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At least 199 records · Page 11

Terahertz 2D coherent spectroscopy for probing and controlling multicorrelations in quantum matter

Terahertz 2D coherent spectroscopy (THz-2DCS) is an emerging technique that brings multidimensional resolution to the ultrafast spectral–temporal dynamics of non-equilibrium quantum phases of matter, enabling new capabilities for precise coherent control in many-body dynamics and multiorder correlations. Here, by mapping and disentangling complex excitation and detection pathways across distinct time and frequency dimensions, THz-2DCS provides a form of coherence tomography of light-induced quantum matter — revealing multiquantum coherences, separating nonlinear response functions and capturing collective modes and quantum kinetics on ultrafast THz timescales. This Perspective discusses the technical capabilities of THz-2DCS, provides a comparison to other multidimensional and coherent transient spectroscopies and looks ahead towards opportunities for advancing THz-2DCS instrumentation and experimental strategies towards new frontier discoveries.

Huang, Chuankun [Ames Laboratory (AMES), Ames, IA ↗

Entangled Photon Spectroscopy

Conspectus The enhanced interest in quantum-related phenomena has provided new opportunities for chemists to push the limits of detection and analysis of chemical processes. As some have called this the second quantum revolution, a time has come to apply the rules learned from previous research in quantum phenomena toward new methods and technologies important to chemists. While there has been great interest recently in quantum information science (QIS), the quest to understand how nonclassical states of light interact with matter has been ongoing for more than two decades. Our entry into this field started around this time with the use of materials to produce nonclassical states of light. Here, the process of multiphoton absorption led to photon-number squeezed states of light, where the photon statistics are sub-Poissonian. In addition to the great interest in generating squeezed states of light, there was also interest in the formation of entangled states of light. While much of the effort is still in foundational physics, there are numerous new avenues as to how quantum entanglement can be applied to spectroscopy, imaging, and sensing. These opportunities could have a large impact on the chemical community for a broad spectrum of applications. Here, we discuss the use of entangled (or quantum) light for spectroscopy as well as applications in microscopy and interferometry. The potential benefits of the use of quantum light are discussed in detail. From the first experiments in porphyrin dendrimer systems by Dr. Dong-Ik Lee in our group to the measurements of the entangled two photon absorption cross sections of biological systems such as flavoproteins, the usefulness of entangled light for spectroscopy has been illustrated. These early measurements led the way to more advanced measurements of the unique characteristics of both entangled light and the entangled photon absorption cross-section, which provides new control knobs for manipulating excited states in molecules. The first reports of fluorescence-induced entangled processes were in organic chromophores where the entangled photon cross-section was measured. These results would later have widespread impact in applications such as entangled two-photon microscopy. From our design, construction and implementation of a quantum entangled photon excited microscope, important imaging capabilities were achieved at an unprecedented low excitation intensity of 10 7 photons/s, which is 6 orders of magnitude lower than the excitation level for the classical two-photon image. New reports have also illustrated an advantage of nonclassical light in Raman imaging as well. From a standpoint of more precise measurements, the use of entangled photons in quantum interferometry may offer new opportunities for chemistry research. Experiments that combine molecular spectroscopy and quantum interferometry, by utilizing the correlations of entangled photons in a Hong–Ou–Mandel (HOM) interferometer, have been carried out. The initial experiment showed that the HOM signal is sensitive to the presence of a resonant organic sample placed in one arm of the interferometer. In addition, parameters such as the dephasing time have been obtained with the opportunity for even more advanced phenomenology in the future.

36 MATERIALS SCIENCE↗

Controlling the dopant profile for SRH suppression at low current densities in λ ≈ 1330 nm GaInAsP light-emitting diodes

The quantum efficiency of double hetero-junction light-emitting diodes (LEDs) can be significantly enhanced at low current density by tailoring the spatial profile of dopants to suppress Shockley–Read–Hall recombination. To demonstrate this effect, we model, design, grow, fabricate, and test a GaInAsP LED (λ≈ 1330 nm) with an unconventional dopant profile. Compared against that of our control design, which is a conventional n + -n - p + double hetero-junction LED, the dopant profile near the n - p + hetero-structure of the design displaces the built-in electric field in such a way that the J 02 space charge recombination current is suppressed. The design principle generalizes to other material systems and could be applicable to efforts to observe and exploit electro-luminescent refrigeration at practical power densities.

