Ultrafast imaging of photoelectron packets generated from graphite surface

We present an electron projection imaging method to study the ultrafast evolution of photoelectron density distribution and transient fields near the surface. The dynamical profile of the photoelectrons from graphite reveals an origin of a thermionic emission, followed by an adiabatic process leading to electron acceleration and cooling before a freely expanding cloud is established. The hot electron emission is found to couple with a surface charge dipole layer formation, with a sheet density several orders of magnitude higher than that of the vacuum emitted cloud.Comment: 9 pages, 4 figures. Applied Physics Letter, in pres

Coherent modulation of the electron temperature and electron-phonon couplings in a 2D material

Ultrashort light pulses can selectively excite charges, spins and phonons in materials, providing a powerful approach for manipulating their properties. Here we use femtosecond laser pulses to coherently manipulate the electron and phonon distributions, and their couplings, in the charge density wave (CDW) material 1T-TaSe$_2$. After exciting the material with a short light pulse, spatial smearing of the electrons launches a coherent lattice breathing mode, which in turn modulates the electron temperature. This indicates a bi-directional energy exchange between the electrons and the strongly-coupled phonons. By tuning the laser excitation fluence, we can control the magnitude of the electron temperature modulation, from ~ 200 K in the case of weak excitation, to ~ 1000 K for strong laser excitation. This is accompanied by a switching of the dominant mechanism from anharmonic phonon-phonon coupling to coherent electron-phonon coupling, as manifested by a phase change of $\pi$ in the electron temperature modulation. Our approach thus opens up possibilities for coherently manipulating the interactions and properties of quasi-2D and other quantum materials using light.Comment: 15 pages, 4 figure

Active spintronic-metasurface terahertz emitters with tunable chirality

The ability to manipulate the electric-field vector of broadband terahertz waves is essential for applications of terahertz technologies in many areas, and can open up new possibilities for nonlinear terahertz spectroscopy and coherent control. Here, we propose a novel laser-driven terahertz emitter, consisting of metasurface-patterned magnetic multilayer heterostructures. Such hybrid terahertz emitters can combine the advantages of spintronic emitters for being ultrabroadband, efficient and flexible, as well as those of metasurfaces for the unique capability to manipulate terahertz waves with high precision and degree of freedom. Taking a stripe-patterned metasurface as an example, we demonstrate the generation of broadband terahertz waves with tunable chirality. Based on experimental and theoretical studies, the interplay between the laser-induced spintronic-origin currents and the metasurface-induced transient charges/currents are investigated, revealing the strong influence on the device functionality originated from both the light-matter interactions in individual metasurface units and the dynamic coupling between them. Our work not only offers a flexible, reliable and cost-effective solution for chiral terahertz wave generation and manipulation, but also opens a new pathway to metasurface-tailored spintronic devices for efficient vector-control of electromagnetic waves in the terahertz regime

Flexible generation of structured terahertz fields via programmable exchange-biased spintronic emitters

Structured light, particularly in the terahertz frequency range, holds considerable potential for a diverse range of applications. However, the generation and control of structured terahertz radiation pose major challenges. In this work, we demonstrate a novel programmable spintronic emitter that can flexibly generate a variety of structured terahertz waves. This is achieved through the precise and high-resolution programming of the magnetization pattern on the emitter surface, utilizing laser-assisted local field cooling of an exchange-biased ferromagnetic heterostructure. Moreover, we outline a generic design strategy for realizing specific complex structured terahertz fields in the far field. Our device successfully demonstrates the generation of terahertz waves with diverse structured polarization states, including spatially separated circular polarizations, azimuthal or radial polarization states, and a full Poincare beam. This innovation opens a new avenue for designing and generating structured terahertz radiations, with potential applications in terahertz microscopy, communication, quantum information, and light-matter interactions

Solitary beam propagation in a nonlinear optical resonator enables high-efficiency pulse compression and mode self-cleaning

Generating intense ultrashort pulses with high-quality spatial modes is crucial for ultrafast and strong-field science. This can be accomplished by controlling propagation of femtosecond pulses under the influence of Kerr nonlinearity and achieving stable propagation with high intensity. In this work, we propose that the generation of spatial solitons in periodic layered Kerr media can provide an optimum condition for supercontinuum generation and pulse compression using multiple thin plates. With both the experimental and theoretical investigations, we successfully identify these solitary modes and reveal a universal relationship between the beam size and the critical nonlinear phase. Space-time coupling is shown to strongly influence the spectral, spatial and temporal profiles of femtosecond pulses. Taking advantage of the unique characters of these solitary modes, we demonstrate single-stage supercontinuum generation and compression of femtosecond pulses from initially 170 fs down to 22 fs with an efficiency ~90%. We also provide evidence of efficient mode self-cleaning which suggests rich spatial-temporal self-organization processes of laser beams in a nonlinear resonator

