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Role of Equilibrium Fluctuations in Light-Induced Order
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. Overall, 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.
Distinct Optical Excitation Mechanisms of a Coherent Magnon in a van der Waals Antiferromagnet
The control of antiferromagnets with ultrashort optical pulses has emerged as a prominent field of research. Tailored laser excitation can launch coherent spin waves at terahertz frequencies, yet a comprehensive description of their generation mechanisms is still lacking despite extensive efforts. Using terahertz emission spectroscopy, we investigate the generation of a coherent magnon mode in the van der Waals antiferromagnet NiPS 3 under a range of photoexcitation conditions. By tuning the pump photon energy from transparency to resonant with a 𝑑−𝑑 transition, we reveal a striking change in the coherent magnon’s dependence on the pump polarization, indicating two distinct excitation mechanisms. Furthermore, our findings provide a strategy for the manipulation of magnetic modes via photoexcitation around subgap electronic states.
Ultrafast nonequilibrium dynamics and high-harmonic generation in two-dimensional quantum spin Hall materials
For this work, we develop the theoretical framework of nonequilibrium ultrafast photonics in monolayer quantum spin Hall insulators supporting a multitude of topological states. In these materials, ubiquitous strong light-matter interactions in the femtosecond scale lead to nonadiabatic quantum dynamics, resulting in topology-dependent nonlinear optoelectronic transport phenomena. We investigate the mechanism driving topological Dirac fermions interacting with strong ultrashort light pulses and uncover various experimentally accessible physical quantities that encode fingerprints of the quantum material's topological electronic state from the high-harmonic generated spectrum. Our work sets the theoretical cornerstones to realize the full potential of time-resolved harmonic spectroscopy for understanding nonequilibrium processes in quantum topological systems and identifying topological invariants in two-dimensional quantum spin Hall solid state systems.
Magneto-opto-phononic inverse Faraday effect
Nonlinear frequency conversion processes, such as optical rectification, difference-frequency generation, and sum-frequency generation, are fundamental for producing electromagnetic radiation at diverse frequencies. In this work, we demonstrate that coherently excited infrared-active phonons can act as transducers for generating nonlinear magnetizations through phonon-magnon interactions, analogous to nonlinear optical frequency conversion. We derive analytical solutions for the time-dependent magnetizations arising from the second-order response to the electric field component of an ultrashort laser pulse. These solutions enable us to define second-order nonlinear magneto-electric susceptibilities, which describe rectification, impulsive excitation, and sum-frequency excitation of coherent magnons. Our theoretical framework naturally incorporates the conventional magneto-optic and phonon inverse Faraday effects and predicts a hybrid magneto-opto-phononic inverse Faraday effect involving photon-phonon-magnon scattering. This work highlights nonlinear phononics as a pathway for controlling magnetization in solids.
Light field–controlled PHz currents in intrinsic metals
Oriented electric currents in metals are routinely driven by applying an external electric potential. Although the response of electrons to the external electric fields occurs within attoseconds, conventional electronics do not use this speed potential. Ultrashort laser pulses with controlled shapes of electric fields that switch direction at petahertz frequencies open perspectives for driving currents in metals. Light field–driven currents were demonstrated in various media including dielectrics, semiconductors, and topological insulators. Now, our research question is whether we can drive and control orders of magnitude more charge carriers in metals enabling ultrafast switching with practically low-energy, picojoule-level pulses. Here, we demonstrate the interaction of light with nanometer-thick metallic layers, which leads to a generation of light field–controlled electric currents. We show that the implantation of metallic layers into a dielectric matrix leads to up to 40 times increase of the sensitivity in contrast to a bare dielectric, decreasing the intensity threshold for lightwave electronics.
