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DOE OSTI2022

Wavefront preserving X-ray optics for Synchrotron and Free Electron Laser photon beam transport systems

We report in the last two decades, after the first light from the new Free Electron Lasers, either in the UV (FLASH and FERMI@Elettra) or X-ray (LCLS and SACLA), more and more new diffraction limited sources have been either constructed or planned. Third generation storage rings are upgraded to provide a more collimated, brighter, and coherent light for the next generation experimental techniques. X-ray optics are the bridge between the light sources and the experimental stations. They are the key to the success of advanced experiments but also the potential bottleneck preventing the exploitation of the full characteristics of the source. The beam degradation originated by any mirror defect (either from mirror polishing or from contamination) is amplified with a coherent source. Delivering diffraction-limited spots, including the option for variable spot sizes in and out of focus, requires the control of the surface of the optics at the 1 nm rms level, if not better. At LCLS, only very recently an almost perfectly uniform beam out of focus has been obtained in the hard X-rays. It has been obtained after two 1-m long mirrors with 0.5 nm rms shape precision (after installation). Those mirrors were not readily available just a decade ago. But, thanks to the pioneering work performed at the Osaka University, those optics are now commercially available with arbitrary tangential profiles. This new generation of mirrors permits achieving unprecedented results. However, they do not remove all road blocks to a perfect photon transport system. Instead, they highlighted the critical importance of mirror mounting, handling of the thermal deformation, and the need of advanced diagnostics to properly exploit all the new potentiality of these optics. Besides the need of “perfect” mirrors, other aspects of the beamline design and elements may impact the quality of the beam in the experimental station, from the lack of blaze gratings to the need of advanced simulation tools, just to cite two. In this article, after a brief historical excursus, we will present the current state of the art of mirrors, gratings, crystals, lenses, diagnostics, and simulation tools. The main problems yet to solve and a look ahead at what would be achievable in the next decade will give the reader an idea on the search for an almost ideal photon transport system and how the path toward experiments, not conceivable today, will unfold.

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

Structural properties of aqueous grown polydopamine thin films determined by neutron reflectometry

Here, in this work, neutron reflectometry (NR) studies of the bio-mimetic polymer, polydopamine (PDA), deposited from differing initial concentrations of precursor material dopamine hydrochloride for a range of polymerization times, is reported. PDA can form a complex and highly versatile polymer film, with many structure studies having been performed previously, but a comprehensive structural determination of PDA by NR is lacking in the literature. It was found that simple box models were incapable of fully explaining the observed data, necessitating the use of a composite model consisting of the weighted average of both the 1 and 2 box models to fully capture the heterogeneous nature of the PDA film structure. Confocal laser scanning microscopy (CLSM) and atomic force microscopy (AFM) were performed to capture the surface structure and relative mechanical difference between the separate domains of the PDA. The CLSM results provide evidence that the PDA domains are larger than the coherent scattering length of a neutron used in these measurements, 10μm, supporting the need for a composite model. The AFM measurements show complex structure below the coherence length provide physical justification for the two box model. It was determined that film structure and quality are both heavily impacted by the initial concentration of dopamine hydrochloride and the polymerization time, giving confidence to the highly customizable nature of PDA as an adhesion promoting interface treatment in composite systems, such as plastic bonded explosives (PBX).

36 MATERIALS SCIENCE↗

DOE OSTI2020

Metal-embedded fiber optic sensor packaging and signal demodulation scheme towards high-frequency dynamic measurements in harsh environments

