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Evidence for sodium-rich alkaline water in the Tagish Lake parent body and implications for amino acid synthesis and racemization 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2020, 117 (21) : 11217-11219
作者:  White, Lee F.;  Tait, Kimberly T.;  Langelier, Brian;  Lymer, Elizabeth A.;  Cernok, Ana;  Kizovski, Tanya V.;  Ma, Chi;  Tschauner, Oliver;  Nicklin, Richard I.
收藏  |  浏览/下载:8/0  |  提交时间:2020/05/13
Tagish Lake  framboidal magnetite  atom probe tomography  amino acid  
Molecular tuning of CO2-to-ethylene conversion 期刊论文
NATURE, 2020, 577 (7791) : 509-+
作者:  Li, Fengwang;  39;Brien, Colin P.
收藏  |  浏览/下载:13/0  |  提交时间:2020/07/03

The electrocatalytic reduction of carbon dioxide, powered by renewable electricity, to produce valuable fuels and feedstocks provides a sustainable and carbon-neutral approach to the storage of energy produced by intermittent renewable sources(1). However, the highly selective generation of economically desirable products such as ethylene from the carbon dioxide reduction reaction (CO2RR) remains a challenge(2). Tuning the stabilities of intermediates to favour a desired reaction pathway can improve selectivity(3-5), and this has recently been explored for the reaction on copper by controlling morphology(6), grain boundaries(7), facets(8), oxidation state(9) and dopants(10). Unfortunately, the Faradaic efficiency for ethylene is still low in neutral media (60 per cent at a partial current density of 7 milliamperes per square centimetre in the best catalyst reported so far(9)), resulting in a low energy efficiency. Here we present a molecular tuning strategy-the functionalization of the surface of electrocatalysts with organic molecules-that stabilizes intermediates for more selective CO2RR to ethylene. Using electrochemical, operando/in situ spectroscopic and computational studies, we investigate the influence of a library of molecules, derived by electro-dimerization of arylpyridiniums(11), adsorbed on copper. We find that the adhered molecules improve the stabilization of an '  atop-bound'  CO intermediate (that is, an intermediate bound to a single copper atom), thereby favouring further reduction to ethylene. As a result of this strategy, we report the CO2RR to ethylene with a Faradaic efficiency of 72 per cent at a partial current density of 230 milliamperes per square centimetre in a liquid-electrolyte flow cell in a neutral medium. We report stable ethylene electrosynthesis for 190 hours in a system based on a membrane-electrode assembly that provides a full-cell energy efficiency of 20 per cent. We anticipate that this may be generalized to enable molecular strategies to complement heterogeneous catalysts by stabilizing intermediates through local molecular tuning.


Electrocatalytic reduction of CO2 over copper can be made highly selective by '  tuning'  the copper surface with adsorbed organic molecules to stabilize intermediates for carbon-based fuels such as ethylene


  
Observation of Bose-Einstein condensates in an Earth-orbiting research lab 期刊论文
NATURE, 2020, 582 (7811) : 103-+
作者:  Yamamoto, Keisuke;  Venida, Anthony;  Yano, Julian;  Biancur, Douglas E.;  Kakiuchi, Miwako;  Gupta, Suprit;  Sohn, Albert S. W.;  Mukhopadhyay, Subhadip;  Lin, Elaine Y.;  Parker, Seth J.;  Banh, Robert S.;  Paulo, Joao A.;  Wen, Kwun Wah;  Debnath, Jayanta;  Kim, Grace E.;  Mancias, Joseph D.;  Fearon, Douglas T.;  Perera, Rushika M.;  Kimmelman, Alec C.
收藏  |  浏览/下载:25/0  |  提交时间:2020/07/03

