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1.
Nature ; 628(8008): 515-521, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38509374

RESUMO

The convergence of topology and correlations represents a highly coveted realm in the pursuit of new quantum states of matter1. Introducing electron correlations to a quantum spin Hall (QSH) insulator can lead to the emergence of a fractional topological insulator and other exotic time-reversal-symmetric topological order2-8, not possible in quantum Hall and Chern insulator systems. Here we report a new dual QSH insulator within the intrinsic monolayer crystal of TaIrTe4, arising from the interplay of its single-particle topology and density-tuned electron correlations. At charge neutrality, monolayer TaIrTe4 demonstrates the QSH insulator, manifesting enhanced nonlocal transport and quantized helical edge conductance. After introducing electrons from charge neutrality, TaIrTe4 shows metallic behaviour in only a small range of charge densities but quickly goes into a new insulating state, entirely unexpected on the basis of the single-particle band structure of TaIrTe4. This insulating state could arise from a strong electronic instability near the van Hove singularities, probably leading to a charge density wave (CDW). Remarkably, within this correlated insulating gap, we observe a resurgence of the QSH state. The observation of helical edge conduction in a CDW gap could bridge spin physics and charge orders. The discovery of a dual QSH insulator introduces a new method for creating topological flat minibands through CDW superlattices, which offer a promising platform for exploring time-reversal-symmetric fractional phases and electromagnetism2-4,9,10.

2.
Nature ; 595(7868): 521-525, 2021 07.
Artigo em Inglês | MEDLINE | ID: mdl-34290425

RESUMO

Whereas ferromagnets have been known and used for millennia, antiferromagnets were only discovered in the 1930s1. At large scale, because of the absence of global magnetization, antiferromagnets may seem to behave like any non-magnetic material. At the microscopic level, however, the opposite alignment of spins forms a rich internal structure. In topological antiferromagnets, this internal structure leads to the possibility that the property known as the Berry phase can acquire distinct spatial textures2,3. Here we study this possibility in an antiferromagnetic axion insulator-even-layered, two-dimensional MnBi2Te4-in which spatial degrees of freedom correspond to different layers. We observe a type of Hall effect-the layer Hall effect-in which electrons from the top and bottom layers spontaneously deflect in opposite directions. Specifically, under zero electric field, even-layered MnBi2Te4 shows no anomalous Hall effect. However, applying an electric field leads to the emergence of a large, layer-polarized anomalous Hall effect of about 0.5e2/h (where e is the electron charge and h is Planck's constant). This layer Hall effect uncovers an unusual layer-locked Berry curvature, which serves to characterize the axion insulator state. Moreover, we find that the layer-locked Berry curvature can be manipulated by the axion field formed from the dot product of the electric and magnetic field vectors. Our results offer new pathways to detect and manipulate the internal spatial structure of fully compensated topological antiferromagnets4-9. The layer-locked Berry curvature represents a first step towards spatial engineering of the Berry phase through effects such as layer-specific moiré potential.

3.
Phys Rev Lett ; 128(15): 153001, 2022 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-35499899

RESUMO

Electronic interactions play a fundamental role in atoms, molecular structure and reactivity. We introduce a general concept to control the effective electronic exchange interaction with intense laser fields via coupling to excited states. As an experimental proof of principle, we study the SF_{6} molecule using a combination of soft x-ray and infrared (IR) laser pulses. Increasing the IR intensity increases the effective exchange energy of the core hole with the excited electron by 50%, as observed by a characteristic spin-orbit branching ratio change. This work demonstrates altering electronic interactions by targeting many-particle quantum properties.

4.
Phys Rev Lett ; 129(18): 183204, 2022 Oct 28.
Artigo em Inglês | MEDLINE | ID: mdl-36374686

RESUMO

We report the measurement of the photoelectron angular distribution of two-photon single-ionization near the 2p^{2} ^{1}D^{e} double-excitation resonance in helium, benchmarking the fundamental nonlinear interaction of two photons with two correlated electrons. This observation is enabled by the unique combination of intense extreme ultraviolet pulses, delivered at the high-repetition-rate free-electron laser in Hamburg (FLASH), ionizing a jet of cryogenically cooled helium atoms in a reaction microscope. The spectral structure of the intense self-amplified spontaneous emission free-electron laser pulses has been resolved on a single-shot level to allow for post selection of pulses, leading to an enhanced spectral resolution, and introducing a new experimental method. The measured angular distribution is directly compared to state-of-the-art theory based on multichannel quantum defect theory and the streamlined R-matrix method. These results and experimental methodology open a promising route for exploring fundamental interactions of few photons with few electrons in general.

