Bulletin of the American Physical Society
54th Annual Meeting of the APS Division of Atomic, Molecular and Optical Physics
Volume 68, Number 7
Monday–Friday, June 5–9, 2023; Spokane, Washington
Session M06: Ultrafast Phenomena in Solid-State |
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Chair: Niranjan Shivaram, Purdue University Room: 206 A |
Wednesday, June 7, 2023 2:00PM - 2:12PM |
M06.00001: Ultrafast electron dynamics in multilayer graphene Nikolay Golubev The light-induced electron motion in atoms, molecules, and solids is the driving force of many phenomena in nature such as photosynthesis and photoelectron effect. While the ultrafast electron dynamics in atoms and molecules has been widely studied in recent years both experimentally and theoretically, the time-resolved measurements and simulations of electron motion in solids are still in their infancy. Here, we present a fully quantum model capable of describing the field-induced electron motion dynamics in multilayer graphene in real time and space. We demonstrate the application of our model to interpret a recent pioneering experiment measuring the ultrafast quantum dynamics in graphene by attosecond electron diffraction imaging technique. |
Wednesday, June 7, 2023 2:12PM - 2:24PM |
M06.00002: Carrier Envelope Phase Dependence of High-order Harmonics from Monolayer MoS2 Christian A Cabello, Michael Chini, Volodymyr Turkowski The discovery of high-order harmonic generation (HHG) in solids has enabled new approaches to analyze and control electron dynamics and quantum properties in condensed matter systems. Here, we investigate the carrier-envelope phase-dependence of high-order harmonic generation from monolayer MoS2 driven by a high-intensity, mid-infrared, few-cycle pulse through time-dependent density functional theory calculations. Our results show different behavior for harmonics in different spectral ranges and with different polarization states, which suggest interference between multiple conduction bands and effects arising from the Berry curvature of the band structure. These results which are supported by experimental studies may provide new insight into sub-cycle topological control in 2D systems. |
Wednesday, June 7, 2023 2:24PM - 2:36PM Withdrawn |
M06.00003: Orbital perspective of high harmonic generation in ReS2 Álvaro Jiménez-Galán, Chandler Bossaer, Guilmot Ernotte, Andrew Parks, Rui Silva, David M Villeneuve, Andre Staudte, Thomas Brabec, Adina A Luican-Mayer, Giulio Vampa High harmonic generation has allowed unparalleled monitoring and control of coherent electron dynamics. In atoms and molecules, this has been made possible thanks to a theoretical framework based on a time-domain and real-space perspective of the highly non-perturbative light-matter interaction, linking the characteristics of the emitted harmonic radiation to sub-laser-cycle dynamics of atomic and molecular orbitals. In solids, high harmonic generation is understood using a similar framework, albeit exchanging the real-space perspective for one in reciprocal-space. This band structure perspective has proven very insightful, for example, to reconstruct the dispersion in ZnO, or to explain multiple plateaus observed in the HHG spectrum of rare-gas solids. |
Wednesday, June 7, 2023 2:36PM - 2:48PM |
M06.00004: Ultrafast Laser-Driven Dynamics in Metal-Insulator Interface Abdallah AlShafey, Gerard McCaul, Yuan-Ming Lu, Xu-Yan Jia, Shou-Shu Gong, Zachariah M Addison, Denys I Bondar, Mohit Randeria, Alexandra S Landsman Mott insulators are examples of strongly correlated solid-state systems with complex properties resulting from the many-body physics at play. Here, we probe the ultrafast dynamics of metal-insulator (MI) interfaces by coupling a free chain to the Mott insulator. We study the effect of an increased interfacial coupling on the electronic and magnetic properties in the insulator, the underlying microscopic mechanisms at play, and the resulting effect on the optical response in the high-harmonic spectrum. |
Wednesday, June 7, 2023 2:48PM - 3:00PM |
M06.00005: Imaging Singlet Fission using Angle-Resolved Photoemission Zachary H Withers, Sergii Chernov, Jin Bakalis, Alice Kunin, Michael G White, Gerd Schönhense, Thomas K Allison Zachary H. Withers1, Sergey Chernov1, Jin Bakalis1, Alice Kunin1, Michael G. White2, Gerd Schönhense3, and Thomas K. Allison1,2 |
Wednesday, June 7, 2023 3:00PM - 3:12PM |