Nonrelativistic and nonmagnetic control of terahertz charge currents via electrical anisotropy in RuO2 and IrO2

Precise and ultrafast control over photo-induced charge currents across nanoscale interfaces could lead to important applications in energy harvesting, ultrafast electronics, and coherent terahertz sources. Recent studies have shown that several relativistic mechanisms, including inverse spin-Hall effect, inverse Rashba-Edelstein effect and inverse spin-orbit-torque effect, can convert longitudinally injected spin-polarized currents from magnetic materials to transverse charge currents, thereby harnessing these currents for terahertz generation. However, these mechanisms typically require external magnetic fields and suffer from low spin-polarization rates and low efficiencies of relativistic spin-to-charge conversion. In this work, we present a novel nonrelativistic and nonmagnetic mechanism that directly utilizes the photo-excited high-density charge currents across the interface. We demonstrate that the electrical anisotropy of conductive oxides RuO2 and IrO2 can effectively deflect injected charge currents to the transverse direction, resulting in efficient and broadband terahertz radiation. Importantly, this new mechanism has the potential to offer much higher conversion efficiency compared to previous methods, as conductive materials with large electrical anisotropy are readily available, whereas further increasing the spin-Hall angle of heavy-metal materials would be challenging. Our new findings offer exciting possibilities for directly utilizing these photo-excited high-density currents across metallic interfaces for ultrafast electronics and terahertz spectroscopy

Influence of microscopic and macroscopic effects on attosecond pulse generation using two-color laser fields

Attosecond pulses and pulse trains generated by high-order harmonic generation are finding broad applications in advanced spectroscopies and imaging, enabling sub-femtosecond electron dynamics to be probed in atomic, molecular and material systems. To date, isolated attosecond pulses have been generated either by using very short few-cycle driving pulses, or by using temporal and polarization gating, or by taking advantage of phase-matching gating. Here we show that by driving high harmonics with a two-color linearly polarized laser field, the temporal window for time-gated phase matching is shorter than for the equivalent singe-color driving laser. As a result, we can generate quasi-isolated attosecond pulses with a peak width of ∼ 450 as using relatively long 26 femtosecond laser pulses. Our experimental data are in good agreement with theoretical simulations, and show that the phase matching window decreases by a factor of 4 - from four optical cycles in the case of a single-color fundamental driving laser, to one optical cycle in the case of two-color (ω-2ω) laser drivers. Finally, we also demonstrate that by changing the relative delay between the two-color laser fields, we can control the duration of the attosecond bursts from 450 as to 1.2 fs.National Science Foundation (NSF) (1125844); Air Force Office of Scientific Research (FA9550-16-1-0121); REA (328334); Junta de Castilla y León (SA046U16); MINECO (FIS2013-44174-P, FIS2016-75652-P)

Tomographic reconstruction of circularly polarized high-harmonic fields: 3D attosecond metrology

Bright, circularly polarized, extreme ultraviolet (EUV) and soft x-ray high-harmonic beams can now be produced using counter-rotating circularly polarized driving laser fields. Although the resulting circularly polarized harmonics consist of relatively simple pairs of peaks in the spectral domain, in the time domain, the field is predicted to emerge as a complex series of rotating linearly polarized bursts, varying rapidly in amplitude, frequency, and polarization. We extend attosecond metrology techniques to circularly polarized light by simultaneously irradiating a copper surface with circularly polarized high-harmonic and linearly polarized infrared laser fields. The resulting temporal modulation of the photoelectron spectra carries essential phase information about the EUV field. Utilizing the polarization selectivity of the solid surface and by rotating the circularly polarized EUV field in space, we fully retrieve the amplitude and phase of the circularly polarized harmonics, allowing us to reconstruct one of the most complex coherent light fields produced to date.This work was done at JILA. We gratefully acknowledge support from the NSF through the Physics Frontiers Centers Program with grant no. PHY1125844 and the Gordon and Betty Moore Foundation EPiQS (Emergent Phenomena in Quantum Systems) Initiative through Grant GBMF4538 to M.M. C.H.-G. acknowledges support from the Marie Curie International Outgoing Fellowship within the European Union Seventh Framework Programme for Research and Technological Development (2007–2013), under Research Executive Agency grant agreement no. 328334. R.K. acknowledges the Swedish Research Council (VR) for financial support. A.J.-B. was supported by grants from the U.S. NSF (grant nos. PHY-1125844 and PHY-1068706). C.H.-G. and L.P. acknowledge support from Junta de Castilla y León (project SA116U13) and MINECO (Ministerio de Econom a y Competitividad) (FIS2013-44174-P and FIS2015-71933-REDT). This work used the Janus supercomputer, which is supported by the U.S. NSF (grant no. CNS-0821794) and the University of Colorado, Boulder. P.G. acknowledges support from the Deutsche Forschungsgemeinschaft (no. GR 4234/1-1)