Quantum mechanics governs the microscopic world, where low mass and momentum reveal a natural wave-particle duality. Magnifying quantum behaviour to macroscopic scales is a major strength of the technique of cooling and trapping atomic gases, in which low momentum is engineered through extremely low temperatures. Advances in this field have achieved such precise control over atomic systems that gravity, often negligible when considering individual atoms, has emerged as a substantial obstacle. In particular, although weaker trapping fields would allow access to lower temperatures(1,2), gravity empties atom traps that are too weak. Additionally, inertial sensors based on cold atoms could reach better sensitivities if the free-fall time of the atoms after release from the trap could be made longer(3). Planetary orbit, specifically the condition of perpetual free-fall, offers to lift cold-atom studies beyond such terrestrial limitations. Here we report production of rubidium Bose-Einstein condensates (BECs) in an Earth-orbiting research laboratory, the Cold Atom Lab. We observe subnanokelvin BECs in weak trapping potentials with free-expansion times extending beyond one second, providing an initial demonstration of the advantages offered by a microgravity environment for cold-atom experiments and verifying the successful operation of this facility. With routine BEC production, continuing operations will support long-term investigations of trap topologies unique to microgravity(4,5), atom-laser sources(6), few-body physics(7,8)and pathfinding techniques for atom-wave interferometry(9-12).


  
Exploring dynamical phase transitions with cold atoms in an optical cavity 期刊论文
NATURE, 2020, 580 (7805) : 602-+
作者:  Halbach, Rebecca;  Miesen, Pascal;  Joosten, Joep;  Taskopru, Ezgi;  Rondeel, Inge;  Pennings, Bas;  Vogels, Chantal B. F.;  Merkling, Sarah H.;  Koenraadt, Constantianus J.;  Lambrechts, Louis;  van Rij, Ronald P.
收藏  |  浏览/下载:8/0  |  提交时间:2020/07/03

Interactions between light and an ensemble of strontium atoms in an optical cavity can serve as a testbed for studying dynamical phase transitions, which are currently not well understood.


Interactions between atoms and light in optical cavities provide a means of investigating collective (many-body) quantum physics in controlled environments. Such ensembles of atoms in cavities have been proposed for studying collective quantum spin models, where the atomic internal levels mimic a spin degree of freedom and interact through long-range interactions tunable by changing the cavity parameters(1-4). Non-classical steady-state phases arising from the interplay between atom-light interactions and dissipation of light from the cavity have previously been investigated(5-11). These systems also offer the opportunity to study dynamical phases of matter that are precluded from existence at equilibrium but can be stabilized by driving a system out of equilibrium(12-16), as demonstrated by recent experiments(17-22). These phases can also display universal behaviours akin to standard equilibrium phase transitions(8,23,24). Here, we use an ensemble of about a million strontium-88 atoms in an optical cavity to simulate a collective Lipkin-Meshkov-Glick model(25,26), an iconic model in quantum magnetism, and report the observation of distinct dynamical phases of matter in this system. Our system allows us to probe the dependence of dynamical phase transitions on system size, initial state and other parameters. These observations can be linked to similar dynamical phases in related systems, including the Josephson effect in superfluid helium(27), or coupled atomic(28) and solid-state polariton(29) condensates. The system itself offers potential for generation of metrologically useful entangled states in optical transitions, which could permit quantum enhancement in state-of-the-art atomic clocks(30,31).


  
Laser spectroscopy of pionic helium atoms 期刊论文
NATURE, 2020, 581 (7806) : 37-+
作者:  Shang, Jian;  Ye, Gang;  Shi, Ke;  Wan, Yushun;  Luo, Chuming;  Aihara, Hideki;  Geng, Qibin;  Auerbach, Ashley;  Li, Fang
收藏  |  浏览/下载:21/0  |  提交时间:2020/07/03

Charged pions(1) are the lightest and longest-lived mesons. Mesonic atoms are formed when an orbital electron in an atom is replaced by a negatively charged meson. Laser spectroscopy of these atoms should permit the mass and other properties of the meson to be determined with high precision and could place upper limits on exotic forces involving mesons (as has been done in other experiments on antiprotons(2-9)). Determining the mass of the pi(-) meson in particular could help to place direct experimental constraints on the mass of the muon antineutrino(10-13). However, laser excitations of mesonic atoms have not been previously achieved because of the small number of atoms that can be synthesized and their typically short (less than one picosecond) lifetimes against absorption of the mesons into the nuclei(1). Metastable pionic helium (pi He-4(+)) is a hypothetical(14-16) three-body atom composed of a helium-4 nucleus, an electron and a pi(-) occupying a Rydberg state of large principal (n approximate to 16) and orbital angular momentum (l approximate to n - 1) quantum numbers. The pi He-4(+) atom is predicted to have an anomalously long nanosecond-scale lifetime, which could allow laser spectroscopy to be carried out(17). Its atomic structure is unique owing to the absence of hyperfine interactions(18,19) between the spin-0 pi(-) and the He-4 nucleus. Here we synthesize pi He-4(+) in a superfluid-helium target and excite the transition (n, l) = (17, 16) -> (17, 15) of the pi(-)-occupied pi He-4(+) orbital at a near-infrared resonance frequency of 183,760 gigahertz. The laser initiates electromagnetic cascade processes that end with the nucleus absorbing the pi(-) and undergoing fission(20,21). The detection of emerging neutron, proton and deuteron fragments signals the laser-induced resonance in the atom, thereby confirming the presence of pi He-4(+). This work enables the use of the experimental techniques of quantum optics to study a meson.


