Stephen R. Leone
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View article: Different Rise Times of Atomic Br M$_{4,5}$ 3d$_{3/2,5/2}$ Core Level Absorptions during Br$_{2}$ C $^{1}Π_{u}$ $1_{u}$ State Dissociation via Extreme Ultraviolet Transient Absorption Spectroscopy
Different Rise Times of Atomic Br M$_{4,5}$ 3d$_{3/2,5/2}$ Core Level Absorptions during Br$_{2}$ C $^{1}Π_{u}$ $1_{u}$ State Dissociation via Extreme Ultraviolet Transient Absorption Spectroscopy Open
The reported ''dissociation times'' for the Br$_{2}$ C ($^{1}Π_{u}$ $1_{u}$) state by various measurement methods differ widely across the literature (30 to 340 fs). We consider this issue by investigating attosecond extreme ultraviolet (X…
View article: Open-source simulation program for extreme ultraviolet and soft x-ray sources based on high-harmonic generation
Open-source simulation program for extreme ultraviolet and soft x-ray sources based on high-harmonic generation Open
Light sources based on high-harmonic generation (HHG) underpin ultrafast spectroscopy experiments across a large range of photon energies, spanning from the extreme ultraviolet to the soft x-ray. To this day, their design, implementation, …
View article: Tracing Long-Lived Atomic Coherences Generated via Molecular Conical Intersections
Tracing Long-Lived Atomic Coherences Generated via Molecular Conical Intersections Open
Accessing coherences is key to fully understand and control ultrafast dynamics of complex quantum systems like molecules. Most photochemical processes are mediated by conical intersections, which generate coherences between electronic stat…
View article: All-optical logic gates for extreme ultraviolet switching via attosecond four-wave mixing
All-optical logic gates for extreme ultraviolet switching via attosecond four-wave mixing Open
All-optical logic-gate-based switching is a prerequisite for photonic computing. This article introduces a logic-gate protocol for noncollinear four-wave mixing (FWM) of one attosecond extreme ultraviolet (XUV) with two few-femtosecond nea…
View article: Attosecond Optical Orientation
Attosecond Optical Orientation Open
Circularly polarized light offers opportunities to probe symmetry-dependent properties of matter such as chirality and spin. Circular dichroism measurements typically require further intrinsic or extrinsic breaking of symmetry by e.g. enan…
View article: Coherently coupled carrier and phonon dynamics in elemental tellurium probed by extreme ultraviolet transient absorption
Coherently coupled carrier and phonon dynamics in elemental tellurium probed by extreme ultraviolet transient absorption Open
The narrow band-gap semiconductor elemental tellurium (Te) has a unique electronic structure due to strong spin-orbit splitting and a lack of inversion symmetry of its helical lattice. Using broadband extreme ultraviolet core-level transie…
View article: Capturing Ring Opening in Photoexcited Enolic Acetylacetone upon Hydrogen Bond Dissociation by Ultrafast Electron Diffraction
Capturing Ring Opening in Photoexcited Enolic Acetylacetone upon Hydrogen Bond Dissociation by Ultrafast Electron Diffraction Open
Photoinduced biological and chemical reactions are often based on key structural transformations of a molecule driven across multiple electronic states. Acetylacetone (AcAc) is a prototypical system for complex chemical pathways involving …
View article: Polarization-resolved core exciton dynamics in LiF using attosecond transient absorption spectroscopy
Polarization-resolved core exciton dynamics in LiF using attosecond transient absorption spectroscopy Open
The ability to control absorption by modifying the polarization of light presents an exciting opportunity to experimentally determine the orbital alignment of absorption features. Here, attosecond extreme ultraviolet (XUV) transient absorp…
View article: Tracing long-lived atomic coherences generated via molecular conical intersections
Tracing long-lived atomic coherences generated via molecular conical intersections Open
Accessing coherences is key to fully understand and control ultrafast dynamics of complex quantum systems like molecules. Most photochemical processes are mediated by conical intersections (CIs), which generate coherences between electroni…
View article: Attosecond Transient Grating Spectroscopy with Near-Infrared Grating Pulses and an Extreme Ultraviolet Diffracted Probe
