MeV Ultrafast Electron Diffraction Research Articles

Non-adiabatic dynamics of photoexcited cyclobutanone: Predicting structural measurements from trajectory surface hopping with XMS-CASPT2 simulations.

Over the years, theoretical calculations and scalable computer simulations have complemented ultrafast experiments, as they offer the advantage of overcoming experimental restrictions and having access to the whole dynamics. This synergy between theory and experiment promises to yield a deeper understanding of photochemical processes, offering valuable insights into the behavior of complex systems at the molecular level. However, the ability of theoretical models to predict ultrafast experimental outcomes has remained largely unexplored. In this work, we aim to predict the electron diffraction signals of an upcoming ultrafast photochemical experiment using high-level electronic structure calculations and non-adiabatic dynamics simulations. In particular, we perform trajectory surface hopping with extended multi-state complete active space with second order perturbation simulations for understanding the photodissociation of cyclobutanone (CB) upon excitation at 200nm. Spin-orbit couplings are considered for investigating the role of triplet states. Our simulations capture the bond cleavage after ultrafast relaxation from the 3s Rydberg state, leading to the formation of the previously observed primary photoproducts: CO + cyclopropane/propene (C3 products), ketene, and ethene (C2 products). The ratio of the C3:C2 products is found to be about 1:1. Within 700fs, the majority of trajectories transition to their electronic ground state, with a small fraction conserving the initial cyclobutanone ring structure. We found a minimal influence of triplet states during the early stages of the dynamics, with their significance increasing at later times. We simulate MeV-ultrafast electron diffraction (UED) patterns from our trajectory results, linking the observed features with specific photoproducts and the underlying structural dynamics. Our analysis reveals highly intense features in the UED signals corresponding to the photochemical processes of CB. These features offer valuable insights into the experimental monitoring of ring opening dynamics and the formation of C3 and C2 photoproducts.

Multi-objective Bayesian active learning for MeV-ultrafast electron diffraction

Ultrafast electron diffraction using MeV energy beams(MeV-UED) has enabled unprecedented scientific opportunities in the study of ultrafast structural dynamics in a variety of gas, liquid and solid state systems. Broad scientific applications usually pose different requirements for electron probe properties. Due to the complex, nonlinear and correlated nature of accelerator systems, electron beam property optimization is a time-taking process and often relies on extensive hand-tuning by experienced human operators. Algorithm based efficient online tuning strategies are highly desired. Here, we demonstrate multi-objective Bayesian active learning for speeding up online beam tuning at the SLAC MeV-UED facility. The multi-objective Bayesian optimization algorithm was used for efficiently searching the parameter space and mapping out the Pareto Fronts which give the trade-offs between key beam properties. Such scheme enables an unprecedented overview of the global behavior of the experimental system and takes a significantly smaller number of measurements compared with traditional methods such as a grid scan. This methodology can be applied in other experimental scenarios that require simultaneously optimizing multiple objectives by explorations in high dimensional, nonlinear and correlated systems.

MeV electron bunch compression and timing jitter suppression using a THz-driven resonator

THz-driven electron bunch compression and manipulation have significantly progressed and shown great potential in recent years. This paper presents a THz-driven resonator capable of bunch compression and timing jitter suppression with the inherent advantages such as field enhancement and laser synchronization. The resonance behavior of the resonator is studied to deduce the expression of the resonance frequency. Using the particle-tracking simulation, we study the performance of the THz-driven resonator in a MeV ultrafast electron diffraction beamline, and conclude that a bunch length (rms) of 15.40 ± 4.86 fs and timing jitter of 10.1 fs (rms) is achievable, which enables a temporal resolution below 25 fs in theory. Moreover, the THz-regime resonating field in the THz resonator allows for direct manipulation of each microbunch of a bunch train with picosecond bunch spacing. Particle-tracking simulation shows that simultaneous multi-bunch compression can be realized with a frequency-customized THz resonator. We expect this novel method to be applied in multi-bunch applications such as the coherent Smith–Purcell radiation.

