Resolving Nonlinear Recombination Dynamics in Semiconductors via Ultrafast Excitation Correlation Spectroscopy: Photoluminescence versus Photocurrent Detection
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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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Determination of the Raman polarizability tensor in the optically anisotropic crystal potassium dihydrogen phosphate and its deuterated analog
Abstract The Raman tensor of the dominant A 1 modes of the nonlinear optical crystalline material potassium dihydrogen phosphate and its 70% deuterated analog have been ascertained. Challenges in determining the A 1 mode tensor element values based on previous reports have been resolved using a specially designed experimental setup that makes use of spherical crystal samples. This novel experimental design enabled the determination of measurement artifacts, including polarization rotation of the pump and/or scattered light propagating through the sample and the contribution of additional overlapping phonon modes, which have hindered previous efforts. Results confirmed that the polarization tensor is diagonal, and matrix elements were determined with high accuracy.
36 MATERIALS SCIENCE↗
Probing lithium mobility at a solid electrolyte surface
Abstract Solid-state electrolytes overcome many challenges of present-day lithium ion batteries, such as safety hazards and dendrite formation 1,2 . However, detailed understanding of the involved lithium dynamics is missing due to a lack of in operando measurements with chemical and interfacial specificity. Here we investigate a prototypical solid-state electrolyte using linear and nonlinear extreme-ultraviolet spectroscopies. Leveraging the surface sensitivity of extreme-ultraviolet-second-harmonic-generation spectroscopy, we obtained a direct spectral signature of surface lithium ions, showing a distinct blueshift relative to bulk absorption spectra. First-principles simulations attributed the shift to transitions from the lithium 1 s state to hybridized Li- s /Ti- d orbitals at the surface. Our calculations further suggest a reduction in lithium interfacial mobility due to suppressed low-frequency rattling modes, which is the fundamental origin of the large interfacial resistance in this material. Our findings pave the way for new optimization strategies to develop these electrochemical devices via interfacial engineering of lithium ions.
25 ENERGY STORAGE↗
Characterization of mechanical deformation in aluminum by optical second harmonic generation
Second harmonic generation (SHG), a laser-based surface technique, was used to characterize near-surface defect evolution associated with mechanical deformation in 2024-T3 aluminum due to tensile loads. Electron backscatter diffraction (EBSD) measurements were also performed to determine the geometrically necessary dislocation density before and after tensile deformation. Comparison of the EBSD and SHG results found that dislocation density and SHG signal are inversely proportional; tensile deformation in the plastic regime led to an increase in dislocation density and a decrease in SHG response. A similar trend was seen in the SHG results on as-received (unpolished) Al samples; SHG response decreases with extent of plastic deformation. Furthermore, this study suggests that SHG has potential as a nondestructive evaluation technique.
36 MATERIALS SCIENCE↗
Role of dipole-forbidden autoionizing resonances in nonresonant one-color two-photon single ionization of N 2
We present an experimental and theoretical energy- and angle-resolved study on the photoionization dynamics of non-resonant one-color two-photon single valence ionization of neutral N$_2$ molecules. Using 9.3 eV photons produced via high harmonic generation and a 3-D momentum imaging spectrometer, we detect the photoelectrons and ions produced from one-color two-photon ionization in coincidence. Photoionization of N$_2$ populates the X $^2\Sigma^+_g$, A $^2\Pi_u$, and B $^2\Sigma^+_u$ ionic states of N$_2^+$, where the photoelectron angular distributions associated with the X $^2\Sigma^+_g$ and A $^2\Pi_u$ states both vary with changes in photoelectron kinetic energy of only a few hundred meV. We attribute the rapid evolution in the photoelectron angular distributions to the excitation and decay of dipole-forbidden autoionizing resonances that belong to series of different symmetries, all of which are members of the Hopfield series, and compete with the direct two-photon single ionization.
74 ATOMIC AND MOLECULAR PHYSICS↗
Nanofocused attosecond hard x-ray free-electron laser with intensity exceeding 10 19 W/cm 2
Attosecond hard x-ray pulses from the LCLS are focused to nanometer-sized spots using an advanced Kirkpatrick Baez mirror system. Peak intensity at the focal point exceeds 10 19 W/cm 2 , enabling a suite of damage-free nonlinear x-ray spectroscopy.
Inoue, Ichiro [RIKEN SPring-8 Center, Sayo (Japan)↗
Dispersion of the Nonlinear Susceptibility of MoS2 and WS2 from Second-Harmonic Scattering Spectroscopy
Dispersion of the absolute second-order susceptibility of both MoS2 and WS2 is assessed on a wide spectral excitation range (710–1300 nm) by using second-harmonic scattering spectroscopy (SHS). SHS is an accurate ensemble measurement here applied on well-dispersed suspensions of monodisperse liquid-exfoliated nanosheets showing a high monolayer content. The as-derived, high susceptibility values shed light on the discrepancies between available literature values while evidencing resonances associated with the main excitonic transitions.
CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SU↗
Observation of cupratelike nonlinear terahertz responses in superconducting infinite-layer nickelates via two-dimensional coherent spectroscopy
The 𝑑-wave pairing symmetry in newly discovered infinite-layer nickelates remains highly debated compared to the widely accepted 𝑑-wave superconductivity in cuprates, despite recent intense efforts using equilibrium optical and electrical transport measurements. A complementary approach involves characterizing THz coherent nonlinear responses, which is currently lacking but needed, as it would offer new insights into the superconducting gap structure by characterizing Higgs modes and quasiparticle excitations. Here, in this study, we report THz 2D coherent spectroscopy (THz-2DCS) responses from the superconducting state in an infinite-layer nickelate. The 2D spectra clearly demonstrate the absence of hallmark signatures of 𝑠-wave pairing symmetry, such as resonant 2Δ peaks at superconducting gaps. Instead, we observe gapless 2D spectra in the nickelate, centered around the THz driving frequency, with no noticeable shift as the temperature increases. These findings closely resemble the nodal superconductivity behavior expected in cuprates. Together with our simulations, these findings suggest that 2Δ signatures in the 2D spectra of 𝑑-wave gap structures can be obscured by significant nodal quasiparticle excitations at arbitrarily low energies. This contrasts with the long-lived Higgs modes, observed as distinct 2Δ peaks in a controlled THz-2DCS experiment on niobium, a representative example of dirty-limit s-wave superconductors. Our results have implications for understanding the unconventional superconductivity in nickelates and highlight the need to explore their coherent nonlinear dynamics.
Pairing mechanisms↗
Instantaneous difference frequency locking observed during toroidicity-induced Alfvén eigenmode coupling in the DIII-D tokamak
In magnetic confinement fusion, toroidicity-induced Alfvén eigenmodes (TAEs) are well-studied, weakly stable solutions of the linearized ideal magnetohydrodynamic equations. Driven unstable by suprathermal populations of energetic particles, TAE pose a key vulnerability to the confinement of high-energy alpha particles generated by fusion reactions. Hence, it is paramount to understand TAE dynamics if a working reactor is to be realized. In this work, we detect and characterize signatures of nonstationary nonlinear coupling between TAE using a novel, time-resolved bispectral analysis; results are supported by analytic signal of band-passed data. Crucially, a stationary phase relationship between two TAE and a nascent low frequency fluctuation is observed precisely when the triple product of magnetic fluctuation amplitudes is enhanced. Local mode number and frequency spectrum, gleaned from beam-emission spectroscopy, corroborates simultaneous satisfaction of nonlinear matching conditions, and provides a tool to identify theorized pathways of energy transfer, e.g. TAE parametric instability.
bispectral analysis↗
Revealing the frequency-dependent oscillations in the nonlinear terahertz response induced by the Josephson current
ABSTRACT Nonlinear responses of superconductors to intense terahertz radiation has been an active research frontier. Using terahertz pump-terahertz probe spectroscopy, we investigate the c-axis nonlinear optical response of a high-temperature superconducting cuprate. After excitation by a single-cycle terahertz pump pulse, the reflectivity of the probe pulse oscillates as the pump-probe delay is varied. Interestingly, the oscillatory central frequency scales linearly with the probe frequency, a fact widely overlooked in pump-probe experiments. By theoretically solving the nonlinear optical reflection problem on the interface, we show that our observation is well explained by the Josephson-type third-order nonlinear electrodynamics, together with the emission coefficient from inside the material into free space. The latter results in a strong enhancement of the emitted signal whose physical frequency is around the Josephson plasma edge. Our result offers a benchmark for and new insights into strong-field terahertz spectroscopy of related quantum materials.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Multidimensional four-wave-mixing spectroscopy with squeezed light
A set of nonlinear spectroscopic measurements with quantum light is presented here. It involves a strong pump with frequency ω pu and a weak probe atω pr interacting with a solid state target to generate a conjugated beam ω c =2ω pu -ω pr via nondegenerate four-wave mixing. The $\chi^{(3)}$ susceptibility can be measured by the noise spectra of the intensity difference of the squeezed beams. We discuss three spectroscopic setups based on squeezed light: first, single four-wave mixing in a single crystal; second, cascading scheme involving two crystals; third, an $\textit{SU}$(1, 1) interferometer based on two separate four-wave mixing processes. We further investigate the microscopic noise and optical losses in all three setups. Simulations are presented for silicon-vacancy color centers in diamond.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
Direct uranium enrichment assay in gaseous uranium hexafluoride with laser induced breakdown spectroscopy
A set of eleven U atomic emission lines, between 421.099 and 421.460 nm, were characterized for direct enrichment assay of gaseous UF 6 samples with laser induced breakdown spectroscopy (LIBS). Several iterative, multivariate nonlinear spectral-fitting algorithms were evaluated for their efficacies to extract the enrichment information from the measured LIBS spectra. Furthermore, wavelength-dependent weight factors, which take into consideration of the spectral-line position in the fitting model, the determined isotopic ratio, and the isotopic shift of the emission line, are essential for the spectral-fitting model to function adequately. The analytical accuracies and precision were typically within 0.5% in absolute [ 235 U/( 235 U + 238 U)] ratios.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Spatiotemporal dispersion compensation for a 200-THz noncollinear optical parametric amplifier
A noncollinear optical parametric amplifier (NOPA) can produce few-cycle femtosecond laser pulses that are ideally suited for time-resolved optical spectroscopy measurements. However, the nonlinear-optical process giving rise to ultrabroadband pulses is susceptible to spatiotemporal dispersion problems. Here, we detail refinements, including chirped-pulse amplification (CPA) and pulse-front matching (PFM), that minimize spatiotemporal dispersion and thereby improve the properties of ultrabroadband pulses produced by a NOPA. Here, the description includes a rationale behind the choices of optical and optomechanical components, as well as assessment protocols. We demonstrate these techniques using a 1 kHz, second-harmonic Ti:sapphire pump configuration, which produces ~5-fs duration pulses that span from about 500 to 800 nm with a bandwidth of about 200 THz. To demonstrate the utility of the CPA-PFM-NOPA, we measure vibrational quantum beats in the transient–absorption spectrum of methylene blue, a dye molecule that serves as a reference standard.