Attosecond Transient Grating Spectroscopy with Near-Infrared Grating Pulses and an Extreme Ultraviolet Diffracted Probe Open
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 attoseco…
View article: Probing soft X-ray induced photoreduction of a model Mn-complex at cryogenic conditions
Probing soft X-ray induced photoreduction of a model Mn-complex at cryogenic conditions Open
Soft X-ray absorption spectroscopy of first row transition elements at their respective L -edges provides important information about the oxidation and spin states of the metal centers. However, the associated sample damage in radiation-se…
View article: Polarization-Resolved Core Exciton Dynamics in LiF Using Attosecond Transient Absorption Spectroscopy
Polarization-Resolved Core Exciton Dynamics in LiF Using Attosecond Transient Absorption Spectroscopy Open
The ability to control absorption by modifying the polarization of light presents an exciting opportunity to experimentally determine the orbital alignment of absorption features. Here, attosecond extreme ultraviolet (XUV) transient absorp…
View article: Extracting doubly excited state lifetimes in helium directly in the time domain with attosecond noncollinear four-wave-mixing spectroscopy
Extracting doubly excited state lifetimes in helium directly in the time domain with attosecond noncollinear four-wave-mixing spectroscopy Open
The helium atom, with one nucleus and two electrons, is a prototypical system to study quantum many-body dynamics. Doubly excited states, or quantum states in which both electrons are excited by one photon, showcase electronic-correlation …
View article: Attosecond Probing of Coherent Vibrational Dynamics in CBr<sub>4</sub>
Attosecond Probing of Coherent Vibrational Dynamics in CBr<sub>4</sub> Open
A coherent vibrational wavepacket is launched and manipulated in the symmetric stretch (a1) mode of CBr4, by impulsive stimulated Raman scattering (ISRS) from nonresonant 400 nm laser pump pulses with various peak int…
View article: UV-Induced Reaction Pathways in Bromoform Probed with Ultrafast Electron Diffraction
UV-Induced Reaction Pathways in Bromoform Probed with Ultrafast Electron Diffraction Open
For many chemical reactions, it remains notoriously difficult to predict and experimentally determine the rates and branching ratios between different reaction channels. This is particularly the case for reactions involving short-lived int…
View article: Measurement of coherent vibrational dynamics with X-ray Transient Absorption Spectroscopy simultaneously at the Carbon K- and Chlorine L2,3- edges
Measurement of coherent vibrational dynamics with X-ray Transient Absorption Spectroscopy simultaneously at the Carbon K- and Chlorine L2,3- edges Open
View article: Spin Dynamics across Metallic Layers on the Few-Femtosecond Timescale
Spin Dynamics across Metallic Layers on the Few-Femtosecond Timescale Open
We measure the light-driven response of a magnetic multilayer structure made of thin alternating layers of cobalt and platinum at the few-femtosecond timescale. Using attosecond magnetic circular dichroism, we observe how light rearranges …
View article: Extracting doubly-excited state lifetimes in helium directly in the time domain with attosecond noncollinear four-wave-mixing spectroscopy
Extracting doubly-excited state lifetimes in helium directly in the time domain with attosecond noncollinear four-wave-mixing spectroscopy Open
The helium atom, with one nucleus and two electrons, is a prototypical system to study quantum many-body dynamics. Doubly-excited states, or quantum states in which both electrons are excited by one photon, are showcase scenarios of electr…
View article: Attosecond transient grating spectroscopy with near-infrared grating pulses and an extreme ultraviolet diffracted probe
Attosecond transient grating spectroscopy with near-infrared grating pulses and an extreme ultraviolet diffracted probe Open
Transient grating spectroscopy has become a mainstay among metal and semiconductor characterization techniques. Here we extend the technique towards the shortest achievable timescales by using tabletop high-harmonic generation of attosecon…
View article: Initial electron thermalization in metals measured by attosecond transient absorption spectroscopy
Initial electron thermalization in metals measured by attosecond transient absorption spectroscopy Open
