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At least 559 records · Page 31

Energy-resolved and time-dependent unimolecular dissociation of hydroperoxyalkyl radicals (˙QOOH)

Hydroperoxyalkyl radicals (˙QOOH) are transient intermediates in the atmospheric oxidation of volatile organic compounds and combustion of hydrocarbon fuels in low temperature (<1000 K) environments. The carbon-centered ˙QOOH radicals are a critical juncture in the oxidation mechanism, but have generally eluded direct experimental observation of their structure, stability, and dissociation dynamics. Recently, this laboratory demonstrated that a prototypical ˙QOOH radical [˙CH 2 (CH 3 ) 2 COOH] can be synthesized by an alternative route, stabilized in a pulsed supersonic expansion, and characterized by its infrared (IR) spectroscopic signature and unimolecular dissociation rate to OH radical and cyclic ether products. The present study focuses on a partially deuterated ˙QOOD analog ˙CH 2 (CH 3 ) 2 COOD, generated in the laboratory by H-atom abstraction from partially deuterated tert-butyl hydroperoxide, (CH 3 ) 3 COOD. IR spectral features associated with jet-cooled and isolated ˙QOOD radicals are observed in the vicinity of the transition state (TS) barrier leading to OD radical and cyclic ether products. Furthermore, the overtone OD stretch (2ν OD ) of ˙QOOD is identified by IR action spectroscopy with UV laser-induced fluorescence detection of OD products. Direct time-domain measurement of the unimolecular dissociation rate for ˙QOOD (2ν OD ) extends prior rate measurements for ˙QOOH. Partial deuteration results in a small increase in the TS barrier predicted by high level electronic structure calculations due to changes in zero-point energies; the imaginary frequency is unchanged. Comparison of the unimolecular decay rates obtained experimentally with those predicted theoretically for both ˙QOOH and ˙QOOD confirm that unimolecular decay is enhanced by heavy-atom tunneling involving simultaneous O–O bond elongation and C–C–O angle contraction along the reaction pathway.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Radiative properties of advanced spacecraft heat shield materials

Experimental results are presented to show the effects of simulated reentry exposure by convective heating and by radiant heating on spectral and total emittance of statically oxidized Inconel 617 and Haynes HS188 superalloys to 1260 K and a silicide coatea (R512E) columbium 752 alloy to 1590 K. Convective heating exposures were conducted in a supersonic arc plasma wind tunnel using a wedge-shaped specimen configuration. Radiant tests were conducted at a pressure of .003 atmospheres of dry air at a flow velocity of several meters per second. Convective heating specimens were subjected to 8, 20, and 38 15-min heating cycles, and radiant heating specimens were tested for 10, 20, 50, and 100 30-min heating cycles. Changes in radiative properties are explained in terms of changes in composition resulting from simulated reentry tests. The methods used to evaluate morphological, compositional and crystallographic changes include: Auger electron spectroscopy; scanning electron microscopy; X-ray diffraction analysis; and electron microprobe analysis.

Cunnington, G. R.↗

Cr silicate as a prototype for engineering magnetic phases in air-stable two-dimensional transition-metal silicates

Abstract Identifying environmentally inert, ferromagnetic two-dimensional (2D) materials with high Curie temperatures ( T c ) down to the single layer limit has been an obstacle to fundamental studies of 2D magnetism and application of 2D heterostructures to spin-polarized devices. To address this challenge, the growth, structure and magnetic properties of a 2D Cr-silicate single layer on Pt(111) was investigated experimentally and theoretically. The layer was grown by sequentially depositing SiO and Cr followed by annealing in O 2 . Scanning tunneling microscopy (STM), low-energy electron diffraction (LEED), and low energy electron microscopy all indicated a well-ordered layer that uniformly covered the surface, with STM and LEED indicating that the silicate relaxed to its favored lattice constant. Further experimental characterizations demonstrated that the Cr was nominally 3+ but with a lower electron density than typical trivalent Cr compounds. Comparison with theory identified a Cr 2 Si 2 O 9 structure that resembles a single layer of a dehydrogenated dioctahedral silicate. Magnetic circular dichroism in x-ray absorption spectroscopy revealed a ferromagnetically ordered state up to at least 80 K. Theoretical analysis revealed that the Cr in a dehydrogenated Cr-silicate/Pt(111) is more oxidized than Cr in freestanding Cr 2 Si 2 O 9 H 4 layers. This greater oxidation was found to enhance ferromagnetic coupling and suggests that the magnetism may be tuned by doping. The 2D Cr-silicate is the first member of a broad series of possible layered first-row transition metal silicates with magnetic order; thus, this paper introduces a new platform for investigating 2D ferromagnetism and the development of magnetoelectronic and spintronic devices by stacking 2D atomic layers.

