The Liquid Jet Endstation for Hard X-ray Scattering and Spectroscopy at the Linac Coherent Light Source.

The ability to study chemical dynamics on ultrafast timescales has greatly advanced with the introduction of X-ray free electron lasers (XFELs) providing short pulses of intense X-rays tailored to probe atomic structure and electronic configuration. Fully exploiting the full potential of XFELs requires specialized experimental endstations along with the development of techniques and methods to successfully carry out experiments. The liquid jet endstation (LJE) at the Linac Coherent Light Source (LCLS) has been developed to study photochemistry and biochemistry in solution systems using a combination of X-ray solution scattering (XSS), X-ray absorption spectroscopy (XAS), and X-ray emission spectroscopy (XES). The pump-probe setup utilizes an optical laser to excite the sample, which is subsequently probed by a hard X-ray pulse to resolve structural and electronic dynamics at their intrinsic femtosecond timescales. The LJE ensures reliable sample delivery to the X-ray interaction point via various liquid jets, enabling rapid replenishment of thin samples with millimolar concentrations and low sample volumes at the 120 Hz repetition rate of the LCLS beam. This paper provides a detailed description of the LJE design and of the techniques it enables, with an emphasis on the diagnostics required for real-time monitoring of the liquid jet and on the spatiotemporal overlap methods used to optimize the signal. Additionally, various scientific examples are discussed, highlighting the versatility of the LJE.

Compact Ho:YLF-pumped ZnGeP2-based optical parametric amplifiers tunable in the molecular fingerprint regime.

We report on a compact mid-infrared laser architecture, comprising a chain of $ {\rm ZnGeP}_2 $ZnGeP2-based optical parametric amplifiers (OPAs), which afford a higher energy yield ($ \mathbin{\lower.3ex\hbox{$\buildrel \lt \over{\smash{\scriptstyle\sim}\vphantom{_x}}$}} 60\;\unicode{x00B5} {\rm J} $∼x<60µJ at 1 kHz) compared to most conventional OPA gain media transparent in the 2-8-µm wavelength range. Specifically, our OPA scheme allows ready tunability in the molecular fingerprint regime and is tailored for strong-field excitation and coherent control of both stretch and bend (or torsional) vibrational modes in molecules. The OPAs are pumped and directly seeded (via supercontinuum generation) by a 2-µm, 3-ps Ho:YLF regenerative amplifier. The compressibility of the OPA output is demonstrated by a representative measurement of the near-Gaussian temporal profile of a dispersion-compensated 105-fs idler pulse at a central wavelength of 5.1 µm, corresponding to ${\sim}6 $∼6 optical cycles. Detailed numerical simulations closely corroborate the experimental measurements, providing a benchmark and a platform to further explore the parameter space for future design, optimization, and implementation of high-energy, ultrafast, mid-infrared laser schemes.

Multi-octave supercontinuum generation in YAG pumped by mid-infrared, multi-picosecond pulses.

High-energy, multi-octave supercontinuum (SC) generation in bulk media pumped with picosecond pulses in the mid-infrared, though pivotal in a myriad of applications, poses severe constraints due to wavelength scaling of the critical power criterion and the propensity to induce avalanche-ionization-seeded breakdown mechanisms. Here, we demonstrate a simple experimental geometry, relying on a very low numerical aperture for the pump pulse, and a crystal length commensurate with the Rayleigh length of the focusing geometry, generating a multi-octave, stable SC in yttrium aluminum garnet (YAG). The SC ranges from 500 nm to 3.5 µm (measured at -30 dB with spectral components at wavelengths up to 4.5 µm) when pumped by a 3 ps pulse centered at 2.05 µm in the anomalous dispersion regime. We also investigate the dynamics of filament formation in this interaction regime by monitoring the spectral and temporal evolution of the pulse during its propagation through the length of the crystal.

Mapping the Damping Dynamics of Mega-Ampere Electron Pulses Inside a Solid.

