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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

DOE Support for the 8th International Conference on Attosecond Science (Final Technical Report)

The 8th International Conference on Attosecond Science and Technology (ATTO VIII) was held on the campus of the University of Central Florida in Orlando, FL from July 10-16, 2022. The main objectives of the conference were (i) to outline the state of the art of attosecond research; (ii) to jump-start national and international collaborations that had been hindered by the pandemic; (iii) to promote recruiting and training of postdocs and tenure-track candidates; and (iv) to consolidate the global and diverse identity of the attosecond community.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Complex Attosecond Waveform Synthesis at FEL FERMI

Free-electron lasers (FELs) can produce radiation in the short wavelength range extending from the extreme ultraviolet (XUV) to the X-rays with a few to a few tens of femtoseconds pulse duration. These facilities have enabled significant breakthroughs in the field of atomic, molecular, and optical physics, implementing different schemes based on two-color photoionization mechanisms. In this article, we present the generation of attosecond pulse trains (APTs) at the seeded FEL FERMI using the beating of multiple phase-locked harmonics. We demonstrate the complex attosecond waveform shaping of the generated APTs, exploiting the ability to manipulate independently the amplitudes and the phases of the harmonics. The described generalized attosecond waveform synthesis technique with an arbitrary number of phase-locked harmonics will allow the generation of sub-100 as pulses with programmable electric fields.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Electron choreography at the attosecond time scale

Abstract In this work, we report on coherent control of electron dynamics in atoms via attosecond pulse-shaping. We show that the photoelectron emission from argon gas produced by absorption of an attosecond pulse train (APT) made of odd and even harmonics can be manipulated along the direction of polarization of the light by tuning the spectral components (amplitude and phase) of the pulse. In addition, we show that APTs produced with a two-color (400- plus 800 nm) femtosecond driving field exhibit high temporal tunability, which is optimized for an intensity ratio between the two colors in the range of 0.1 to 5%.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Attosecond Transient Grating Spectroscopy with Near-Infrared Grating Pulses and an Extreme Ultraviolet Diffracted Probe

Transient grating spectroscopy has become a mainstay among metal and semiconductor characterization techniques. Here, we extend the technique toward the shortest achievable time scales by using tabletop high-harmonic generation of attosecond extreme ultraviolet (XUV) pulses that diffract from transient gratings generated with sub-5 fs near-infrared (NIR) pulses. We demonstrate the power of attosecond transient grating spectroscopy (ATGS) by investigating the ultrafast photoexcited dynamics in an Sb semimetal thin film. ATGS provides an element-specific, background-free signal unfettered by spectral congestion, in contrast to transient absorption spectroscopy. With ATGS measurements in Sb polycrystalline thin films, we observe the generation of coherent phonons and investigate the lattice and carrier dynamics. Among the latter processes, we extract carrier thermalization, hot carrier cooling, and electron-hole recombination, which are on the order of 20 fs, 50 fs, and 2 ps time scales, respectively. Furthermore, the simultaneous collection of transient absorption and transient grating data allows us to extract the total complex dielectric constant in the sample dynamics with a single measurement, including the real-valued refractive index, from which we are also able to investigate carrier-phonon interactions and longer-lived phonon dynamics. The outlined experimental technique expands the capabilities of transient grating spectroscopy and attosecond spectroscopies by providing a wealth of information concerning carrier and lattice dynamics with an element-selective technique at the shortest achievable time scales.

Quintero-Bermudez, Rafael↗
DOE OSTI2021

Generation of isolated soft x-ray attosecond pulses with mid-infrared driving lasers via transient phase-matching gating

Abstract Isolated attosecond pulses (IAPs) in the soft x-ray (SXR) region are highly desirable for attosecond time-resolved experiments. Here we identify a transient phase matching gating method for the generation of such IAPs with mid-infrared (MIR) lasers. This gating method works when a loosely focused, long-duration MIR Gaussian driving beam is slightly reshaped during its propagation in the gas medium under the ‘critical’ ionization condition. Quantitatively, the calculated coherence length of high harmonic is used to analyze the mechanism of the gating method, by using one-dimensional plane-wave beams and by comparing 2000 nm and 800 nm lasers. The robustness of the generation method is checked by varying laser’s carrier-envelope-phase and gas pressure. This gating method provides with an alternative route to efficiently produce tabletop ultrashort attosecond SXR light sources with the emerging MIR lasers.