2D materials↗

A survey of simulation and diagnostic techniques for hypersonic nonequilibrium flows

The possible means of simulating nonequilibrium reacting flows in hypersonic environments, and the required diagnostic techniques, are surveyed in two categories: bulk flow behavior and determination of chemical rate parameters. Flow visualization of shock shapes for validation of computational-fluid dynamic calculations is proposed. The facilities and the operating conditions necessary to produce the required nonequilibrium conditions, the suitable optical techniques, and their sensitivity requirements, are surveyed. Shock-tubes, shock-tunnels, and ballistic ranges in a wide range of sizes and strengths are found to be useful for this purpose, but severe sensitivity requirements are indicated for the optical instruments, which can be met only by using highly-collimated laser sources. Likewise, for the determination of chemical parameters, this paper summarizes the quantities that need to be determined, required facilities and their operating conditions, and the suitable diagnostic techniques and their performance requirements. Shock tubes of various strengths are found to be useful for this purpose. Vacuum ultraviolet absorption and fluorescence spectroscopy and coherent anti-Stokes Raman spectroscopy are found to be the techniques best suited for the measurements of the chemical data.

Sharma, Surendra P.↗

Simulations of Attosecond Metallization in Quartz and Diamond Probed with Inner-Shell Transient Absorption Spectroscopy

When dielectrics are hit with intense infrared (IR) laser pulses, transient metalization can occur. The initial attosecond dynamics behind this metallization are not entirely understood. Therefore, simulations are needed to understand this process and to help interpret experimental observations of it, such as with attosecond transient absorption (ATA). In this paper, we present first-principles simulations of ATA based on bulk-mimicking clusters and real-time time-dependent density functional theory (RT-TDDFT), with Koopmans-tuned range-separated hybrid functionals and Gaussian basis sets. Our method gives good agreement with the experiment for the breakdown threshold in silica and diamond. This breakdown voltage corresponds to a Keldysh parameter of approximately one and thus involves a transition to a regime where the dynamics are driven by tunneling. Pumping at an amplitude just below this value causes a mixture of multiphoton and tunneling excitations across the band gap to occur. The computed extreme ultraviolet and X-ray attosecond transient spectra also agree well with the experiment and show a decrease in optical density due to the transient population of the conduction band from the IR field. First-principles approaches such as this are valuable for interpreting the complicated modulations in a spectrum and for guiding future attosecond experiments on solids.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Scanning Tunneling Microscopy Studies of Diamond Films and Optoelectronic Materials

We present a summary of the research, citations of publications resulting from the research and abstracts of such publications. We have made no inventions in the performance of the work in this project. The main goals of the project were to set up a Chemical Vapor Deposition (CVD) diamond growth system attached to an UltraHigh Vacuum (UHV) atomic resolution Scanning Tunneling Microscopy (STM) system and carry out experiments aimed at studying the properties and growth of diamond films using atomic resolution UHV STM. We successfully achieved these goals. We observed, for the first time, the atomic structure of the surface of CVD grown epitaxial diamond (100) films using UHV STM. We studied the effects of atomic hydrogen on the CVD diamond growth process. We studied the electronic properties of the diamond (100) (2x1) surface, and the effect of alkali metal adsorbates such as Cs on the work function of this surface using UHV STM spectroscopy techniques. We also studied, using STM, new electronic materials such as carbon nanotubes and gold nanostructures. This work resulted in four publications in refereed scientific journals and five publications in refereed conference proceedings.

Perez, Jose M.↗

Human-in-the-Loop: The Future of Machine Learning in Automated Electron Microscopy

Machine learning (ML) methods are progressively gaining acceptance in the electron microscopy community for de-noising, semantic segmentation, and dimensionality reduction of data post-acquisition. The introduction of the application programming interfaces (APIs) by major instrument manufacturers now allows the deployment of ML workflows in microscopes, not only for data analytics but also for real-time decision-making and feedback for microscope operation. However, the number of use cases for real-time ML remains remarkably small. Furthermore, we discuss some considerations in designing ML-based active experiments and pose that the likely strategy for the next several years will be human-in-the-loop automated experiments (hAE). In this paradigm, the ML learning agent directly controls beam position and image and spectroscopy acquisition functions, and a human operator monitors experiment progression in real and feature space of the system and tunes the policies of the ML agent to steer the experiment toward specific objectives.