We report the lifetime of intense-laser (2×10^{19} W/cm^{2}) generated relativistic electron pulses in solids by measuring the time evolution of their Cherenkov emission. Using a picosecond resolution optical Kerr gating technique, we demonstrate that the electrons remain relativistic as long as 50 picoseconds-more than 1000 times longer than the incident light pulse. Numerical simulations of the propagation of relativistic electrons and the emitted Cherenkov radiation with Monte Carlo geant4 package reproduce the striking experimental findings.

Intense femtosecond laser driven collimated fast electron transport in a dielectric medium-role of intensity contrast.

Ultra-high intensity (> 1018 W/cm2), femtosecond (~30 fs) laser induced fast electron transport in a transparent dielectric has been studied for two laser systems having three orders of magnitude different peak to pedestal intensity contrast, using ultrafast time-resolved shadowgraphy. Use of a 400 nm femtosecond pulse as a probe enables the exclusive visualization of the dynamics of highest density electrons (> 7 × 1021 cm-3) observed so far. High picosecond contrast (~109) results in greater coupling of peak laser energy to the plasma electrons, enabling long (~1 mm), collimated (divergence angle ~2°) transport of fast electrons inside the dielectric medium at relativistic speeds (~0.66c). In comparison, the laser system with a contrast of ~106 has a large pre-plasma, limiting the coupling of laser energy to the solid and yielding limited fast electron injection into the dielectric. In the lower contrast case, bulk of the electrons expand as a cloud inside the medium with an order of magnitude lower speed than that of the fast electrons obtained with the high contrast laser. The expansion speed of the plasma towards vacuum is similar for the two contrasts.

Enhanced x-ray emission from nano-particle doped bacteria.

Recently, it has been greatly appreciated that intense light matter interaction is modified due to the nano- and microstructures in the target by--surface plasmons, laser energy localization scattering etc. Extreme laser intensities produce dense plasmas and collective mechanisms generate energetic electrons, ions and hard x-rays. Recently, it is postulated that the anharmonic electron motion, driven by ultrashort, high-intensity laser pulses, provides a universal mechanism for the laser absorption. Here, we provide the first demonstration of anharmonic-resonance-aided high laser-absorption in a biological system. At intensities of ∼ 10¹6⁻¹8 W/cm², 40 fs pulses excite a plasma formed with E. coli bacteria. The density-inhomogeneities due to the micro- and nanostructures in the bacterial target increase anharmonic resonance (AHR) heating and result in a 104-fold enhancement in the hard x-ray yield compared to plain solid targets. These observations lead to novel high-energy x-ray sources that have implications to lithography, imaging and medical applications.

Overcoming bifurcation instability in high-repetition-rate Ho:YLF regenerative amplifiers.

We demonstrate a Ho:YLF regenerative amplifier (RA) overcoming bifurcation instability and consequently achieving high extraction energies of 6.9 mJ at a repetition rate of 1 kHz with pulse-to-pulse fluctuations of 1.1%. Measurements of the output pulse energy, corroborated by numerical simulations, identify an operation point (OP) that allows high-energy pulse extraction at a minimum noise level. Complete suppression of the onset of bifurcation was achieved by gain saturation after each pumping cycle in the Ho:YLF crystal via lowering the repetition rate and cooling the crystal. Even for moderate cooling, a significant temperature dependence of the Ho:YLF RA performance was observed.

Terahertz acoustics in hot dense laser plasmas.

We present a hitherto unobserved facet of hydrodynamics, namely the generation of an ultrahigh frequency acoustic disturbance in the terahertz frequency range, whose origins are purely hydrodynamic in nature. The disturbance is caused by differential flow velocities down a density gradient in a plasma created by a 30 fs, 800 nm high-intensity laser (∼5×10(16) W/cm(2)). The picosecond scale observations enable us to capture these high frequency oscillations (1.9±0.6 THz) which are generated as a consequence of the rapid heating of the medium by the laser. Adoption of two complementary techniques, namely pump-probe reflectometry and pump-probe Doppler spectrometry provides unambiguous identification of this terahertz acoustic disturbance. Hydrodynamic simulations well reproduce the observations, offering insight into this process.

