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1.
Nat Nanotechnol ; 18(1): 29-35, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-36543882

RESUMO

Photoinduced charge transfer in van der Waals heterostructures occurs on the 100 fs timescale despite weak interlayer coupling and momentum mismatch. However, little is understood about the microscopic mechanism behind this ultrafast process and the role of the lattice in mediating it. Here, using femtosecond electron diffraction, we directly visualize lattice dynamics in photoexcited heterostructures of WSe2/WS2 monolayers. Following the selective excitation of WSe2, we measure the concurrent heating of both WSe2 and WS2 on a picosecond timescale-an observation that is not explained by phonon transport across the interface. Using first-principles calculations, we identify a fast channel involving an electronic state hybridized across the heterostructure, enabling phonon-assisted interlayer transfer of photoexcited electrons. Phonons are emitted in both layers on the femtosecond timescale via this channel, consistent with the simultaneous lattice heating observed experimentally. Taken together, our work indicates strong electron-phonon coupling via layer-hybridized electronic states-a novel route to control energy transport across atomic junctions.

2.
Adv Mater ; : e2206997, 2022 Nov 28.
Artigo em Inglês | MEDLINE | ID: mdl-36440651

RESUMO

One central challenge in understanding phonon thermal transport is a lack of experimental tools to investigate frequency-resolved phonon transport. Although recent advances in computation lead to frequency-resolved information, it is hindered by unknown defects in bulk regions and at interfaces. Here, a framework that can uncover microscopic phonon transport information in heterostructures is presented, integrating state-of-the-art ultrafast electron diffraction (UED) with advanced scientific machine learning (SciML). Taking advantage of the dual temporal and reciprocal-space resolution in UED, and the ability of SciML to solve inverse problems involving O ( 10 3 ) $\mathcal{O}({10^3})$ coupled Boltzmann transport equations, the frequency-dependent interfacial transmittance and frequency-dependent relaxation times of the heterostructure from the diffraction patterns are reliably recovered. The framework is applied to experimental Au/Si UED data, and a transport pattern beyond the diffuse mismatch model is revealed, which further enables a direct reconstruction of real-space, real-time, frequency-resolved phonon dynamics across the interface. The work provides a new pathway to probe interfacial phonon transport mechanisms with unprecedented details.

3.
Nano Lett ; 2022 Nov 30.
Artigo em Inglês | MEDLINE | ID: mdl-36450036

RESUMO

Relaxor ferroelectrics have been intensely studied for decades based on their unique electromechanical responses which arise from local structural heterogeneity involving polar nanoregions or domains. Here, we report first studies of the ultrafast dynamics and reconfigurability of the polarization in freestanding films of the prototypical relaxor 0.68PbMg1/3Nb2/3O3-0.32PbTiO3 (PMN-0.32PT) by probing its atomic-scale response via femtosecond-resolution, electron-scattering approaches. By combining these structural measurements with dynamic phase-field simulations, we show that femtosecond light pulses drive a change in both the magnitude and direction of the polarization vector within polar nanodomains on few-picosecond time scales. This study defines new opportunities for dynamic reconfigurable control of the polarization in nanoscale relaxor ferroelectrics.

4.
Adv Mater ; : e2202841, 2022 Oct 03.
Artigo em Inglês | MEDLINE | ID: mdl-36189841

RESUMO

Magnetism in topological materials creates phases exhibiting quantized transport phenomena with potential technological applications. The emergence of such phases relies on strong interaction between localized spins and the topological bands, and the consequent formation of an exchange gap. However, this remains experimentally unquantified in intrinsic magnetic topological materials. Here, this interaction is quantified in MnBi2 Te4 , a topological insulator with intrinsic antiferromagnetism. This is achieved by optically exciting Bi-Te p states comprising the bulk topological bands and interrogating the consequent Mn 3d spin dynamics, using a multimodal ultrafast approach. Ultrafast electron scattering and magneto-optic measurements show that the p states demagnetize via electron-phonon scattering at picosecond timescales. Despite being energetically decoupled from the optical excitation, the Mn 3d spins, probed by resonant X-ray scattering, are observed to disorder concurrently with the p spins. Together with atomistic simulations, this reveals that the exchange coupling between localized spins and the topological bands is at least 100 times larger than the superexchange interaction, implying an optimal exchange gap of at least 25 meV in the surface states. By quantifying this exchange coupling, this study validates the materials-by-design strategy of utilizing localized magnetic order to manipulate topological phases, spanning static to ultrafast timescales.

