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At least 127 records · Page 7

A cavity-enhanced spectroscopist's lens on molecular polaritons

Polariton chemistry has been hailed as a potential new route to direct molecular processes with electromagnetic fields. To make further strides, the community needs to clarify which unusual polaritonic phenomena are true hallmarks of cavity quantum electrodynamics and which can be rationalized with classical optical physics. Here, in this work, we provide a tutorial perspective on the formation, spectroscopy, and behavior of molecular polaritons using classical optics. Where possible, we draw connections to cavity-enhanced spectroscopy and recast open questions in terms that may be more familiar to the broader community of physical chemists.

Cavity quantum electrodynamics↗

Floquet engineering of polaritonic amplification in dispersive photonic time crystals

In this study, we investigate the dynamics of dispersive photonic time crystals (PTCs) and their potential applications for controlling light-matter interaction. Using the Lorentz-Drude as dispersive material model, we analyze the effects of periodic modulation of dispersion parameters through both theoretical and numerical analysis, revealing the emergence of hybrid bandgaps from the interaction of polaritonic branches with distinctive characteristics. Our study demonstrates that dispersive PTCs offer novel excitation channels and amplification possibilities, that require lower modulation frequencies compared to nondispersive systems thus alleviating experimental challenges for the realization of PTCs in the optical regime. These findings pave the way for advancements in polaritonic lasing and resonant Raman scattering.

Classical optics↗

Design of Ionization Profile Monitors at the Integrable Optics Test Accelerator Facility at Fermilab

The Integrable Optics Test Accelerator (IOTA) at Fermilab is transitioning from an electron beam facility to a proton beam facility for studies in nonlinear accelerator optics and space-charge dominated proton beams. This project involves the commissioning and fabrication of Ionization Profile Monitors (IPMs) to enable beam profile measurements at IOTA. In general, IPMs work on principle of residual gas ionization by the beam to generate beam profile. This work focuses on a mechanical design that leverages a controlled injection of noble gases, primarily Argon, as the ultra-high vacuum of the IOTA ring provides insufficient residual gas for ionization. Efforts to understand vacuum integration to ensure compatibility with the storage ring environment, the integration of real-time data acquisition systems and the commissioning of the IPMs will be discussed. This project provides a versatile diagnostic tool, supporting IOTA’s role as a testbed for larger-scale accelerator facilities and contributing to the broader understanding of beam physics in high-intensity, high-space-charge regimes.

Mwaniki, M. W. [IIT, Chicago] (ORCID:0000000169057↗

Many-body enhancement of high-harmonic generation in monolayer MoS2

Abstract Many-body effects play an important role in enhancing and modifying optical absorption and other excited-state properties of solids in the perturbative regime, but their role in high harmonic generation (HHG) and other nonlinear response beyond the perturbative regime is not well-understood. We develop here an ab initio many-body method to study nonperturbative HHG based on the real-time propagation of the non-equilibrium Green’s function with the GW self energy. We calculate the HHG of monolayer MoS 2 and obtain good agreement with experiment, including the reproduction of characteristic patterns of monotonic and nonmonotonic harmonic yield in the parallel and perpendicular responses, respectively. Here, we show that many-body effects are especially important to accurately reproduce the spectral features in the perpendicular response, which reflect a complex interplay of electron-hole interactions (or exciton effects) in tandem with the many-body renormalization and Berry curvature of the independent quasiparticle bandstructure.

36 MATERIALS SCIENCE↗

Soft x-ray high-harmonic generation in an anti-resonant hollow core fiber driven by a 3 μ m ultrafast laser

High-harmonic upconversion driven by a mid-infrared femtosecond laser can generate coherent soft x-ray beams in a tabletop-scale setup. Here, we report on a compact ytterbium-pumped optical parametric chirped pulse amplifier (OPCPA) laser system seeded by an all-fiber front-end and employing periodically poled lithium niobate (PPLN) nonlinear media operated near the pulse fluence limits of current commercially available PPLN crystals. The OPCPA delivers 3 µm wavelength pulses with 775 µJ energy at 1 kHz repetition rate, with transform-limited 120 fs pulse duration, diffraction-limited beam quality, and ultrahigh 0.33% rms energy stability over >18 h. Using this laser, we generate soft x-ray high harmonics (HHG) in argon gas by focusing into a low-loss, high-pressure gas-filled anti-resonant hollow core fiber (ARHCF), generating coherent light at photon energies up to the argon L-edge (250 eV) and carbon K-edge (284 eV), with high beam quality and ∼1% rms energy stability. This work demonstrates soft x-ray HHG in a high-efficiency guided-wave phase matched geometry, overcoming the high losses inherent to mid-IR propagation in unstructured waveguides, or the short interaction lengths of gas cells or jets. The ARHCF can operate in the long term without damage and with the repetition rate, stability, and robustness required for demanding applications in spectromicroscopy and imaging. Finally, we discuss routes for further optimizing the soft x-ray HHG flux by driving He at higher laser intensities using either the signal (1.5 μm) or idler wavelengths (3 μm).

