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Very regular high-frequency pulsation modes in young intermediate-mass stars 期刊论文
NATURE, 2020, 581 (7807) : 147-+
作者:  Zhao, Chuangqi;  Zhang, Pengchao;  Zhou, Jiajia;  Qi, Shuanhu;  Yamauchi, Yoshihiro;  Shi, Ruirui;  Fang, Ruochen;  Ishida, Yasuhiro;  Wang, Shutao;  Tomsia, Antoni P.;  Jiang, Lei;  Liu, Mingjie
收藏  |  浏览/下载:21/0  |  提交时间:2020/07/03

Asteroseismology probes the internal structures of stars by using their natural pulsation frequencies(1). It relies on identifying sequences of pulsation modes that can be compared with theoretical models, which has been done successfully for many classes of pulsators, including low-mass solar-type stars(2), red giants(3), high-mass stars(4) and white dwarfs(5). However, a large group of pulsating stars of intermediate mass-the so-called delta Scuti stars-have rich pulsation spectra for which systematic mode identification has not hitherto been possible(6,7). This arises because only a seemingly random subset of possible modes are excited and because rapid rotation tends to spoil regular patterns(8-10). Here we report the detection of remarkably regular sequences of high-frequency pulsation modes in 60 intermediate-mass main-sequence stars, which enables definitive mode identification. The space motions of some of these stars indicate that they are members of known associations of young stars, as confirmed by modelling of their pulsation spectra.


The pulsation spectra of intermediate-mass stars (so-called delta Scuti stars) have been challenging to analyse, but new observations of 60 such stars reveal remarkably regular sequences of high-frequency pulsation modes.


  
Spin squeezing of 10(11) atoms by prediction and retrodiction measurements 期刊论文
NATURE, 2020, 581 (7807) : 159-+
作者:  Lan, Jun;  Ge, Jiwan;  Yu, Jinfang;  Shan, Sisi;  Zhou, Huan;  Fan, Shilong;  Zhang, Qi;  Shi, Xuanling;  Wang, Qisheng;  Zhang, Linqi;  Wang, Xinquan
收藏  |  浏览/下载:33/0  |  提交时间:2020/07/03

The measurement sensitivity of quantum probes using N uncorrelated particles is restricted by the standard quantum limit(1), which is proportional to 1/root N. This limit, however, can be overcome by exploiting quantum entangled states, such as spin-squeezed states(2). Here we report the measurement-based generation of a quantum state that exceeds the standard quantum limit for probing the collective spin of 10(11) rubidium atoms contained in a macroscopic vapour cell. The state is prepared and verified by sequences of stroboscopic quantum non-demolition (QND) measurements. We then apply the theory of past quantum states(3,4) to obtain spin state information from the outcomes of both earlier and later QND measurements. Rather than establishing a physically squeezed state in the laboratory, the past quantum state represents the combined system information from these prediction and retrodiction measurements. This information is equivalent to a noise reduction of 5.6 decibels and a metrologically relevant squeezing of 4.5 decibels relative to the coherent spin state. The past quantum state yields tighter constraints on the spin component than those obtained by conventional QND measurements. Our measurement uses 1,000 times more atoms than previous squeezing experiments(5-10), with a corresponding angular variance of the squeezed collective spin of 4.6 x 10(-13) radians squared. Although this work is rooted in the foundational theory of quantum measurements, it may find practical use in quantum metrology and quantum parameter estimation, as we demonstrate by applying our protocol to quantum enhanced atomic magnetometry.


  
A general carbonyl alkylative amination for tertiary amine synthesis 期刊论文
NATURE, 2020
作者:  Ouyang, David;  He, Bryan;  Ghorbani, Amirata;  Yuan, Neal;  Ebinger, Joseph;  Langlotz, Curtis P.;  Heidenreich, Paul A.;  Harrington, Robert A.;  Liang, David H.;  Ashley, Euan A.;  Zou, James Y.
收藏  |  浏览/下载:26/0  |  提交时间:2020/07/03

The ubiquity of tertiary alkylamines in pharmaceutical and agrochemical agents, natural products and small-molecule biological probes(1,2) has stimulated efforts towards their streamlined synthesis(3-9). Arguably the most robust method for the synthesis of tertiary alkylamines is carbonyl reductive amination(3), which comprises two elementary steps: the condensation of a secondary alkylamine with an aliphatic aldehyde to form an all-alkyl-iminium ion, which is subsequently reduced by a hydride reagent. Direct strategies have been sought for a '  higher order'  variant of this reaction via the coupling of an alkyl fragment with an alkyl-iminium ion that is generated in situ(10-14). However, despite extensive efforts, the successful realization of a '  carbonyl alkylative amination'  has not yet been achieved. Here we present a practical and general synthesis of tertiary alkylamines through the addition of alkyl radicals to all-alkyl-iminium ions. The process is facilitated by visible light and a silane reducing agent, which trigger a distinct radical initiation step to establish a chain process. This operationally straightforward, metal-free and modular transformation forms tertiary amines, without structural constraint, via the coupling of aldehydes and secondary amines with alkyl halides. The structural and functional diversity of these readily available precursors provides a versatile and flexible strategy for the streamlined synthesis of complex tertiary amines.


