Engineering topics

Shivaram, Niranjan

Publications and source records attributed to Shivaram, Niranjan.

8 records

DOE OSTI2022

The DREAM Endstation at the Linac Coherent Light Source

Free-electron lasers (FEL), with their ultrashort pulses, ultrahigh intensities, and high repetition rates at short wavelength, have provided new approaches to Atomic and Molecular Optical Science. One such approach is following the birth of a photo electron to observe ion dynamics on an ultrafast timescale. Such an approach presents the opportunity to decipher the photon-initiated structural dynamics of an isolated atomic and molecular species. It is a fundamental step towards understanding single- and non-linear multi-photon processes and coherent electron dynamics in atoms and molecules, ultimately leading to coherent control following FEL research breakthroughs in pulse shaping and polarization control. A key aspect for exploring photoinduced quantum phenomena is visualizing the collective motion of electrons and nuclei in a single reaction process, as dynamics in atoms/ions proceed at femtosecond (10 –15 s) timescales while electronic dynamics take place in the attosecond timescale (10 –18 s). Here, we report on the design of a Dynamic Reaction Microscope (DREAM) endstation located at the second interaction point of the Time-Resolved Molecular and Optical (TMO) instrument at the Linac Coherent Light Source (LCLS) capable of following the photon–matter interactions by detecting ions and electrons in coincidence. The DREAM endstation takes advantage of the pulse properties and high repetition rate of LCLS-II to perform gas-phase soft X-ray experiments in a wide spectrum of scientific domains. With its design ability to detect multi-ions and electrons in coincidence while operating in step with the high repetition rate of LCLS-II, the DREAM endstation takes advantage of the inherent momentum conservation of reaction product ions with participating electrons to reconstruct the original X-ray photon–matter interactions. In this report, we outline in detail the design of the DREAM endstation and its functionality, with scientific opportunities enabled by this state-of-the-art instrument.

47 OTHER INSTRUMENTATION↗

DOE OSTI2022

The time-resolved atomic, molecular and optical science instrument at the Linac Coherent Light Source

The newly constructed time-resolved atomic, molecular and optical science instrument (TMO) is configured to take full advantage of both linear accelerators at SLAC National Accelerator Laboratory, the copper accelerator operating at a repetition rate of 120 Hz providing high per-pulse energy as well as the superconducting accelerator operating at a repetition rate of about 1 MHz providing high average intensity. Both accelerators power a soft X-ray free-electron laser with the new variable-gap undulator section. With this flexible light source, TMO supports many experimental techniques not previously available at LCLS and will have two X-ray beam focus spots in line. Thereby, TMO supports atomic, molecular and optical, strong-field and nonlinear science and will also host a designated new dynamic reaction microscope with a sub-micrometer X-ray focus spot. The flexible instrument design is optimized for studying ultrafast electronic and molecular phenomena and can take full advantage of the sub-femtosecond soft X-ray pulse generation program.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2021

Aggregation of solutes in bosonic versus fermionic quantum fluids

Quantum fluid droplets made of helium-3 ( 3 He) or helium-4 ( 4 He) isotopes have long been considered as ideal cryogenic nanolabs, enabling unique ultracold chemistry and spectroscopy applications. The droplets were believed to provide a homogeneous environment in which dopant atoms and molecules could move and react almost as in free space but at temperatures close to absolute zero. Here, we report ultrafast x-ray diffraction experiments on xenon-doped 3 He and 4 He nanodroplets, demonstrating that the unavoidable rotational excitation of isolated droplets leads to highly anisotropic and inhomogeneous interactions between the host matrix and enclosed dopants. Superfluid 4 He droplets are laced with quantum vortices that trap the embedded particles, leading to the formation of filament-shaped clusters. In comparison, dopants in 3 He droplets gather in diffuse, ring-shaped structures along the equator. The shapes of droplets carrying filaments or rings are direct evidence that rotational excitation is the root cause for the inhomogeneous dopant distributions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

SILIA: software implementation of a multi-channel, multi-frequency lock-in amplifier for spectroscopy and imaging applications

In this work, we describe a software implementation of a multi-channel, multi-frequency Lock-in Amplifier (SILIA) to extract modulated signals from noisy data distributed over multiple channels of arbitrary number and size. This software implementation emulates the functionality of a multi-channel, multi-frequency lock-in amplifier in a post-processing step following data acquisition. Unlike most traditional lock-in amplifiers, SILIA can work with any number of input channels and is especially useful to analyze data distributed over many channels. We demonstrate the versatility and performance for extracting weak signals in spectroscopy and fluorescence microscopy. We also discuss more general applications and exhibit a method to automatically estimate error from a lock-in result.