Optical fiber-based sensors are commonly used for industrial monitoring and control processes due to their small size, resistance to electromagnetic interference, and ability to perform a wide variety of high-precision measurements. However, implementing optical fiber sensors in harsh environments is challenging because they are small and fragile. Proper packaging of fiber-optic sensors could extend their use to harsh environments, including at high temperature and under high radiation. Furthermore, conventional fiber optic-based measurement systems often use computationally expensive signal processing algorithms which hinder their use in high-frequency dynamic applications. This work reports on the design of an optical fiber-pressure sensor system based on low-coherence interferometry that uses a metal-embedded optical fiber to provide a robust sensor package. Additionally, a novel phase demodulation scheme is proposed to extract length changes from the deformation of a thin diaphragm within a Fabry–Pérot cavity to measure pressure. The sensor has been tested to ±100 kPa, has a theoretical linear response over a 270 kPa dynamic range (24 dB maximum signal-to-noise ratio), and can resolve pressure transients up to 3910 kPa/s. Sampling at 100 kHz, the present sensor can resolve 2 kPa dynamic pressures at frequencies up to 2 kHz. Faster transients on the order of tens to hundreds of kHz can theoretically be resolved at the expense of decreasing the maximum resolvable amplitude. A methodology for designing a LCI pressure sensor for a given application is outlined based on the limitations imposed by the Nyquist criterion, the diaphragm's resonant frequency, the LCI optoelectronics, and the phase demodulation scheme. The sensor is the first to implement a low-coherence light source and a Fabry–Pérot interferometer designed to provide real-time high-fidelity pressure measurements using a metal-embedded optical fiber. The demonstrated sensor provides a platform for sensing in harsh conditions such as in nuclear and energy applications.

47 OTHER INSTRUMENTATION↗

DOE OSTI2020

Temporal dynamics of large-scale structures for turbulent Rayleigh–Bénard convection in a moderate aspect-ratio cylinder

We investigate the spatial organization and temporal dynamics of large-scale, coherent structures in turbulent Rayleigh–Bénard convection via direct numerical simulation of a 6.3 aspect-ratio cylinder with Rayleigh and Prandtl numbers of 9.6×10 7 and 6.7, respectively. Fourier modal decomposition is performed to investigate the structural organization of the coherent turbulent motions by analysing the length scales, time scales and the underlying dynamical processes that are ultimately responsible for the large-scale structure formation and evolution. We observe a high level of rotational symmetry in the large-scale structure in this study and that the structure is well described by the first four azimuthal Fourier modes. Two different large-scale organizations are observed during the duration of the simulation and these patterns are dominated spatially and energetically by azimuthal Fourier modes with frequencies of 2 and 3. Studies of the transition between these two large-scale patterns, radial and vertical variations in the azimuthal energy spectra, as well as the spatial and modal variations in the system's correlation time are conducted. Rotational dynamics are observed for individual Fourier modes and the global structure with strong similarities to the dynamics that have been reported for unit aspect-ratio domains in prior works. It is shown that the large-scale structures have very long correlation time scales, on the order of hundreds to thousands of free-fall time units, and that they are the primary source for a horizontal inhomogeneity within the system that can be observed during a finite, but a very long-time simulation or experiment.

42 ENGINEERING↗

DOE OSTI2024

Reynolds-number scaling of wall-pressure–velocity correlations in wall-bounded turbulence

Wall-pressure fluctuations are a practically robust input for real-time control systems aimed at modifying wall-bounded turbulence. The scaling behaviour of the wall-pressure–velocity coupling requires investigation to properly design a controller with such input data so that it can actuate upon the desired turbulent structures. A comprehensive database from direct numerical simulations (DNS) of turbulent channel flow is used for this purpose, spanning a Reynolds-number range$Re_\tau \approx 550\unicode{x2013}5200$. Spectral analysis reveals that the streamwise velocity is most strongly coupled to the linear term of the wall pressure, at a Reynolds-number invariant distance-from-the-wall scaling of$\lambda _x/y \approx 14$(and$\lambda _x/y \approx 8$for the wall-normal velocity). When extending the analysis to both homogeneous directions in$x$and$y$, the peak coherence is centred at$\lambda _x/\lambda _z \approx 2$and$\lambda _x/\lambda _z \approx 1$for$p_w$and$u$, and$p_w$and$v$, respectively. A stronger coherence is retrieved when the quadratic term of the wall pressure is concerned, but there is only little evidence for a wall-attached-eddy type of scaling. An experimental dataset comprising simultaneous measurements of wall pressure and velocity complements the DNS-based findings at one value of$Re_\tau \approx 2$k, with ample evidence that the DNS-inferred correlations can be replicated with experimental pressure data subject to significant levels of (acoustic) facility noise. It is furthermore shown that velocity-state estimations can be achieved with good accuracy by including both the linear and quadratic terms of the wall pressure. An accuracy of up to 72 % in the binary state of the streamwise velocity fluctuations in the logarithmic region is achieved; this corresponds to a correlation coefficient of$\approx$0.6. This thus demonstrates that wall-pressure sensing for velocity-state estimation – e.g. for use in real-time control of wall-bounded turbulence – has merit in terms of its realization at a range of Reynolds numbers.

