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At least 199 records · Page 11

Phase noise limited frequency shift impulsive Raman spectroscopy

We introduce a method to enable optical amplification of a coherent Raman spectroscopy signal, which we call radio frequency (RF) Doppler Raman spectroscopy. In this article, we consider the perturbation of a probe pulse in a sample due to an excited Raman vibrational coherence as a generalized Doppler shift, which connects a time-varying optical path length (the product of the propagation length and refractive index, OPL = n ℓ) with an optical frequency shift. Amplification of a Raman signal outside of the focused interaction is enabled by converting the Doppler frequency shift experienced by a laser probe pulse into a periodic timing jitter. This transit time perturbation is detected through the phase of a RF electronic signal measured at a harmonic of the probe pulse train with a method adapted from precision metrology techniques used to measure laser pulse train timing jitter. Measurement of a timing jitter allows access to much lower noise floors than other coherent Raman techniques, and by exploiting the new capability to scale the signal of a coherent Raman spectroscopic signal, this method opens the potential to detect very weak Raman signals that are currently not observable due to limits of illumination intensity imposed by laser damage to the specimen and noise.

47 OTHER INSTRUMENTATION↗

Optical constants of magnetron sputtered aluminum in the range 17–1300 eV with improved accuracy and ultrahigh resolution in the L absorption edge region

This work determines a new set of EUV/x-ray optical constants for aluminum (Al), one of the most important materials in science and technology. Absolute photoabsorption (transmittance) measurements in the 17–1300 eV spectral range were performed on freestanding Al films protected by carbon (C) layers, to prevent oxidation. The dispersive portion of the refractive index was obtained via the Kramers–Kronig transformation. Our data provide significant improvements in accuracy compared to previously tabulated values and reveal fine structure in the Al L 1 and L 2,3 regions, with photon energy step sizes as small as 0.02 eV. The implications of this work in the successful realization of EUV/x-ray instruments and in the validation of atomic and molecular physics models are also discussed.

74 ATOMIC AND MOLECULAR PHYSICS↗

Acousto-optic modulators of high-power laser radiation on the basis of KGW and KYW crystals

Different modifications of acousto-optic modulators (AOMs) based on KG(WO{sub 4}){sub 2} (KGW) and KY(WO{sub 4}){sub 2} (KYW) crystals, designed for Q switching of high-power pulsed lasers, is developed and investigated. It is shown that AOMs based on these crystals are universal, can be combined with different lasers in the wavelength range of 1 – 3 μm, and have a high radiation resistance in the absence of antireflection coatings and light input at Brewster’s angle. The operation efficiency of KGW-based AOMs is experimentally demonstrated. Solid-state lasers based on Cr : Er : YSGG (λ = 2.78 μm), Cr : Yb : Ho : YSGG (λ = 2.87 μm), Cr : Tm : Ho : YSGG (λ = 2.09 μm), and Nd : YAG (λ = 1.064 μm) crystals with active acousto-optic Q switching, operating in the repetitively pulsed regime with a high beam quality and without surface destruction, are investigated. Lasing pulses (30 – 60)-ns long with energy up to 32 mJ at a repetition rate from 1 to 1000 Hz are obtained. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Quantum nanophotonic interface for tin-vacancy centers in thin-film diamond

The negatively charged tin-vacancy center in diamond (SnV − ) is an excellent solid state qubit with optically-addressable transitions and a long electron spin coherence time at elevated (∼1.7 K). However, implementing scalable quantum nodes with high-fidelity optical readout of the electron spin state requires efficient photon emission and collection from the system. Here, in this manuscript, we report a quantum photonic interface for SnV−centers based on one-dimensional photonic crystal cavities fabricated in diamond thin films. Furthermore, we provide a rigorous description of the spontaneous emission dynamics of our system, taking into account individual contributions from both the C and D transitions of the emitter. This allows for determination of Purcell factors per transition and, by extension, the C/D branching ratio SnV− zero phonon line. We observe quality factors up to ~6000 across this sample, and measure up to a 12-fold lifetime reduction, which translates into a Purcell factor of 𝐹 𝐶 =26.2±1.5 for a targeted C transition. By considering the cavity mode polarization alignment with the C and D transition dipole moments, we validate the C/D branching ratio to be 𝜂 BR =0.75±0.01, in line with previous theoretical and experimental findings.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Entanglement-enhanced matter-wave interferometry in a high-finesse cavity