42 ENGINEERING↗

Photonic integration of Er 3+ :Y 2 SiO 5 with thin-film lithium niobate by flip chip bonding

Rare earth ions are known as promising candidates for building quantum light-matter interface. However, tunable photonic cavity access to rare earth ions in their desired host crystal remains challenging. Here, we demonstrate the integration of erbium doped yttrium orthosilicate (Er 3+ :Y 2 SiO 5 ) with thin-film lithium niobate photonic circuit by plasma-activated direct flip chip bonding. Resonant coupling to erbium ions is realized by on-chip electro-optically tuned high Q lithium niobate micro-ring resonators. Fluorescence and absorption of erbium ions at 1536.48 nm are measured in the waveguides, while the collective ion-cavity cooperativity with micro-ring resonators is assessed to be 0.36. This work presents a versatile scheme for future rare earth ion integrated quantum devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Low-loss millimeter-wave resonators with an improved coupling structure

Millimeter-wave superconducting resonators are a useful tool for studying quantum device coherence in a new frequency domain. However, improving resonators is difficult without a robust and reliable method for coupling millimeter-wave signals to 2D structures. We develop and characterize a tapered transition structure coupling a rectangular waveguide to a planar slotline waveguide with better than 0.5 dB efficiency over 14 GHz, and use it to measure ground-shielded resonators in the W band (75–110 GHz). Having decoupled the resonators from radiative losses, we consistently achieve single-photon quality factors above 10 5 , with a two-level-system loss limit above 10 6 , and verify the effectiveness of oxide removal treatments to reduce loss. These values are 4–5 times higher than those previously reported in the W band, and much closer to typical planar microwave resonators. The improved losses demonstrated by these on-chip millimeter-wave devices shed new light on quantum decoherence in a different frequency regime, offer increased selectivity for high-frequency detectors, and enables new possibilities for hybrid quantum experiments integrating millimeter-wave frequencies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Environmentally Robust Quantum Dot Down Converters for Highly Efficient Solid State Lighting

This project contributes fundamental understanding of the chemical synthesis of cadmium free quantum dots (QDs) designed for solid state lighting (SSL). Methods to incorporate gallium into quantum dot architectures were explored, which led to more stable and brighter solid state lighting devices. These findings will help advance the incorporation of quantum dots in highly energy efficient lighting devices with a warm color spectrum. Such Cd-free lighting devices can greatly accelerate the adoption of high efficiency, warm spectrum lighting in buildings. The project targeted InP/GaP/ZnS colloidal quantum dots that more effectively absorb the blue light produced by light emitting diode packages and emit monochromatic red light with near perfect efficiency. While significant improvements in the QD absorptivity were demonstrated, the absorbance increase achieved was 3x rather than the targeted 10x increase. Similarly, the luminescence from these QDs achieved about half of the target photoluminescence quantum yield (PLQY) and twice the desired spectral width, a measure of the color purity of their luminescence. While the target characteristics and some of the year 2/2 milestones were not met, the new QD architectures did lead to greater stability on SSL packages, a sign of the long term promise of the technology.

36 MATERIALS SCIENCE↗

Wavelength-Selective Reactivity of Iron(III) Halide Salts in Photocatalytic C–H Functionalization

The utility of halogen radicals in hydrocarbon functionalization extends from early examples of photochemical halogenation to recent reports using photoredox catalysis with iridium complexes and simple transition metal salts such as FeCl 3 . The majority of these methods (uncatalyzed and iron-catalyzed) require UV light (λ ≤ 390 nm), and systematic efforts to enable the use of visible light remain valuable. We report the use of a simple Fe(III) salt that enables a C–H to C–C and C–N functionalization under visible light. The reactivity and selectivity profile using different light sources demonstrates wavelength-selective behavior, which was further investigated with deuterium kinetic isotope effect experiments and DFT calculations. These results show that control over the reactive intermediates in this iron-catalyzed reaction can be achieved through proper choice of the wavelength of irradiation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Deterministic modeling of hybrid nonlinear effects in epsilon-near-zero thin films

In nonlinear optics, significant effort is concentrated on improving the strength and efficiency of interactions; however, experimentally investigating nonlinear materials is a complex, time-consuming, and costly investment. Moreover, it is often challenging to isolate, study, and optimize material parameters in an experiment due to complexities in the growth process. Recently, epsilon-near-zero materials have received a great deal of attention as promising nonlinear optical materials, but like many up-and-coming materials, the ability to explore and optimize their properties has been challenging. Here, we establish a framework to rapidly evaluate the performance of nonlinear epsilon-near-zero materials for both inter- and intraband effects in silico, requiring only an energy-momentum (E-k) diagram, linear optical properties, and experimental conditions. Measured nonlinear reflection and transmission in gallium-doped zinc oxide films are compared to the numerical framework for both intra- and interband excitation to verify accuracy across wavelength and irradiance while two figures of merit (FoMs) are introduced to quickly evaluate the performance of films without a full numerical framework. This capability is used to predict the performance of highly doped gallium nitride, cadmium oxide, zinc oxide, and indium tin oxide films, and efficient intra- and interband operation conditions are identified. Through this numerical framework and the FoMs, the exploration of unstudied epsilon-near-zero materials is enabled without the need for a nonlinear experiment, thereby accelerating the search for more efficient nonlinear materials and excitation conditions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Non-Gaussian photonic state engineering with the quantum frequency processor