Mechanics↗

DOE OSTI2025

Vortical interactions in turbulent thermoacoustic systems

This study examines the dynamics of vortical interactions and their implications for mitigating thermoacoustic instability in a turbulent combustor. The regions of intense vortical interactions are identified as vortical communities in the network space of weighted directed vortical networks constructed from two-dimensional experimental velocity data. One can expect vortical interactions in the combustor to be strongest near the moment of vortex shedding, as the shed vortices gradually weaken due to dissipation while convecting downstream. However, we show that, during the state of thermoacoustic instability, there is a non-trivial consistent phase lag of approximately 52° between the shedding of the coherent structures from the backward-facing step and the time instant when the vortical interactions attain their local maximum value. We explain this phase lag by investigating the correlation between acoustic pressure fluctuations, spatio-temporal dynamics of coherent structures and vortical interactions in the reaction field of the combustor. We also show the aperiodic variation of vortical interactions during the states of combustion noise and aperiodic epochs of intermittency. Furthermore, the spatio-temporal evolution of pairs of vortical communities with the maximum inter-community interactions provides insight into explaining the critical regions detected in the reaction field during the states of intermittency and thermoacoustic instability, also identified in previous studies. As a result, we further show that the most efficient suppression of thermoacoustic instability via air microjet injection is achieved when steady air jets are introduced to disrupt the maximum inter-community interactions present during the state of thermoacoustic instability.

Sahay, Ankit [Indian Institute of Technology Madra↗

DOE OSTI2026

Modulation induced by very-large-scale motions on the inclination angle of wall-attached eddies: an atmospheric surface layer experiment

The forward leaning inclination angle, 𝛾, of coherent turbulent structures is a well-known feature of wall-bounded turbulent flows. Although invariant across friction Reynolds numbers within the range 𝑅𝑒 𝜏 =10 3 −10 6 , 𝛾 can vary significantly across turbulent scales within a high-Reynolds-number flow. Very-large-scale motions (VLSMs) are known to induce significant changes in the instantaneous shear profile, which is a conditioning event that could trigger variability in the inclination angle of smaller coherent turbulent structures. Although this aspect has been extensively studied via numerical and laboratory experiments, few studies have explored this feature for a very-high-Reynolds-number atmospheric flow. In this work, the inclination angle of turbulent structures within the atmospheric surface layer at a very high Reynolds number (𝑅𝑒 𝜏 =7.9 ×10 5 ) is investigated by deploying a scanning Doppler light detection and ranging and a super large particle image velocimetry (SLPIV) apparatus. The inclination angle of wall-attached eddies is inferred either from the two-point correlation of streamwise velocity (𝛾 =41.1∘) or with a scale-dependent approach through the spectral linear stochastic estimator (SLSE). The SLSE (and, thus, the scale-dependent inclination angle) is conditionally evaluated based on the high- and low-momentum events induced by VLSMs, both in the streamwise (𝑢′𝑉𝐿𝑆𝑀) and in the vertical (𝑤′ 𝑉𝐿𝑆𝑀) velocity components. As a result, lower inclination angles (𝛾 =30° −50°) are found for 𝑢$^{'}_{VLSM}$ >0 (𝑤$^{'}_{VLSM}$ <0), while higher values (50° −85°) are ascribed to 𝑢$^{'}_{VLSM}$ <0 (𝑤$^{'}_{VLSM}$ >0). This result emphasises the primary role that VLSMs play in shaping the wall-attached eddy geometry, which, in turn, is crucial to determine the Reynolds stress balance within the wall-attached eddy range.

