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At least 271 records · Page 15

Probing coherence in nanoscale energy transport with high spatial-temporal resolution. Final Technical Report for DOE Award Number DE-SC0019244

The overarching goal of this project is to understand how the phase coherence of phonons and the interaction of phonons with other microscopic degrees of freedom in nanomaterials, such as 2D materials, can affect the energy transport properties and eventually lead to control of energy transport by manipulating phonon interference and phonon scatterings. On the computational side, we are developing and applying first-principles methods to study emerging phonon properties in nanomaterials, including coherent phonons, resonant bonding and gate-tunable phonon-electron scatterings, which hold the promise of enabling significant tunability of energy transport processes with external fields for a wide range of applications. On the experimental side, we are developing ultrafast transient grating spectroscopy and scanning ultrafast electron microscopy (SUEM) to directly probe the coherent phonon transport and phonon-electron interaction processes in nanomaterials with high combined spatial-temporal resolutions. This program will not only provide new insights into the microscopic transport and interaction processes of fundamental energy carriers, but also open new venue towards energy-relevant applications such as thermal switches and coherent energy harvesters.

42 ENGINEERING↗

Spectrotemporal Shaping of Attosecond X-Ray Pulses with a Fresh-Slice Free-Electron Laser

We propose a scheme allowing coherent shaping, i.e., controlling both the amplitude and phase, of attosecond x-ray pulses at free-electron lasers. Here, we show that by seeding an FEL with a short coherent seed that overfills the amplification bandwidth, one can shape the Wigner function of the pulse by controlling the undulator taper profile. The examples of controllable pulse pairs and trains, as well as isolated spectrotemporally shaped pulses with very broad bandwidths are examined in detail. Existing attosecond XFELs can achieve these experimental conditions in a two-stage cascade, in which the seed is generated by a short current spike in an electron bunch and shaped in an unspoiled region within the same bunch. We experimentally demonstrate the production and control of phase-stable pulse trains using this method at the Linac Coherent Light Source II.

47 OTHER INSTRUMENTATION↗

Light-wave control of correlated materials using quantum magnetism during time-periodic modulation of coherent transport

Light–wave quantum electronics utilizes the oscillating carrier wave to control electronic properties with intense laser pulses. Without direct light–spin interactions, however, magnetic properties can only be indirectly affected by the light electric field, mostly at later times. A grand challenge is how to establish a universal principle for quantum control of charge and spin fluctuations, which can allow for faster-than-THz clock rates. Using quantum kinetic equations for the density matrix describing non–equilibrium states of Hubbard quasiparticles, here we show that time–periodic modulation of electronic hopping during few cycles of carrier–wave oscillations can dynamically steer an antiferromagnetic insulating state into a metalic state with transient magnetization. While nonlinearities associated with quasi-stationary Floquet states have been achieved before, magneto–electronics based on quasiparticle acceleration by time–periodic multi–cycle fields and quantum femtosecond/attosecond magnetism via strongly–coupled charge–spin quantum excitations represents an alternative way of controlling magnetic moments in sync with quantum transport.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Nanometer-scale prebunched electron beams generated from all-optical plasma-based acceleration

High-quality and prebunched electron beams can produce coherent x-rays with high intensity and narrow bandwidth, which are essential for modern light sources. An all-optical scheme based on plasma-based acceleration for producing bright electron beams that are prebunched on the nanometer scale is proposed. By using a density modulation created by two low intensity counterpropagating lasers, the phase velocity of the plasma wake excited by an intense driver laser in a uniform plasma can be modulated at a frequency twice that of the colliding lasers, thus turning the injection on and off. The injected electrons are microbunched at the Doppler-shifted modulated wavelength, corresponding to the phase velocity of the gradually expanding wakefield. It is demonstrated that by controlling the properties of the drive and colliding lasers, beams with exotic prebunched structures can be produced, which may have critical applications in ultrafast high power x-rays. This extremely compact, all-optical scheme for producing ultrabright prebunched electron beams may therefore enable novel applications for ultrafast x-ray users and arouse general interest in various fields.