5.
Phys Chem Chem Phys ; 24(25): 15416-15427, 2022 Jun 29.
Artigo em Inglês | MEDLINE | ID: mdl-35707953

RESUMO

The structural dynamics of photoexcited gas-phase carbon disulfide (CS2) molecules are investigated using ultrafast electron diffraction. The dynamics were triggered by excitation of the optically bright 1B2(1Σu+) state by an ultraviolet femtosecond laser pulse centred at 200 nm. In accordance with previous studies, rapid vibrational motion facilitates a combination of internal conversion and intersystem crossing to lower-lying electronic states. Photodissociation via these electronic manifolds results in the production of CS fragments in the electronic ground state and dissociated singlet and triplet sulphur atoms. The structural dynamics are extracted from the experiment using a trajectory-fitting filtering approach, revealing the main characteristics of the singlet and triplet dissociation pathways. Finally, the effect of the time-resolution on the experimental signal is considered and an outlook to future experiments provided.

6.
Sci Adv ; 8(13): eabn0523, 2022 04.
Artigo em Inglês | MEDLINE | ID: mdl-35363518

RESUMO

Magnetic nanoparticles such as FePt in the L10 phase are the bedrock of our current data storage technology. As the grains become smaller to keep up with technological demands, the superparamagnetic limit calls for materials with higher magnetocrystalline anisotropy. This, in turn, reduces the magnetic exchange length to just a few nanometers, enabling magnetic structures to be induced within the nanoparticles. Here, we describe the existence of spin-wave solitons, dynamic localized bound states of spin-wave excitations, in FePt nanoparticles. We show with time-resolved x-ray diffraction and micromagnetic modeling that spin-wave solitons of sub-10 nm sizes form out of the demagnetized state following femtosecond laser excitation. The measured soliton spin precession frequency of 0.1 THz positions this system as a platform to develop novel miniature devices.

7.
Nat Commun ; 13(1): 1929, 2022 Apr 08.
Artigo em Inglês | MEDLINE | ID: mdl-35396393

RESUMO

The emergence of magnetism in quantum materials creates a platform to realize spin-based applications in spintronics, magnetic memory, and quantum information science. A key to unlocking new functionalities in these materials is the discovery of tunable coupling between spins and other microscopic degrees of freedom. We present evidence for interlayer magnetophononic coupling in the layered magnetic topological insulator MnBi2Te4. Employing magneto-Raman spectroscopy, we observe anomalies in phonon scattering intensities across magnetic field-driven phase transitions, despite the absence of discernible static structural changes. This behavior is a consequence of a magnetophononic wave-mixing process that allows for the excitation of zone-boundary phonons that are otherwise 'forbidden' by momentum conservation. Our microscopic model based on density functional theory calculations reveals that this phenomenon can be attributed to phonons modulating the interlayer exchange coupling. Moreover, signatures of magnetophononic coupling are also observed in the time domain through the ultrafast excitation and detection of coherent phonons across magnetic transitions. In light of the intimate connection between magnetism and topology in MnBi2Te4, the magnetophononic coupling represents an important step towards coherent on-demand manipulation of magnetic topological phases.

8.
Lab Chip ; 22(7): 1365-1373, 2022 03 29.
Artigo em Inglês | MEDLINE | ID: mdl-35234235

RESUMO

We report on the design and testing of glass nozzles used to produce liquid sheets. The sheet nozzles use a single converging channel chemically etched into glass wafers by standard lithographic methods. Operation in ambient air and vacuum was demonstrated. The measured sheet thickness ranges over one order of magnitude with the smallest thickness of 250 nm and the largest of 2.5 µm. Sheet thickness was shown to be independent of liquid flow rate, and dependent on the nozzle outlet area. Sheet surface roughness was dependent on nozzle surface finish and was on the order of 10 nm for polished nozzles. Electron transmission data is presented for various sheet thicknesses near the MeV mean free path and the charge pair distribution function for D2O is determined from electron scattering data.