Ultrafast optics of solid density plasma using multicolor probes.

We present time-resolved reflectivity and transmissivity of hot, overdense plasma by employing a multicolor probe beam, consisting of harmonics at wavelengths of 800 nm, 400 nm and 266 nm. The hot-dense plasma, formed by exciting a fused silica target with a 30 fs, 2 × 10(17) W cm(-2) intensity pulse, shows a sub-picosecond transition in reflectivity (transmissivity), and a wavelength-dependent fall (rise) in the reflected (transmitted) signal. A simple model of probe absorption in the plasma via inverse bremsstrahlung is used to determine electron-ion collision frequency at different plasma densities.

A versatile high-average-power ultrafast infrared driver tailored for high-harmonic generation and vibrational spectroscopy.

We report on an ultrafast infrared optical parametric chirped-pulse amplifier (OPCPA), pumped by a 200-W thin-disk Yb-based regenerative amplifier at a repetition rate of 100 kHz. The OPCPA is tunable in the spectral range 1.4-3.9 [Formula: see text]m, generating up to 23 W of < 100-fs signal and 13 W of < 200-fs idler pulses for infrared spectroscopy, with additional spectral filtering capabilities for Raman spectroscopy. The OPCPA can also yield 19 W of 49-fs 1.75-[Formula: see text]m signal or 5 W of 62-fs 2.8-[Formula: see text]m idler pulses with active carrier-to-envelope-phase (CEP) stabilisation for high-harmonic generation (HHG). We illustrate the versatility of the laser design, catering to various experimental requirements for probing ultrafast science.

A bright point source of ultrashort hard x-ray pulses using biological cells.

We demonstrate that the interaction of intense femtosecond light on a plain solid substrate can be substantially altered by a few micron layer coating of bacterial cells, live or dead. Using E. Coli cells, we show that at an intensity of 10(16)W cm(-2), the bremsstraahlung hard x-ray emission (up to 300 keV), is increased by more than two orders of magnitude as compared to a plain glass slab. Particle-in-cell simulations carried out by modeling the bacterial cells as ellipsoidal particles show that the hot electron generation is indeed enhanced by the presence of microstructures. This new methodology should pave way for using microbiological systems of varied shapes to control intense laser produced plasmas for EUV/x-ray generation.

Macroscopic transport of mega-ampere electron currents in aligned carbon-nanotube arrays.

We demonstrate that aligned carbon-nanotube arrays are efficient transporters of laser-generated mega-ampere electron currents over distances as large as a millimeter. A direct polarimetric measurement of the temporal and the spatial evolution of the megagauss magnetic fields (as high as 120 MG) at the target rear at an intensity of (10(18)-10(19)) W/cm2 was corroborated by the rear-side hot electron spectra. Simulations show that such high magnetic flux densities can only be generated by a very well collimated fast electron bunch.

Torsionally broken symmetry assists infrared excitation of biomimetic charge-coupled nuclear motions in the electronic ground state.

The concerted interplay between reactive nuclear and electronic motions in molecules actuates chemistry. Here, we demonstrate that out-of-plane torsional deformation and vibrational excitation of stretching motions in the electronic ground state modulate the charge-density distribution in a donor-bridge-acceptor molecule in solution. The vibrationally-induced change, visualised by transient absorption spectroscopy with a mid-infrared pump and a visible probe, is mechanistically resolved by ab initio molecular dynamics simulations. Mapping the potential energy landscape attributes the observed charge-coupled coherent nuclear motions to the population of the initial segment of a double-bond isomerization channel, also seen in biological molecules. Our results illustrate the pivotal role of pre-twisted molecular geometries in enhancing the transfer of vibrational energy to specific molecular modes, prior to thermal redistribution. This motivates the search for synthetic strategies towards achieving potentially new infrared-mediated chemistry.