Physics↗
DOE OSTI2023

Generation of multiple attosecond sub-bursts in femtosecond pulse trains by long-wavelength driving lasers

High-order harmonics generated by a long intense femtosecond laser are known experimentally to create attosecond pulse trains (APTs). In the time domain, an APT consists of a sequence of sharp attosecond bursts that are equally separated by each half optical cycle. Here, in this work, we show that such well-known features can be modified when a longer wavelength driving laser is used. From our simulations, we show that multiple shorter attosecond sub-bursts exist in the femtosecond pulse train within each half optical cycle and the duration of each sub-burst scales approximately as $λ^{–2}_0$ with the driving laser wavelength λ 0 . We show that such sub-bursts can be found using quantitative rescattering model for harmonics generated from a single atom, and their origin is due to the interference of the quantum orbits from first two returns of the recombining electron. We further show that such sub-bursts can be phase matched under proper laser focusing condition and the position of the gas cell, thus, such new features should be observable experimentally.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Measuring autoionization decay lifetimes of optically forbidden inner valence excited states in neon atoms with attosecond noncollinear four-wave-mixing spectroscopy

Attosecond noncollinear four-wave-mixing spectroscopy with one attosecond extreme ultraviolet (XUV) pulse and two few-cycle near-infrared (NIR) pulses was used to measure the autoionization decay lifetimes of inner valence electronic excitations in neon atoms. After a 43-48-eV XUV photon excites a 2s electron into the 2s2p 6 (np) Rydberg series, broadband NIR pulses couple the 2s2p 6 3p XUV-bright state to neighboring 2s2p 6 3s and 2s2p 6 3d XUV-dark states. Controllable delays of one or both NIR pulses with respect to the attosecond XUV pulse reveal the temporal evolution of either the dark or bright states, respectively. Experimental lifetimes for the 3s, 3p, and 3d states are measured to be 7±2, 48±8, and 427±40 fs, respectively, with 95% confidence. Accompanying calculations with two independent ab initio theoretical methods, newstock and astra, verify the findings. The results support the expected trend that the autoionization lifetime should be longer for states that have a smaller penetration in the radial region of the 2s core hole, which in this case is for the higher angular momentum Rydberg orbitals. In conclusion, the underlying theory thus links the lifetime results to electron correlation and provides an assessment of the direct and exchange terms in the autoionization process.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Bond-length dependence of attosecond ionization delays in O 2 arising from electron correlation to a shape resonance

We experimentally and theoretically demonstrate that electron correlation can cause the bond-length sensitivity of a shape resonance to induce an unexpected vibrational state–dependent ionization delay in a nonresonant channel. This discovery was enabled by a high-resolution attosecond-interferometry experiment based on a 400-nm driving and dressing wavelength. The short-wavelength driver results in a 6.2–electron volt separation between harmonics, markedly reducing the spectral overlap in the measured interferogram. We demonstrate the promise of this method on O 2 , a system characterized by broad vibrational progressions and a dense photoelectron spectrum. We measure a 40-attosecond variation of the photoionization delays over the X 2 Π g vibrational progression. Multichannel calculations show that this variation originates from a strong bond-length dependence of the energetic position of a shape resonance in the b 4 Σ$^{-}_{g}$ channel, which translates to the observed effects through electron correlation. The unprecedented energy resolution and delay accuracies demonstrate the promise of visible-light–driven molecular attosecond interferometry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Attosecond impulsive stimulated X-ray Raman scattering in liquid water

We report the measurement of impulsive stimulated x-ray Raman scattering in neutral liquid water. An attosecond pulse drives the excitations of an electronic wavepacket in water molecules. The process comprises two steps: a transition to core-excited states near the oxygen atoms accompanied by transition to valence-excited states. Thus, the wavepacket is impulsively created at a specific atomic site within a few hundred attoseconds through a nonlinear interaction between the water and the x-ray pulse. We observe this nonlinear signature in an intensity-dependent Stokes Raman sideband at 526 eV. Our measurements are supported by our state-of-the-art calculations based on the polarization response of water dimers in bulk solvation and propagation of attosecond x-ray pulses at liquid density.