Beam injection, extraction & transport↗

Correlation-driven attosecond photoemission delay in the plasmonic excitation of C60 fullerene

Extreme light confinement in plasmonic nanosystems enables novel applications in photonics, sensor technology, energy harvesting, biology, and quantum information processing. Fullerenes represent an extreme case for nanoplasmonics: they are sub-nanometer carbon- based molecules showing high-energy and ultrabroad plasmon resonances, however the fundamental mechanisms driving the plasmonic response and the corresponding collective electron dynamics are still elusive. Here, we uncover the dominant role of electron correlations in the dynamics of the giant plasmon resonance (GPR) of the sub-nanometer system C60 by employing attosecond photoemission chronoscopy. We find a characteristic photoemission delay of up to about 300 attoseconds that is purely induced by coherent large-scale electron correlations in the plasmonic potential. These results provide novel insights into the nature of the plasmon resonances in sub-nanometer systems and open new perspectives for advancing nanoplasmonic applications.

Biswas, Shubhadeep [SLAC National Accelerator Labo↗

Towards Mitigating Electron Beam-Induced Damage in MOFs Using Low Dose Electron Microscopy for In-Situ Room-Temperature Measurements

Metal-Organic Frameworks (MOFs) have emerged as a versatile class of materials with applications in gas storage and separation, catalysis, and drug delivery [1]. Understanding their damage mechanisms in under various environmental conditions is crucial for optimizing performance and stability [2]. This study employs a combination of Length Structural Coherence (LSC) analysis in electron scattering and Electron Energy Loss Spectroscopy (EELS) to elucidate the damage mechanisms in two representative MOFs. MIL101(Fe), and MIL101(Cr). Here, the primary objective is to reveal structural and chemical changes that occur under electron beam irradiation in Scanning Transmission Electron Microscopy (STEM), both in the pristine state and during in-situ CO and CO 2 adsorption. By combining LSC in Radial Distribution Function (RDF) analysis with EELS, comprehensive insights into the nanoscale alterations are obtained and correlated to the electron dose rate.

dos Santos, Gabriel T. [Northwestern University, E↗

Stroboscopic ultrafast imaging using RF strip-lines in a commercial transmission electron microscope

The development of ultrafast electron microscopy (UEM), specifically stroboscopic imaging, has brought the study of structural dynamics to a new level by overcoming the spatial limitations of ultrafast spectroscopy and the temporal restrictions of traditional TEM simultaneously. Combining the concepts governing both techniques has enabled direct visualization of dynamics with spatiotemporal resolutions in the picosecond-nanometer regime. Here, in this study, we push the limits of imaging using a pulsed electron beam via RF induced transverse deflection based on the newly developed 200 keV frequency-tunable strip-line pulser. We demonstrate 0.2 nm spatial resolution at high magnifications and elucidation of Lorentz imaging using the phase-microscopy method. We also present beam coherence measurements and expand our study using the breathing modes of a silicon interdigitated comb under RF excitation which achieves improved temporal synchronization between the electron pulse-train and electric field. A new RF holder has also been developed with impedance matching to the RF signal to minimize transmission power loss to samples and its performance is compared with a conventional sample holder.

47 OTHER INSTRUMENTATION↗

High-resolution analogue of time-domain phonon spectroscopy in the transmission electron microscope

Femtosecond photoexcitation of semiconducting materials leads to the generation of coherent acoustic phonons (CAPs), the behaviours of which are linked to intrinsic and engineered electronic, optical and structural properties. While often studied with pump-probe spectroscopic techniques, the influence of nanoscale structure and morphology on CAP dynamics can be challenging to resolve with these all-optical methods. Here, we used ultrafast electron microscopy (UEM) to resolve variations in CAP dynamics caused by differences in the degree of crystallinity in as-prepared and annealed GaAs lamellae. Following in situ femtosecond photoexcitation, we directly imaged the generation and propagation dynamics of hypersonic CAPs in a mostly amorphous and, following an in situ photothermal anneal, a mostly crystalline lamella. Subtle differences in both the initial hypersonic velocities and the asymptotic relaxation behaviours were resolved via construction of space-time contour plots from phonon wavefronts. Comparison to bulk sound velocities in crystalline and amorphous GaAs reveals the influence of the mixed amorphous-crystalline morphology on CAP dispersion behaviours. Further, an increase in the asymptotic velocity following annealing establishes the sensitivity of quantitative UEM imaging to both structural and compositional variations through differences in bonding and elasticity. Lastly, implications of extending the methods and results reported here to elucidating correlated electronic, optical and structural behaviours in semiconducting materials are discussed.