47 OTHER INSTRUMENTATION↗
Hole‐Carrier‐Dominant Transport in 2D Single‐Crystal Copper
Abstract In 2D noble metals like copper, the carrier scattering at grain boundaries has obscured the intrinsic nature of electronic transport. However, it is demonstrated that the intrinsic nature of transport by hole carriers in 2D copper can be revealed by growing thin films without grain boundaries. As even a slight deviation from the twin boundary is perceived as grain boundaries by electrons, it is only through the thorough elimination of grain boundaries that the hidden hole‐like attribute of 2D single‐crystal copper can be unmasked. Two types of Fermi surfaces, a large hexagonal Fermi surface centered at the zone center and the triangular Fermi surface around the zone corner, tightly matching to the calculated Fermi surface topology, confirmed by angle‐resolved photoemission spectroscopy (ARPES) measurements and vivid nonlinear Hall effects of the 2D single‐crystal copper account for the presence of hole carriers experimentally. This breakthrough suggests the potential to manipulate the majority carrier polarity in metals by means of grain boundary engineering in a 2D geometry.
36 MATERIALS SCIENCE↗
Enabling robust, stable, and accurate nonlinear optical measurements from squeezed light generated in hot rubidium vapor
The feasibility of nonlinear optical (NLO) imaging and spectroscopy using low intensity quantum states of light including entangled photon and squeezed light sources, such as those driven by two-photon absorption (TPA), has been a topic of ongoing debate. An unambiguous identification of the appreciable quantum advantage in such quantum light applications could enable NLO imaging of biological samples without photodegradation and phototoxicity. Recently, we have constructed a two-mode squeezed light source based on four-wave mixing in 85Rb vapor, which is capable of 7.9 dB of intensity-difference squeezing (IDS), corresponding to 8.7 dB upon electronic noise correction. In this talk, we discuss the stability of our system, including implementation details on achieving and maintaining 8.7 dB of IDS for several hours, and ensuring the two spatially multimode beams are properly overlapped in a sample with minimal optical loss.
Allen, Harry [ORNL] (ORCID:0000000190253914)↗
Terahertz stimulated parametric downconversion of a magnon mode in an antiferromagnet
Parametric amplification, where one signal is enhanced by the action of another, offers both practical utility for boosting weak signals and fundamental insights into the nonlinear coupling between degrees of freedom. In condensed matter systems, interactions between collective modes offer avenues for nonlinear coherent manipulation of coupled excitations and quantum phases. Antiferromagnets, with inherently coupled magnon modes, provide a promising platform for nonlinear control of spin waves and magnetization. However, nonlinear magnon-magnon interactions have been only partially elaborated, leaving key gaps in the prospects for potential ultrahigh-bandwidth magnonic signal processing. Here, we excite two distinct coherent magnon modes in an antiferromagnet and find that the magnon mode with a lower frequency undergoes amplification when the higher-frequency mode is driven. We unveil the nonlinear excitation pathways of this stimulated parametric downconversion process by using polarization-selective two-dimensional terahertz spectroscopy. Our work provides fundamental insights into nonlinear magnonics in antiferromagnets, laying the groundwork for forthcoming spintronic and magnonic devices.
Science & Technology - Other Topics↗
Nonlinear dielectric relaxation of polar liquids
Molecular dynamics of two water models, SPC/E and TIP3P, at a number of temperatures are used to test the Kivelson-Madden equation connecting single-particle and collective dielectric relaxation times through the Kirkwood factor. The relation is confirmed by simulations and used to estimate the nonlinear effect of the electric field on the dielectric relaxation time. We show that the main effect of the field comes through slowing down of the single-particle rotational dynamics and the relative contribution of the field-induced alteration of the Kirkwood factor is insignificant for water. Theories of nonlinear dielectric relaxation need to mostly account for the effect of the field on rotations of a single dipole in a polar liquid.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