Science & Technology - Other Topics↗
DOE OSTI2022

Attosecond coherent electron motion in Auger-Meitner decay

In quantum systems, coherent superpositions of electronic states evolve on ultrafast time scales (few femtoseconds to attoseconds; 1 attosecond = 0.001 femtoseconds = 10 -18 seconds), leading to a time-dependent charge density. Here we performed time-resolved measurements using attosecond soft x-ray pulses produced by a free-electron laser, to track the evolution of a coherent core-hole excitation in nitric oxide. Using an additional circularly polarized infrared laser pulse, we created a clock to time-resolve the electron dynamics and demonstrated control of the coherent electron motion by tuning the photon energy of the x-ray pulse. Core-excited states offer a fundamental test bed for studying coherent electron dynamics in highly excited and strongly correlated matter.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Kramers–Kronig relation in attosecond transient absorption spectroscopy

The Kramers–Kronig relation (KKR) has a wide range of applications in extreme ultraviolet (XUV) and x-ray spectroscopy. However, the validity of KKR for many of these applications has not been systematically studied, while it is known to require careful attention in nonlinear and pump–probe experiments in optical domain spectroscopy. Here, we study the validity of KKR in XUV attosecond transient absorption spectroscopy pump–probe measurements both experimentally and theoretically using argon Fano resonances as a case study. Experiments are enabled by a phase-resolved method dubbed Complex Attosecond Transient-absorption Spectroscopy (CATS). Although the estimations based on the rotating-wave approximation suggest that KKR violation could be expected in the studied case, our results validate KKR and provide a solid basis for its application in a broad range of attosecond spectroscopy experiments.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

Student Support for the “Frontiers in Attosecond & Ultrafast X-ray Science” School

The new millennium witnessed two revolutionary breakthroughs in ultrafast x-ray science: table-top XUV sources based on high harmonic generation in gases ushered in the attosecond era while facility-based x-ray free-electron lasers opened the path for intense, femtosecond hard x-rays. This award requested scholarship funds for a 2019 and 2023 School whose prime objective was the training of young scientists in these emerging complementary areas both relevant to DOE BES mission. The school entitled the “Frontiers of Attosecond and Ultrafast X-ray Science (FAXS)” (http://www.erice-attosecond.it/) was the second and fourth in a series, which began in 2017. The two Schools were held during March 10-16, 2019 and March 26-31, 2023 at the Ettore Majorana Foundation and Centre for Scientific Culture (http://www.ccsem.infn.it/) in Erice, Sicily. The DOE funds supported the registration fee for young scientists (graduate students and postdocs) from US institutions. The registration fees included School participation, lodging and meals over the duration of the School. Note, the third addition of the School was held in 2022 as a virtual event due to the pandemic, DOE funds were not necessary for this event. The FAXS School is a course of the 62th and 63rd International School of Quantum Electronics under the directorship of Prof. Diederik Wiersma (University of Florence). The Directors for the FAXS School are Louis DiMauro (The Ohio State University, USA) and Mauro Nisoli (Politecnico di Milano, Italy). The FAXS School program consisted of approximately 10 lectures by leading experts in attosecond and x-ray science (see attached list). Most lecturers delivered a series of three 1-hour lectures. The lecturers were required to spend the full 5 days at the school so to promote interaction with the students. The Erice Majorana Center venue accommodated ~75 young scientists. The registration fee covered the cost of participating in the school, lodging and meals for the entire duration of the school. The schedule consisted of lectures every morning and afternoon except for one afternoon that was reserved for an archaeological excursion. Every evening had a student/postdoc poster session and social gatherings at the Majorana Center to encourage further interaction of all participants and lecturers. The two FAXS Schools attracted an international group of young scientists. The DOE funds supported the registration fee for 11 students/postdocs from US institutions (5 supported in 2019 and 6 supported in 2023). The management of the DOE fellowships were administered through the Research Foundation of The Ohio State University. FAXS scholarships for European students/postdocs were provided by European funding sources administered by co-Director, Prof. Nisoli. All students/postdocs were encouraged to present a poster. Travel expenses to the FAXS School were the responsibility of the student/postdoc home institution.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2026

Probing Attosecond Bound Electron Dynamics Driven by Strong-Field Light Transients

The project aimed to drive strong-field excitation of bound electronic coherences in gas-phase atoms and molecules using a novel source of near-single-cycle optical field transients, based on industrial-grade Yb:solid-state laser technology. Key objectives included generating near-single cycle field transients and isolated attosecond pulses, reconstructing time-dependent wave packets in atoms and molecules, probing their decoherence using attosecond interferometry, and controlling the dynamic evolution of systems on attosecond to few-femtosecond timescales. A secondary goal of the project was to develop field-resolved measurement platforms as a novel approach for studying electron dynamics in atomic and molecular systems.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Circularly Polarized Attosecond Pulses Enabled by an Azimuthal Phase and Polarization Grating