Assuntos
Vidro , Vácuo
9.
Phys Rev Lett ; 128(3): 036401, 2022 Jan 21.
Artigo em Inglês | MEDLINE | ID: mdl-35119886

RESUMO

Hysteresis underlies a large number of phase transitions in solids, giving rise to exotic metastable states that are otherwise inaccessible. Here, we report an unconventional hysteretic transition in a quasi-2D material, EuTe_{4}. By combining transport, photoemission, diffraction, and x-ray absorption measurements, we observe that the hysteresis loop has a temperature width of more than 400 K, setting a record among crystalline solids. The transition has an origin distinct from known mechanisms, lying entirely within the incommensurate charge density wave (CDW) phase of EuTe_{4} with no change in the CDW modulation periodicity. We interpret the hysteresis as an unusual switching of the relative CDW phases in different layers, a phenomenon unique to quasi-2D compounds that is not present in either purely 2D or strongly coupled 3D systems. Our findings challenge the established theories on metastable states in density wave systems, pushing the boundary of understanding hysteretic transitions in a broken-symmetry state.

10.
Nat Commun ; 13(1): 1055, 2022 Feb 25.
Artigo em Inglês | MEDLINE | ID: mdl-35217665

RESUMO

Plasticity is ubiquitous and plays a critical role in material deformation and damage; it inherently involves the atomistic length scale and picosecond time scale. A fundamental understanding of the elastic-plastic deformation transition, in particular, incipient plasticity, has been a grand challenge in high-pressure and high-strain-rate environments, impeded largely by experimental limitations on spatial and temporal resolution. Here, we report femtosecond MeV electron diffraction measurements visualizing the three-dimensional (3D) response of single-crystal aluminum to the ultrafast laser-induced compression. We capture lattice transitioning from a purely elastic to a plastically relaxed state within 5 ps, after reaching an elastic limit of ~25 GPa. Our results allow the direct determination of dislocation nucleation and transport that constitute the underlying defect kinetics of incipient plasticity. Large-scale molecular dynamics simulations show good agreement with the experiment and provide an atomic-level description of the dislocation-mediated plasticity.

11.
Phys Rev Lett ; 127(22): 227401, 2021 Nov 24.
Artigo em Inglês | MEDLINE | ID: mdl-34889631

RESUMO

Engineering novel states of matter with light is at the forefront of materials research. An intensely studied direction is to realize broken-symmetry phases that are "hidden" under equilibrium conditions but can be unleashed by an ultrashort laser pulse. Despite a plethora of experimental discoveries, the nature of these orders and how they transiently appear remain unclear. To this end, we investigate a nonequilibrium charge density wave (CDW) in rare-earth tritellurides, which is suppressed in equilibrium but emerges after photoexcitation. Using a pump-pump-probe protocol implemented in ultrafast electron diffraction, we demonstrate that the light-induced CDW consists solely of order parameter fluctuations, which bear striking similarities to critical fluctuations in equilibrium despite differences in the length scale. By calculating the dynamics of CDW fluctuations in a nonperturbative model, we further show that the strength of the light-induced order is governed by the amplitude of equilibrium fluctuations. These findings highlight photoinduced fluctuations as an important ingredient for the emergence of transient orders out of equilibrium. Our results further suggest that materials with strong fluctuations in equilibrium are promising platforms to host hidden orders after laser excitation.

12.
Science ; 373(6552): 352-355, 2021 07 16.
Artigo em Inglês | MEDLINE | ID: mdl-34437156

RESUMO

Understanding the pathways and time scales underlying electrically driven insulator-metal transitions is crucial for uncovering the fundamental limits of device operation. Using stroboscopic electron diffraction, we perform synchronized time-resolved measurements of atomic motions and electronic transport in operating vanadium dioxide (VO2) switches. We discover an electrically triggered, isostructural state that forms transiently on microsecond time scales, which is shown by phase-field simulations to be stabilized by local heterogeneities and interfacial interactions between the equilibrium phases. This metastable phase is similar to that formed under photoexcitation within picoseconds, suggesting a universal transformation pathway. Our results establish electrical excitation as a route for uncovering nonequilibrium and metastable phases in correlated materials, opening avenues for engineering dynamical behavior in nanoelectronics.

