Zhensheng Tao

Direct time-domain observation of attosecond final-state lifetimes in photoemission from solids

Clocking electrons as they exit a metal Einstein earned his Nobel Prize for a quantum-mechanical explanation of electron ejection from metals by light. More than a century later, attosecond spectroscopy has let researchers explore that process in real time. Tao et al. used attosecond pulse trains to distinguish the dynamics of electrons excited from a nickel surface into discrete states versus free space (see the Perspective by Bovensiepen and Liggues). They succeeded in resolving a time delay of ∼200 as that was associated with excitation into unoccupied band states. Science, this issue p. 62; see also p. 28 Attosecond pulses resolve the quantum mechanical delays associated with electron photoejection from a nickel surface. Attosecond spectroscopic techniques have made it possible to measure differences in transport times for photoelectrons from localized core levels and delocalized valence bands in solids. We report the application of attosecond pulse trains to directly and unambiguously measure the difference in lifetimes between photoelectrons born into free electron–like states and those excited into unoccupied excited states in the band structure of nickel (111). An enormous increase in lifetime of 212 ± 30 attoseconds occurs when the final state coincides with a short-lived excited state. Moreover, a strong dependence of this lifetime on emission angle is directly related to the final-state band dispersion as a function of electron transverse momentum. This finding underscores the importance of the material band structure in determining photoelectron lifetimes and corresponding electron escape depths.

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

Circularly polarized attosecond pulse trains in the EUV region were reconstructed using 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.

Space charge effects in ultrafast electron diffraction and imaging

Understanding space charge effects is central for the development of high-brightness ultrafast electron diffraction and microscopy techniques for imaging material transformation with atomic scale detail at the fs to ps timescales. We present methods and results for direct ultrafast photoelectron beam characterization employing a shadow projection imaging technique to investigate the generation of ultrafast, non-uniform, intense photoelectron pulses in a dc photo-gun geometry. Combined with N-particle simulations and an analytical Gaussian model, we elucidate three essential space-charge-led features: the pulse lengthening following a power-law scaling, the broadening of the initial energy distribution, and the virtual cathode threshold. The impacts of these space charge effects on the performance of the next generation high-brightness ultrafast electron diffraction and imaging systems are evaluated.

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.

The nature of photoinduced phase transition and metastable states in vanadium dioxide

Photoinduced threshold switching processes that lead to bistability and the formation of metastable phases in photoinduced phase transition of VO2 are elucidated through ultrafast electron diffraction and diffusive scattering techniques with varying excitation wavelengths. We uncover two distinct regimes of the dynamical phase change: a nearly instantaneous crossover into an intermediate state and its decay led by lattice instabilities over 10 ps timescales. The structure of this intermediate state is identified to be monoclinic, but more akin to M2 rather than M1 based on structure refinements. The extinction of all major monoclinic features within just a few picoseconds at the above-threshold-level (~20%) photoexcitations and the distinct dynamics in diffusive scattering that represents medium-range atomic fluctuations at two photon wavelengths strongly suggest a density-driven and nonthermal pathway for the initial process of the photoinduced phase transition. These results highlight the critical roles of electron correlations and lattice instabilities in driving and controlling phase transformations far from equilibrium.

Distinguishing attosecond electron–electron scattering and screening in transition metals

Significance Electron–electron interactions are among the fastest processes in materials that determine their fascinating properties, occurring on attosecond timescales on up (1 as = 10−18 s). The recent development of attosecond angle-resolved photoemission spectroscopy (atto-ARPES) using high harmonic generation has opened up the possibility of probing electron–electron interactions in real time. In this paper, we distinguish electron–electron screening and charge scattering in the time domain in individual energy bands within a solid. These results open up new possibilities for probing fundamental electron–electron interactions in a host of materials including magnetic, superconducting, and advanced quantum materials. Electron–electron interactions are the fastest processes in materials, occurring on femtosecond to attosecond timescales, depending on the electronic band structure of the material and the excitation energy. Such interactions can play a dominant role in light-induced processes such as nano-enhanced plasmonics and catalysis, light harvesting, or phase transitions. However, to date it has not been possible to experimentally distinguish fundamental electron interactions such as scattering and screening. Here, we use sequences of attosecond pulses to directly measure electron–electron interactions in different bands of different materials with both simple and complex Fermi surfaces. By extracting the time delays associated with photoemission we show that the lifetime of photoelectrons from the d band of Cu are longer by ∼100 as compared with those from the same band of Ni. We attribute this to the enhanced electron–electron scattering in the unfilled d band of Ni. Using theoretical modeling, we can extract the contributions of electron–electron scattering and screening in different bands of different materials with both simple and complex Fermi surfaces. Our results also show that screening influences high-energy photoelectrons (≈20 eV) significantly less than low-energy photoelectrons. As a result, high-energy photoelectrons can serve as a direct probe of spin-dependent electron–electron scattering by neglecting screening. This can then be applied to quantifying the contribution of electron interactions and screening to low-energy excitations near the Fermi level. The information derived here provides valuable and unique information for a host of quantum materials.