Ultimate bunch length and emittance performance of an MeV ultrafast electron diffraction apparatus with a dc gun and a multicavity superconducting rf linac

We present the design of a high repetition rate MeV energy ultrafast electron diffraction instrument based on a DC photoelectron gun and an SRF linac with multiple independently controlled accelerating and bunching cavities. The design is based on the existing Cornell photoinjector, which can readily be applied to the presented findings. Using particle tracking simulations in conjunction with multiobjective genetic algorithm optimization, we explore the smallest bunch lengths, emittance, and probe spot sizes achievable. We present results for both stroboscopic conditions (with single electrons per pulse) and with $10^5$ electrons/bunch which may be suitable for single-shot diffraction images. In the stroboscopic case, the flexibility provided by the many-cavity bunching and acceleration allows for longitudinal phase space linearization without a higher harmonic field, providing sub-fs bunch lengths at the sample. Given low emittance photoemission conditions, these small bunch lengths can be maintained with probe transverse sizes at the single micron scale and below. In the case of $10^5$ electrons per pulse, we simulate state-of the art 5D brightness conditions: rms bunch lengths of 10 fs with 3 nm normalized emittances, while now permitting repetition rates as high as 1.3 GHz. Finally, to aid in the design of new SRF-based UED machines, we simulate the trade-off between the number of cavities used and achievable bunch length and emittance.

Photoinduced evolution of lattice orthorhombicity and conceivably enhanced ferromagnetism in LaMnO3 membranes

Ultrashort laser pulses have been utilized to dynamically drive phase transitions in correlated quantum materials. Of particular interest is whether phases not achievable in thermal equilibrium can be induced in complex oxides with intricately coupled lattice, electron and spin degrees of freedom. Here, we tracked atomic motions in LaMnO3 following photoexcitation with MeV ultrafast electron diffraction (MeV-UED) technique. We found that the light excited state exhibits numerous signatures different from thermal equilibrium ones, including nearly conserved Bragg intensities, strongly suppressed La cation and oxygen anion displacements, and the long-range lattice orthorhombicity evolution. Furthermore, using first-principles calculations, we predict that the ferromagnetic ordering and conductivity are both enhanced upon laser excitation due to the reduction of the lattice orthorhombicity. This work benefits from recent advance in fabrication of membrane films with high epitaxial quality and in MeV-UED with large momentum space access and high temporal resolution.

Development of a 1.4-cell RF photocathode gun for single-shot MeV ultrafast electron diffraction devices with femtosecond resolution

The MeV ultrafast electron diffraction (UED) has proven to be a powerful tool for exploring the ultrafast process at the atomic level with femtosecond resolution. However, MeV UED facilities are struggling to achieve sub-100 fs temporal resolution at pC level charges due to the rapid and severe bunch lengthening near the cathode region. Both analytical work and simulation show that the bunch lengthening near the cathode originates from both the strong space charge effect (SCE) within the sub-relativistic electron beam and the bunch tail trailing due to the mirror charge effect (MCE). In this paper, we report the development of a new 1.4-cell RF gun that significantly increases the extraction field at the cathode to suppress both the SCE and the MCE. Compared to the conventional 1.6-cell RF gun, the new 1.4-cell RF gun is more suitable to produce an electron beam with a shorter bunch length and less distorted longitudinal phase space. The shorter bunch length leads directly to a temporal resolution improvement in UEDs. Meanwhile, the beam longitudinal phase space with better linearity ensures a smaller compressed bunch length when the bunch compression schemes are applied.

How to realize an ultrafast electron diffraction experiment with a terahertz pump: A theoretical study

To integrate a terahertz pump into an ultrafast electron diffraction (UED) experiment has attracted much attention due to its potential to initiate and detect the structural dynamics both directly. However, the deflection of the electron probe by the electromagnetic field of the terahertz pump alters the incident angle of the electron probe on the sample, impeding it from recording structural information afterwards. In this article, we studied this issue by a theoretical simulation of the terahertz-induced deflection effect on the electron probe, and came up with several possible schemes to reduce such effect. As a result, a terahertz-pump-electron-probe UED experiment with a temporal resolution comparable to the terahertz period is realized. We also found that MeV UED was more suitable for such terahertz pump experiment.