5.
Faraday Discuss ; 228(0): 519-536, 2021 May 27.
Artigo em Inglês | MEDLINE | ID: mdl-33575691

RESUMO

The emergence of ultra-intense extreme-ultraviolet (XUV) and X-ray free-electron lasers (FELs) has opened the door for the experimental realization of non-linear XUV and X-ray spectroscopy techniques. Here we demonstrate an experimental setup for an all-XUV transient absorption spectroscopy method for gas-phase targets at the FEL. The setup combines a high spectral resolving power of E/ΔE ≈ 1500 with sub-femtosecond interferometric resolution, and covers a broad XUV photon-energy range between approximately 20 and 110 eV. We demonstrate the feasibility of this setup firstly on a neon target. Here, we intensity- and time-resolve key aspects of non-linear XUV-FEL light-matter interactions, namely the non-resonant ionization dynamics and resonant coupling dynamics of bound states, including XUV-induced Stark shifts of energy levels. Secondly, we show that this setup is capable of tracking the XUV-initiated dissociation dynamics of small molecular targets (oxygen and diiodomethane) with site-specific resolution, by measuring the XUV transient absorption spectrum. In general, benefitting from a single-shot detection capability, we show that the setup and method provides single-shot phase-locked XUV pulse pairs. This lays the foundation to perform, in the future, experiments as a function of the XUV interferometric time delay and the relative phase, which enables advanced coherent non-linear spectroscopy schemes in the XUV and X-ray spectral range.

6.
J Phys Chem A ; 125(47): 10138-10143, 2021 Dec 02.
Artigo em Inglês | MEDLINE | ID: mdl-34788037

RESUMO

We performed a time-resolved spectroscopy experiment on the dissociation of oxygen molecules after the interaction with intense extreme-ultraviolet (XUV) light from the free-electron laser in Hamburg at Deutsches Elektronen-Synchrotron. Using an XUV-pump/XUV-probe transient-absorption geometry with a split-and-delay unit, we observe the onset of electronic transitions in the O2+ cation near 50 eV photon energy, marking the end of the progression from a molecule to two isolated atoms. We observe two different time scales of 290 ± 53 and 180 ± 76 fs for the emergence of different ionic transitions, indicating different dissociation pathways taken by the departing oxygen atoms. With regard to the emerging opportunities of tuning the central frequencies of pump and probe pulses and of increasing the probe-pulse bandwidth, future pump-probe transient-absorption experiments are expected to provide a detailed view of the coupled nuclear and electronic dynamics during molecular dissociation.

7.
Nature ; 516(7531): 374-8, 2014 Dec 18.
Artigo em Inglês | MEDLINE | ID: mdl-25519135

RESUMO

The concerted motion of two or more bound electrons governs atomic and molecular non-equilibrium processes including chemical reactions, and hence there is much interest in developing a detailed understanding of such electron dynamics in the quantum regime. However, there is no exact solution for the quantum three-body problem, and as a result even the minimal system of two active electrons and a nucleus is analytically intractable. This makes experimental measurements of the dynamics of two bound and correlated electrons, as found in the helium atom, an attractive prospect. However, although the motion of single active electrons and holes has been observed with attosecond time resolution, comparable experiments on two-electron motion have so far remained out of reach. Here we show that a correlated two-electron wave packet can be reconstructed from a 1.2-femtosecond quantum beat among low-lying doubly excited states in helium. The beat appears in attosecond transient-absorption spectra measured with unprecedentedly high spectral resolution and in the presence of an intensity-tunable visible laser field. We tune the coupling between the two low-lying quantum states by adjusting the visible laser intensity, and use the Fano resonance as a phase-sensitive quantum interferometer to achieve coherent control of the two correlated electrons. Given the excellent agreement with large-scale quantum-mechanical calculations for the helium atom, we anticipate that multidimensional spectroscopy experiments of the type we report here will provide benchmark data for testing fundamental few-body quantum dynamics theory in more complex systems. They might also provide a route to the site-specific measurement and control of metastable electronic transition states that are at the heart of fundamental chemical reactions.