Non-Gaussian quantum states of light are critical resources for optical quantum information processing, but methods to generate them efficiently remain challenging to implement. Here we introduce a generic approach for non-Gaussian state production from input states populating discrete frequency bins. Based on controllable unitary operations with a quantum frequency processor, followed by photon-number-resolved detection of ancilla modes, our method combines recent developments in both frequency-based quantum information and non-Gaussian state preparation. Leveraging and refining the K-function representation of quantum states in the coherent basis, we develop a theoretical model amenable to numerical optimization and, as specific examples, design quantum frequency processor circuits for the production of Schrödinger cat states, exploring the performance tradeoffs for several combinations of ancilla modes and circuit depth. Our scheme provides a valuable framework for producing complex quantum states in frequency bins, paving the way for single-spatial-mode, fiber-optic-compatible non-Gaussian resources.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Dynamics of Spin Polarization in Tilted Polariton Rings

We have observed the effect of pseudomagnetic field originating from the polaritonic analog of spin-orbit coupling [transverse electric and transverse magnetic (TE-TM) splitting] on a polariton condensate in a ring-shaped microcavity. The effect gives rise to a stable four-leaf pattern around the ring as seen from the linear polarization measurements of the condensate photoluminescence. This pattern is found to originate from the interplay of the cavity potential, energy relaxation, and TE-TM splitting in the ring. Our observations are compared to the dissipative one-dimensional spinor Gross-Pitaevskii equation with the TE-TM splitting energy, which shows good qualitative agreement.

CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS↗

Observation of biexciton emission from single semiconductor nanoplatelets

Quasi-two-dimensional semiconductor nanoplatelets (NPLs) are intriguing systems for studying the influence of Auger recombination processes on the multiexciton emission efficiencies in the weak in-plane confinement regime. We investigate CdSe/CdS core/shell NPLs using cryogenic temperature single particle spectroscopy and observe bright biexciton emission at high excitation powers. The average binding energy of the biexcitons is determined to be 16.5 meV. The observed switching between the biexciton and trion states indicates charging-decharging dynamics of the NPLs mediated by the Auger ionization process. These findings are highly relevant for harvesting efficient biexciton emission for energy, lighting, and quantum applications.

36 MATERIALS SCIENCE↗

Role of Matter Interactions in Superradiant Phenomena

The superradiant phenomenon, usually described by the Dicke model, is a hallmark of strong light-matter interaction. Here, we explore how matter-matter interactions influence this phenomenon by performing ground-state simulations of Dicke-like models with both isotropic and anisotropic interactions. We find that Ising-type interactions produce two qualitatively distinct phase boundaries, one of which gives rise to an antiferromagnetic-normal phase connected to the superradiant regime via a first-order phase transition. Under anisotropic couplings, we uncover a strongly correlated phase where in-plane spin order coexists with superradiance, exhibiting sublinear scaling of the photon occupation per site and power-law decay of spin correlations. Furthermore, superradiance is strengthened by tuning either isotropic or anisotropic interactions, highlighting the role of intrinsic many-body correlations in shaping light-matter quantum phases.

Dicke model↗

3D quantum ghost imaging microscope

Quantum ghost imaging uses quantum-entangled photons to generate a two-dimensional image with only a bucket detector at the sample. Here we expand on this approach to generate a three-dimensional image without scanning. A quantum-entangled light source directly links information between a pair of 2D sensors, one of which captures a standard image from one perspective and a second sensor which captures a ghost image from a perpendicular perspective. By correlating the spatial information from the two detectors for each photon pair, we obtain three dimensions of spatial information (x, y, and z) for each scattered photon. We demonstrate that this system can study microscopic environments by imaging scattering from metallic nanoparticle clusters. This approach has the potential to greatly reduce the flux of light required to obtain a 3D image of a biological sample and thereby extend the number of images that can be obtained before photodamaging the sample.

Eshun, Audrey [Lawrence Livermore National Laborat↗