47 OTHER INSTRUMENTATION↗

Revealing CO 2 dissociation pathways at vicinal copper (997) interfaces

Size- and shape-tailored copper (Cu) nanocrystals can offer vicinal planes for facile carbon dioxide (CO 2 ) activation. Despite extensive reactivity benchmarks, a correlation between CO 2 conversion and morphology structure has not yet been established at vicinal Cu interfaces. Herein, ambient pressure scanning tunneling microscopy reveals step-broken Cu nanocluster evolutions on the Cu(997) surface under 1 mbar CO 2 (g). The CO 2 dissociation reaction produces carbon monoxide (CO) adsorbate and atomic oxygen (O) at Cu step-edges, inducing complicated restructuring of the Cu atoms to compensate for increased surface chemical potential energy at ambient pressure. The CO molecules bound at under-coordinated Cu atoms contribute to the reversible Cu clustering with the pressure gap effect, whereas the dissociated oxygen leads to irreversible Cu faceting geometries. Synchrotron-based ambient pressure X-ray photoelectron spectroscopy identifies the chemical binding energy changes in CO-Cu complexes, which proves the characterized real-space evidence for the step-broken Cu nanoclusters under CO(g) environments. Our in situ surface observations provide a more realistic insight into Cu nanocatalyst designs for efficient CO 2 conversion to renewable energy sources during C 1 chemical reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Contributions to the BeEST sterile neutrino search

Sterile neutrinos are hypothetical right-handed leptons that have been postulated as extensions to the Standard Model to help explain the origin of neutrino masses and the matter-antimatter asymmetry in the Universe. Sterile neutrinos with keV-scale masses are also a promising candidate for dark matter. LLNL and the Colorado School of Mines are developing an experiment to search for sterile neutrinos by measuring the \Beryllium-7 Electron capture in Superconducting Tunnel junctions (STJs)" (the \BeEST" Experiment). When 7 Be implanted into STJ radiation detectors decays by electron capture, the neutrino escapes and the energy of the recoiling 7 Li nucleus can be measured with high accuracy. Using conservation of energy and momentum, the mass of the emitted neutrino can then be found. Sterile keV neutrinos would generate additional peaks in the spectrum, and the experiment uses high-resolution STJs to observe such a potential signal. During my internship, I contributed to different aspects of the BeEST experiment. I designed a UHV setup for X-ray spectroscopy analysis with STJs. It will allow high-resolution X-ray spectroscopy of different materials to examine the broadening in the BeEST spectra, the origins of which are unknown but may be related to material effects inside the STJ detectors. The design accounts for the specific demands of the BeEST project, but provides a degree of flexibility that makes it useful for other potential STJ projects. Additionally, to test the accuracy of the electronics and data analysis routine, an arbitrary waveform generator (AWG) will be used to generate simulated spectra that contain sterile neutrino signals of a specified mass and admixture. For this I programmed an AWG to output random STJ signals whose amplitudes follow the appropriate user-de ned probability distribution. The AWG signals can be input into the 32-channel preamplifier to simulate any spectrum of interest and test the uniformity of the amplifier chain, as well as the sensitivity of the data analysis.

42 ENGINEERING↗

Light-induced electron spin qubit coherences in the purple bacteria reaction center protein