Measurement and control of optical nonlinearities in dispersive dielectric multilayers
Dispersive dielectric multilayer mirrors, high-dispersion chirped mirrors in particular, are widely used in modern ultrafast optics to manipulate spectral chirps of ultrashort laser pulses. Dispersive mirrors are routinely designed for dispersion compensation in ultrafast lasers and are assumed to be linear optical components. In this work, we report the experimental characterization of an unexpectedly strong nonlinear response in these chirped mirrors. At modest peak intensities <2 TW/cm 2 —well below the known laser-induced damage threshold of these dielectric structures—we observed a strong reflectivity decrease, local heating, transient spectral modifications, and time-dependent absorption of the incident pulse. Through computational analysis, we found that the incident laser field can be enhanced by an order of magnitude in the dielectric layers of the structure. The field enhancement leads to a wavelength-dependent nonlinear absorption, that shows no signs of cumulative damage before catastrophic failure. The nonlinear absorption is not a simply two-photon process but instead is likely mediated by defects that facilitate two-photon absorption. To mitigate this issue, we designed and fabricated a dispersive multilayer design that strategically suppresses the field enhancement in the high-index layers, shifting the high-field regions to the larger-bandgap, low-index layers. This strategy significantly increases the maximum peak intensity that the mirror can sustain. However, our finding of an onset of nonlinear absorption even at ‘modest’ fluence and peak intensity has significant implications for numerous past published experimental works employing dispersive mirrors. Additionally, our results will guide future ultrafast experimental work and ultrafast laser design.
High-energy X-ray radiography with apodized petawatt laser beams
We have produced laser wakefield-accelerated electron beams with energies of 2 GeV in Target Area 1 of the ZEUS facility. These electron beams oscillate in the accelerating structure that is produced in the wake of an ultrashort laser pulse (25 fs). These ’betatron’ oscillations result in the emission of a collimated (4 mrad divergence) beam of high-energy X-ray/gamma photons (on the order of several hundred keV). In this work, we demonstrate the capabilities of the ZEUS laser system by showing that apodizing the laser beam in the near field allows for the production of high-quality betatron X-rays for radiography purposes. This demonstrates that a high-power, large-aperture laser beam could be split into multiple parts to drive betatron X-ray sources from multiple angles or temporal delays into a High Energy Density (HED) target to be probed, enabling pump-probe measurements at multiple temporal delays or tomography on a single shot.
Millisecond-long suppression of spectroscopic optical signals using laser filamentation
Ultrashort laser pulse filamentation in air can extend the delivery of focused laser energy to distances greatly exceeding the Rayleigh length. In this way, remote measurements can be conducted using many standard methods of analytical spectroscopy. The performance of spectroscopic techniques can be enhanced by temporal gating, which rejects the unwanted noise and background. In the present work, we investigate the thermal relaxation of air in the wake of single-filament plasmas using shadowgraphy. Here, we demonstrate that the transient change in refractive index associated with relaxation of the gas can be used to reject both continuous and time-varying spectroscopic signals, including emission from laser-produced plasmas. This method can augment temporal gating of simple optical detectors.
Probing electron-hole coherence in strongly driven 2D materials using high-harmonic generation
Under strong electromagnetic excitation, electron–hole (e-h) pairs may be generated in solids, which are subsequently driven to high energy and high momentum, producing high harmonics (HH) of the driving field. The HH efficiency depends on the degree of coherence between the driven electron and hole created by the laser field. Here, we disrupt this e-h coherence in an atomically thin semiconductor by photodoping via incoherent e-h pairs. We observe a strong, systematic harmonic order-dependent intensity reduction. This trend is explained by an exponential decay of the inter-band polarization, proportional to the sub-cycle excursion time of the e-h pair. Our study provides a platform to probe the importance of many-body effects, such as excitation density-dependent decoherence time for strongly driven electrons without the need of ultrashort laser pulses.