Photoinduced anisotropic lattice dynamic response and domain formation in thermoelectric SnSe

Identifying and understanding the mechanisms behind strong phonon–phonon scattering in condensed matter systems is critical to maximizing the efficiency of thermoelectric devices. To date, the leading method to address this has been to meticulously survey the full phonon dispersion of the material in order to isolate modes with anomalously large linewidth and temperature-dependence. Here we combine quantitative MeV ultrafast electron diffraction (UED) analysis with Monte Carlo based dynamic diffraction simulation and first-principles calculations to directly unveil the soft, anharmonic lattice distortions of model thermoelectric material SnSe. A small single-crystal sample is photoexcited with ultrafast optical pulses and the soft, anharmonic lattice distortions are isolated using MeV-UED as those associated with long relaxation time and large displacements. We reveal that these modes have interlayer shear strain character, induced mainly by c-axis atomic displacements, resulting in domain formation in the transient state. These findings provide an innovative approach to identify mechanisms for ultralow and anisotropic thermal conductivity and a promising route to optimizing thermoelectric devices.

Fast attenuation of high-frequency acoustic waves in bicontinuous nanoporous gold

We studied the formation and attenuation of GHz elastic waves in free-standing nanoporous gold films by MeV ultrafast electron diffraction and finite element simulations. By tracing the evolution of the high frequency acoustic waves in time domain, we found that the bicontinuous nanoporous structure in nanoporous gold films results in three-dimensionally acoustic response with low coherence, leading to fast attenuation of the elastic waves in comparison with solid gold films. The morphologically dominated dynamics indicates the nanoporosity plays an important role in the high-frequency acoustic energy relaxation, which shines a light on the applications of dealloyed nanoporous materials in nanodevices and sensors as GHz and THz acoustic filters and dampers.

Noninvasive time-sorting in radio frequency-compressed ultrafast electron diffraction.

We demonstrate a noninvasive time-sorting method for ultrafast electron diffraction (UED) experiments with radio frequency (rf)-compressed electron beams. We show that electron beam energy and arrival time at the sample after the rf compression are strongly correlated, such that the arrival time jitter may be corrected through the measurement of the beam energy. The method requires minimal change to the infrastructure of most of the UED machines and is applicable to both keV and MeV UED. In our experiment with ∼3 MeV beam, the timing jitter after the rf compression is corrected with a 35-fs root mean square (rms) accuracy, limited by the energy stability. For keV UED with a high energy stability, sub-10 fs accuracy in time-sorting should be readily achievable. This time-sorting technique allows us to retrieve the 2.5 THz oscillation related to coherent A1g phonon in the laser-excited Bismuth film and extends the temporal resolution of UED to a regime far beyond the 100–200 fs rms jitter limitation.

Simulation study of first and second harmonic photocathode bimodal gun

The increasing demands for electron beams with high quality and low timing jitter for accelerator-based applications such as ultrafast electron microscopy (UEM) and ultrafast electron diffraction (UED) have stimulated active efforts to develop suitable injectors for these accelerators. One promising direction in this regard is using of a bimodal rf gun operating in fundamental mode and a phase-locked harmonically-related higher mode. Work reported in this paper is on analysis and design of a bimodal rf gun operating in S-band as the fundamental and C-band as the second-harmonic modes. The rf design for such an rf gun includes the new design like directional coupler and rectangular mode launcher, which presented good transmission, low reflective cross-talk, and allowed multiple iterations of the modification. Compared to the fundamental mode, the new design achieved reduction in rf emittance and energy spread for MeV UEM initial distribution, and reduction in slope of flight time as function of injection phase for MeV UED applications.

Dogleg design for an MeV Ultra-fast electron Diffraction beamline for the hybrid Photo-emitted RF GUN at Ariel University

A secondary parallel beamline is proposed for the construction of a Mega electron Volt Ultrafast electron Diffraction (Mev UED) facility, based on the novel hybrid 6 MeV RF-GUN in the Schlesinger center for compact accelerators in Ariel University. The Addition of a second beamline requires kicking the beam sideways and back, using a dogleg section. In order to change the trajectory of the beam, while preserving as much as possible the quality of the relativistic electron beam, requires a careful design and simulation process. Start-to-end comprehensive simulations of the dogleg design were performed using GPT (General Particle Tracer) software followed by analysis and optimization for the simulations in order to achieve optimal beam parameters in the second beamline. This paper presents the results of the dogleg design and optimization.