Photosynthetic reaction center proteins (RCs) provide ideal model systems for studying quantum entanglement between multiple spins, a quantum mechanical phenomenon wherein the properties of the entangled particles become inherently correlated. Following light-generated sequential electron transfer, RCs generate spin-correlated radical pairs (SCRPs), also referred to as entangled spin qubit (radical) pairs (SQPs). Understanding and controlling coherence mechanisms in SCRP/SQPs is important for realizing practical uses of electron spin qubits in quantum sensing applications. The bacterial RC (bRC) provides an experimental system for exploring quantum effects in the SCRP P 865 + Q A − , where P 865 , a special pair of bacteriochlorophylls, is the primary donor, and Q A is the primary quinone acceptor. In this study, we focus on understanding how local molecular environments and isotopic substitution, particularly deuteration, influence spin coherence times (T M ). Using high-frequency electron paramagnetic resonance (EPR) spectroscopy, we observed that the local environment surrounding P 865 and Q A plays a significant role in determining T M . Our findings show that while deuteration led to a modest increase in T M , particularly at low temperatures, but the effect was substantially smaller than predicted by classical nuclear spin diffusion alone. This result is in contrast to our previous study of the photosystem I (PSI) RC, where no increase in T M was observed upon deuteration. Theoretical modeling identified several methyl groups at key distances from the spin centers of both bRC and PSI, and methyl group tunneling at low temperatures has been previously suggested as a mechanism for enhanced spin decoherence. Additionally, our study revealed a strong dependence of spin coherence on the orientation of the external magnetic field, highlighting the influence of the protein microenvironment on spin dynamics. In conclusion, these results offer new insights for optimizing coherence times in quantum system design for quantum information science and sensing applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Controlling the Fluctuating Tip-Enhanced Raman Spectra of Chloramben on Silver Nanocubes

Tip-enhanced Raman (TER) scattering from molecules residing at plasmonic junctions can be used to detect, identify, and image single molecules. This is most evident for flat molecules interrogated under extreme conditions of temperatures and pressure. It is also the case for (bio)molecular systems that feature preferred orientations/conformations under ambient laboratory conditions. More complex molecules that can adopt multiple conformations and/or that feature different protonation and/or charge states give rise to complex TER spectra. Here we illustrate how the latter can be controlled in the case of chloramben molecules coated onto plasmonic silver nanocubes. We show that characteristic molecular Raman spectra cannot be obtained when tunneling plasmons are operative, i.e., when the tip is in direct contact with the chemically functionalized plasmonic nanoparticles. We rationalize these observations and propose an approach to less invasive, and hence, more analytical TER spectral imaging.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Light-Induced Melting of Competing Stripe Orders without Introducing Superconductivity in La 2 − x Ba x CuO 4

The ultrafast manipulation of quantum material has led to many novel and significant discoveries. Among them, the light-induced transient superconductivity in cuprates achieved by melting competing stripe orders represents a highly appealing accomplishment. However, recent investigations have shown that the notion of photoinduced superconductivity remains a topic of controversy, and its elucidation solely through c -axis time-resolved terahertz spectroscopy remains an arduous task. Here, we measure the in-plane and out-of-plane transient terahertz responses simultaneously in the stripe-ordered nonsuperconducting La 2 − x Ba x CuO 4 after near-infrared excitations. We find that although a pump-induced reflectivity edge appears in the c -axis reflectance spectrum, the reflectivity along the CuO 2 planes decreases simultaneously, indicating an enhancement in the scattering rate of quasiparticles. This in-plane transient response is clearly distinct from the features associated with superconducting condensation. Therefore, we conclude the out-of-plane transient responses cannot be explained by an equivalent of Josephson tunneling. Notably, those pump-induced terahertz responses remain consistent even when we vary the near-infrared optical pump wavelengths and hole concentrations. Our results provide critical evidence that transient three-dimensional superconductivity cannot be induced by melting the competing stripe orders with pump pulses whose photon energy is much higher than the superconducting gap of cuprates. Published by the American Physical Society 2024

36 MATERIALS SCIENCE↗

A-site occupancy effects on structure, ionic conductivity, and thermodynamic stability of KxMgx/2Ti8−x/2O16

Abstract K x Mg x /2 Ti 8− x /2 O 16 (1.54 ≤ x ≤ 2) hollandite samples synthesized using a conventional solid-state route were used to investigate the effect of structure, ionic conductivity, and thermodynamic stability as a function of A-site (K) occupancy. The ionic conductivity, as measured using AC impedance spectroscopy, decreased as the A-site occupancy (and K content) increased. Titanate hollandite, of the form K x Mg x /2 Ti 8− x /2 O 16 , was measured using high-temperature oxide melt solution calorimetry in sodium molybdate (3Na 2 O $$\bullet$$ ∙ 4MoO 3 ) solvent at 804 $$^\circ{\rm C}$$ ∘ C . The enthalpies of formation are strongly exothermic indicating that they are thermodynamically stable relative to their constituent oxides. Previous studies have demonstrated increased stability with an increase in Cs content at fixed A-site occupancy. This work demonstrated an increase in the stability for the K-bearing hollandite samples with an increase in K content and tunnel occupancy. The measured enthalpies of formation (∆ H f,ox ) were in good agreement with density functional theory (DFT) predictions. Graphical abstract

