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At least 91 records · Page 5

Information encoding in the spatial correlations of entangled twin beams

The ability to use the temporal and spatial degrees of freedom of quantum states of light to encode and transmit information is crucial for a robust and efficient quantum network. In particular, the potential offered by the large dimensionality of the spatial degree of freedom remains unfulfilled, as the necessary level of control required to encode information remains elusive. We encode information in the distribution of the spatial correlations of entangled twin beams by taking advantage of their dependence on the angular spectrum of the pump needed for four-wave mixing. We show that the encoded information can only be extracted through joint spatial measurements of the twin beams and not through individual beam measurements and that the temporal quantum correlations are not modified. The ability to engineer the spatial properties of twin beams will enable high-capacity quantum networks and quantum-enhanced spatially resolved sensing and imaging.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Excitation and detection of coherent nanoscale spin waves via extreme ultraviolet transient gratings

The advent of free electron lasers has opened the opportunity to explore interactions between extreme ultraviolet (EUV) photons and collective excitations in solids. While EUV transient grating spectroscopy, a noncollinear four-wave mixing technique, has already been applied to probe coherent phonons, the potential of EUV radiation for studying nanoscale spin waves has not been harnessed. Here we report EUV transient grating experiments with coherent magnons in Fe/Gd ferrimagnetic multilayers. Magnons with tens of nanometers wavelengths are excited by a pair of femtosecond EUV pulses and detected via diffraction of a probe pulse tuned to an absorption edge of Gd. The results unlock the potential of nonlinear EUV spectroscopy for studying magnons and provide a tool for exploring spin waves in a wave vector range not accessible by established inelastic scattering techniques.

Science & Technology - Other Topics↗

Heterodyne spectrometer sensitivity limit for quantum networking

We report optical heterodyne detection-based spectrometers are attractive due to their relatively simple construction and ultrahigh resolution. Here we demonstrate a proof-of-principle single-mode optical-fiber-based heterodyne spectrometer that has picometer resolution and quantum-limited sensitivity around 1550 nm. Moreover, we report a generalized quantum limit of detecting broadband multispectral-temporal-mode light using heterodyne detection, which provides a sensitivity limit on a heterodyne detection-based optical spectrometer. We then compare this sensitivity limit to several spectrometer types and dim light sources of interest such as spontaneous parametric downconversion, Raman scattering, and spontaneous four-wave mixing. We calculate that the heterodyne spectrometer is significantly less sensitive than a single-photon detector and is unable to detect these dim light sources, except for the brightest and narrowest-bandwidth examples.

47 OTHER INSTRUMENTATION↗

Spatially Multiplexed Cluster State Generation

We demonstrate the use of spatially multimode two-mode squeezed states (TMSSs) interfered at beamsplitters to generate an arbitrarily large cluster state. A four-mode state is generated using two TMSSs, leveraging spatial modes of four-wave mixing.

Leger, Zacharie [ORNL] (ORCID:0000000179044775)↗

Multimode description of self-mode locking in a single-section quantum-dot laser

This paper describes a theory for mode locking and frequency comb generation by four-wave mixing in a semiconductor quantum-dot active medium. The derivation uses a multimode semiclassical laser theory that accounts for fast carrier collisions within an inhomogeneous distribution of quantum dots. Numerical simulations are presented to illustrate the role of active medium nonlinearities in mode competition, gain saturation, carrier-induced refractive index and creation of combination tones that lead to locking of beat frequencies among lasing modes in the presence of cavity material dispersion.

Chow, Weng W.↗

Measuring an ultrashort, ultraviolet pulse in a slowly responding, absorbing medium