An ensemble of atoms can operate as a quantum sensor by placing atoms in a superposition of two different states. Upon measurement of the sensor, each atom is individually projected into one of the two states. Creating quantum correlations between the atoms, that is entangling them, could lead to resolutions surpassing the standard quantum limit set by projections of individual atoms. Large amounts of entanglement involving the internal degrees of freedom of laser-cooled atomic ensembles have been generated in collective cavity quantum-electrodynamics systems, in which many atoms simultaneously interact with a single optical cavity mode. Here we report a matter-wave interferometer in a cavity quantum-electrodynamics system of 700 atoms that are entangled in their external degrees of freedom. In our system, each individual atom falls freely under gravity and simultaneously traverses two paths through space while entangled with the other atoms. In this work, we demonstrate both quantum non-demolition measurements and cavity-mediated spin interactions for generating squeezed momentum states with directly observed sensitivity $3.4^{+1.1}_{–0.9}$dB and $2.5^{+0.6}_{–0.6}$dB below the standard quantum limit, respectively. We successfully inject an entangled state into a Mach–Zehnder light-pulse interferometer with directly observed sensitivity $1.7^{+0.5}_{–0.5}$dB below the standard quantum limit. The combination of particle delocalization and entanglement in our approach may influence developments of enhanced inertial sensors, searches for new physics, particles and fields, future advanced gravitational wave detectors and accessing beyond mean-field quantum many-body physics.

74 ATOMIC AND MOLECULAR PHYSICS↗

Attosecond light-field control of high-density plasmas (Final Scientific/Technical Report)

Sub-optical-cycle dynamics of dense electron bunches in relativistic-intensity laser—solid interactions (relativistic plasma mirrors) lead to the emission of high-order harmonics and attosecond light pulses. The aim of this project was to advance our understanding of the fundamental principles underlying high-energy-density physics behind this phenomenon. We achieved this goal by conducting experiments and a comprehensive theoretical analysis of harmonics driven by specially tailored light waveforms providing precise control over the sub-laser-cycle trajectories of the emitting electron bunches. The multi-color laser waveforms, generated in our experiments in a cascaded plasma mirror configuration, allowed us to manipulate (enhance and suppress) harmonic generation in relativistic laser-solid interactions by adjusting the relative phase between the colors.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Gradient Field Detection Using Interference of Stimulated Microwave Optical Sidebands

Here, we demonstrate that stimulated microwave optical sideband generation using parametric frequency conversion can be utilized as a powerful technique for coherent state detection in atomic physics experiments. The technique has advantages over traditional absorption or polarization rotation-based measurements and enables the isolation of signal photons from probe photons. We outline a theoretical framework that accurately models sideband generation using a density matrix formalism. Using this technique, we demonstrate a novel intrinsic magnetic gradiometer that detects magnetic gradient fields between two spatially separated vapor cells by measuring the frequency of the beat note between sidebands generated within each cell. The sidebands are produced with high efficiency using parametric frequency conversion of a probe beam interacting with 87 Rb atoms in a coherent superposition of magnetically sensitive hyperfine ground states. Interference between the sidebands generates a low-frequency beat note whose frequency is determined by the magnetic field gradient between the two vapor cells. In contrast to traditional gradiometers the intermediate step of measuring the magnetic field experienced by the two vapor cells is unnecessary. We show that this technique can be readily implemented in a practical device by demonstrating a compact magnetic gradiometer sensor head with a sensitivity of 25 fT/cm/ √ Hz with a 4.4 cm baseline, while operating in a noisy laboratory environment unshielded from Earth’s field.