42 ENGINEERING↗

DOE OSTI2021

Bispectral analysis of broadband turbulence and geodesic acoustic modes in the T-10 tokamak

Local fluctuations of electrostatic potential, poloidal electric field, magnetic potential and electron density are simultaneously measured in the T-10 tokamak by a heavy ion beam probe (HIBP) having a five-slit energy analyser, which allows an estimate of the turbulent particle flux and $\boldsymbol {E}\times \boldsymbol {B}$ rotation velocity in the off-minor-axis gradient zone of the toroidal plasma column. The high spatial and temporal resolution of the modern multichannel HIBP makes it an effective tool to study plasma oscillations. Motivated by previous work that has documented time-resolved interactions between measured plasma parameters using correlation analysis (coherence of $E_{\textrm {pol}}$ and density $n_e$ , and cross-phase), a new result from bicorrelation analysis (bicoherence of magnetic potential $A_\zeta$ and density $n_e$ , and biphase) is reported for documenting the evidence of wave–wave coupling and energy transfer associated with the interaction between geodesic acoustic modes (GAM) and broadband, quasi-coherent modes.

Physics↗

DOE OSTI2020

Flowthrough Pretreatment of Softwood under Water-only and Alkali Conditions

Flowthrough pretreatment provides valuable insight in the fundamentals of deconstruction of plant biomass. In this study, the potential softwood degradation pathways under water-only and alkali conditions were determined by elucidating the deconstructed biomass-derived products at 0-270 °C for 2-10 min at a flow rate of 25 mL/min with water-only or alkaline at initial pH of 8, 9, 11, and 12, respectively. Results indicated that the initial pH value was a convenient indicator along with the severity parameter to control biomass degradation through the non-oxidative (pH<9) and oxidative (pH=9) pathways. Up to 100 % of hemi-sugars, 90 % of cellulose, and 70 % of lignin were derived from softwood under non-oxidative conditions at severity parameter LogR0 around 5.5, respectively. On the contrary, at pH 12, the oxidative degradation resulted in pretreated hydrolysate rich in monomeric and oligomeric phenolic products as well as glycolic acid, acetic acid, and formic acid from carbohydrates. The two dimensional 1H-13C heteronuclear single quantum coherence (HSQC) nuclear magnetic resonance (NMR) analysis revealed that non-oxidative degradation at initial pH values lower than 9 mainly cleaved ß-O-4, all of the ß-ß, and ß-5/a-O-4 linkages, whereas substantial aromatic ring structures with limited ß-O-4 structures remaining at pH 12 through oxidative degradation.

Zhang, Libing↗

DOE OSTI2020

Revisiting the Hole Size in Double Helical DNA with Localized Orbital Scaling Corrections

The extent of electronic wave function delocalization for the charge carrier (electron or hole) in double helical DNA plays an important role in determining the DNA charge transfer mechanism and kinetics. The size of the charge carrier’s wave function delocalization is regulated by the solvation induced localization and the quantum delocalization among the π stacked base pairs at any instant of time. Using a newly developed localized orbital scaling correction (LOSC) density functional theory method, we accurately characterized the quantum delocalization of the hole wave function in double helical B-DNA. This approach can be used to diagnose the extent of delocalization in fluctuating DNA structures. Our studies indicate that the hole state tends to delocalize among 4 guanine–cytosine (GC) base pairs and among 3 adenine–thymine (AT) base pairs when these adjacent bases fluctuate into degeneracy. The relatively small delocalization in AT base pairs is caused by the weaker π–π interaction. This extent of delocalization has significant implications for assessing the role of coherent, incoherent, or flickering coherent carrier transport in DNA.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Many-Exciton Quantum Dynamics in a Ruddlesden–Popper Tin Iodide

We present a study on the many-body exciton interactions in a Ruddlesden–Popper tin halide, namely, (PEA) 2 SnI 4 (PEA = phenylethylammonium), using coherent two-dimensional electronic spectroscopy. The optical dephasing times of the third-order polarization observed in these systems are determined by exciton many-body interactions and lattice fluctuations. We investigate the excitation-induced dephasing (EID) and observe a significant reduction of the dephasing time with increasing excitation density as compared to its lead counterpart (PEA) 2 PbI 4 , which we have previously reported in a separate publication [J. Chem. Phys. 2020, 153, 164706]. Surprisingly, we find that the EID interaction parameter is four orders of magnitude higher in (PEA) 2 SnI 4 than that in (PEA) 2 PbI 4 . This increase in the EID rate may be due to exciton localization arising from a more statically disordered lattice in the tin derivative. This is supported by the observation of multiple closely spaced exciton states and the broadening of the linewidth with increasing population time (spectral diffusion), which suggests a static disordered structure relative to the highly dynamic lead-halide. Additionally, we find that the exciton nonlinear coherent lineshape shows evidence of a biexcitonic state with low binding energy (<10 meV) not observed in the lead system. We model the lineshapes based on a stochastic scattering theory that accounts for the interaction with a nonstationary population of dark background excitations. Our study provides evidence of differences in the exciton quantum dynamics between tin- and lead-based Ruddlesden–Popper metal halides (RPMHs) and links them to the exciton–exciton interaction strength and the static disorder aspect of the crystalline structure.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Spin Decoherence in VOPc@graphene Nanoribbon Complexes