Reaction nanoscopy of ion emission from sub-wavelength propanediol droplets
Abstract Droplets provide unique opportunities for the investigation of laser-induced surface chemistry. Chemical reactions on the surface of charged droplets are ubiquitous in nature and can provide critical insight into more efficient processes for industrial chemical production. Here, we demonstrate the application of the reaction nanoscopy technique to strong-field ionized nanodroplets of propanediol (PDO). The technique’s sensitivity to the near-field around the droplet allows for the in-situ characterization of the average droplet size and charge. The use of ultrashort laser pulses enables control of the amount of surface charge by the laser intensity. Moreover, we demonstrate the surface chemical sensitivity of reaction nanoscopy by comparing droplets of the isomers 1,2-PDO and 1,3-PDO in their ion emission and fragmentation channels. Referencing the ion yields to gas-phase data, we find an enhanced production of methyl cations from droplets of the 1,2-PDO isomer. Density functional theory simulations support that this enhancement is due to the alignment of 1,2-PDO molecules on the surface. The results pave the way towards spatio-temporal observations of charge dynamics and surface reactions on droplets.
Spatiotemporal imaging and manipulation of surface plasmons
Abstract Surface plasmon polaritons (SPPs) are travelling surface waves that have shown promise for applications in nanophotonics as they provide a direct route toward photon-mediated electrical signal generation – a central paradigm for speeding up and scaling down photonic elements. SPP waves have also generated fundamental interest due to their high-field strength and sub-wavelength confinement, properties that have enabled the surface-enhanced Raman effect. Over the last decade, photoemission electron microscopy (PEEM) has emerged as a pioneering technique for imaging surface electric fields through ultrashort laser pulse mediated electron emission and has therefore become an indispensable tool for characterizing plasmonic phenomena at interfaces in a variety of materials. PEEM offers nanometer spatial resolution and femtosecond temporal resolution, allowing SPPs to be prepared, monitored, and manipulated on the nanometer-femtosecond scale. Through a brief review of recent reports, we aim to introduce PEEM-based SPP imaging and manipulation modalities and highlight their utility in the context of emerging nanoscale and quantum materials science advancements.
Laser-Induced Polarization for the Electron-Ion Collider
The use of an intense ultrashort laser pulse to induce electron polarization has been proposed in existing literature. Utilizing the Python programming language, a code has been developed to recreate the local constant crossed field approximation (LCFA) with the aim of determining values for transverse polarization given a nonzero initial polarization. It has been shown that over multiple laser shots, lower values of the quantum efficiency parameter are associated with higher transverse polarization output, yet require a greater number of shots to attain maximal polarization. Moreover, the quantum efficiency parameter has been rede fined as a function of intensity for Ti:sapphire laser necessary to induce polarization in the Electron-Ion Collider.
Fragmentation Dynamics of Fluorene Explored Using Ultrafast XUV-Vis Pump-Probe Spectroscopy
We report on the use of extreme ultraviolet (XUV, 30.3 nm) radiation from the Free-electron LASer in Hamburg (FLASH) and visible (Vis, 405 nm) photons from an optical laser to investigate the relaxation and fragmentation dynamics of fluorene ions. The ultrashort laser pulses allow to resolve the molecular processes occurring on the femtosecond timescales. Fluorene is a prototypical small polycyclic aromatic hydrocarbon (PAH). Through their infrared emission signature, PAHs have been shown to be ubiquitous in the universe, and they are assumed to play an important role in the chemistry of the interstellar medium. Our experiments track the ionization and dissociative ionization products of fluorene through time-of-flight mass spectrometry and velocity-map imaging. Multiple processes involved in the formation of each of the fragment ions are disentangled through analysis of the ion images. The relaxation lifetimes of the excited fluorene monocation and dication obtained through the fragment formation channels are reported to be in the range of a few tens of femtoseconds to a few picoseconds.