42 ENGINEERING↗

Single-Shot Readout and Weak Measurement of a Tin-Vacancy Qubit in Diamond

The negatively charged tin-vacancy center in diamond (SnV − ) is an emerging platform for building the next generation of long-distance quantum networks. This is due to the SnV − ’s favorable optical and spin properties including bright emission, insensitivity to electronic noise, and long spin coherence times at temperatures above 1 K. Here, we demonstrate measurement of a single SnV − electronic spin with a single-shot readout fidelity of 87.4%, which can be further improved to 98.5% by conditioning on multiple readouts. In the process, we develop understanding of the relationship between strain, magnetic field, spin readout, and microwave spin control. We show that high-fidelity readout is compatible with rapid microwave spin control, demonstrating a favorable parameter regime for use of the SnV − center as a high-quality spin-photon interface. Finally, we use weak quantum measurement to study measurement-induced dephasing; this illuminates the fundamental interplay between measurement and decoherence in quantum mechanics, and provides a universal method to characterize the efficiency of color-center spin readout. Taken together, these results overcome an important hurdle in the development of the SnV − -based quantum technologies and, in the process, develop techniques and understanding broadly applicable to the study of solid-state quantum emitters.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Online and Offline Data Quality Monitoring for the Mu2e Calorimeter

This thesis presents the design, implementation, and validation of a calorimeter Data Quality Monitoring (DQM) toolchain for the Mu2e experiment at Fermilab. Mu2e searches for charged lepton flavor violation via coherent muon-to-electron conversion in the field of an aluminum nucleus, $\mu^- Al \rightarrow e^-Al$, a process whose observation would constitute clear evidence of physics beyond the Standard Model. Achieving target sensitivity requires stringent control of detector performance and data integrity during acquisition, as subtle issues in readout configuration, data formatting, or electronics behavior can compromise reconstruction and bias downstream analyzes. To address these challenges, this work develops a multi-layer DQM approach spanning both raw data validation and reconstructed digi-level diagnostics. At the low level, a fragment analysis component performs word- and bit-field decoding of calorimeter readout blocks, enabling sanity checks of the expected structure and producing detailed error and integrity statistics useful for commissioning and troubleshooting. At the digi level, the CaloDigiDQM analyzer is implemented within the art framework and transforms each CaloDigiCollection into a structured hierarchy of ROOT histograms designed for fast drill-down diagnostics. The module generates coherent monitoring views at global, disk, board, and channel granularity, including occupancy, waveform-derived features (baseline, RMS, peak amplitude and position), and left-right sensor consistency metrics. Detector-aware channel-to-electronics mapping is performed through the conditions system (CaloDAQMap), ensuring that diagnostics remain aligned with hardware identifiers used in operations. For end-to-end testing without reliance on live DAQ data, a synthetic CaloDigi producer is developed to generate realistic waveforms with controlled noise and pulse shapes. The resulting system supports both offline ROOT-file production and online operation, including optional histogram streaming through otsdaq via ots::HistoSender. This toolchain provides a practical and scalable foundation for calorimeter commissioning and stable data collection, enabling early detection of anomalies and reducing operational risk for Mu2e.

Vakulenko, Mark [Drew U.] (ORCID:0009000276197818)↗

Imaging coherent phonons and precursor dynamics in LaFeAsO with 4D ultrafast electron microscopy

In this work, we used 4D ultrafast electron microscopy (UEM) to directly image femtosecond photoinduced structural dynamics in single-crystal LaFeAsO at initial temperatures of 300 and 100 K, above and below the known structural and magnetic phase-transition temperatures, respectively. With nanometer-picosecond resolution, we resolved an initial (precursor) sigmoidlike response arising from photothermal expansion and lattice reorientation that precedes the onset of propagating coherent acoustic phonons (CAPs). In the specific regions probed, the precursor response at 100 K is shorter than at 300 K ($t$ 0.5;100 K = 11.3ps vs $t$ 0.5;300 K = 17.8ps), and the CAP oscillation frequency is lowered with cooling (ƒ CAP;100 K = 12 GHz vs ƒ CAP;300 K = 21 GHz), correlated to known lattice softening due to the structural phase change. The transient CAP behaviors at 300 K are dispersive, displaying an exponentially decaying phase velocity over the first nanosecond. Further, the CAP symmetry at 300 K matches a first-order antisymmetric shear mode (A 1 ), while at 100 K it is best matched by a mostly nondispersive zero-order symmetric mode (S 0 ). These findings illustrate the sensitivity of UEM imaging to spatially heterogeneous dynamics in the Fe-pnictide materials and more broadly in other quantum materials.