The synthesis of tertiary amines is achieved through a carbonyl alkylative amination reaction facilitated by visible light, in which an aldehyde and an amine condense to form an iminium ion that subsequently reacts with alkyl radical.


  
Late-stage oxidative C(sp(3))-H methylation 期刊论文
NATURE, 2020, 580 (7805) : 621-+
作者:  Fessler, Evelyn;  Eckl, Eva-Maria;  Schmitt, Sabine;  Mancilla, Igor Alves;  Meyer-Bender, Matthias F.;  Hanf, Monika;  Philippou-Massier, Julia;  Krebs, Stefan;  Zischka, Hans;  Jae, Lucas T.
收藏  |  浏览/下载:71/0  |  提交时间:2020/07/03

Frequently referred to as the '  magic methyl effect'  , the installation of methyl groups-especially adjacent (alpha) to heteroatoms-has been shown to dramatically increase the potency of biologically active molecules(1-3). However, existing methylation methods show limited scope and have not been demonstrated in complex settings(1). Here we report a regioselective and chemoselective oxidative C(sp(3))-H methylation method that is compatible with late-stage functionalization of drug scaffolds and natural products. This combines a highly site-selective and chemoselective C-H hydroxylation with a mild, functional-group-tolerant methylation. Using a small-molecule manganese catalyst, Mn(CF3PDP), at low loading (at a substrate/catalyst ratio of 200) affords targeted C-H hydroxylation on heterocyclic cores, while preserving electron-neutral and electron-rich aryls. Fluorine- or Lewis-acid-assisted formation of reactive iminium or oxonium intermediates enables the use of a mildly nucleophilic organoaluminium methylating reagent that preserves other electrophilic functionalities on the substrate. We show this late-stage C(sp(3))-H methylation on 41 substrates housing 16 different medicinally important cores that include electron-rich aryls, heterocycles, carbonyls and amines. Eighteen pharmacologically relevant molecules with competing sites-including drugs (for example, tedizolid) and natural products-are methylated site-selectively at the most electron rich, least sterically hindered position. We demonstrate the syntheses of two magic methyl substrates-an inverse agonist for the nuclear receptor RORc and an antagonist of the sphingosine-1-phosphate receptor-1-via late-stage methylation from the drug or its advanced precursor. We also show a remote methylation of the B-ring carbocycle of an abiraterone analogue. The ability to methylate such complex molecules at late stages will reduce synthetic effort and thereby expedite broader exploration of the magic methyl effect in pursuit of new small-molecule therapeutics and chemical probes.


A manganese-catalysed oxidative C(sp(3))-H methylation method allows a methyl group to be selectively installed into medicinally important heterocycles, providing a way to improve pharmaceuticals and better understand the '  magic methyl effect'  .


  
Spontaneous gyrotropic electronic order in a transition-metal dichalcogenide 期刊论文
NATURE, 2020, 578 (7796) : 545-+
作者:  Kum, Hyun S.;  Lee, Hyungwoo;  Kim, Sungkyu;  Lindemann, Shane;  Kong, Wei;  Qiao, Kuan;  Chen, Peng;  Irwin, Julian;  Lee, June Hyuk;  Xie, Saien;  Subramanian, Shruti;  Shim, Jaewoo;  Bae, Sang-Hoon;  Choi, Chanyeol;  Ranno, Luigi;  Seo, Seungju;  Lee, Sangho;  Bauer, Jackson;  Li, Huashan;  Lee, Kyusang;  Robinson, Joshua A.;  Ross, Caroline A.;  Schlom, Darrell G.;  Rzchowski, Mark S.;  Eom, Chang-Beom;  Kim, Jeehwan
收藏  |  浏览/下载:24/0  |  提交时间:2020/07/03