Long-lived pionic helium atoms (composed of a helium-4 nucleus, an electron and a negatively charged pion) are synthesized in a superfluid-helium target, as confirmed by laser spectroscopy involving the pion-occupied orbitals.


  
Exotic helium atom lit up 期刊论文
NATURE, 2020, 581 (7806) : 32-33
作者:  Rabkin, Eugen
收藏  |  浏览/下载:4/0  |  提交时间:2020/07/03

Laser excitation of pionic helium.


An elusive type of atom known as pionic helium has been directly excited by laser light for the first time. The work establishes a promising experimental platform for probing fundamental physics.


  
Submicrosecond entangling gate between trapped ions via Rydberg interaction 期刊论文
NATURE, 2020, 580 (7803) : 345-+
作者:  Chatterjee, Sourav;  Guidi, Mara;  Seeberger, Peter H.;  Gilmore, Kerry
收藏  |  浏览/下载:17/0  |  提交时间:2020/07/03

Generating quantum entanglement in large systems on timescales much shorter than the coherence time is key to powerful quantum simulation and computation. Trapped ions are among the most accurately controlled and best isolated quantum systems(1) with low-error entanglement gates operated within tens of microseconds using the vibrational motion of few-ion crystals(2,3). To exceed the level of complexity tractable by classical computers the main challenge is to realize fast entanglement operations in crystals made up of many ions (large ion crystals)(4). The strong dipole-dipole interactions in polar molecule(5) and Rydberg atom(6,7) systems allow much faster entangling gates, yet stable state-independent confinement comparable with trapped ions needs to be demonstrated in these systems(8). Here we combine the benefits of these approaches: we report a two-ion entangling gate with 700-nanosecond gate time that uses the strong dipolar interaction between trapped Rydberg ions, which we use to produce a Bell state with 78 per cent fidelity. The sources of gate error are identified and a total error of less than 0.2 per cent is predicted for experimentally achievable parameters. Furthermore, we predict that residual coupling to motional modes contributes an approximate gate error of 10(-4) in a large ion crystal of 100 ions. This provides a way to speed up and scale up trapped-ion quantum computers and simulators substantially.


  
Collisional cooling of ultracold molecules 期刊论文
NATURE, 2020, 580 (7802) : 197-+
作者:  Wang, Qinyang;  Wang, Yupeng;  Ding, Jingjin;  Wang, Chunhong;  Zhou, Xuehan;  Gao, Wenqing;  Huang, Huanwei;  Shao, Feng;  Liu, Zhibo
收藏  |  浏览/下载:13/0  |  提交时间:2020/07/03

Since the original work on Bose-Einstein condensation(1,2), the use of quantum degenerate gases of atoms has enabled the quantum emulation of important systems in condensed matter and nuclear physics, as well as the study of many-body states that have no analogue in other fields of physics(3). Ultracold molecules in the micro- and nanokelvin regimes are expected to bring powerful capabilities to quantum emulation(4) and quantum computing(5), owing to their rich internal degrees of freedom compared to atoms, and to facilitate precision measurement and the study of quantum chemistry(6). Quantum gases of ultracold atoms can be created using collision-based cooling schemes such as evaporative cooling, but thermalization and collisional cooling have not yet been realized for ultracold molecules. Other techniques, such as the use of supersonic jets and cryogenic buffer gases, have reached temperatures limited to above 10 millikelvin(7,8). Here we show cooling of NaLi molecules to micro- and nanokelvin temperatures through collisions with ultracold Na atoms, with both molecules and atoms prepared in their stretched hyperfine spin states. We find a lower bound on the ratio of elastic to inelastic molecule-atom collisions that is greater than 50-large enough to support sustained collisional cooling. By employing two stages of evaporation, we increase the phase-space density of the molecules by a factor of 20, achieving temperatures as low as 220 nanokelvin. The favourable collisional properties of the Na-NaLi system could enable the creation of deeply quantum degenerate dipolar molecules and raises the possibility of using stretched spin states in the cooling of other molecules.