Cassell, Nakeshma S.↗

Simulated 'On-Line' Wear Metal Analysis of Lubricating Oils by X-Ray Fluorescence Spectroscopy

The objective of this project was to assess the sensitivity of X-ray Fluorescence Spectroscopy (XFS) for quantitative evaluation of metal particle content in engine oil suspensions and the feasibility of real-time, dynamic wear metal analysis. The study was focused on iron as the majority wear metal component. Variable parameters were: particle size, particle concentration and oil velocity. A commercial XFS spectrometer equipped with interchangeable static/dynamic (flow cell) sample chambers was used. XFS spectra were recorded for solutions of Fe-organometallic standard and for a series of DTE oil suspensions of high purity spherical iron particles of 2g, 4g, and 8g diameter, at concentrations from 5 ppm to 5,000 ppm. Real contaminated oil samples from Langley Air Force Base aircraft engines and NASA Langley Research Center wind tunnels were also analyzed. The experimental data conform the reliability of XFS as the analytical method of choice for this project. Intrinsic inadequacies of the instrument for precise analytic work at low metal concentrations were identified as being related to the particular x-ray beam definition, system geometry, and flow-cell materials selection. This work supports a proposal for the design, construction and testing of a conceptually new, miniature XFS spectrometer with superior performance, dedicated to on-line, real-time monitoring of lubricating oils in operating engines. Innovative design solutions include focalization of the incident x-ray beam, non-metal sample chamber, and miniaturization of the overall assembly. The instrument would contribute to prevention of catastrophic engine failures. A proposal for two-year funding has been presented to NASA Langley Research Center Internal Operation Group (IOG) Management, to continue the effort begun by this summer's project.

Kelliher, Warren C.↗

Using Quasiparticle Poisoning To Detect Photons

According to a proposal, a phenomenon associated with excitation of quasiparticles in certain superconducting quantum devices would be exploited as a means of detecting photons with exquisite sensitivity. The phenomenon could also be exploited to perform medium-resolution spectroscopy. The proposal was inspired by the observation that Coulomb blockade devices upon which some quantum logic gates are based are extremely sensitive to quasiparticles excited above the superconducting gaps in their leads. The presence of quasiparticles in the leads can be easily detected via the charge states. If quasiparticles could be generated in the leads by absorption of photons, then the devices could be used as very sensitive detectors of electromagnetic radiation over the spectral range from x-rays to submillimeter waves. The devices in question are single-Cooper-pair boxes (SCBs), which are mesoscopic superconducting devices developed for quantum computing. An SCB consists of a small superconducting island connected to a reservoir via a small tunnel junction and connected to a voltage source through a gate capacitor. An SCB is an artificial two-level quantum system, the Hamiltonian of which can be controlled by the gate voltage. One measures the expected value of the charge of the eigenvectors of this quantum system by use of a radio-frequency single-electron transistor. A plot of this expected value of charge as a function of gate voltage resembles a staircase that, in the ideal case, consists of steps of height 2 e (where e is the charge of one electron). Experiments have shown that depending on the parameters of the device, quasiparticles in the form of "broken" Cooper pairs present in the reservoir can tunnel to the island, giving rise to steps of 1 e. This effect is sometimes called "poisoning." Simulations have shown that an extremely small average number of quasiparticles can generate a 1-e periodic signal. In a device according to the proposal, this poisoning would be turned to advantage. Depending on the wavelength, an antenna or other component would be used to couple radiation into the reservoir, wherein the absorption of photons would break Cooper pairs, thereby creating quasiparticles that, in turn, would tunnel to the island, creating a 1-e signal. On the basis of conservative estimates of device parameters derived from experimental data and computational simulations that fit the data, it has been estimated that the noise equivalent power of a device according to the proposal could be as low as 6 10(exp -22) W/Hz(exp 1/2). It has also been estimated that the spectroscopic resolution (photon energy divided by increment of photon energy) of such a device in visible light would exceed 100.