47 OTHER INSTRUMENTATION↗

DOE OSTI2020

Electronic Population Transfer via Impulsive Stimulated X-Ray Raman Scattering with Attosecond Soft-X-Ray Pulses

Free electron lasers provide a source of X-ray pulses short enough and intense enough to drive nonlinearities in molecular systems. Impulsive interactions driven by these X-ray pulses provide a way to create and probe valence electron motions with high temporal and spatial resolution. Observing these electronic motions is crucial to understand the role of electronic coherence in chemical processes. A simple nonlinear technique for probing electronic motion, impulsive stimulated X-ray Raman scattering (ISXRS), involves a single impulsive interaction to produce a coherent superposition of electronic states. In this work, we demonstrate electronic population transfer via ISXRS using broad bandwidth (5.5 eV full width at half maximum) attosecond X-ray pulses produced by the Linac Coherent Light Source (LCLS). The impulsive excitation is resonantly enhanced by the oxygen 1s → 2π* resonance of nitric oxide (NO), and excited state neutral molecules are probed with a time-delayed UV laser pulse.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2020

Shapes of rotating normal fluid He-3 versus superfluid He-4 droplets in molecular beams

Previous single-pulse extreme ultraviolet and X-ray coherent diffraction studies revealed that superfluid 4He droplets obtained in free jet expansion acquire sizable angular momentum, resulting in significant centrifugal distortion. Similar experiments with normal fluid 3He droplets may help elucidating the origin of the of the large degree of rotational excitation and highlight similarities and differences of dynamics in normal and superfluid droplets. Here, we present the first comparison of the shapes of isolated 3He and 4He droplets following expansion of the corresponding fluids in vacuum at temperatures as low as ~ 2 K. Large 3He and 4He droplets with average radii of ~160 nm and ~350 nm, respectively, were produced. We find that the majority of the 3He droplets in the beam correspond to rotating oblate spheroids with reduced average angular momentum ($\Lambda$) and reduced angular velocities ($\Omega$) similar to that of 4He droplets. Given the different physical nature of 3He and 4He, this similarity in $\Lambda$ and $\Omega$ may be surprising and suggest that similar mechanisms induce rotation regardless of the isotope. We hypothesized that the observed distribution of droplet sizes and angular momenta stem from processes in the dense region close to the nozzle. In this region, the significant velocity spread and collisions between the droplets induce excessive rotation followed by droplet fission. The process may repeat itself several times before the droplets enter the collision-fee high vacuum region further downstream.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Time-Resolved Ultrafast Transient Polarization Spectroscopy to Investigate Nonlinear Processes and Dynamics in Electronically Excited Molecules on the Femtosecond Time Scale

Here, we report a novel experimental technique to investigate ultrafast dynamics in photoexcited molecules by probing the third-order nonlinear optical susceptibility. A non-colinear 3-pulse scheme is developed to probe the ultrafast dynamics of excited electronic states using the optical Kerr effect by time-resolved polarization spectroscopy. Optical heterodyne and optical homodyne detection are demonstrated to measure the third-order nonlinear optical response for the S 1 excited state of liquid nitrobenzene, which is populated by 2-photon absorption of a 780 nm 35 fs excitation pulse.

47 OTHER INSTRUMENTATION↗

DOE OSTI2020

Ultrafast Dynamics of Excited Electronic States in Nitrobenzene Measured by Ultrafast Transient Polarization Spectroscopy

We investigate ultrafast dynamics of the lowest singlet excited electronic state in liquid nitrobenzene using ultrafast transient polarization spectroscopy, extending the well-known technique of optical Kerr effect spectroscopy to excited electronic states. The third-order nonlinear response of the excited molecular ensemble is measured using a pair of femtosecond pulses following a third femtosecond pulse that populates the S 1 excited state. By measuring this response, which is highly sensitive to details of the excited state character and structure, as a function of time delays between the three pulses involved, we extract the dephasing time of the wave packet on the excited state. The dephasing time, measured as a function of time delay after pump excitation, shows oscillations indicating oscillatory wave packet dynamics on the excited state. Finally, from the experimental measurements and supporting theoretical calculations, we deduce that the wave packet completely leaves the S 1 state potential energy surface after three traversals of the intersystem crossing between the singlet S 1 and triplet T 2 states.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