13.
Nature ; 596(7873): 531-535, 2021 08.
Artigo em Inglês | MEDLINE | ID: mdl-34433948

RESUMO

Water is one of the most important, yet least understood, liquids in nature. Many anomalous properties of liquid water originate from its well-connected hydrogen bond network1, including unusually efficient vibrational energy redistribution and relaxation2. An accurate description of the ultrafast vibrational motion of water molecules is essential for understanding the nature of hydrogen bonds and many solution-phase chemical reactions. Most existing knowledge of vibrational relaxation in water is built upon ultrafast spectroscopy experiments2-7. However, these experiments cannot directly resolve the motion of the atomic positions and require difficult translation of spectral dynamics into hydrogen bond dynamics. Here, we measure the ultrafast structural response to the excitation of the OH stretching vibration in liquid water with femtosecond temporal and atomic spatial resolution using liquid ultrafast electron scattering. We observed a transient hydrogen bond contraction of roughly 0.04 Å on a timescale of 80 femtoseconds, followed by a thermalization on a timescale of approximately 1 picosecond. Molecular dynamics simulations reveal the need to treat the distribution of the shared proton in the hydrogen bond quantum mechanically to capture the structural dynamics on femtosecond timescales. Our experiment and simulations unveil the intermolecular character of the water vibration preceding the relaxation of the OH stretch.

14.
Adv Mater ; 33(37): e2101875, 2021 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-34331368

RESUMO

On-chip dynamic strain engineering requires efficient micro-actuators that can generate large in-plane strains. Inorganic electrochemical actuators are unique in that they are driven by low voltages (≈1 V) and produce considerable strains (≈1%). However, actuation speed and efficiency are limited by mass transport of ions. Minimizing the number of ions required to actuate is thus key to enabling useful "straintronic" devices. Here, it is shown that the electrochemical intercalation of exceptionally few lithium ions into WTe2 causes large anisotropic in-plane strain: 5% in one in-plane direction and 0.1% in the other. This efficient stretching of the 2D WTe2 layers contrasts to intercalation-induced strains in related materials which are predominantly in the out-of-plane direction. The unusual actuation of Lix WTe2 is linked to the formation of a newly discovered crystallographic phase, referred to as Td', with an exotic atomic arrangement. On-chip low-voltage (<0.2 V) control is demonstrated over the transition to the novel phase and its composition. Within the Td'-Li0.5- δ WTe2 phase, a uniaxial in-plane strain of 1.4% is achieved with a change of δ of only 0.075. This makes the in-plane chemical expansion coefficient of Td'-Li0.5-δ WTe2 far greater than of any other single-phase material, enabling fast and efficient planar electrochemical actuation.

15.
Nat Commun ; 12(1): 1860, 2021 Mar 25.
Artigo em Inglês | MEDLINE | ID: mdl-33767138

RESUMO

Nonradiative processes limit optoelectronic functionality of nanocrystals and curb their device performance. Nevertheless, the dynamic structural origins of nonradiative relaxations in such materials are not understood. Here, femtosecond electron diffraction measurements corroborated by atomistic simulations uncover transient lattice deformations accompanying radiationless electronic processes in colloidal semiconductor nanocrystals. Investigation of the excitation energy dependence in a core/shell system shows that hot carriers created by a photon energy considerably larger than the bandgap induce structural distortions at nanocrystal surfaces on few picosecond timescales associated with the localization of trapped holes. On the other hand, carriers created by a photon energy close to the bandgap of the core in the same system result in transient lattice heating that occurs on a much longer 200 picosecond timescale, dominated by an Auger heating mechanism. Elucidation of the structural deformations associated with the surface trapping of hot holes provides atomic-scale insights into the mechanisms deteriorating optoelectronic performance and a pathway towards minimizing these losses in nanocrystal devices.

16.
Nano Lett ; 21(19): 8051-8057, 2021 Oct 13.
Artigo em Inglês | MEDLINE | ID: mdl-34529439

RESUMO

Vertically stacked transition metal dichalcogenide-graphene heterostructures provide a platform for novel optoelectronic applications with high photoresponse speeds. Photoinduced nonequilibrium carrier and lattice dynamics in such heterostructures underlie these applications but have not been understood. In particular, the dependence of these photoresponses on the twist angle, a key tuning parameter, remains elusive. Here, using ultrafast electron diffraction, we report the simultaneous visualization of charge transfer and electron-phonon coupling in MoS2-graphene heterostructures with different stacking configurations. We find that the charge transfer timescale from MoS2 to graphene varies strongly with twist angle, becoming faster for smaller twist angles, and show that the relaxation timescale is significantly shorter in a heterostructure as compared to a monolayer. These findings illustrate that twist angle constitutes an additional tuning knob for interlayer charge transfer in heterobilayers and deepen our understanding of fundamental photophysical processes in heterostructures, of importance for future applications in optoelectronics and light harvesting.