Femtosecond lasers↗

Dephasingless two-color terahertz generation

A laser pulse composed of a fundamental and an appropriately phased second harmonic can drive a time-dependent current of photoionized electrons that generates broadband THz radiation. Over the propagation distances relevant to many experiments, dispersion causes the relative phase between the harmonics to evolve. This “dephasing” slows the accumulation of THz energy and results in a multi-cycle THz pulse with significant angular dispersion. Here, we introduce a novel optical configuration that compensates the relative phase evolution, allowing for the formation of a half-cycle THz pulse with almost no angular dispersion. The configuration uses the spherical aberration of an axilens to map a prescribed radial phase variation in the near field to a desired longitudinal phase variation in the far field. Simulations that combine this configuration with an ultrashort flying focus demonstrate the formation of a half-cycle THz pulse with a controlled emission angle and 1/4 the angular divergence of the multi-cycle pulse created by a conventional optical configuration.

47 OTHER INSTRUMENTATION↗

Experimental measurements for extracting nonlinear invariants

Nonlinear integrable optics are a promising alternative approach to lattice design. The integrable optics test accelerator (IOTA) at Fermilab has been constructed for dedicated studies of magnetostatic elliptical elements as described by Danilov and Nagaitsev. The most compelling verification of correct implementation of the NIO lattice is direct observation of the analytically expected invariants. This report outlines the experimental and analytical methods for extracting the nonlinear invariants of motion from data gathered in the last IOTA run.

43 PARTICLE ACCELERATORS↗

Broken symmetries associated with a Kagome chiral charge order

Chirality, or handedness, is ubiquitous in science, from cell biology to physics, and in condensed matter can underlie exotic phases such as chiral charge density waves and chiral superconductivity. However, detecting subtle broken symmetries that define such states is challenging, leading to debate and controversy. Here, using second-order optical response, we reveal the broken symmetries of a chiral charge density wave in the Kagome lattice KV 3 Sb 5 . Polarization-dependent mid-infrared photocurrent microscopy uncovers a longitudinal, helicity-dependent photocurrent associated with the charge order, indicating broken inversion and mirror symmetries. These findings, supported by theoretical analysis, directly establish the intrinsic chiral nature of the ordered state. Moreover, the absence of a circular photogalvanic effect perpendicular to the incident light imposes stringent constraints on the point-group symmetries. Our study not only visualizes the chiral nature of the Kagome charge order, but also highlights the nonlinear photogalvanic effect as a sensitive probe for detecting subtle symmetry breakings.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Shock compression of diamond single crystals to 120 GPa: Refractive index and nonlinear photoelasticity

The optical response of transparent solids at extreme conditions is important for both fundamental science and many applications. Strong transparent solids are of particular interest for use as optical windows in dynamic compression experiments. Due to diamond’s exceptional strength and optical properties, laser-driven shock experiments and plate impact experiments were carried out to examine the diamond optical response for shock wave compression along two different crystal orientations. Using laser interferometry at 532 nm and 1550 nm wavelengths, optical transparency was observed and refractive indices were determined for [100] diamond at stresses up to 119 GPa and for [111] diamond at stresses up to 87 GPa. From these results, the nonlinear photoelastic response for [100] and [111] diamond was determined, revealing significant dependence on both crystal orientation and laser wavelength. To enable [100] diamond as an interferometry window in dynamic compression experiments, the requisite window corrections were determined for 532 nm and 1550 nm wavelengths. Because of diamond’s excellent x-ray transparency, the present findings will be particularly useful for incorporating [100] diamonds as windows in dynamic compression experiments involving x-ray diffraction or other x-ray diagnostics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

A 1-km photonic link connecting superconducting circuits in two dilution refrigerators