Computational and experimental characterization of high-brightness beams for femtosecond electron imaging and spectroscopy

Using a multilevel fast multipole method, coupled with the shadow imaging of femtosecond photoelectron pulses for validation, we quantitatively elucidate the photocathode, space charge, and virtual cathode physics, which fundamentally limit the spatiotemporal and spectroscopic resolution and throughput of ultrafast electron microscope (UEM) systems. We present a simple microscopic description to capture the nonlinear beam dynamics based on a two-fluid picture and elucidate an unexpected dominant role of image potential pinning in accelerating the emittance growth process. These calculations set theoretical limits on the performance of UEM systems and provide useful guides for photocathode design for high-brightness electron beam systems.

Critical behavior within 20 fs drives the out-of-equilibrium laser-induced magnetic phase transition in nickel

High-harmonic spectroscopies reveal that fast energy transfer within 20 fs triggers ultrafast magnetic phase transition in Ni. It has long been known that ferromagnets undergo a phase transition from ferromagnetic to paramagnetic at the Curie temperature, associated with critical phenomena such as a divergence in the heat capacity. A ferromagnet can also be transiently demagnetized by heating it with an ultrafast laser pulse. However, to date, the connection between out-of-equilibrium and equilibrium phase transitions, or how fast the out-of-equilibrium phase transitions can proceed, was not known. By combining time- and angle-resolved photoemission with time-resolved transverse magneto-optical Kerr spectroscopies, we show that the same critical behavior also governs the ultrafast magnetic phase transition in nickel. This is evidenced by several observations. First, we observe a divergence of the transient heat capacity of the electron spin system preceding material demagnetization. Second, when the electron temperature is transiently driven above the Curie temperature, we observe an extremely rapid change in the material response: The spin system absorbs sufficient energy within the first 20 fs to subsequently proceed through the phase transition, whereas demagnetization and the collapse of the exchange splitting occur on much longer, fluence-independent time scales of ~176 fs. Third, we find that the transient electron temperature alone dictates the magnetic response. Our results are important because they connect the out-of-equilibrium material behavior to the strongly coupled equilibrium behavior and uncover a new time scale in the process of ultrafast demagnetization.

Active control of bright electron beams with RF optics for femtosecond microscopy

A frontier challenge in implementing femtosecond electron microscopy is to gain precise optical control of intense beams to mitigate collective space charge effects for significantly improving the throughput. Here, we explore the flexible uses of an RF cavity as a longitudinal lens in a high-intensity beam column for condensing the electron beams both temporally and spectrally, relevant to the design of ultrafast electron microscopy. Through the introduction of a novel atomic grating approach for characterization of electron bunch phase space and control optics, we elucidate the principles for predicting and controlling the phase space dynamics to reach optimal compressions at various electron densities and generating conditions. We provide strategies to identify high-brightness modes, achieving ∼100 fs and ∼1 eV resolutions with 106 electrons per bunch, and establish the scaling of performance for different bunch charges. These results benchmark the sensitivity and resolution from the fundamental beam brightness perspective and also validate the adaptive optics concept to enable delicate control of the density-dependent phase space structures to optimize the performance, including delivering ultrashort, monochromatic, high-dose, or coherent electron bunches.

The Differential Algebra Based Multiple Level Fast Multipole Algorithm for 3D Space Charge Field Calculation and Photoemission Simulation

Coulomb interaction between charged particles inside a bunch is one of the most important collective effects in beam dynamics, becoming even more significant as the energy of the particle beam is lowered to accommodate analytical and low-Z material imaging purposes such as in the time resolved Ultrafast Electron Microscope (UEM) development currently underway at Michigan State University. Space charge effects are the key limiting factor in the development of ultrafast atomic resolution electron imaging and diffraction technologies [1-4] and are also correlated with an irreversible growth in rms beam emittance due to fluctuating components of the nonlinear electron dynamics. In the short pulse regime used in the UEM, space charge effects also lead to virtual cathode (VC) formation in which the negative charge of the electrons emitted at earlier times, combined with the attractive surface field, hinders further emission of particles and causes a degradation of the pulse properties. Space charge and virtual cathode effects and their remediation are core issues for the development of the next generation of high-brightness UEMs [5-9]. Since the analytical models are only applicable for special cases, numerical simulations, in addition to experiments, are usually necessary to accurately understand the space charge effect. In this paper we will introduce a grid-free differential algebra (DA) based multiple level fast multipole algorithm (MLFMA), which calculates the 3D space charge field for n charged particles in arbitrary distribution with an efficiency of O(n) [10], and the implementation of the DA based MLFMA to a simulation code for space charge dominated photoemission process.