Toward nonthermal control of excited quantum materials: framework and investigations by ultrafast electron scattering and imaging
Quantum material systems upon applying ultrashort laser pulses provide a rich platform to access excited material phases and their transformations that are not entirely like their equilibrium counterparts. The addressability and potential controls of metastable or long-trapped out-of-equilibrium phases have motivated interests both for the purposes of understanding the nonequilibrium physics and advancing the quantum technologies. Thus far, the dynamical spectroscopic probes eminently focus on microscopic electronic and phonon responses. For characterizing the long-range dynamics, such as order parameter fields and fluctuation effects, the ultrafast scattering probes offer direct sensitivity. Bridging the connections between the microscopic dynamics and macroscopic responses is central toward establishing the nonequilibrium physics behind the light-induced phases. Here, we present a path toward such understanding by cross-examining the structure factors associated with different dynamical states obtained from ultrafast electron scattering, imaging, and modeling. We give the basic theoretical framework on describing the non-equilibrium scattering problems and briefly describe how such framework relates to the out-of-equilibrium phenomena. We give effective models outlining the emergences of nonthermal critical points, hidden phases, and non-equilibrium relaxational responses from vacuum-suspended rare-earth tritellurides, tantalum disulfides thin films, and vanadium dioxide nanocrystalline materials upon light excitations.
Search for High-Pressure Silicon Phases: Reaching the Extreme Conditions with High-Intensity Laser Irradiation
Controlling electronic and optical properties of semiconducting materials could substantially expand their functionality and enable new pathways for the formation of ‘smart’ materials for emerging innovative applications. An emerging new path for the synthesis of exotic silicon (Si) polymorphs is irradiation of bulk diamond-cubic Si by ultrashort laser pulses at relativistic intensity above 1019 W/cm2. Exotic polymorphs are formed due to interaction with MeV-energy electrons generated in laser-produced high-temperature plasma state. The unusual Si structures are found in the form of 5–10 nm nanoparticles confined deep in the bulk of 500-μm-thick Si samples. Raman spectroscopy, electron microscopy and X-ray diffraction studies provide an unequivocal evidence of exotic Si phase formation. A key advantage of such relativistic irradiation lies thereby in the fact that large quantities of such exotic Si is synthesised embedded within the bulk diamond-cubic Si and that further the formed Si polymorphs are stable at ambient temperature and pressure. They are thus available for further studies for electronic applications in selective band gap engineering.
Subnanosecond phase transition dynamics in laser-shocked iron
Iron is one of the most studied chemical elements due to its sociotechnological and planetary importance; hence, understanding its structural transition dynamics is of vital interest. By combining a short pulse optical laser and an ultrashort free electron laser pulse, we have observed the subnanosecond structural dynamics of iron from high-quality x-ray diffraction data measured at 50-ps intervals up to 2500 ps. We unequivocally identify a three-wave structure during the initial compression and a two-wave structure during the decaying shock, involving all of the known structural types of iron (α-, γ-, and ε-phase). In the final stage, negative lattice pressures are generated by the propagation of rarefaction waves, leading to the formation of expanded phases and the recovery of γ-phase. Our observations demonstrate the unique capability of measuring the atomistic evolution during the entire lattice compression and release processes at unprecedented time and strain rate.
Ghost-imaging-enhanced noninvasive spectral characterization of stochastic x-ray free-electron-laser pulses
Abstract High-intensity ultrashort X-ray free-electron laser (XFEL) pulses are revolutionizing the study of fundamental nonlinear x-ray matter interactions and coupled electronic and nuclear dynamics. To fully exploit the potential of this powerful tool for advanced x-ray spectroscopies, a noninvasive spectral characterization of incident stochastic XFEL pulses with high resolution is a key requirement. Here we present a methodology that combines high-acceptance angle-resolved photoelectron time-of-flight spectroscopy and ghost imaging to enhance the quality of spectral characterization of x-ray free-electron laser pulses. Implementation of this noninvasive high-resolution x-ray diagnostic can greatly benefit the ultrafast x-ray spectroscopy community by functioning as a transparent beamsplitter for applications such as transient absorption spectroscopy in averaging mode as well as covariance-based x-ray nonlinear spectroscopies in single-shot mode where the shot-to-shot fluctuations inherent to a self-amplified spontaneous emission (SASE) XFEL pulse are a powerful asset.