ConspectusThe invention of the laser marked a milestone in modern science and technology. Inorganic second-order nonlinear optical (NLO) crystals, with their unique frequency conversion capabilities, play a critical role in extending laser wavelength ranges. These materials are indispensable in laser science, information transmission, and other fields such as the industrial Internet. As Moore's Law drives the demand for shorter wavelengths and higher-precision laser sources, the development of high-performance short-wave ultraviolet (UV) (<300 nm) NLO materials for UV solid-state lasers has become increasingly important. While researchers have synthesized a variety of NLO crystals, their discovery has largely relied on trial-and-error approaches, which are not only time-consuming but also serendipitous rather than based on rational design principles. Moreover, the complexity of designing these materials is compounded by the need to meet several strict functional criteria, including a short UV cutoff edge, a strong second-harmonic generation (SHG) effect, and moderate birefringence, all of which hinder efficient synthesis. The rational design and controlled synthesis of high-performance short-wave UV NLO crystals, therefore, remains a significant scientific challenge.In this Account, we propose a three-step strategy to address this challenge: (1) Rational screening of highly polar functional groups, particularly new NLO-active groups with novel bonding characteristics (π-localized distorted [O] anions, highly polarizable cations such as Zn, Cd, and Hg, and cations containing stereochemically active lone pairs (SCALP) including Ge, Sn, Sb, and Pb) that exhibit significantly enhanced polarization anisotropy and hyperpolarizability, to replace traditional anionic groups (planar π-conjugated groups such as [BO], [CO], and [NO], and non-π-conjugated tetrahedral anions, such as [SO] and [PO]). (2) Precise regulation of crystal structures to sequentially construct functional groups using two methods: (a) a template-oriented synthesis strategy, which is a method that guides the formation of desired materials through crystal engineering, based on ideal structural models, and (b) a multifunctional primitive module assembly strategy, by identifying and designing multifunctional modules with specific structural configurations to achieve ordered arrangement, which facilitates the creation of high-performance materials. (3) Controlled synthesis of target compounds through synthesis method innovation. These strategies have successfully guided the discovery of several high-performance short-wave UV NLO crystals, including GeHPO, ASbXSO (A = K, Rb, Cs, NH; X = F, Cl), ASb(PO)F (A = K, Rb), HgOSO, AVO(O)CO (A = Rb, Cs), YO(OH)(CO)Cl, and ANO(OH) (A = Ba, Sr), among others. Finally, we summarize these strategies and offer perspectives on the future development of high-performance short-wave UV NLO materials, providing insights into their potential to advance this critical field.
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http://dx.doi.org/10.1021/acs.accounts.4c00704 | DOI Listing |
J Phys Chem Lett
December 2024
Institute of Optoelectronic Technology, Fuzhou University, Fuzhou 350116, China.
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December 2024
Oxford University, Department of Chemistry, UNITED KINGDOM OF GREAT BRITAIN AND NORTHERN IRELAND.
With a view towards the development of molecular spintronics, non-linear optics, and qubits, a great amount of research effort aims to establish the factors which govern the spin classification of diradicals. Electron spin resonance (ESR) is an indispensable tool for such research. However, in some cases, the mere presence of an ESR spectrum is insufficient to ascertain that the presumed diradical is indeed a triplet state.
View Article and Find Full Text PDFPhys Rev Lett
December 2024
University of Vienna, Faculty of Physics, Vienna Center for Quantum Science and Technology, Boltzmanngasse 5, 1090 Vienna, Austria.
From a quantum information perspective, verifying quantum coherence in a quantum experiment typically requires adjusting measurement settings or changing inputs. A paradigmatic example is that of a double-slit experiment, where observing the interference pattern on the screen in a series of experimental settings where one, the other, and both slits are open unambiguously proves quantum coherence. Here we show that this is not necessary by verifying quantum coherence in a network scenario without the need for inputs.
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December 2024
Key Laboratory of Materials Physics, Institute of Solid State Physics, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei 230031, China.
Nonlinear optics plays important roles in the research of fundamental physics and the applications of high-performance optoelectronic devices. The bulk nonlinear optical responses arise from the uniform light absorption in noncentrosymmetric crystals, and hence are usually considered to be the collective phenomena of all atoms. Here we show, in contrast to this common expectation, the nonlinear optical responses in antiferromagnets can be selectively accumulated near the surfaces, representing a skin effect.
View Article and Find Full Text PDFPhys Rev Lett
December 2024
Université Paris Cité, CNRS, Laboratoire Matériaux et Phénomènes Quantiques, 75013 Paris, France.
Harnessing high-dimensional entangled states of light presents a frontier for advancing quantum information technologies, from fundamental tests of quantum mechanics to enhanced computation and communication protocols. In this context, the spatial degree of freedom stands out as particularly suited for on-chip integration. But while traditional demonstrations produce and manipulate path-entangled states sequentially with discrete optical elements, continuously coupled nonlinear waveguide systems offer a promising alternative where photons can be generated and interfere along the entire propagation length, unveiling novel capabilities within a reduced footprint.
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