Chirality is ubiquitous in nature, and populations of opposite chiralities are surprisingly asymmetric at fundamental levels(1,2). Examples range from parity violation in the subatomic weak force to homochirality in biomolecules. The ability to achieve chirality-selective synthesis (chiral induction) is of great importance in stereochemistry, molecular biology and pharmacology(2). In condensed matter physics, a crystalline electronic system is geometrically chiral when it lacks mirror planes, space-inversion centres or rotoinversion axes(1). Typically, geometrical chirality is predefined by the chiral lattice structure of a material, which is fixed on formation of the crystal. By contrast, in materials with gyrotropic order(3-6), electrons spontaneously organize themselves to exhibit macroscopic chirality in an originally achiral lattice. Although such order-which has been proposed as the quantum analogue of cholesteric liquid crystals-has attracted considerable interest(3-15), no clear observation or manipulation of gyrotropic order has been achieved so far. Here we report the realization of optical chiral induction and the observation of a gyrotropically ordered phase in the transition-metal dichalcogenide semimetal 1T-TiSe2. We show that shining mid-infrared circularly polarized light on 1T-TiSe2 while cooling it below the critical temperature leads to the preferential formation of one chiral domain. The chirality of this state is confirmed by the measurement of an out-of-plane circular photogalvanic current, the direction of which depends on the optical induction. Although the role of domain walls requires further investigation with local probes, the methodology demonstrated here can be applied to realize and control chiral electronic phases in other quantum materials(4,16).


Optical chiral induction and spontaneous gyrotropic electronic order are realized in the transition-metal chalcogenide 1T-TiSe2 by using illumination with mid-infrared circularly polarized light and simultaneous cooling below the critical temperature.


  
Ion Heating by Electromagnetic Ion Cyclotron Waves and Magnetosonic Waves in the Earth's Inner Magnetosphere 期刊论文
GEOPHYSICAL RESEARCH LETTERS, 2019, 46 (12) : 6258-6267
作者:  Ma, Q.;  Li, W.;  Yue, C.;  Thorne, R. M.;  Bortnik, J.;  Kletzing, C. A.;  Kurth, W. S.;  Hospodarsky, G. B.;  Reeves, G. D.;  Spence, H. E.
收藏  |  浏览/下载:26/0  |  提交时间:2019/11/26
ion heating  electromagnetic ion cyclotron waves  ring current  resonant interaction in plasmasphere  Van Allen Probes observation  quasilinear modeling  
EMIC Waves Converted From Equatorial Noise Due to M/Q=2 Ions in the Plasmasphere: Observations From Van Allen Probes and Arase 期刊论文
GEOPHYSICAL RESEARCH LETTERS, 2019, 46 (11) : 5662-5669
作者:  Miyoshi, Y.;  Matsuda, S.;  Kurita, S.;  Nomura, K.;  Keika, K.;  Shoji, M.;  Kitamura, N.;  Kasahara, Y.;  Matsuoka, A.;  Shinohara, I.;  Shiokawa, K.;  Machida, S.;  Santolik, O.;  Boardsen, S. A.;  Horne, R. B.;  Wygant, J. F.
收藏  |  浏览/下载:33/0  |  提交时间:2019/11/26
EMIC  magnetsonic waves  Arase  Van Allen Probes  plasmasphere  M  Q=2 ions  
Magnetospheric Signatures of STEVE: Implications for the Magnetospheric Energy Source and Interhemispheric Conjugacy 期刊论文
GEOPHYSICAL RESEARCH LETTERS, 2019, 46 (11) : 5637-5644
作者:  Nishimura, Y.;  Gallardo-Lacourt, B.;  Zou, Y.;  Mishin, E.;  Knudsen, D. J.;  Donovan, E. F.;  Angelopoulos, V.;  Raybell, R.
收藏  |  浏览/下载:18/0  |  提交时间:2019/11/26
STEVE  SAPS  interhemispheric conjugate phenomena  storm and ring current  THEMIS  Van Allen Probes (RBSP)  
Van Allen Probes Observations of Chorus Wave Vector Orientations: Implications for the Chorus-to-Hiss Mechanism 期刊论文
GEOPHYSICAL RESEARCH LETTERS, 2019, 46 (5) : 2337-2346
作者:  Hartley, D. P.;  Kletzing, C. A.;  Chen, L.;  Horne, R. B.;  Santolik, O.
收藏  |  浏览/下载:15/0  |  提交时间:2019/11/26
Van Allen Probes  EMFISIS  chorus waves  plasmaspheric hiss  plasmaspheric plumes  wave normal angle  
What Causes Radiation Belt Enhancements: A Survey of the Van Allen Probes Era 期刊论文
GEOPHYSICAL RESEARCH LETTERS, 2018, 45 (11) : 5253-5259
作者:  Boyd, A. J.;  Turner, D. L.;  Reeves, G. D.;  Spence, H. E.;  Baker, D. N.;  Blake, J. B.
收藏  |  浏览/下载:21/0  |  提交时间:2019/04/09
Radiation Belt  Phase Space Density  Local Acceleration  Van Allen Probes  THEMIS