8.
Phys Rev Lett ; 123(16): 163201, 2019 Oct 18.
Artigo em Inglês | MEDLINE | ID: mdl-31702368

RESUMO

We report on the experimental observation of a strong-field dressing of an autoionizing two-electron state in helium with intense extreme-ultraviolet laser pulses from a free-electron laser. The asymmetric Fano line shape of this transition is spectrally resolved, and we observe modifications of the resonance asymmetry structure for increasing free-electron-laser pulse energy on the order of few tens of Microjoules. A quantum-mechanical calculation of the time-dependent dipole response of this autoionizing state, driven by classical extreme-ultraviolet (XUV) electric fields, evidences strong-field-induced energy and phase shifts of the doubly excited state, which are extracted from the Fano line-shape asymmetry. The experimental results obtained at the Free-Electron Laser in Hamburg (FLASH) thus correspond to transient energy shifts on the order of a few meV, induced by strong XUV fields. These results open up a new way of performing nonperturbative XUV nonlinear optics for the light-matter interaction of resonant electronic transitions in atoms at short wavelengths.

9.
Phys Rev Lett ; 123(10): 103001, 2019 Sep 06.
Artigo em Inglês | MEDLINE | ID: mdl-31573300

RESUMO

We demonstrate time-resolved nonlinear extreme-ultraviolet absorption spectroscopy on multiply charged ions, here applied to the doubly charged neon ion, driven by a phase-locked sequence of two intense free-electron laser pulses. Absorption signatures of resonance lines due to 2p-3d bound-bound transitions between the spin-orbit multiplets ^{3}P_{0,1,2} and ^{3}D_{1,2,3} of the transiently produced doubly charged Ne^{2+} ion are revealed, with time-dependent spectral changes over a time-delay range of (2.4±0.3) fs. Furthermore, we observe 10-meV-scale spectral shifts of these resonances owing to the ac Stark effect. We use a time-dependent quantum model to explain the observations by an enhanced coupling of the ionic quantum states with the partially coherent free-electron laser radiation when the phase-locked pump and probe pulses precisely overlap in time.

11.
Opt Lett ; 41(4): 709-12, 2016 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-26872169

RESUMO

Noncollinear four-wave-mixing (FWM) techniques at near-infrared (NIR), visible, and ultraviolet frequencies have been widely used to map vibrational and electronic couplings, typically in complex molecules. However, correlations between spatially localized inner-valence transitions among different sites of a molecule in the extreme ultraviolet (XUV) spectral range have not been observed yet. As an experimental step toward this goal, we perform time-resolved FWM spectroscopy with femtosecond NIR and attosecond XUV pulses. The first two pulses (XUV-NIR) coincide in time and act as coherent excitation fields, while the third pulse (NIR) acts as a probe. As a first application, we show how coupling dynamics between odd- and even-parity, inner-valence excited states of neon can be revealed using a two-dimensional spectral representation. Experimentally obtained results are found to be in good agreement with ab initio time-dependent R-matrix calculations providing the full description of multielectron interactions, as well as few-level model simulations. Future applications of this method also include site-specific probing of electronic processes in molecules.

12.
Opt Lett ; 40(15): 3464-7, 2015 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-26258333

RESUMO

Attosecond transient absorption spectroscopy has thus far been lacking the capability to simultaneously characterize the intense laser pulses at work within a time-resolved quantum-dynamics experiment. However, precise knowledge of these pulses is key to extracting quantitative information in strong-field highly nonlinear light-matter interactions. Here, we introduce and experimentally demonstrate an ultrafast metrology tool based on the time-delay-dependent phase shift imprinted on a strong-field-driven resonance. Since we analyze the signature of the laser pulse interacting with the absorbing spectroscopy target, the laser pulse duration and intensity are determined in situ. As we also show, this approach allows for the quantification of time-dependent bound-state dynamics in one and the same experiment. In the future, such experimental data will facilitate more precise tests of strong-field dynamics theories.

13.
Phys Rev Lett ; 112(10): 103001, 2014 Mar 14.
Artigo em Inglês | MEDLINE | ID: mdl-24679285

RESUMO

Fano line shapes observed in absorption spectra encode information on the amplitude and phase of the optical dipole response. A change in the Fano line shape, e.g., by interaction with short-pulsed laser fields, allows us to extract dynamical modifications of the amplitude and phase of the coupled excited quantum states. We introduce and apply this physical mechanism to near-resonantly coupled doubly excited states in helium. This general approach provides a physical understanding of the laser-induced spectral shift of absorption-line maxima on a sub-laser-cycle time scale as they are ubiquitously observed in attosecond transient-absorption measurements.