Carbon nanoribbons or nanographene qubit arrays can facilitate quantum-to-quantum transduction between light, charge, and spin, making them an excellent testbed for fundamental science in quantum coherent systems and for the construction of higher-level qubit circuits. Here, in this work, we study spin decoherence due to coupling with a surrounding nuclear spin bath of an electronic molecular spin of a vanadyl phthalocyanine (VOPc) molecule integrated onto an armchair-edged graphene nanoribbon (GNR). Density functional theory (DFT) is used to obtain ground-state atomic configurations. Decay of spin coherence in Hahn echo experiments is then simulated using the cluster correlation expansion method with a spin Hamiltonian involving hyperfine and electric field gradient tensors calculated from DFT. We find that the decoherence time T 2 is anisotropic with respect to magnetic field orientation and determined only by the hydrogen nuclear spins on both VOPc and GNR. Large electron spin echo envelope modulation (ESEEM) due to nitrogen and vanadium nuclear spins is present at specific field ranges and can be completely suppressed by tuning the magnetic field. The relation between these field ranges and the hyperfine interactions is analyzed. The effects of interactions with the nuclear quadrupole moments are also studied, validating the applicability and limitations of the spin Hamiltonian when they are disregarded.

Hamiltonians↗

DOE OSTI2026

Laser-Induced Enhancement of Acoustic Mode Quality Factor Revealed by Correlated Single-Particle Optical and Electron Microscopy

Acoustic modes in plasmonic nanostructures provide fundamental insights into their optomechanical behavior at the nanoscale, enabling emerging applications in plasmon-enhanced optomechanics, ultrasensitive sensing, and nanoscale energy transduction. Here we explore the modulation of acoustic phonon dynamics in lithographically fabricated gold nanodisks via laser-induced photothermal annealing. Using a correlated approach that utilizes both single-particle transient extinction spectroscopy and advanced electron microscopy, we directly link nanoscale structural transformations to changes in mechanical properties as probed through the coherence of the excited acoustic modes. Specifically, ultrafast pump–probe microscopy reveals an enhancement in the acoustic mode quality factor of annealed gold nanodisks, indicative of reduced damping and improved vibrational coherence. Structural characterization via scanning electron microscopy and electron backscatter diffraction confirms that photoinduced annealing results in smoother surface morphology and overall enhanced crystallinity. The improved crystalline order reduces defect and crystal boundary scattering, which we suggest as the reason underlying the lower quality factor before annealing. Furthermore, these findings demonstrate that targeted structural engineering at the nanoscale offers a powerful strategy for optimizing the optomechanical performance of plasmonic nanostructures, with broad implications for the design of next-generation nanophotonic and optomechanical systems.

Annealing (metallurgy)↗

DOE OSTI2020

The “Hole” Story in Ionized Water from the Perspective of Ehrenfest Dynamics

The radiolysis of liquid water and the radiation-matter interactions that happen in aqueous environments are important to the elds of chemistry, materials, and environmental sciences, as well as biological and physiological response to extreme conditions and medical treatments. The initial stage of radiolysis is the ultrafast response, or hole dynamics, that trigger chemical processes within complex energetic landscapes that may include reactivity. A fundamental understanding necessitates the use of theoretical methods that are capable of simulating both ultrafast coherence and non-adiabatic energy transfer pathways. In this work, we carry out an ab initio Ehrenfest dynamic study in order to provide a more complete description of the ultrafast dynamics and reactive events initiated by photoionization of water. Furthermore, after sudden ionization, the range of processes that include hole trapping and transfer, large OH oscillations, proton transfer and subsequent relay, formation of the metastable Zundel complex, and long-lived coherence, are identied and new insight into their driving forces are elucidated.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Emulating Quantum Entangled Biphoton Spectroscopy Using Classical Light Pulses