74 ATOMIC AND MOLECULAR PHYSICS↗

Time propagation of electronic wavefunctions using nonorthogonal determinant expansions

The use of truncated configuration interaction in real-time time-dependent simulations of electron dynamics provides a balance of computational cost and accuracy, while avoiding some of the failures associated with real-time time-dependent density functional theory. However, low-order truncated configuration interaction also has limitations, such as overestimation of polarizability in configuration interaction singles, even when perturbative doubles are included. Increasing the size of the determinant expansion may not be computationally feasible, and so, in this work, we investigate the use of nonorthogonality in the determinant expansion to establish the extent to which higher-order substitutions can be recovered, providing an improved description of electron dynamics. Model systems are investigated to quantify the extent to which different methods accurately reproduce the (hyper)polarizability, including the high-harmonic generation spectrum of H 2 , water, and butadiene.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Epitaxial (Al x Ga 1-x-y In y ) 2 O 3 Alloys Lattice Matched to Monoclinic Ga 2 O 3 Substrates

We have epitaxially stabilized a series of monoclinic (Al x Ga 1-x-y In y ) 2 O 3 alloys by careful choice of molecular beam epitaxy growth conditions, which balance alloy growth with suboxide desorption. The films are pseudomorphic to (010) β-Ga 2 O 3 substrates at thicknesses up to 150 nm with compositions ranging from (Al 0.01 Ga 0.83 In 0.16 ) 2 O 3 to (Al 0.24 Ga 0.75 In 0.03 ) 2 O 3 . The absorption edge shifts from approximately 4.62-5.14 eV with coincidently increasing Al and decreasing In mole fractions. J-V measurements reveal an increase in resistivity over four orders of magnitude with a maximum value of 4.2 x 10 5 Ω-cm for (Al 0.17 Ga 0.76 In 0.07 ) 2 O 3 , which has nearly identical lattice parameters (both in-plane and out-of-plane) to the underlying β-Ga 2 O 3 . Scanning transmission electron microscopy of this sample reveals a mostly uniform and single crystalline film, though we identify areas of non-uniform In incorporation and some γ-phase inclusions. This work demonstrates the feasibility of thick layers lattice-matched to β-Ga 2 O 3 with increased bandgap compared to phase-separation limited (Al,Ga) 2 O 3 . These alloys can enable higher bandgap epitaxial dielectrics and high sheet charge density transistors by increasing the conduction band offset with respect to β-Ga 2 O 3 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

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↗

1 / ω electric-field noise in surface ion traps from correlated adsorbate dynamics

Ion traps are promising architectures for implementing quantum computers, but they suffer from excessive “anomalous” ion motional heating that limit their overall coherence and practicality for scalable quantum computing. The exact microscopic origins of anomalous heating remain an open question, but experiments point to adsorbates on trap electrodes as one likely source. Many different models of anomalous heating have been proposed, but these models have yet to pinpoint the atomistic origin of the experimentally observed 1/ω electric-field noise scaling seen in ion traps at frequencies between 0.1–10 MHz. In this work, we show that a model based on previously proposed surface-induced dipole fluctuations on adsorbates, but which also incorporates interparticle interaction dynamics through molecular dynamics simulations of up to multiple monolayers of adsorbates, gives rise to 1/ω frequency scaling at the MHz frequencies typically employed in ion traps. Overall, these results demonstrate that moderate-to-high densities of adsorbates can give rise to a set of activated motions that produce the 1/ω noise observed in ion traps and that collective adsorbate motions produce the observed noise spectra that a noninteracting model does not capture.