Luminous, relativistic, directional electron bunches from an intense laser driven grating plasma.

Bright, energetic, and directional electron bunches are generated through efficient energy transfer of relativistic intense (~ 1019 W/cm2), 30 femtosecond, 800 nm high contrast laser pulses to grating targets (500 lines/mm and 1000 lines/mm), under surface plasmon resonance (SPR) conditions. Bi-directional relativistic electron bunches (at 40° and 150°) are observed exiting from the 500 lines/mm grating target at the SPR conditions. The surface plasmon excited grating target enhances the electron flux and temperature by factor of 6.0 and 3.6, respectively, compared to that of the plane substrate. Particle-in-Cell simulations indicate that fast electrons are emitted in different directions at different stages of the laser interaction, which are related to the resultant surface magnetic field evolution. This study suggests that the SPR mechanism can be used to generate multiple, bright, ultrafast relativistic electron bunches for a variety of applications.

Nucleic Acid Strand Displacement with Synthetic mRNA Inputs in Living Mammalian Cells.

Strand displacement reactions are widely used in DNA nanotechnology as a building block for engineering molecular computers and machines. Here, we demonstrate that strand displacement-based probes can be triggered by RNA expressed in mammalian cells, thus taking a step toward adapting the DNA nanotechnology toolbox to a cellular environment. We systematically compare different probe architectures in order to identify a design that works robustly in living cells. Our optimized strand displacement probe combines chemically modified nucleic acids that enhance stability to degradation by cellular nucleases with structural elements that improve probe retention in the cytoplasm. We visualize probe binding to individual mRNA carrying 96 repeats of a target sequence in the 3'UTR. We find that RNA counts based on live cell imaging using a strand displacement probe are comparable to counts from independent measurement based on fluorescence in situ hybridization experiments. We used probes with scrambled toeholds and scrambled binding domains to demonstrate that target recognition indeed occurs through toehold-mediated strand displacement. Our results demonstrate that strand displacement probes can work reliably in mammalian cells and lay the groundwork for future applications of such probes for live-cell imaging and molecular computing.

A spatially localized architecture for fast and modular DNA computing.

Cells use spatial constraints to control and accelerate the flow of information in enzyme cascades and signalling networks. Synthetic silicon-based circuitry similarly relies on spatial constraints to process information. Here, we show that spatial organization can be a similarly powerful design principle for overcoming limitations of speed and modularity in engineered molecular circuits. We create logic gates and signal transmission lines by spatially arranging reactive DNA hairpins on a DNA origami. Signal propagation is demonstrated across transmission lines of different lengths and orientations and logic gates are modularly combined into circuits that establish the universality of our approach. Because reactions preferentially occur between neighbours, identical DNA hairpins can be reused across circuits. Co-localization of circuit elements decreases computation time from hours to minutes compared to circuits with diffusible components. Detailed computational models enable predictive circuit design. We anticipate our approach will motivate using spatial constraints for future molecular control circuit designs.

Magnetic turbulence in a table-top laser-plasma relevant to astrophysical scenarios.

Turbulent magnetic fields abound in nature, pervading astrophysical, solar, terrestrial and laboratory plasmas. Understanding the ubiquity of magnetic turbulence and its role in the universe is an outstanding scientific challenge. Here, we report on the transition of magnetic turbulence from an initially electron-driven regime to one dominated by ion-magnetization in a laboratory plasma produced by an intense, table-top laser. Our observations at the magnetized ion scale of the saturated turbulent spectrum bear a striking resemblance with spacecraft measurements of the solar wind magnetic-field spectrum, including the emergence of a spectral kink. Despite originating from diverse energy injection sources (namely, electrons in the laboratory experiment and ion free-energy sources in the solar wind), the turbulent spectra exhibit remarkable parallels. This demonstrates the independence of turbulent spectral properties from the driving source of the turbulence and highlights the potential of small-scale, table-top laboratory experiments for investigating turbulence in astrophysical environments.