36 MATERIALS SCIENCE↗

Quantum coherent energy transport in the Fenna–Matthews–Olson complex at low temperature

In the primary step of natural light harvesting, the solar photon energy is captured in a photoexcited electron–hole pair, or an exciton, in chlorophyll. Its conversion to chemical potential occurs in the special pair reaction center, which is reached by downhill ultrafast excited-state energy transport through a network of chromophores. Being inherently quantum, transport could in principle occur via a matter wave, with vast implications for efficiency. How long a matter wave remains coherent is determined by the intensity by which the exciton is disturbed by the noisy biological environment. The stronger this is, the stronger the electronic coupling between chromophores must be to overcome the fluctuations and phase shifts. The current consensus is that under physiological conditions, quantum coherence vanishes on the 10-fs time scale, rendering it irrelevant for the observed picosecond transfer. Yet, at low-enough temperature, quantum coherence should in principle be present. Here, we reveal the onset of longer-lived electronic coherence at extremely low temperatures of ∼20 K. Using two-dimensional electronic spectroscopy, we determine the exciton coherence times in the Fenna–Matthew–Olson complex over an extensive temperature range. At 20 K, coherence persists out to 200 fs (close to the antenna) and marginally up to 500 fs at the reaction center. It decays markedly faster with modest increases in temperature to become irrelevant above 150 K. At low temperature, the fragile electronic coherence can be separated from the robust vibrational coherence, using a rigorous theoretical analysis. We believe that by this generic principle, light harvesting becomes robust against otherwise fragile quantum effects.

59 BASIC BIOLOGICAL SCIENCES↗

A numerically exact description of ultrafast vibrational decoherence in vibration-coupled electron transfer

Broadband pump–probe spectroscopy has been widely used to measure vibrational decoherence associated with the reaction coordinate in photoinduced ultrafast vibration-coupled electron transfer (VCET) reactions. These experiments provide insight into the interplay of intramolecular coordinates along the reaction coordinate. However, a general theoretical foundation for analyzing, and even for explaining rigorously, these data is lacking. In this work, we study vibrational decoherence in a model VCET reaction using the nearly exact time-dependent density matrix renormalization group simulation method. We explore how analyzing the density matrix with quantum information measures can help elucidate the evolution of vibrational coherence in simulations of dynamics. We examine how vibrational coherence is affected by electron transfer on the timescale of approximately 100 femtoseconds. Our results suggest that electron transfer, in the nonadiabatic model, changes the vibrational equilibrium position abruptly—an example of a “quantum quench” event. This explains the concomitant vibrational decoherence. We find that abrupt vibrational decoherence can be mitigated by wavepacket motion occurring on the timescale of the electron transfer.

Science & Technology - Other Topics↗

Impact of Arsenic- and Indium-Terminated InGaAs Stressors on Carrier Confinement, Strain, Defects, and Transport Properties of Tensile-Strained Ge

Device-quality tensile-strained Ge (ε-Ge) grown on a large bandgap semiconductor with superior electrical and optical carrier confinement is essential for group-IV-based optoelectronics. Properties of ε-Ge active layers synthesized on In 0.24 Ga 0.76 As buffers with two different surface terminations─arsenic-rich and indium-rich─were experimentally demonstrated, highlighting the factors not considered in theoretical calculations. High-resolution X-ray diffraction and Raman spectroscopy analyses of these ε-Ge/In 0.24 Ga 0.76 As heterostructures confirmed the fully strained (1.6%) and partially relaxed (0.82%) nature of the ε-Ge bonded with arsenic-terminated (Ge As-terminated ) and indium-terminated (Ge In-terminated ) In 0.24 Ga 0.76 As stressors, respectively. High-resolution cross-sectional transmission electron microscopy showed a coherent, sharp, and fully strained ε-Ge/In 0.24 Ga 0.76 As heterointerface in the Ge As-terminated heterostructure, whereas microtwin defects were present in the Ge In-terminated heterostructure. These heterostructures were further characterized by evaluating the minority carrier lifetimes, high for Ge As-terminated (525 ns) and low for Ge In-terminated (69 ns), using the photoconductive decay technique. Moreover, band alignment was constructed using X-ray photoelectron spectroscopy, where the Ge As-terminated heterostructure revealed that both holes and electrons were confined within the ε-Ge active layer as a type-I band alignment with ΔE V, As-terminated = 0.22 eV and ΔE C,As-terminated = 0.38 eV. On the other hand, the Ge In-terminated heterostructure exhibited a type-II band alignment with ΔE V,In-terminated = – 0.02 eV and ΔE C,In-terminated = 0.53 eV. Furthermore, the magnetotransport properties revealed high mobility (321 cm 2 /(V s)) with single-electron transport in Ge As-terminated heterostructure and low mobility (3.34 cm 2 /(V s)) with multihole transport in the Ge In-terminated heterostructure. Therefore, preferring the ε-Ge on the arsenic-rich surface of In 0.24 Ga 0.76 As stressor over the indium-rich surface during material synthesis offers device-quality materials with high carrier lifetime and superior carrier confinement, which can provide an opportunity to fabricate efficient group-IV-based optoelectronic devices.