M06.00006: Controlling the polarization and phase of high-order harmonics with a plasmonic metasurface Sohail A Jalil, Kashif M Awan, Idriss A Ali, Sabaa Rashid, Joshua Baxter, Aleksey Korobenko, Guilmot Ernotte, Andrei Y Naumov, David M Villeneuve, Andre Staudte, Pierre Berini, Lora Ramunno, Giulio Vampa Metasurfaces have been utilized to enhance the emission of high-order harmonics of femtosecond infrared laser pulses, by enhancing the incident field, and to shape the emitted high harmonics in space. Here we show control of the polarization and phase of high harmonics with a plasmonic Pancharatnam–Berry phase metasurface. The latter generates circularly polarized deep-ultraviolet high harmonics, from a circularly polarized infrared driver, providing a simple path for achieving circular emission from patterned crystals. Our metasurface enhances the circularly polarized harmonics up to ∼43 times when compared to the unpatterned surface. |
Wednesday, June 7, 2023 3:12PM - 3:24PM |
M06.00007: Photo-Induced Plasmonic Light Harvesting Dynamics and Chemical Transformations Monitored Via Picosecond Time-Resolved Ambient-Pressure X-ray Photoelectron Spectroscopy (TRAPXPS) Sahan Neelakanni Mudiyanselage, Zachery Donnellan, Lars Hoffmann, Soumyadeep Ghosh, Jin Qian, Sasawat Jamnuch, Tod A Pascal, Friedrich Roth, Wolfgang Eberhardt, Oliver Gessner Combining plasmonic nanostructures with semiconductor catalysts is a promising strategy to enhance both optical and electronic characteristics of photocatalytic devices. However, improving device efficiencies requires more detailed knowledge of processes such as light-induced charge injection, carrier separation, as well as back electron transfer and electron-hole recombination. We employ picosecond time-resolved X-ray photoemission spectroscopy to probe charge-carrier dynamics and chemical transformations in gold nanoparticle (AuNPs) sensitized TiO2 under UHV and near-ambient H2O pressure conditions suitable for photoelectrochemical water splitting. The experiments provide an absolute measure of the amount of charge injected from AuNPs into the TiO2 substrate as well as the back electron transfer dynamics from the perspective of the electron donor. Under UHV conditions, approximately two electrons are injected per NP and charge recombination is complete within less than 1 ns. The presence of water has a significant impact on interfacial dynamics. Recombination timescales are increased by up to several ns and accompanied by indications for more efficient charge injection. Both effects are beneficial for the photocatalytic efficiency of the heterosystem as they potentially increase exposure of reactants to interfacial charges. The results underline the importance of characterizing fundamental interfacial electron and chemical dynamics under reaction-like conditions. Experiments are complemented by ongoing theoretical efforts to disentangle the physics underlying the observed charge transfer dynamics using a combination of molecular dynamics simulations and density functional theory. |
Wednesday, June 7, 2023 3:24PM - 3:36PM |
M06.00008: In Situ Control and Nanofocusing of Extreme Ultraviolet Solid-State High Harmonics Aleksey Korobenko, Sabaa Rashid, Christian Heide, Andrei Y Naumov, David A Reis, Pierre Berini, Paul B Corkum, Giulio Vampa Extreme ultraviolet (XUV), electromagnetic radiation with a wavelength of ~100 nm, is one of the key technologies of ultrafast science. A lot of progress has been made in developing high-brightness and high-energy coherent XUV sources, including the ones based on solid state materials. However, efficient manipulation and focusing of XUV photons to their ultimate diffraction limit remains a formidable challenge because of the precision of the focusing by curved optical surfaces. |
Wednesday, June 7, 2023 3:36PM - 3:48PM |
M06.00009: Electric field measurement of four-wave mixing signals in magnesium oxide with attosecond resolution Francis F Walz, Shashank Kumar, Siddhant Pandey, Yuyan Zhong, Rudro R Biswas, Niranjan Shivaram We present measurements of the electric field emitted from a third order nonlinear interaction in crystalline magnesium oxide (MgO). Using a sensitive interferometric technique known as TADPOLE, we measure the complete femtosecond electric field of the weak nonlinear signal generated using a degenerate four wave mixing (DFWM) scheme. In this scheme, three femtosecond pulses of the same wavelength (800 nm) interact with MgO and emit a signal pulse. Two of the pulses are time delayed with respect to the third which allows us to extract dynamical information about the system. Using a specific geometry of the incoming beams, the signal pulse is spatially separated from the incoming beams to allow for a background-free measurement. We observe modulations in the temporal phase of the emitted electric field on attosecond timescales. With help from theoretical calculations, the source of such modulations, arising from a modulation in the nonlinear response of the material, will be discussed. |
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