Micron-scale mapping of megagauss magnetic fields using optical polarimetry to probe hot electron transport in petawatt-class laser-solid interactions.

The transport of hot, relativistic electrons produced by the interaction of an intense petawatt laser pulse with a solid has garnered interest due to its potential application in the development of innovative x-ray sources and ion-acceleration schemes. We report on spatially and temporally resolved measurements of megagauss magnetic fields at the rear of a 50-µm thick plastic target, irradiated by a multi-picosecond petawatt laser pulse at an incident intensity of ~1020 W/cm2. The pump-probe polarimetric measurements with micron-scale spatial resolution reveal the dynamics of the magnetic fields generated by the hot electron distribution at the target rear. An annular magnetic field profile was observed ~5 ps after the interaction, indicating a relatively smooth hot electron distribution at the rear-side of the plastic target. This is contrary to previous time-integrated measurements, which infer that such targets will produce highly structured hot electron transport. We measured large-scale filamentation of the hot electron distribution at the target rear only at later time-scales of ~10 ps, resulting in a commensurate large-scale filamentation of the magnetic field profile. Three-dimensional hybrid simulations corroborate our experimental observations and demonstrate a beam-like hot electron transport at initial time-scales that may be attributed to the local resistivity profile at the target rear.

Contrasting levels of absorption of intense femtosecond laser pulses by solids.

The absorption of ultraintense, femtosecond laser pulses by a solid unleashes relativistic electrons, thereby creating a regime of relativistic optics. This has enabled exciting applications of relativistic particle beams and coherent X-ray radiation, and fundamental leaps in high energy density science and laboratory astrophysics. Obviously, central to these possibilities lies the basic problem of understanding and if possible, manipulating laser absorption. Surprisingly, the absorption of intense light largely remains an open question, despite the extensive variations in target and laser pulse structures. Moreover, there are only few experimental measurements of laser absorption carried out under very limited parameter ranges. Here we present an extensive investigation of absorption of intense 30 femtosecond laser pulses by solid metal targets. The study, performed under varying laser intensity and contrast ratio over four orders of magnitude, reveals a significant and non-intuitive dependence on these parameters. For contrast ratio of 10(-9) and intensity of 2 × 10(19)W cm(-2), three observations are revealed: preferential acceleration of electrons along the laser axis, a ponderomotive scaling of electron temperature, and red shifting of emitted second-harmonic. These point towards the role of J × B absorption mechanism at relativistic intensity. The experimental results are supported by particle-in-cell simulations.

High-resolution measurements of the spatial and temporal evolution of megagauss magnetic fields created in intense short-pulse laser-plasma interactions.

A pump-probe polarimetric technique is demonstrated, which provides a complete, temporally and spatially resolved mapping of the megagauss magnetic fields generated in intense short-pulse laser-plasma interactions. A normally incident time-delayed probe pulse reflected from its critical surface undergoes a change in its ellipticity according to the magneto-optic Cotton-Mouton effect due to the azimuthal nature of the ambient self-generated megagauss magnetic fields. The temporal resolution of the magnetic field mapping is typically of the order of the pulsewidth, limited by the laser intensity contrast, whereas a spatial resolution of a few µm is achieved by this optical technique. High-harmonics of the probe can be employed to penetrate deeper into the plasma to even near-solid densities. The spatial and temporal evolution of the megagauss magnetic fields at the target front as well as at the target rear are presented. The µm-scale resolution of the magnetic field mapping provides valuable information on the filamentary instabilities at the target front, whereas probing the target rear mirrors the highly complex fast electron transport in intense laser-plasma interactions.