Understanding initial electron thermalization has relevance to both fundamental scientific knowledge and application to the construction of novel devices. In this study, attosecond transient absorption is used to directly measure initial e…
View article: Measurement of Coherent Vibrational Dynamics with X-ray Transient Absorption Spectroscopy Simultaneously at the Carbon K- and Chlorine L$_{2,3}$- Edges
Measurement of Coherent Vibrational Dynamics with X-ray Transient Absorption Spectroscopy Simultaneously at the Carbon K- and Chlorine L$_{2,3}$- Edges Open
X-ray Transient Absorption Spectroscopy near the carbon K-edge (1s, $\sim$ 285 eV) and chlorine L$_{2,3}$ edges (2p, $\sim$ 200 eV) is used to study the nuclear dynamics of CCl$_4$ vibrationally activated by impulsive stimulated Raman scat…
View article: Capturing ring opening in photoexcited enolic acetylacetone upon hydrogen bond dissociation by ultrafast electron diffraction
Capturing ring opening in photoexcited enolic acetylacetone upon hydrogen bond dissociation by ultrafast electron diffraction Open
Photoinduced biological and chemical reactions are often based on key structural transformations of a molecule driven across multiple electronic states. Acetylacetone (AcAc) is a prototypical system for complex chemical pathways involving …
View article: Profile of Pierre Agostini, Anne L’Huillier, and Ferenc Krausz: 2023 Nobel laureates in Physics
Profile of Pierre Agostini, Anne L’Huillier, and Ferenc Krausz: 2023 Nobel laureates in Physics Open
View article: Spin Coupling Effect on Geometry-Dependent X-Ray Absorption of Diradicals
Spin Coupling Effect on Geometry-Dependent X-Ray Absorption of Diradicals Open
We theoretically investigate the influence of diradical electron spin coupling on the time-resolved X-ray absorption spectra of the photochemical ring opening of furanone. We predict geometry-dependent carbon K-edge signals involving trans…
View article: Dynamics via Attosecond Four-Wave Mixing
Dynamics via Attosecond Four-Wave Mixing Open
Attosecond four-wave mixing spectroscopy is a relatively new technique for studying ultrafast dynamics of highly excited states with exquisite temporal precision and spectral resolution. The attosecond four-wave mixing technique, as descri…
View article: Reinvented: An Attosecond Chemist
Reinvented: An Attosecond Chemist Open
Attosecond science requires a substantial rethinking of how to make measurements on very short timescales; how to acquire the necessary equipment, technology, and personnel; and how to build a set of laboratories for such experiments. This…
View article: Experimental and theoretical analysis of ultrafast electron diffraction (UED) data for acetylacetone
Experimental and theoretical analysis of ultrafast electron diffraction (UED) data for acetylacetone Open
Here, in two archives with data for ultrafast electron diffraction (UED) study of the acetylacetone. AcAc_UED_theoretical.zip contains the results of theoretical simulations. AcAc_UED_experimental.zip contains raw and processed experimenta…
View article: Experimental and theoretical analysis of ultrafast electron diffraction (UED) data for acetylacetone
Experimental and theoretical analysis of ultrafast electron diffraction (UED) data for acetylacetone Open
Here, in two archives with data for ultrafast electron diffraction (UED) study of the acetylacetone. AcAc_UED_theoretical.zip contains the results of theoretical simulations. AcAc_UED_experimental.zip contains raw and processed experimenta…
View article: On the Onset of Coherent Phonon Motion in Peierls-Distorted Antimony by Attosecond Transient Absorption
On the Onset of Coherent Phonon Motion in Peierls-Distorted Antimony by Attosecond Transient Absorption Open
Attosecond extreme-ultraviolet (XUV) transient absorption spectroscopy measurements on the Peierls-distorted phase of the semimetal antimony (Sb) are presented. After excitation by an ultrashort, broad band near-infrared (NIR) pulse, the d…
View article: Spin Coupling Effect on Geometry-Dependent X-ray Absorption of Diradicals
Spin Coupling Effect on Geometry-Dependent X-ray Absorption of Diradicals Open
We theoretically investigate the influence of diradical electron spin coupling on the time-resolved X-ray absorption spectra of the photochemical ring opening of furanone. We predict geometry dependent carbon K-edge signals involving trans…