More Like this

1. Lithium niobate photonics: Unlocking the electromagnetic spectrum

   https://doi.org/10.1126/science.abj4396  

   Boes, Andreas ; Chang, Lin ; Langrock, Carsten ; Yu, Mengjie ; Zhang, Mian ; Lin, Qiang ; Lončar, Marko ; Fejer, Martin ; Bowers, John ; Mitchell, Arnan ( January 2023 , Science)

   BACKGROUND Electromagnetic (EM) waves underpin modern society in profound ways. They are used to carry information, enabling broadcast radio and television, mobile telecommunications, and ubiquitous access to data networks through Wi-Fi and form the backbone of our modern broadband internet through optical fibers. In fundamental physics, EM waves serve as an invaluable tool to probe objects from cosmic to atomic scales. For example, the Laser Interferometer Gravitational-Wave Observatory and atomic clocks, which are some of the most precise human-made instruments in the world, rely on EM waves to reach unprecedented accuracies. This has motivated decades of research to develop coherent EM sources over broad spectral ranges with impressive results: Frequencies in the range of tens of gigahertz (radio and microwave regimes) can readily be generated by electronic oscillators. Resonant tunneling diodes enable the generation of millimeter (mm) and terahertz (THz) waves, which span from tens of gigahertz to a few terahertz. At even higher frequencies, up to the petahertz level, which are usually defined as optical frequencies, coherent waves can be generated by solid-state and gas lasers. However, these approaches often suffer from narrow spectral bandwidths, because they usually rely on well-defined energy states of specific materials, which results inmore »a rather limited spectral coverage. To overcome this limitation, nonlinear frequency-mixing strategies have been developed. These approaches shift the complexity from the EM source to nonresonant-based material effects. Particularly in the optical regime, a wealth of materials exist that support effects that are suitable for frequency mixing. Over the past two decades, the idea of manipulating these materials to form guiding structures (waveguides) has provided improvements in efficiency, miniaturization, and production scale and cost and has been widely implemented for diverse applications. ADVANCES Lithium niobate, a crystal that was first grown in 1949, is a particularly attractive photonic material for frequency mixing because of its favorable material properties. Bulk lithium niobate crystals and weakly confining waveguides have been used for decades for accessing different parts of the EM spectrum, from gigahertz to petahertz frequencies. Now, this material is experiencing renewed interest owing to the commercial availability of thin-film lithium niobate (TFLN). This integrated photonic material platform enables tight mode confinement, which results in frequency-mixing efficiency improvements by orders of magnitude while at the same time offering additional degrees of freedom for engineering the optical properties by using approaches such as dispersion engineering. Importantly, the large refractive index contrast of TFLN enables, for the first time, the realization of lithium niobate–based photonic integrated circuits on a wafer scale. OUTLOOK The broad spectral coverage, ultralow power requirements, and flexibilities of lithium niobate photonics in EM wave generation provides a large toolset to explore new device functionalities. Furthermore, the adoption of lithium niobate–integrated photonics in foundries is a promising approach to miniaturize essential bench-top optical systems using wafer scale production. Heterogeneous integration of active materials with lithium niobate has the potential to create integrated photonic circuits with rich functionalities. Applications such as high-speed communications, scalable quantum computing, artificial intelligence and neuromorphic computing, and compact optical clocks for satellites and precision sensing are expected to particularly benefit from these advances and provide a wealth of opportunities for commercial exploration. Also, bulk crystals and weakly confining waveguides in lithium niobate are expected to keep playing a crucial role in the near future because of their advantages in high-power and loss-sensitive quantum optics applications. As such, lithium niobate photonics holds great promise for unlocking the EM spectrum and reshaping information technologies for our society in the future. Lithium niobate spectral coverage. The EM spectral range and processes for generating EM frequencies when using lithium niobate (LN) for frequency mixing. AO, acousto-optic; AOM, acousto-optic modulation; χ (2) , second-order nonlinearity; χ (3) , third-order nonlinearity; EO, electro-optic; EOM, electro-optic modulation; HHG, high-harmonic generation; IR, infrared; OFC, optical frequency comb; OPO, optical paramedic oscillator; OR, optical rectification; SCG, supercontinuum generation; SHG, second-harmonic generation; UV, ultraviolet.« less
2. Miniature light-driven nanophotonic electron acceleration and control

   https://doi.org/10.1364/AOP.461142  

   Shiloh, Roy ; Schönenberger, Norbert ; Adiv, Yuval ; Ruimy, Ron ; Karnieli, Aviv ; Hughes, Tyler ; Joel England, R. ; Leedle, Kenneth James ; Black, Dylan S. ; Zhao, Zhexin ; et al ( January 2022 , Advances in Optics and Photonics)

   Dielectric laser accelerators (DLAs) are fundamentally based on the interaction of photons with free electrons, where energy and momentum conservation are satisfied by mediation of a nanostructure. In this scheme, the photonic nanostructure induces near-fields which transfer energy from the photon to the electron, similar to the inverse-Smith–Purcell effect described in metallic gratings. This, in turn, may provide ground-breaking applications, as it is a technology promising to miniaturize particle accelerators down to the chip scale. This fundamental interaction can also be used to study and demonstrate quantum photon-electron phenomena. The spontaneous and stimulated Smith–Purcell effect and the photon-induced near-field electron-microscopy (PINEM) effect have evolved to be a fruitful ground for observing quantum effects. In particular, the energy spectrum of the free electron has been shown to have discrete energy peaks, spaced with the interacting photon energy. This energy spectrum is correlated to the photon statistics and number of photon exchanges that took place during the interaction. We give an overview of DLA and PINEM physics with a focus on electron phase-space manipulation.
3. Efficient pathway to NaCs ground state molecules

   https://doi.org/10.1088/1367-2630/acd411  

   Warner, Claire ; Bigagli, Niccolò ; Lam, Aden Z. ; Yuan, Weijun ; Zhang, Siwei ; Stevenson, Ian ; Will, Sebastian ( June 2023 , New Journal of Physics)