17.
Phys Chem Chem Phys ; 23(2): 1308-1316, 2021 Jan 21.
Artigo em Inglês | MEDLINE | ID: mdl-33367391

RESUMO

Electron scattering on liquid samples has been enabled recently by the development of ultrathin liquid sheet technologies. The data treatment of liquid-phase electron scattering has been mostly reliant on methodologies developed for gas electron diffraction, in which theoretical inputs and empirical fittings are often needed to account for the atomic form factor and remove the inelastic scattering background. In this work, we present an alternative data treatment method that is able to retrieve the radial distribution of all the charged particle pairs without the need of either theoretical inputs or empirical fittings. The merits of this new method are illustrated through the retrieval of real-space molecular structure from experimental electron scattering patterns of liquid water, carbon tetrachloride, chloroform, and dichloromethane.

18.
ACS Nano ; 14(7): 8449-8458, 2020 Jul 28.
Artigo em Inglês | MEDLINE | ID: mdl-32538617

RESUMO

The inspection of Friedel's law in ultrafast electron diffraction (UED) is important to gain a comprehensive understanding of material atomic structure and its dynamic response. Here, monoclinic gallium telluride (GaTe), as a low-symmetry, layered crystal in contrast to many other 2D materials, is investigated by mega-electronvolt UED. Strong out-of-phase oscillations of Bragg peak intensities are observed for Friedel pairs, which does not obey Friedel's law. As evidenced by the preserved mirror symmetry and supported by both kinematic and dynamic scattering simulations, the intensity oscillations are provoked by the lowest-order longitudinal acoustic breathing phonon. Our results provide a generalized understanding of Friedel's law in UED and demonstrate that by designed misalignment of surface normal and primitive lattice vectors, coherent lattice wobbling and effective shear strain can be generated in crystal films by laser pulse excitation, which is otherwise hard to achieve and can be further utilized to dynamically tune and switch material properties.

19.
Science ; 368(6493): 885-889, 2020 05 22.
Artigo em Inglês | MEDLINE | ID: mdl-32439793

RESUMO

Simultaneous observation of nuclear and electronic motion is crucial for a complete understanding of molecular dynamics in excited electronic states. It is challenging for a single experiment to independently follow both electronic and nuclear dynamics at the same time. Here we show that ultrafast electron diffraction can be used to simultaneously record both electronic and nuclear dynamics in isolated pyridine molecules, naturally disentangling the two components. Electronic state changes (S1→S0 internal conversion) were reflected by a strong transient signal in small-angle inelastic scattering, and nuclear structural changes (ring puckering) were monitored by large-angle elastic diffraction. Supported by ab initio nonadiabatic molecular dynamics and diffraction simulations, our experiment provides a clear view of the interplay between electronic and nuclear dynamics of the photoexcited pyridine molecule.

20.
ACS Nano ; 14(4): 4792-4804, 2020 Apr 28.
Artigo em Inglês | MEDLINE | ID: mdl-32208676

RESUMO

Metal nanocrystals exhibit important optoelectronic and photocatalytic functionalities in response to light. These dynamic energy conversion processes have been commonly studied by transient optical probes to date, but an understanding of the atomistic response following photoexcitation has remained elusive. Here, we use femtosecond resolution electron diffraction to investigate transient lattice responses in optically excited colloidal gold nanocrystals, revealing the effects of nanocrystal size and surface ligands on the electron-phonon coupling and thermal relaxation dynamics. First, we uncover a strong size effect on the electron-phonon coupling, which arises from reduced dielectric screening at the nanocrystal surfaces and prevails independent of the optical excitation mechanism (i.e., inter- and intraband). Second, we find that surface ligands act as a tuning parameter for hot carrier cooling. Particularly, gold nanocrystals with thiol-based ligands show significantly slower carrier cooling as compared to amine-based ligands under intraband optical excitation due to electronic coupling at the nanocrystal/ligand interfaces. Finally, we spatiotemporally resolve thermal transport and heat dissipation in photoexcited nanocrystal films by combining electron diffraction with stroboscopic elastic scattering microscopy. Taken together, we resolve the distinct thermal relaxation time scales ranging from 1 ps to 100 ns associated with the multiple interfaces through which heat flows at the nanoscale. Our findings provide insights into optimization of gold nanocrystals and their thin films for photocatalysis and thermoelectric applications.

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