High-harmonic generation (HHG) is an extreme nonlinear optical process that can map the properties of an infrared driving laser beam onto short wavelength attosecond pulse trains. However, current techniques for generating circularly polarized high harmonics for probing magnetic materials and chiral systems have limitations: two-color collinear counter-rotating driving lasers result in a low cutoff photon energy, while single-color non-collinear counter-rotating schemes suffer from low conversion efficiency. In this work, we generate circularly polarized attosecond pulse trains by using a structured laser driver which has a rotating polarization and phase grating along the azimuthal coordinate. Furthermore, our experimental and numerical results demonstrate the production of left and right circularly polarized harmonics, which naturally separate upon propagation. Our approach uses a single laser color in a collinear geometry, that can be scaled for high efficiency. Simulations show this scheme can extend into the soft x-ray region when driven by mid-infrared driving lasers, while preserving the same high phase-matching cutoff photon energy as for linearly-polarized high harmonics.

attosecond science↗
DOE OSTI2021

Terawatt attosecond x-ray source driven by a plasma accelerator

Plasma accelerators can generate ultra-high-brightness electron beams that open the door to light sources with a smaller physical footprint and properties un-achievable with conventional accelerator technology. In this paper, we show that electron beams from Plasma WakeField Accelerators can generate few-cycle coherent tunable soft x-ray pulses with TW peak power and a duration of tens of attoseconds, an order of magnitude more powerful, shorter, and with better stability than state-of-the-art X-ray Free Electron Lasers (XFELs). Such a light source would significantly enhance the ability to experimentally investigate electron dynamics on ultrafast timescales, having a broad-ranging impact across multiple scientific fields. Rather than starting from noise as in typical XFELs, the x-ray emission in this approach is driven by coherent radiation from a pre-bunched, high peak current electron beam of attosecond duration. This relaxes the restrictive tolerances that have hindered progress toward utilizing plasma accelerators as coherent x-ray drivers thus far, presenting a new paradigm for advanced accelerator light source applications.

43 PARTICLE ACCELERATORS↗
DOE OSTI2021

Analysis of two-color photoelectron spectroscopy for attosecond metrology at seeded free-electron lasers

The generation of attosecond pulse trains at free-electron lasers opens new opportunities in ultrafast science, as it gives access, for the first time, to reproducible, programmable, extreme ultraviolet (XUV) waveforms with high intensity. In this work, we present a detailed analysis of the theoretical model underlying the temporal characterization of the attosecond pulse trains recently generated at the free-electron laser FERMI. In particular, the validity of the approximations used for the correlated analysis of the photoelectron spectra generated in the two-color photoionization experiments are thoroughly discussed. The ranges of validity of the assumptions, in connection with the main experimental parameters, are derived.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Attosecond time delay in atomic photoionization: Angular-dependent transition from dipole to quadrupole and spin-flip dynamics

The angular distribution of attosecond Wigner time delay has been investigated including both quadrupole and relativistic effects using the relativistic-random-phase approximation that is based on the Dirac equation and includes significant aspects of many-body correlations. Here the results show a dramatic evolution of the time delay from (essentially nonrelativistic) dipole to quadrupole and spin-flip dynamics as a function of angle, thereby providing a venue for studying these interactions at the attosecond level.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Generation of Intense Low-Divergence Isolated Soft-X-Ray Attosecond Pulses in a Gas-Filled Waveguide Using Three-Color Synthesized Laser Pulses

Isolated attosecond pulses (IAPs) in the soft-x-ray (SXR) region have been successfully produced via high-order harmonic generation in a gas medium at several laboratories, but pulse energies are much lower compared to the IAPs in the extreme ultraviolet. Here, we show that in a gas-filled hollow waveguide, an efficient gating method using a few-cycle three-color synthesizer is able to generate stronger SXR IAPs. We show that an 104-as IAP in the SXR region (central energy of 210 eV) with a higher pulse energy (0.9 nJ) and a lower divergence (within 1.5 mrad) can be generated with a three-color laser beam for input pulse energy at 0.62 mJ, under the condition of optimal gas pressure and waveguide length. The enhancement of the IAP is attributed to favorable phase matching of SXR high harmonics caused by the evolution of the three-color waveform during its propagation in the waveguide, which can be understood by analyzing the time shift of the waveform due to the interplay of the waveguide mode, atomic dispersion, and plasma dispersion. We check that the gating method is quite robust with respect to the phase jitter in the waveform. The advantage of this method is further demonstrated by comparing the generation of SXR high harmonics and attosecond pulses with two other schemes: the three-color waveform in a gas cell and a previously optimized two-color waveform in a gas-filled waveguide.

74 ATOMIC AND MOLECULAR PHYSICS↗