Photoinduced Dirac semimetal in ZrTe5

Novel phases of matter with unique properties that emerge from quantum and topological protection present an important thrust of modern research. Of particular interest is to engineer these phases on demand using ultrafast external stimuli, such as photoexcitation, which offers prospects of their integration into future devices compatible with optical communication and information technology. Here, we use MeV Ultrafast Electron Diffraction (UED) to show how a transient three-dimensional (3D) Dirac semimetal state can be induced by a femtosecond laser pulse in a topological insulator ZrTe5. We observe marked changes in Bragg diffraction, which are characteristic of bond distortions in the photoinduced state. Using the atomic positions refined from the UED, we perform density functional theory (DFT) analysis of the electronic band structure. Our results reveal that the equilibrium state of ZrTe5 is a topological insulator with a small band gap of ~ 25 meV, consistent with angle-resolved photoemission (ARPES) experiments. However, the gap is closed in the presence of strong spin-orbit coupling (SOC) in the photoinduced transient state, where massless Dirac fermions emerge in the chiral band structure. The time scale of the relaxation dynamics to the transient Dirac semimetal state is remarkably long, τ ~ 160 ps, which is two orders of magnitude longer than the conventional phonon-driven structural relaxation. The long relaxation is consistent with the vanishing density of states in Dirac spectrum and slow spin-repolarization of the SOC-controlled band structure accompanying the emergence of Dirac fermions.

Ultrafast formation of a transient two-dimensional diamondlike structure in twisted bilayer graphene

Due to the absence of matching carbon atoms at honeycomb centers with carbon atoms in adjacent graphene sheets, theorists predicted that a sliding process is needed to form AA, AB, or ABC stacking when directly converting graphite into sp3 bonded diamond. Here, using twisted bilayer graphene, which naturally provides AA and AB stacking configurations, we report the ultrafast formation of a transient 2D diamond-like structure (which is not observed in aligned graphene) under femtosecond laser irradiation. This photo-induced phase transition is evidenced by the appearance of new bond lengths of 1.94A and 3.14A in the time-dependent differential pair distribution function using MeV ultrafast electron diffraction. Molecular dynamics and first principles calculation indicate that sp3 bonds nucleate at AA and AB stacked areas in moire pattern. This work sheds light on the direct graphite-to-diamond transformation mechanism, which has not been fully understood for more than 60 years.

Breaking 50 Femtosecond Resolution Barrier in MeV Ultrafast Electron Diffraction with a Double Bend Achromat Compressor.

We propose and demonstrate a novel scheme to produce ultrashort and ultrastable MeV electron beam. In this scheme, the electron beam produced in a photocathode radio frequency (rf) gun first expands under its own Coulomb force with which a positive energy chirp is imprinted in the beam longitudinal phase space. The beam is then sent through a double bend achromat with positive longitudinal dispersion where electrons at the bunch tail with lower energies follow shorter paths and thus catch up with the bunch head, leading to longitudinal bunch compression. We show that with optimized parameter sets, the whole beam path from the electron source to the compression point can be made isochronous such that the time of flight for the electron beam is immune to the fluctuations of rf amplitude. With a laser-driven THz deflector, the bunch length and arrival time jitter for a 20fC beam after bunch compression are measured to be about 29fs (FWHM) and 22fs (FWHM), respectively. Such an ultrashort and ultrastable electron beam allows us to achieve 50 femtosecond (FWHM) resolution in MeV ultrafast electron diffraction where lattice oscillation at 2.6THz corresponding to Bismuth A_{1g} mode is clearly observed without correcting both the short-term timing jitter and long-term timing drift. Furthermore, oscillating weak diffuse scattering signal related to phonon coupling and decay is also clearly resolved thanks to the improved temporal resolution and increased electron flux. We expect that this technique will have a strong impact in emerging ultrashort electron beam based facilities and applications.

