG with rSPG (R2 = 0.99) and ITA (R2 = 0.98); Discussion: Laser-rSPG and LED-rPPG produced different waveforms in reflection, but not in transmission. We created the concept of ITA to investigate this behavior. Conclusions: Reflective Laser-SPG truly originated from coherence. Transmissive Laser-rSPG showed a loss of speckles, accompanied by waveform changes towards rPPG. Diffuse spatial intensity modulation polluted spatial-mode SPG.

Megahertz pulse trains enable multi-hit serial femtosecond crystallography experiments at X-ray free electron lasers

The European X-ray Free Electron Laser (XFEL) and Linac Coherent Light Source (LCLS) II are extremely intense sources of X-rays capable of generating Serial Femtosecond Crystallography (SFX) data at megahertz (MHz) repetition rates. Previous work has shown that it is possible to use consecutive X-ray pulses to collect diffraction patterns from individual crystals. Here, we exploit the MHz pulse structure of the European XFEL to obtain two complete datasets from the same lysozyme crystal, first hit and the second hit, before it exits the beam. The two datasets, separated by <1 µs, yield up to 2.1 Å resolution structures. Comparisons between the two structures reveal no indications of radiation damage or significant changes within the active site, consistent with the calculated dose estimates. This demonstrates MHz SFX can be used as a tool for tracking sub-microsecond structural changes in individual single crystals, a technique we refer to as multi-hit SFX.

Confining Light in Porous Perovskite Heterostructures for Light Amplification

Nanostructured porous media are capable of modulating light transport via diffusion or localization, while their combination with optical gain offers a solution to creating coherent light sources. Herein, we report on the development of a new class of optically active porous medium–porous perovskite heterostructures and demonstrate their potential in confining light via strong scattering for light amplification. Such heterostructures are chemically composed of 2D-networked CsPb2Br5 and 3D-networked CsPbBr3, which are attained upon direct water stimuli of 0D-networked Cs4PbBr6. Optical imaging reveals that light trajectories due to whispering gallery modes are formed in Cs4PbBr6 resonators to offer optical feedback for lasing. In contrast, light scattering due to structural inhomogeneity suppresses whispering gallery modes in porous heterostructures, while light is mainly confined in the pumping region. Despite the poor definition of microscopic cavities due to local disorder, the pump threshold of the porous heterostructure is only 1/3 to 1/5 that of Cs4PbBr6 and comparable to that of CsPbBr3 reported previously. Eigenvalue modeling was performed to analyze the eigenmodes, revealing that porous perovskite heterostructures support high-quality eigenmodes for lasing. The results suggest that perovskite heterostructures with interconnected porous scaffolds serve as promising complex nanophotonic systems for fundamental studies and potential applications.