36 MATERIALS SCIENCE↗

Quantum dynamics of cold atomic gas with SU(1,1) symmetry

Motivated by recent advances in quantum dynamics, we investigate the dynamics of the system with SU(1,1) symmetry. Instead of performing the time-ordered integral for the evolution operator of the time-dependent Hamiltonian, we show that the time evolution operator can be expressed as an SU(1,1) group element. Since the SU(1,1) group describes the “rotation” on a hyperbolic surface, the dynamics can be visualized on a Poincaré disk, a stereographic projection of the upper hyperboloid. As an example, we present the trajectory of the revival of Bose-Einstein condensation and that of the scale-invariant Fermi gas on the Poincaré disk. Further considering quantum gases in an oscillating lattice, we also study the dynamics of the system with time-dependent single-particle dispersion.

74 ATOMIC AND MOLECULAR PHYSICS↗

Robust analytic continuation of Green's functions via projection, pole estimation, and semidefinite relaxation

Green's functions of fermions are described by matrix-valued Herglotz-Nevanlinna functions. Since analytic continuation is fundamentally an ill-posed problem, the causal space described by the matrix-valued Herglotz-Nevanlinna structure can be instrumental in improving the accuracy and in enhancing the robustness with respect to noise. We demonstrate a three-pronged procedure for robust analytic continuation called PES: (1) projection of data to the causal space; (2) estimation of pole locations; and (3) semidefinite relaxation within the causal space. We compare the performance of PES with the recently developed Nevanlinna and Carathéodory continuation methods and find that PES is more robust in the presence of noise and does not require the usage of extended precision arithmetics. We also demonstrate that a causal projection improves the performance of the Nevanlinna and Carathéodory methods. The PES method is generalized to bosonic response functions, for which the Nevanlinna and Carathéodory continuation methods have not yet been developed. Furthermore, it is particularly useful for studying spectra with sharp features, as they occur in the study of molecules and band structures in solids.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Complete Frequency-Bin Bell Basis Synthesizer

Here we report the experimental generation of all four frequency-bin Bell states in a single versatile setup via successive pumping of spontaneous parametric down-conversion with single and dual spectral lines. Our scheme utilizes intensity modulation to control the pump configuration and offers turn-key generation of any desired Bell state using only off-the-shelf telecommunication equipment. We employ Bayesian inference to reconstruct the density matrices of the generated Bell states, finding fidelities ≥97% for all cases. Additionally, we demonstrate the sensitivity of the frequency-bin Bell states to common-mode and differential-mode temporal delays traversed by the photons comprising the state—presenting the potential for either enhanced resolution or nonlocal sensing enabled by our complete Bell basis synthesizer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

3D track reconstruction of low-energy electrons in the MIGDAL low pressure optical time projection chamber

Here, we demonstrate three-dimensional track reconstruction of electrons in a low pressure (50 Torr) optical TPC consisting of two glass GEMs with an ITO strip readout in CF 4 and CF 4 /Ar mixtures. The reconstructed tracks show a variety of event topologies, including short tracks from photoelectrons induced by 55 Fe 5.9 keV X-rays and long tracks from gamma ray interactions and beta decays. Algorithms for event identification and track ridge detection are discussed as well as multiple methods for integrating information from the camera image and ITO waveforms with the goal of full 3D reconstruction of the track.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Low-energy magneto-optics of Tb 2 Ti 2 O 7 in a [111] magnetic field

The pyrochlore magnet Tb 2 Ti 2 O 7 shows a lack of magnetic order to low temperatures and is considered to be a quantum spin liquid candidate. Here we perform time-domain THz spectroscopy on high-quality Tb 2 Ti 2 O 7 crystals and study the low-energy excitations as a function of [111] magnetic field with high energy resolution. The low-energy crystal-field excitations change their energies anomalously under magnetic field. Despite several sharp field-dependent changes, we show that the material's spectrum can be described not by phase transitions but by field-dependent hybridization between the low-energy crystal-field levels. We highlight the strong coupling between spin and lattice degrees of freedom in Tb 2 Ti 2 O 7 as evidenced by the magnetic-field tunable crystal-field environment. Calculations based on single ion physics with field-induced symmetry reduction of the crystal-field environment can reproduce our data.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