Superconducting quantum processors are a leading platform for implementing practical quantum computation algorithms. Although superconducting quantum processors with hundreds of qubits have been demonstrated, their further scale-up is constrained by the physical size and cooling power of dilution refrigerators. This constraint can be overcome by constructing a quantum network to interconnect qubits hosted in different refrigerators, which requires microwave-to-optical transducers to enable low-loss signal transmission over long distances. Although various designs and demonstrations have achieved high-efficiency and low-added-noise transducers, a coherent photonic link between separate refrigerators has not yet been realized. Here, in this work, we experimentally demonstrate coherent signal transfer between two superconducting circuits housed in separate dilution refrigerators, enabled by a pair of frequency-matched aluminium nitride electro-optic transducers connected via a 1-km telecom optical fibre. The optical frequency matching between two transducers is realized by an asymmetric photonic molecule design, and an overall 80 dB improvement in transduction efficiency over commercial electro-optic modulators is achieved, paving the way towards a fully quantum-enabled link. This work provides critical design guidelines for scalable superconducting quantum networks interconnected by photonic links.

nonlinear optics↗

Tomography of longitudinal phase space linearization for the generation of attosecond electron bunches

The generation of electron bunches on the attosecond timescale is important for a multitude of accelerator-based applications. Here, we report on a tomographic measurement of the (pre)linearized longitudinal phase space of a low charge 3 MeV electron bunch generated with the 1.6 cell Pegasus photoinjector for the generation of attosecond bunches. The nonlinear correlations in the longitudinal phase space induced by space charge at the photocathode, radiofrequency field curvature of the gun, and vacuum dispersion are compensated using a compact X-band linearizer. Then, the initial and compensated phase of the picosecond electron bunch is precisely reconstructed by neural network assisted tomographic reconstruction from momentum spectra at varying buncher linac phase. Finally, we combine the measured phase space shape with particle tracking simulations to show that electron bunches as short as 941 as develop downstream the beamline.

Beam control↗

Joint Experimental and Computational Characterization of Sum-Frequency Generation between a Continuous Wave Laser and an Ultrafast Frequency Comb Laser for Tunable Laser Development

Ultrafast optical frequency combs allow for both high spectral and temporal resolution in molecular spectroscopy and have become a powerful tool in many areas of chemistry and physics. Ultrafast lasers and frequency combs generated from ultrafast mode-locked lasers often need to be converted to other wavelengths. Commonly used wavelength conversions are optical parametric oscillators, which require an external optical cavity, and supercontinuum generation combined with optical parametric amplifiers. Whether commercial or home-built, these systems are complex and costly. Here, we investigate an alternative, simple, and easy-to-implement approach to tunable frequency comb ultrafast lasers enabled by new continuous-wave laser technology. Sum-frequency generation between an Nd:YAG continuous-wave laser and a Yb:fiber femtosecond frequency comb in a beta-barium borate (BBO) crystal is explored. The resulting sum-frequency beam is a pulsed frequency comb with the same repetition rate as the Yb:fiber source. SNLO simulation software is used to simulate the results and provide benchmarks for designing future systems to achieve wavelength conversion and tunability in otherwise difficult-to-reach spectral regions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Crystal Growth of Quaternary Rare Earth Selenosilicates by Using the Flux-Assisted Boron Chalcogen Mixture Method: Investigation of Their Magnetic and Optical Properties

A series of rare earth magnesium selenosilicates, RE3Mg 0.5 SiSe 7 (RE = Ce, Pr, Nd, Sm, Gd, Tb, Dy) were obtained as single crystal using the flux assisted boron chalcogen mixture (BCM) method. The structures of the crystals were determined by single-crystal X-ray diffraction. The RE3Mg 0.5 SiSe 7 series crystallizes in the hexagonal crystal system in the space group P6 3 . Polycrystalline powders were synthesized to perform physical property measurements. Magnetic measurements over the 2–300 K temperature range reveal that Ce 3 Mg 0.5 SiSe 7 and Gd 3 Mg 0.5 SiSe 7 exhibit paramagnetic behavior with negative Weiss constants (θ W = −14.50, θ W = −6.13 K, respectively). The optical properties of RE 3 Mg 0.5 SiSe 7 (RE = Ce, Pr, Nd, Sm, Gd) were measured by ultraviolet–visible (UV–vis) diffuse reflectance. Density functional theory (DFT) electronic structure calculations were performed. Furthermore, a second harmonic generation measurement was performed on a polycrystalline powder of Ce 3 Mg 0.5 SiSe 7 and was found to be SHG active with an efficiency of 0.11 times the standard potassium dihydrogen phosphate (KDP).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Determining the complex second-order optical susceptibility in macroscale van der Waals heterobilayers