14.
Sci Adv ; 9(47): eadk1482, 2023 Nov 24.
Artigo em Inglês | MEDLINE | ID: mdl-37992169

RESUMO

The electronic and nuclear dynamics inside molecules are essential for chemical reactions, where different pathways typically unfold on ultrafast timescales. Extreme ultraviolet (XUV) light pulses generated by free-electron lasers (FELs) allow atomic-site and electronic-state selectivity, triggering specific molecular dynamics while providing femtosecond resolution. Yet, time-resolved experiments are either blind to neutral fragments or limited by the spectral bandwidth of FEL pulses. Here, we combine a broadband XUV probe pulse from high-order harmonic generation with an FEL pump pulse to observe dissociation pathways leading to fragments in different quantum states. We temporally resolve the dissociation of a specific O2+ state into two competing channels by measuring the resonances of ionic and neutral fragments. This scheme can be applied to investigate convoluted dynamics in larger molecules relevant to diverse science fields.

15.
J Prim Health Care ; 13(2): 165-170, 2021 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-34620298

RESUMO

INTRODUCTION Peripheral arterial disease is an increasingly prevalent chronic illness globally. The Ankle Brachial Pressure Index (ABPI) is a well-established, simple, relatively quick and non-invasive assessment useful in diagnosing and quantifying peripheral arterial disease. ABPIs may be currently underutilised in general practice. AIM To explore perspectives of health professionals on the role of the ABPI. METHODS One-to-one interviews were conducted with health professionals using snowball sampling. Questions centred around interviewees' education on, experience with and view on the usefulness of the ABPI in general practice. Interviews were recorded and used for thematic analysis. RESULTS Participants consisted of 13 health-care professionals: nine general practitioners, two vascular surgeons and two allied health professionals. Most general practitioners interviewed identified benefits of ABPIs use in primary care, including aiding peripheral arterial disease diagnostics, management, referral and triage. No general practitioners stated they had ever had formal training in undertaking ABPIs. Two of the nine general practitioners stated regular ABPI use in their practice. Participants who did not use ABPIs identified practical barriers to its use in general practice, including cost of equipment, length of time needed and perceived low patient need to justify cost. All interviewees agreed that there was a role for ABPI use in the community if barriers were overcome. DISCUSSION There was consensus among general practitioners that ABPI use is beneficial. Many general practitioners named similar practical barriers to more common use of ABPIs in general practice. They saw a role for ABPIs in primary care, although it may be more practical as a tool for specialised individual clinicians to use for communities, given practical barriers of cost, time and perceived low patient need. Formal training could be considered, as none of the interviewed general practitioners had ever had any.


Assuntos
Tornozelo , Medicina Geral , Hospitais , Humanos , Percepção , Atenção Primária à Saúde
16.
Nat Commun ; 12(1): 643, 2021 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-33510142

RESUMO

High-intensity ultrashort pulses at extreme ultraviolet (XUV) and x-ray photon energies, delivered by state-of-the-art free-electron lasers (FELs), are revolutionizing the field of ultrafast spectroscopy. For crossing the next frontiers of research, precise, reliable and practical photonic tools for the spectro-temporal characterization of the pulses are becoming steadily more important. Here, we experimentally demonstrate a technique for the direct measurement of the frequency chirp of extreme-ultraviolet free-electron laser pulses based on fundamental nonlinear optics. It is implemented in XUV-only pump-probe transient-absorption geometry and provides in-situ information on the time-energy structure of FEL pulses. Using a rate-equation model for the time-dependent absorbance changes of an ionized neon target, we show how the frequency chirp can be directly extracted and quantified from measured data. Since the method does not rely on an additional external field, we expect a widespread implementation at FELs benefiting multiple science fields by in-situ on-target measurement and optimization of FEL-pulse properties.

17.
Rev Sci Instrum ; 90(5): 053108, 2019 May.
Artigo em Inglês | MEDLINE | ID: mdl-31153289

RESUMO

Measuring bound-state quantum dynamics, excited and driven by strong fields, is achievable by time-resolved absorption spectroscopy. Here, a vacuum beamline for spectroscopy in the attosecond temporal and extreme ultraviolet (XUV) spectral range is presented, which is a tool for observing and controlling nonequilibrium electron dynamics. In particular, we introduce a technique to record an XUV absorption signal and the corresponding reference simultaneously, which greatly improves the signal quality. The apparatus is based on a common beam path design for XUV and near-infrared (NIR) laser light in a vacuum. This ensures minimal spatiotemporal fluctuations between the strong NIR laser and the XUV excitation and reference beams, while the grazing incidence optics enable broadband spectral coverage. The apparatus combines high spectral and temporal resolution together with an increase in sensitivity to weak absorption signatures by an order of magnitude. This opens up new possibilities for studying strong-field-driven electron dynamics in bound systems on their natural attosecond time scale.