Frequency-resolved optical gating (FROG) is a common technique for measuring ultrashort laser pulses using an instantaneous, nonlinear-optical interaction as a fast time-gate to measure the pulse intensity and phase. But at high frequencies, materials are often absorbing and it is not always possible to find a medium with a fast nonlinear-optical response. Here we show that an ultrashort, ultraviolet (UV) pulse can be measured in a strongly absorbing medium, using the absorption as the nonlinear-optical time-gate. To do this, we build on our recent implementation of FROG, known as induced-grating cross-correlation FROG (IG XFROG), where an unknown, higher-frequency pulse creates a transient grating that is probed with a lower-frequency, more easily detectable reference pulse. We demonstrate this with an 800 nm reference pulse to characterize 400 nm or 267 nm pulses using ZnS as the nonlinear-optical medium, which is absorptive at and below 400 nm. By scanning the delay between the two UV pulses which create the transient grating, we show that the phase-sensitive instantaneous four-wave-mixing contribution to the nonlinear signal field can be detected and separated from the slower, incoherent part of the response. Measuring a spectrally-resolved cross-correlation in this way and then applying a simple model for the response of the medium, we show that a modified generalized projections (GP) phase-retrieval algorithm can be used to extract the pulse amplitude and phase. We test this approach by measuring chirped UV pulses centered at 400 nm and 267 nm. Since interband absorption (or even photoionization) is not strongly wavelength-dependent, we expect IG XFROG to be applicable deeper into the UV.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Rapid multiplex ultrafast nonlinear microscopy for material characterization

We demonstrate rapid imaging based on four-wave mixing (FWM) by assessing the quality of advanced materials through measurement of their nonlinear response, exciton dephasing, and exciton lifetimes. We use a WSe 2 monolayer grown by chemical vapor deposition as a canonical example to demonstrate these capabilities. By comparison, we show that extracting material parameters such as FWM intensity, dephasing times, excited state lifetimes, and distribution of dark/localized states allows for a more accurate assessment of the quality of a sample than current prevalent techniques, including white light microscopy and linear micro-reflectance spectroscopy. We further discuss future improvements of the ultrafast FWM techniques by modeling the robustness of exponential decay fits to different spacing of the sampling points. Employing ultrafast nonlinear imaging in real-time at room temperature bears the potential for rapid in-situ sample characterization of advanced materials and beyond.

36 MATERIALS SCIENCE↗

Compact fiber-coupled narrowband two-mode squeezed light source

Quantum correlated states of light, such as squeezed states, are a fundamental resource for the development of quantum technologies, as they are needed for applications in quantum metrology, quantum computation, and quantum communications. It is thus critical to develop compact, efficient, and robust sources to generate such states. Here, we report on a compact, narrowband, fiber-coupled source of two-mode squeezed states of light at 795 nm based on four-wave mixing (FWM) in an 85 Rb atomic vapor. The source is designed in a small modular form factor, with two input fiber-coupled beams, the seed and pump beams required for the FWM, and two output fibers, one for each of the modes of the squeezed state. The system is optimized for low pump power (135 mW) to achieve a maximum intensity-difference squeezing of 4.4 dB after the output of fibers at an analysis frequency of 1 MHz. Furthermore, the narrowband nature of the source makes it ideal for atomic-based quantum sensing and quantum networking configurations that rely on atomic quantum memories. Such a source paves the way for a versatile and portable platform for applications in quantum information science.

Jain, Umang [University of Oklahoma, Norman, OK (U↗

Characterizing non-polarization-maintaining highly nonlinear fiber toward squeezed-light generation

Squeezed light, which is easily degraded by loss, could benefit from generation directly in optical fiber. Furthermore, highly nonlinear fiber could offer more efficient generation with lower pump power and shorter fiber lengths than standard single-mode fiber. We investigate non-polarization-maintaining highly nonlinear fiber (HNLF) for squeezed-light generation by characterizing possible sources of excess noise, including its zero-dispersion wavelength (ZDW) variation and polarization noise. We find significant ZDW variation and excess polarization noise. We believe the polarization noise is from non-linear polarization-mode dispersion. We model this polarization noise and find that it is likely to degrade Kerr squeezing but not squeezing from four-wave mixing.

47 OTHER INSTRUMENTATION↗

Interpretable inverse-designed cavity for on-chip nonlinear photon pair generation

Inverse design is a powerful tool in wave physics for compact, high-performance devices. To date, applications in photonics have mostly been limited to linear systems and it has rarely been investigated or demonstrated in the nonlinear regime. In addition, the “black box” nature of inverse design techniques has hindered the understanding of optimized inverse-designed structures. We propose an inverse design method with interpretable results to enhance the efficiency of on-chip photon generation rate through nonlinear processes by controlling the effective phase-matching conditions. We fabricate and characterize a compact, inverse-designed device using a silicon-on-insulator platform that allows a spontaneous four-wave mixing process to generate photon pairs at a rate of 1.1 MHz with a coincidence to accidental ratio of 162. Our design method accounts for fabrication constraints and can be used for scalable quantum light sources in large-scale communication and computing applications.