We show that for a class of quantum light spectroscopy (QLS) experiments using n = 0, 1, 2, ··· classical light pulses and an entangled photon pair (a biphoton state) where one photon acts as a reference without interacting with the matter sample, identical signals can be obtained by replacing the biphotons with classical-like coherent states of light, where these are defined explicitly in terms of the parameters of the biphoton states. An input-output formulation of quantum nonlinear spectroscopy is used to prove this equivalence. We demonstrate the equivalence numerically by comparing a classical pump–quantum probe experiment with the corresponding classical pump–classical probe experiment. This analysis shows that understanding the equivalence between entangled biphoton probes and carefully designed classical-like coherent state probes leads to quantum-inspired classical experiments that yield equivalent signals and provides insights for the future design of QLS experiments that could provide a true quantum advantage.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

T 1 Anisotropy Elucidates Spin Relaxation Mechanisms in an S = 1 Cr(IV) Optically Addressable Molecular Qubit

Paramagnetic molecules offer unique advantages for quantum information science owing to their spatial compactness, synthetic tunability, room-temperature quantum coherence, and potential for optical state initialization and readout. However, current optically addressable molecular qubits are hampered by rapid spin–lattice relaxation ( T 1 ) even at sub-liquid nitrogen temperatures. Here, we use temperature- and orientation-dependent pulsed electron paramagnetic resonance (EPR) to elucidate the negative sign of the ground state zero-field splitting (ZFS) and assign T 1 anisotropy to specific types of motion in an optically addressable S = 1 Cr(o-tolyl) 4 molecular qubit. The anisotropy displays a distinct sin 2 (2θ) functional form that is not observed in S = 1/2 Cu(acac) 2 or other Cu(II)/V(IV) microwave addressable molecular qubits. The Cr(o-tolyl) 4 T 1 anisotropy is ascribed to couplings between electron spins and rotational motion in low-energy acoustic or pseudoacoustic phonons. Our findings suggest that rotational degrees of freedom should be suppressed to maximize the coherence temperature of optically addressable qubits.

magnetic properties↗

DOE OSTI2025

Ultrafast Dynamics and Rearrangement of the EUV Photoacid Generator Phenyl Triflate

Extreme UV photolithography is a high-energy process crucial for modern computer chip fabrication, where photoacid generators (PAGs) enhance radiation exposure by producing reactive chemical species. This study investigates the ultrafast dissociative dynamics of phenyl triflate, a widely used PAG, under high-energy ionizing conditions. The dissociative ionization of the phenyl triflate cation, which includes a molecular rearrangement that releases SO 2 and forms the phenyl trifluoromethyl ether cation, is measured over the first 5 ps. These dynamics reveal vibrational coherence corresponding to a torsional mode of the cation, involving the twisting of the phenyl group into the O–S–C plane. Electronic structure calculations for the radical cation are in good agreement with the experimentally observed vibrational coherence. These findings provide valuable insights into the behavior of phenyl triflate under ionizing conditions similar to its industrial usage.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Interplay between Ultrafast Electronic and Librational Dynamics in Liquid Nitrobenzene Probed with Two-Color Four-Wave Mixing

Here, we present an experimental and theoretical study of the interplay between ultrafast electron dynamics and librational dynamics in liquid nitrobenzene. A femtosecond ultraviolet pulse and two femtosecond near-infrared pulses interact with nitrobenzene molecules, generating a four-wave mixing nonlinear signal measured in the Optical Kerr Effect geometry. The signal is measured to be nonzero only at negative time delays, corresponding to the near-infrared pulses arriving before the ultraviolet pulse. We perform time-dependent Quantum Master Equation calculations with classical libration to simulate the experiment. The simulations support the conclusion that the near-infrared pulses launch librational motion while creating electronic coherences resulting in a libration-modulated electronic nonlinear response. The analysis of the phase-matched four-wave mixing signals suggests a nonparametric process leaving the molecules in an excited electronic state, providing new insight into ultrafast nonlinear optical interactions in liquids and advancing toward probing ultrafast electronic coherences in complex molecular liquids.

Shivaram, Niranjan [Lawrence Berkeley National Lab↗