18.
Int J Oral Maxillofac Implants ; 18(6): 865-72, 2003.
Artigo em Inglês | MEDLINE | ID: mdl-14696662

RESUMO

PURPOSE: The purpose of this study was to compare internal Morse taper connections in 2 separate modes: repeated torque/reverse-torque values and compressive bending at a 30-degree off-axis angle. MATERIALS AND METHODS: Three sample groups (n = 12 in each group)--a solid-screw implant paired with a 5.5-mm solid abutment (SSI), a synOcta implant with a 5.5-mm solid abutment (SOI), and a synOcta implant with a synOcta 5.5-mm solid abutment (SOSA)--were torqued to 35 Ncm, and the reverse torque to remove the abutment was recorded. This was repeated for 3 trials. Additionally, the sample groups were loaded 30 degrees off-axis, and the ultimate compressive values were recorded. RESULTS: There was a significant difference in the initial reverse-torque values. The SOSA setup showed significantly lower torque than the SOI and SSI setups (P < .05). In addition, the compressive bending test showed that the SOSA setup was significantly different (P < .05) from the SSI and SOI setups. Radiographic survey of the test groups following compressive bending revealed no implant fractures, but bending of the implant-abutment complex occurred. DISCUSSION: The alteration within the Morse taper did not reduce the strength of the implant-abutment connection, ie, the reduction in surface area did not significantly reduce the torque properties or tensile properties. The new 2-piece synOcta 5.5-mm solid abutment was shown to have a stronger implant-abutment connection when torqued down a second time. CONCLUSIONS: In this in vitro study, alteration of the Morse taper with an internal octagon indexing did not significantly reduce the strength of the implant connection. Sufficient strength was exhibited, which would indicate this implant-abutment design for anterior as well as posterior edentulous sites.


Assuntos
Dente Suporte , Implantes Dentários , Planejamento de Prótese Dentária , Análise de Variância , Humanos , Teste de Materiais , Microscopia Eletrônica de Varredura , Maleabilidade , Estresse Mecânico , Propriedades de Superfície , Torque , Suporte de Carga
20.
Hum Mol Genet ; 11(23): 2929-40, 2002 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-12393804

RESUMO

Coffin-Lowry syndrome (CLS) is characterized by cognitive impairment, characteristic facial and digital findings and skeletal anomalies. The gene implicated in CLS encodes RSK2, a serine/threonine kinase acting in the Ras/MAPK signalling pathway. In humans, RSK2 belongs to a family of four highly homologous proteins (RSK1-RSK4), encoded by distinct genes. RSK2 mutations in CLS patients are extremely heterogeneous. No consistent relationship between specific mutations and the severity of the disease or the expression of uncommon features has been established. Together, the data suggest an influence of environmental and/or other genetic components on the presentation of the disease. Obvious modifying genes include those encoding other RSK family members. In this study we have determined the expression of RSK1, 2 and 3 genes in various human tissues, during mouse embryogenesis and in mouse brain. The three RSK mRNAs were expressed in all human tissues and brain regions tested, supporting functional redundancy. However, tissue specific variations in levels suggest that they may also serve specific roles. The mouse Rsk3 gene was prominently expressed in the developing neural and sensory tissues, whereas Rsk1 gene expression was the strongest in various other tissues with high proliferative activity, suggesting distinct roles during development. In adult mouse brain, the highest levels of Rsk2 expression were observed in regions with high synaptic activity, including the neocortex, the hippocampus and Purkinje cells. These structures are essential components in cognitive function and learning. Based on the expression levels, our results suggest that in these areas, the Rsk1 and Rsk3 genes may not be able to fully compensate for a lack of Rsk2 function.


Assuntos
Encéfalo/enzimologia , Síndrome de Coffin-Lowry/genética , Cognição/fisiologia , Regulação Enzimológica da Expressão Gênica , Aprendizagem/fisiologia , Mutação , Proteínas Quinases S6 Ribossômicas 90-kDa/genética , Animais , Northern Blotting , Encéfalo/embriologia , Feminino , Humanos , Técnicas Imunoenzimáticas , Hibridização In Situ , Sistema de Sinalização das MAP Quinases , Camundongos , Gravidez , Proteínas Quinases S6 Ribossômicas 90-kDa/metabolismo
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