42 ENGINEERING↗

Ultrafast temporal phase-resolved nonlinear optical spectroscopy in the molecular frame

In an ultrafast nonlinear optical interaction, the electric field of the emitted nonlinear signal provides direct access to the induced nonlinear transient polarization or transient currents and thus carries signatures of ultrafast dynamics in a medium. Measurement of the electric field of such signals offers sensitive observables to track ultrafast electron dynamics in various systems. In this work, we resolve the real-time phase of the electric field of a femtosecond third-order nonlinear optical signal in the molecular frame. The electric field emitted from impulsively pre-aligned gas-phase molecules at room temperature, in a degenerate four-wave mixing scheme, is measured using a spectral interferometry technique. The nonlinear signal is measured around a rotational revival to extract its molecular-frame angle dependence from pump-probe time-delay scans. By comparing these measurements for two linear molecules, carbon dioxide and nitrogen, we show that the measured second-order phase parameter (temporal chirp) of the signal is sensitive to the valence electronic symmetry of the molecules, whereas the amplitude of the signal does not show such sensitivity. We compare measurements to theoretical calculations of the chirp observable in the molecular frame. This work is an important step towards using electric field measurements in nonlinear optical spectroscopy to study ultrafast dynamics of electronically excited molecules in the molecular frame.

47 OTHER INSTRUMENTATION↗

Telecom-to-visible quantum frequency converter on a silicon nitride chip

Quantum frequency conversion serves a key role in the realization of hybrid quantum networks by interfacing between wavelength-incompatible platforms. Here we present what is believed to be the first quantum frequency converter connecting visible and telecom domains on a silicon nitride (SiN) chip, using Bragg-scattering four-wave mixing to upconvert heralded single photons from 1260 to 698 nm, which covers a 192 THz span. We examine the noise sources in SiN and devise approaches to suppress noise photons at the source and target frequencies to enable measurements at the single-photon level. We demonstrate an on-chip conversion efficiency of 5% in photon flux and describe design modifications that can be implemented to significantly improve it. Our results pave the way for the implementation of complementary metal-oxide-semiconductor (CMOS)-compatible devices in quantum networks.

59 BASIC BIOLOGICAL SCIENCES↗

Dynamics of Product Branching from Radical Intermediates in Elementary Combustion Reactions (Final Technical Report)

While the total rate constant for many elementary reactions is well-characterized, understanding the product branching in complex reactions presents a formidable challenge. To gain an incisive probe of such reactions, our experiments investigate the dynamics of the product channels that arise from transient radical intermediates along the bimolecular reaction coordinates. Our recent published work uses the methodology developed in my group in the last fifteen years, using both imaging and scattering apparatuses. The experiments generate a particular isomeric form of an unstable radical intermediate along a bimolecular reaction coordinate and study the branching between the ensuing product channels of the energized radical as a function of its internal rotational and vibrational energy under collision-less conditions. The experiments use a combination of: 1) measurement of product velocity and angular distributions in a crossed laser-molecular beam apparatus, with electron bombardment detection in my lab in Chicago or 2) with tunable vacuum ultraviolet photoionization detection at Taiwan's National Synchrotron Radiation Research Center (NSRRC), and 3) velocity map imaging using state-selective REMPI and single photon VUV ionization of radical intermediates and reaction products. We also employ tunable VUV photoionization detection in our imaging apparatus, using difference frequency four-wave mixing to produce photoionization light tunable from 8 to 10.8 eV. This year of support funded our work to photolytically generate the radical intermediate important in the OH + propene reaction when OH adds to an end carbon. Our other major result this past year was on the photoionization detection of vinoxy radicals. Our experiments at the NSRRC definitively show that vinoxy dissociatively ionizes to both CH 3 + and HCO + , and establishes the absolute partial photoionization cross section of vinoxy to CH 3 + at 10.5 and 11.44 eV. This should allow experimentalists detecting vinoxy radicals produced in bimolecular reactions such as OH + propene to get good branching fractions to that product channel. Finally we initiated studies of the photodissociation of 1-bromo-2-chloroethane and 1,1-bromochloroethane at 193 nm at the NSRRC.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Table-Top High Photon Energy Sources for Chemical Dynamics Investigations