NaLi molecules are cooled to micro- and nanokelvin temperatures through collisions with ultracold Na atoms by using molecules and atoms in stretched hyperfine spin states and applying two evaporation stages.


  
Copper-mediated synthesis of drug-like bicyclopentanes 期刊论文
NATURE, 2020, 580 (7802) : 220-+
作者:  Canavelli, Pierre;  Islam, Saidul;  Powner, Matthew W.
收藏  |  浏览/下载:8/0  |  提交时间:2020/07/03

Multicomponent reactions are relied on in both academic and industrial synthetic organic chemistry owing to their step- and atom-economy advantages over traditional synthetic sequences(1). Recently, bicyclo[1.1.1]pentane (BCP) motifs have become valuable as pharmaceutical bioisosteres of benzene rings, and in particular 1,3-disubstituted BCP moieties have become widely adopted in medicinal chemistry as para-phenyl ring replacements(2). These structures are often generated from [1.1.1]propellane via opening of the internal C-C bond through the addition of either radicals or metal-based nucleophiles(3-13). The resulting propellane-addition adducts are then transformed to the requisite polysubstituted BCP compounds via a range of synthetic sequences that traditionally involve multiple chemical steps. Although this approach has been effective so far, a multicomponent reaction that enables single-step access to complex and diverse polysubstituted drug-like BCP products would be more time efficient compared to current stepwise approaches. Here we report a one-step three-component radical coupling of [1.1.1]propellane to afford diverse functionalized bicyclopentanes using various radical precursors and heteroatom nucleophiles via a metallaphotoredox catalysis protocol. This copper-mediated reaction operates on short timescales (five minutes to one hour) across multiple (more than ten) nucleophile classes and can accommodate a diverse array of radical precursors, including those that generate alkyl, alpha-acyl, trifluoromethyl and sulfonyl radicals. This method has been used to rapidly prepare BCP analogues of known pharmaceuticals, one of which is substantially more metabolically stable than its commercial progenitor.


A one-step, three-component radical coupling of [1.1.1]propellane by a photoredox reaction mediated by a copper catalyst produces drug-like bicyclopentanes.


  
Limits on gas impermeability of graphene 期刊论文
NATURE, 2020, 579 (7798) : 229-+
作者:  Pagano, Justin K.;  Xie, Jing;  Erickson, Karla A.;  Cope, Stephen K.;  Scott, Brian L.;  Wu, Ruilian;  Waterman, Rory;  Morris, David E.;  Yang, Ping;  Gagliardi, Laura;  Kiplinger, Jaqueline L.
收藏  |  浏览/下载:28/0  |  提交时间:2020/07/03

Despite being only one-atom thick, defect-free graphene is considered to be completely impermeable to all gases and liquids(1-10). This conclusion is based on theory(3-8) and supported by experiments(1,9,10) that could not detect gas permeation through micrometre-size membranes within a detection limit of 10(5) to 10(6) atoms per second. Here, using small monocrystalline containers tightly sealed with graphene, we show that defect-free graphene is impermeable with an accuracy of eight to nine orders of magnitude higher than in the previous experiments. We are capable of discerning (but did not observe) permeation of just a few helium atoms per hour, and this detection limit is also valid for all other gases tested (neon, nitrogen, oxygen, argon, krypton and xenon), except for hydrogen. Hydrogen shows noticeable permeation, even though its molecule is larger than helium and should experience a higher energy barrier. This puzzling observation is attributed to a two-stage process that involves dissociation of molecular hydrogen at catalytically active graphene ripples, followed by adsorbed atoms flipping to the other side of the graphene sheet with a relatively low activation energy of about 1.0 electronvolt, a value close to that previously reported for proton transport(11,12). Our work provides a key reference for the impermeability of two-dimensional materials and is important from a fundamental perspective and for their potential applications.