Towards jitter-free ultrafast electron diffraction technology

Stroboscopic visualization of nuclear or electron dynamics in atoms, molecules or solids requires ultrafast pump and probe pulses and a close to perfect synchronization between the two. We have developed a 3 MeV ultrafast electron diffraction (UED) probe technology that nominally reduces the electron bunch duration and the arrival time jitter to the subfemtosecond level. This simple configuration uses a radiofrequency photogun and a 90° achromatic bend and is designed to provide effectively jitter-free conditions. Terahertz streaking measurements reveal an electron bunch duration of 25 fs, even for a charge as high as 0.6 pC, and an arrival time jitter of 7.8 fs, the latter limited by only the measurement accuracy. From pump–probe measurements of photoexcited bismuth films, the instrument response function was determined to be 31 fs. This pioneering jitter-free technique paves the way towards UED of attosecond phenomena in atomic, molecular and solid-state dynamics. An ultrafast electron diffraction facility with an overall temporal resolution of 31 fs root mean square is developed. Even for a charge as high as 0.6 pC, the electron bunch duration and timing jitter are 25 fs and less than 10 fs, respectively.

Improvement of 6D brightness by a 1.4-cell photocathode RF gun for MeV Ultrafast electron diffraction

Recent research indicates that ultrafast electron diffraction and microscopy (UED/M) have unprecedented potential in probing ultrafast dynamic processes, especially in organic and biological materials. However, reaching the required brightness while maintaining high spatiotemporal resolution requires new design of electron source. In order to produce ultrashort electron beam with extreme high brightness, a 1.4-cell RF gun is being developed to reach higher acceleration gradient near the photocathode and thus suppress the space charge effect in the low energy region. Simulation of the 1.4-cell RF photocathode gun shows considerable improvement in bunch length, emittance and energy spread, which all lead to better temporal and spatial resolution comparing to traditional 1.6-cell RF photocathode gun. The results demonstrate the feasibility of sub-ps temporal resolution with normalized emittance less than 0.1 πmm·mrad while maintaining 1 pC electron pulse.

Imaging the ring opening reaction of 1,3-cyclohexadiene with MeV ultrafast electron diffraction

We resolve the structural dynamics of the ultrafast photoinduced ring opening reaction of 1,3-cyclohexadiene in space and time employing megaelectronvolt gas phase ultrafast electron diffraction. We, furthermore, observe coherent large amplitude motions of the photoproduct.

Terahertz Streaking of Few-Femtosecond Relativistic Electron Beams

Streaking of photoelectrons with optical lasers has been widely used for temporal characterization of attosecond extreme ultraviolet pulses. Recently, this technique has been adapted to characterize femtosecond x-ray pulses in free-electron lasers with the streaking imprinted by farinfrared and Terahertz (THz) pulses. Here, we report successful implementation of THz streaking for time-stamping of an ultrashort relativistic electron beam of which the energy is several orders of magnitude higher than photoelectrons. Such ability is especially important for MeV ultrafast electron diffraction (UED) applications where electron beams with a few femtosecond pulse width may be obtained with longitudinal compression while the arrival time may fluctuate at a much larger time scale. Using this laser-driven THz streaking technique, the arrival time of an ultrashort electron beam with 6 fs (rms) pulse width has been determined with 1.5 fs (rms) accuracy. Furthermore, we have proposed and demonstrated a non-invasive method for correction of the timing jitter with femtosecond accuracy through measurement of the compressed beam energy, which may allow one to advance UED towards sub-10 fs frontier far beyond the ~100 fs (rms) jitter.

Stacking order dynamics in the quasi-two-dimensional dichalcogenide 1T-TaS2 probed with MeV ultrafast electron diffraction.

Transitions between different charge density wave (CDW) states in quasi-two-dimensional materials may be accompanied also by changes in the inter-layer stacking of the CDW. Using MeV ultrafast electron diffraction, the out-of-plane stacking order dynamics in the quasi-two-dimensional dichalcogenide 1T-TaS2 is investigated for the first time. From the intensity of the CDW satellites aligned around the commensurate l = 1/6 characteristic stacking order, it is found out that this phase disappears with a 0.3 ps time constant. Simultaneously, in the same experiment, the emergence of the incommensurate phase, with a slightly slower 2.0 ps time constant, is determined from the intensity of the CDW satellites aligned around the incommensurate l = 1/3 characteristic stacking order. These results might be of relevance in understanding the metallic character of the laser-induced metastable “hidden” state recently discovered in this compound.