Adra Carr

Collapse of long-range charge order tracked by time-resolved photoemission at high momenta

Intense femtosecond (10−15 s) light pulses can be used to transform electronic, magnetic and structural order in condensed-matter systems on timescales of electronic and atomic motion. This technique is particularly useful in the study and in the control of materials whose physical properties are governed by the interactions between multiple degrees of freedom. Time- and angle-resolved photoemission spectroscopy is in this context a direct and comprehensive, energy- and momentum-selective probe of the ultrafast processes that couple to the electronic degrees of freedom. Previously, the capability of such studies to access electron momentum space away from zero momentum was, however, restricted owing to limitations of the available probing photon energy. Here, using femtosecond extreme-ultraviolet pulses delivered by a high-harmonic-generation source, we use time- and angle-resolved photoemission spectroscopy to measure the photoinduced vaporization of a charge-ordered state in the potential excitonic insulator 1T-TiSe2 (refs 12, 13). By way of stroboscopic imaging of electronic band dispersions at large momentum, in the vicinity of the edge of the first Brillouin zone, we reveal that the collapse of atomic-scale periodic long-range order happens on a timescale as short as 20 femtoseconds. The surprisingly fast response of the system is assigned to screening by the transient generation of free charge carriers. Similar screening scenarios are likely to be relevant in other photoinduced solid-state transitions and may generally determine the response times. Moreover, as electron states with large momenta govern fundamental electronic properties in condensed matter systems, we anticipate that the experimental advance represented by the present study will be useful to study the ultrafast dynamics and microscopic mechanisms of electronic phenomena in a wide range of materials.

Time-domain classification of charge-density-wave insulators

Distinguishing insulators by the dominant type of interaction is a central problem in condensed matter physics. Basic models include the Bloch-Wilson and the Peierls insulator due to electron-lattice interactions, the Mott and the excitonic insulator caused by electron-electron interactions, and the Anderson insulator arising from electron-impurity interactions. In real materials, however, all the interactions are simultaneously present so that classification is often not straightforward. Here, we show that time- and angle-resolved photoemission spectroscopy can directly measure the melting times of electronic order parameters and thus identify-via systematic temporal discrimination of elementary electronic and structural processes-the dominant interaction. Specifically, we resolve the debates about the nature of two peculiar charge-density-wave states in the family of transition-metal dichalcogenides, and show that Rb intercalated 1T-TaS(2) is a Peierls insulator and that the ultrafast response of 1T-TiSe(2) is highly suggestive of an excitonic insulator.

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.

Self-amplified photo-induced gap quenching in a correlated electron material

Capturing the dynamic electronic band structure of a correlated material presents a powerful capability for uncovering the complex couplings between the electronic and structural degrees of freedom. When combined with ultrafast laser excitation, new phases of matter can result, since far-from-equilibrium excited states are instantaneously populated. Here, we elucidate a general relation between ultrafast non-equilibrium electron dynamics and the size of the characteristic energy gap in a correlated electron material. We show that carrier multiplication via impact ionization can be one of the most important processes in a gapped material, and that the speed of carrier multiplication critically depends on the size of the energy gap. In the case of the charge-density wave material 1T-TiSe2, our data indicate that carrier multiplication and gap dynamics mutually amplify each other, which explains—on a microscopic level—the extremely fast response of this material to ultrafast optical excitation.

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.

Tomographic Reconstruction of Circularly Polarized High Harmonic Fields: 3D Attosecond Metrology

Using laser-dressed photoelectron spectroscopy from solids, we completely characterized the circularly polarized harmonics, allowing us to reconstruct the complex 3D waveform of the circularly polarized attosecond pulse train.

Defect Classification Using Machine Learning

Laser-induced damage growth on the surface of fused silica optics has been extensively studied and has been found to depend on a number of factors including fluence and the surface on which the damage site resides. It has been demonstrated that damage sites as small as a few tens of microns can be detected and tracked on optics installed a fusion-class laser, however, determining the surface of an optic on which a damage site resides in situ can be a significant challenge. In this work demonstrate that a machine-learning algorithm can successfully predict the surface location of the damage site using an expanded set of characteristics for each damage site, some of which are not historically associated with growth rate.

Far above bandgap photonics: attosecond dynamics of highly excited electrons in materials

Tabletop-scale coherent EUV generated through high-harmonic generation (HHG) produces light in the form of an attosecond pulse train that uniquely combines characteristics of good energy resolution (≈100-300meV) with sub-fs time resolution. This makes HHG an ideal source for studying the fastest dynamics in materials. Furthermore, using angle-resolved photoemission spectroscopy (ARPES), it is possible to extract detailed information about electron dynamics over the entire Brillouin zone. In recently published work, we combined HHG with ARPES to identify a sub-femtosecond excited-state lifetime for the first time. Photoemission occurs as a three-step process: 1) An electron is photoexcited from the valence band to far above the Fermi energy; 2) it transports to the surface, and 3) it overcomes the work function and exits. If the electron is promoted into a highlyexcited unoccupied band in the material (as opposed to a free-electron-like state), we observe the electron emission lifetime to increase in a measurable way—the Ni band 22 eV above the Fermi level has a lifetime of 212±30 attoseconds. Furthermore, by comparing photoemission from Cu and Ni, we reveal the influence of attosecond-timescale electron screening vs scattering by the electrons near the fermi surface. This work for the first time demonstrates the relevance of attosecond spectroscopy to the study of intrinsic properties and band structure in materials, as opposed to the strong-field induced dynamics studied extensively to-date.

3D Characterization of Attosecond Pulse Trains with Circular Polarization

Using laser-dressed photoelectron spectroscopy from solids, we fully characterize circularly polarized harmonics for the first time to reconstruct the complex 3D waveform of a circularly polarized attosecond pulse train.