Time-resolved spectroscopies using high-energy photons in the vacuum ultraviolet (VUV) to the X-ray region of the electromagnetic spectrum, have proven to be powerful probes of chemical dynamics. These high-energy photons can access valence and core orbitals of molecules and materials, providing key information on molecular and electronic structure and their time evolution. This report details the development of table-top sources of extreme ultraviolet (XUV) and VUV pulses at Sandia National Laboratories for use in studies of gas phase chemical dynamics. Femtosecond duration XUV pulses are produced using laser-driven high harmonic generation and their detected range span ~40-140 eV photon energies. These pulses are used in conjunction with ultraviolet pulses in a pump-probe scheme to study excited state dynamics of gas phase molecules. VUV pulses at 7.75 eV are generated using a four-wave-mixing scheme driven by 800 nm and 266 nm pulses in an argon-filled hollow-core fiber.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Development of theory and experimental operational framework for Coherent Thomson Scattering (Final Technical Report)

The research carried out explored and proved the feasibility and operational framework of a new diagnostic technique termed Coherent Thomson Scattering (CTS) for electrons in a low temperature plasma. The work is performed in collaboration with the Princeton Collaborative Research Facility (PCRF) at Princeton Plasma Physics Laboratory. The novel technique builds on an established and demonstrated single shot diagnostic method, called Coherent Rayleigh-Brillouin scattering, which has successfully been applied in neutral flows. The proposed novel four wave mixing diagnostic technique of CTS will allow for higher spatial resolution and lower detectable number densities for the electrons than conventional Thomson scattering. In this project we developed the theoretical framework for Coherent Thomson Scattering as well as the specification of the appropriate operational experimental parameters for successful CTS implementation in e.g. a low temperature plasma. Additionally, the mode of operation and the detection limits for a practical CTS experimental demonstration were explored. Ultimately, successful experimental demonstration of CTS can be seen as transformative in a multitude of plasma physics areas, since it will allow for detailed, non-perturbative measurements of electron density and temperature, previously unattainable by other measurement techniques. This project was the first successful step towards this direction.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Detection of trace contaminants released from rapidly heated pulsed power electrodes by laser diagnostics

Development of a capability to measure trace gas contaminants released from pulsed power electrodes would immediately impact Sandia pulsed power research. These releases occur during ultra-fast heating of metal electrodes during pulsed power discharges and can lead to substantial power losses through plasma formation. Detection of contaminants is a formidable challenge due to the need for in-situ spatially and temporally resolved measurements of trace gases in the extreme environment of ultra-fast heated metal surfaces. We investigate the feasibility of laser diagnostics for detecting contaminants, including H-atom, OH, and H 2 O. Laser-induced fluorescence and photofragmentation fluorescence showed significant plasma emission interferences and did not yield any detectable H-atom, OH, or H 2 O. Our newly developed H-atom detection using femtosecond degenerate four-wave mixing suppressed interferences and enabled detection of H-atoms. A few shots showed large signals in the near-surface region of metal foils, suggesting the formation of a wave of H-atoms from the metal.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

A Compact Monolithic Electro-Optic Package for Quantum Microwave-to-Optical Transduction

We present a novel quantum transduction package that integrates a macroscopic electro-optic crystal into a compact, monolithic assembly designed for superconducting quantum processors. The device provides an efficient and scalable interface between microwave and optical domains while preserving cryogenic compatibility. We performed full-wave and quantum dynamical simulations to assess the performance of the hybrid system, focusing on the interaction between a transmon-based microwave cavity and the crystal’s and cavity low-frequency microwave mode. The transmon operates both as an ancilla for the QPU and as a nonlinear element enabling four-wave mixing between cavity and electro-optic crystal microwave fields. Our results indicate that this architecture can coherently mediate quantum information transfer from the cavity to the electro-optic mode, offering a promising platform for on-chip quantum transduction within superconducting quantum networks.

Reineri, Alessandro [Fermilab] (ORCID:000000016175↗