36 MATERIALS SCIENCE↗

Many-body interference in kagome crystals

When electrons in metals act collectively, they enable emergent phenomena and electronic functionalities that transcend the behaviour of individual particles. Coherent collective charge motion has so far been observed primarily in superconductors, in which it arises with the formation of Cooper pairs. Here we report experimental evidence for coherent charge transport in the normal state of the kagome metal CsV 3 Sb 5 , indicative of a distinct collective electronic state. The signature is a set of magnetoresistance oscillations in mesoscopic crystalline pillars under in-plane magnetic fields, with a periodicity determined by the number of magnetic flux quanta h/e threading between adjacent kagome layers—effectively forming an interlayer Aharonov–Bohm interferometer. The cooperative nature of this phenomenon is evidenced by a non-analytic angular dependence characterized by abrupt transitions between discrete oscillation frequencies and its persistence over length scales that exceed the single-particle mean free path. Notably, the oscillation amplitude matches other anomalous electronic responses reported in CsV 3 Sb 5 , pointing to an underlying mechanism that establishes intrinsic coherence. These findings shed new light on the debated nature of correlated order in kagome metals and establish CsV 3 Sb 5 as a platform for realizing long-range coherent charge transport in the absence of superconductivity—opening new directions for coherence in correlated electron systems beyond conventional models.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Optical control of ultrafast structural dynamics in a fluorescent protein

The photoisomerization reaction of a fluorescent protein chromophore occurs on the ultrafast timescale. The structural dynamics that result from femtosecond optical excitation have contributions from vibrational and electronic processes and from reaction dynamics that involve the crossing through a conical intersection. The creation and progression of the ultrafast structural dynamics strongly depends on optical and molecular parameters. When using X-ray crystallography as a probe of ultrafast dynamics, the origin of the observed nuclear motions is not known. Now, high-resolution pump–probe X-ray crystallography reveals complex sub-ångström, ultrafast motions and hydrogen-bonding rearrangements in the active site of a fluorescent protein. However, we demonstrate that the measured motions are not part of the photoisomerization reaction but instead arise from impulsively driven coherent vibrational processes in the electronic ground state. A coherent-control experiment using a two-colour and two-pulse optical excitation strongly amplifies the X-ray crystallographic difference density, while it fully depletes the photoisomerization process. A coherent control mechanism was tested and confirmed the wave packets assignment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Laser-Induced Enhancement of Acoustic Mode Quality Factor Revealed by Correlated Single-Particle Optical and Electron Microscopy

Acoustic modes in plasmonic nanostructures provide fundamental insights into their optomechanical behavior at the nanoscale, enabling emerging applications in plasmon-enhanced optomechanics, ultrasensitive sensing, and nanoscale energy transduction. Here we explore the modulation of acoustic phonon dynamics in lithographically fabricated gold nanodisks via laser-induced photothermal annealing. Using a correlated approach that utilizes both single-particle transient extinction spectroscopy and advanced electron microscopy, we directly link nanoscale structural transformations to changes in mechanical properties as probed through the coherence of the excited acoustic modes. Specifically, ultrafast pump–probe microscopy reveals an enhancement in the acoustic mode quality factor of annealed gold nanodisks, indicative of reduced damping and improved vibrational coherence. Structural characterization via scanning electron microscopy and electron backscatter diffraction confirms that photoinduced annealing results in smoother surface morphology and overall enhanced crystallinity. The improved crystalline order reduces defect and crystal boundary scattering, which we suggest as the reason underlying the lower quality factor before annealing. Furthermore, these findings demonstrate that targeted structural engineering at the nanoscale offers a powerful strategy for optimizing the optomechanical performance of plasmonic nanostructures, with broad implications for the design of next-generation nanophotonic and optomechanical systems.

Annealing (metallurgy)↗