Echternach, Pierre↗

Strong interlayer charge transfer due to exciton condensation in an electrically isolated GaAs quantum well bilayer

We introduce a design of electrically isolated “floating” bilayer GaAs quantum wells (QW), in which application of a large gating voltage controllably and highly reproducibly induces charges that remain trapped in the bilayer after removal of the gating voltage. At smaller gate voltages, the bilayer is fully electrically isolated from external electrodes by thick insulating barriers. This design permits full control of the total and differential densities of two coupled 2D electron systems. The floating bilayer design provides a unique approach for studying systems inaccessible by simple transport measurements. It also provides the ability to measure the charge transfer between the layers, even when the in-plane resistivities of the 2D systems diverge. We measure the capacitance and inter-layer tunneling spectra of the QW bilayer with independent control of the top and bottom layer electron densities. Our measurements display strongly enhanced inter-layer tunneling current at v T =1, a signature of exciton condensation of a strongly interlayer-correlated bilayer system. With fully tunable densities of individual layers, the floating bilayer QW system provides a versatile platform to access previously unavailable information on the quantum phases in electron bilayer systems.

42 ENGINEERING↗

Instanton Effects in Euclidean vacuum, Real Time Production, and in the Light-front Wave Functions

Nontrivial topological structures of non-Abelian gauge fields were discovered in the 1970s. Instanton solutions, describing vacuum tunneling through topological barriers, have fermionic zero modes which are at the origin of ‘t Hooft effective Lagrangian. In the 1980s, instanton ensembles have been used to explain chiral symmetry breaking. In the 1990s, a large set of numerical simulations were performed deriving Euclidean correlation functions. The special role of scalar diquarks in nucleons and color superconductivity in dense quark matter has been elucidated. In these lectures, we discuss further developments of physics related to gauge topology. We show that the instanton–anti-instanton “streamline” configurations describe “sphaleron transitions” in high-energy collisions, which result in production of hadronic clusters with nontrivial topological/chiral charges. (They are not yet observed, but discussions of dedicated experiments at the LHC and RHIC are ongoing.) Another new direction is instanton effects in hadronic spectroscopy, both in the rest frame and on the light front. We will discuss their role in central and spin-dependent potentials, form factors and antiquark nuclear “sea”. Finally, we summarize the advances in the semiclassical theory of deconfinement, and chiral phase transitions at finite temperature, in QCD, and in some of its “deformed” versions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Studies of surface adsorbate electronic structure and femtochemistry at the fundamental length and time scales. Final report

The electronic structure and ultrafast (10-15 s-femtosecond timescale) electron dynamics were investigated for clean and atom/molecule covered metal surfaces. The studies were performed by scanning tunneling microscopy (STM) to measure the structure of adsorbed atoms and molecules on metal surfaces, and to investigate their electronic properties. The electronic structure of the observed molecular networks was calculated by electronic structure theory in collaboration with Prof. Jin Zhao, who is a long-time collaborator, a Professor at the University of Science and Technology of China, and holds an Adjunct Professorship at the University of Pittsburgh. We also investigated the electronic properties of C60 molecules when they are templated by corrugated black phosphorous surfaces. We found unexpected charge delocalization that is enabled by the templating. This research was done in collaboration with Professor Min Feng at the Wuhan University, and who also holds an Adjunct Professorship at the University of Pittsburgh. Moreover, the electronic structure and electron dynamics in metal surfaces were investigated by time-resolved photoemission electron spectroscopy. The focus of ultrafast spectroscopy has been on the plasmonic response of silver surfaces. One direction has been to develop multidimensional (energy, momentum, and time) photoelectron spectroscopy of the coherent response of solid surfaces. This method was applied to study the collective electron excitations known generally as plasmons, which screen optical fields from penetration into metals. Although this collective response has been known for more than 60 years and is used extensively to deposit optical energy into metals, how this happens is poorly known. We investigated the plasmonic response of silver at the point where the dielectric response passes through zero and bulk plasmon is excited by light. We discovered that the plasmon excitation decays by exciting electrons from the Fermi level of a metal, which is contrary to what is believed in the plasmonic science community. This research has been performed in collaboration with Dr. Marcel Reutzel, who was a postdoctoral fellow working on this research at the University of Pittsburgh, and now has a faculty position at the University of Göttingen in Germany. Prof. Branko Gumhalter from the Institute of Physics in Zagreb contributed on the theory of plasmonic decay processes. Furthermore, we investigated the Floquet engineering of electronic bands in metals leading to multiphoton photoemission and above threshold photoemission. Finally, we demonstrated that it is possible to change the electronic structure of metals by application of optical fields. Our studies indicated that this happens on subfemtosecond time scale and could potentially be used in ultrafast information processing and quantum computation. Related document information

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