In this work, we report on the experimental characterization of the second-order susceptibility in MoSe 2 /WS 2 heterobilayers, including their hidden complex phases. To this end, we developed a heterodyne-detection scheme for second-harmonic generation and applied it to macroscale heterobilayer samples prepared using the gold-tape exfoliation method. The heterodyne scheme enabled us to distinguish the relative orientation of the crystal domains, and furthermore, it allowed us to characterize the complex phases of the susceptibility relative to a reference quartz sample. By comparing the results from the monolayer regions and the heterobilayer region over several hundred microns of the sample area, we determined that the contribution of interlayer effects to second-harmonic generation is within the experimental uncertainty arising from the sample inhomogeneity. The results here provide fundamental quantitative information necessary for the precise design of nanophotonic systems based on stacking engineering.

2D materials↗

Extreme-ultraviolet spatiotemporal vortices via high harmonic generation

Spatiotemporal optical vortices (STOVs) are space–time structured light pulses with a unique topology that couples spatial and temporal domains and carry transverse orbital angular momentum (OAM). Up to now, their generation has been limited to the visible and infrared regions of the spectrum. During the last decade, it was shown that through the process of high-order harmonic generation, it is possible to upconvert spatial optical vortices that carry longitudinal OAM from the near-infrared into the extreme-ultraviolet (EUV), thereby producing vortices with distinct femtosecond and attosecond structure. In this work, we demonstrate theoretically and experimentally the generation of EUV spatiotemporal and spatiospectral vortices using near-infrared STOV driving laser pulses. Here, we use analytical expressions for focused STOVs to perform macroscopic calculations of high-order harmonic generation that are directly compared to the experimental results. As STOV beams are not eigenmodes of propagation, we characterize the highly charged EUV STOVs in both the near and far fields to show that they represent conjugated spatiotemporal and spatiospectral vortex pairs. Our work provides high-frequency light beams topologically coupled at the nanometre/attosecond scales domains with transverse OAM that could be suitable to explore electronic dynamics in magnetic materials, chiral media and nanostructures.

High-harmonic generation↗

Peculiar Magnetic and Magneto-Transport Properties in a Noncentrosymmetric Self-Intercalated van der Waals Ferromagnet Cr 5 Te 8

Trigonal Cr 5 Te 8 , a self-intercalated van der Waals ferromagnet with an out-of-plane magnetic anisotropy, has long been known to crystallize in a centrosymmetric structure. However, optical second harmonic generation experiments, together with comprehensive structural analysis, indicate that this compound rather adopts a noncentrosymmetric structure. Lorentz transmission electron microscopy reveals the presence of Néel-type skyrmions, consistent with its noncentrosymmetric structure. A large anomalous Hall conductivity of 102 Ω –1 cm –1 at low temperature stems from intrinsic origin, which is larger than any previously reported values in the bulk Cr–Te system. Notably, spontaneous topological Hall resistivity arising from the skyrmionic phase has been observed. Here, our findings not only elucidate the unique magnetic and magneto-transport properties of noncentrosymmetric trigonal Cr 5 Te 8 , but also open new avenues for investigating the effects of broken inversion symmetry on material properties and their potential applications.

crystal structure↗

Quantum control of Hubbard excitons

Quantum control of the many-body wavefunction is a central challenge in quantum materials research, as it could yield a precise control knob to manipulate emergent phenomena. Floquet engineering, the coherent dressing of quantum states with periodic non-resonant optical fields, has become an important strategy for quantum control. Most applications to solid-state systems have targeted weakly interacting or single-ion states, leaving the manipulation of many-body wavefunctions largely unexplored. Here, in this work, we use Floquet engineering to achieve quantum control of a strongly correlated Hubbard exciton in the one-dimensional Mott insulator Sr 2 CuO 3 . A nonresonant midinfrared optical field coherently dresses the exciton wavefunction, driving its rotation between bright and dark states. We use resonant third-harmonic generation to quantify ultrafast π/2 rotations on the Bloch sphere spanned by these exciton states. Our work advances the quest towards programmable control of correlated states and exciton-based quantum sensing.

36 MATERIALS SCIENCE↗