   We present a study of two-photon pathways for the transfer of NaCs molecules to their rovibrational ground state. Starting from NaCs Feshbach molecules, we perform bound-bound excited state spectroscopy in the wavelength range from 900 nm to 940 nm, covering more than 30 vibrational states of the$c^3{\mathrm{\Sigma }}^{+}$,$b^3\mathrm{\Pi }$, and$B^1\mathrm{\Pi }$electronic states. Analyzing the rotational substructure, we identify the highly mixed$c^3{\mathrm{\Sigma }}_1^{+}|v=22⟩\sim b^3{\mathrm{\Pi }}_1|v=54⟩$state as an efficient bridge for stimulated Raman adiabatic passage. We demonstrate transfer into the NaCs ground state with an efficiency of up to 88(4)%. Highly efficient transfer is critical for the realization of many-body quantum phases of strongly dipolar NaCs molecules and high fidelity detection of single molecules, for example, in spin physics experiments in optical lattices and quantum information experiments in optical tweezer arrays.
4. Time-resolved relaxation and fragmentation of polycyclic aromatic hydrocarbons investigated in the ultrafast XUV-IR regime

   https://doi.org/10.1038/s41467-021-26193-z  

   Lee, J. W. ; Tikhonov, D. S. ; Chopra, P. ; Maclot, S. ; Steber, A. L. ; Gruet, S. ; Allum, F. ; Boll, R. ; Cheng, X. ; Düsterer, S. ; et al ( December 2021 , Nature Communications)

   Abstract Polycyclic aromatic hydrocarbons (PAHs) play an important role in interstellar chemistry and are subject to high energy photons that can induce excitation, ionization, and fragmentation. Previous studies have demonstrated electronic relaxation of parent PAH monocations over 10–100 femtoseconds as a result of beyond-Born-Oppenheimer coupling between the electronic and nuclear dynamics. Here, we investigate three PAH molecules: fluorene, phenanthrene, and pyrene, using ultrafast XUV and IR laser pulses. Simultaneous measurements of the ion yields, ion momenta, and electron momenta as a function of laser pulse delay allow a detailed insight into the various molecular processes. We report relaxation times for the electronically excited PAH * , PAH +* and PAH 2+* states, and show the time-dependent conversion between fragmentation pathways. Additionally, using recoil-frame covariance analysis between ion images, we demonstrate that the dissociation of the PAH 2+ ions favors reaction pathways involving two-body breakup and/or loss of neutral fragments totaling an even number of carbon atoms.
5. The Reactivity of Ambident Nucleophiles: Marcus Theory or Hard and Soft Acids and Bases Principle?

   https://doi.org/10.1002/jcc.26052  

   Wang, Yi‐Gui ; Barnes, Ericka C. ; Kaya, Savaș ; Sharma, Vinit ( August 2019 , Journal of Computational Chemistry)

   The model reactions CH₃X + (NH—CH=O)M ➔ CH₃—NH—NH═O or NH═CH—O—CH₃ + MX (M = none, Li, Na, K, Ag, Cu; X = F, Cl, Br) are investigated to demonstrate the feasibility of Marcus theory and the hard and soft acids and bases (HSAB) principle in predicting the reactivity of ambident nucleophiles. The delocalization indices (DI) are defined in the framework of the quantum theory of atoms in molecules (QT‐AIM), and are used as the scale of softness in the HSAB principle. To react with the ambident nucleophile NH═CH—O⁻, the carbocation H₃C⁺from CH₃X (F, Cl, Br) is actually a borderline acid according to the DI values of the forming C…N and C…O bonds in the transition states (between 0.25 and 0.49), while the counter ions are divided into three groups according to the DI values of weak interactions involving M (M…X, M…N, and M…O): group I (M = none, and Me₄N) basically show zero DI values; group II species (M = Li, Na, and K) have noticeable DI values but the magnitudes are usually less than 0.15; and group III species (M = Ag and Cu(I)) have significant DI values (0.30–0.61). On a relative basis, H₃C⁺is a soft acid with respect to group I andmore »group II counter ions, and a hard acid with respect to group III counter ions. Therefore, N‐regioselectivity is found in the presence of group I and group II counter ions (M = Me₄N, Li, Na, K), while O‐regioselectivity is observed in the presence of the group III counter ions (M = Ag, and Cu(I)). The hardness of atoms, groups, and molecules is also calculated with new functions that depend on ionization potential (I) and electron affinity (A) and use the atomic charges obtained from localization indices (LI), so that the regioselectivity is explained by the atomic hardness of reactive nitrogen atoms in the transition states according to the maximum hardness principle (MHP). The exact Marcus equation is derived from the simple harmonic potential energy parabola, so that the concepts of activation free energy, intrinsic activation barrier, and reaction energy are completely connected. The required intrinsic activation barriers can be either estimated fromab initiocalculations on reactant, transition state, and product of the model reactions, or calculated from identity reactions. The counter ions stabilize the reactant through bridging N‐ and O‐site of reactant of identity reactions, so that the intrinsic barriers for the salts are higher than those for free ambident anions, which is explained by the increased reorganization parameter Δr. The proper application of Marcus theory should quantitatively consider all three terms of Marcus equation, and reliably represent the results with potential energy parabolas for reactants and all products. For the model reactions, both Marcus theory and HSAB principle/MHP principle predict the N‐regioselectivity when M = none, Me₄N, Li, Na, K, and the O‐regioselectivity when M = Ag and Cu(I). © 2019 Wiley Periodicals, Inc.

   « less