Aaron LaForge
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View article: Machine-learning calibration of intense x-ray free-electron-laser pulses using Bayesian optimization
Machine-learning calibration of intense x-ray free-electron-laser pulses using Bayesian optimization Open
X-ray free-electron lasers (XFELs) have brought new ways to probe and manipulate atomic and molecular dynamics with unprecedented spatial and temporal resolutions. A quantitative comparison of experimental results with their simulated theo…
View article: Diffraction imaging of light induced dynamics in xenon-doped helium nanodroplets
Diffraction imaging of light induced dynamics in xenon-doped helium nanodroplets Open
We explore the light induced dynamics in superfluid helium nanodroplets with wide-angle scattering in a pump–probe measurement scheme. The droplets are doped with xenon atoms to facilitate the ignition of a nanoplasma through irradiation w…
View article: Diffraction imaging of light induced dynamics in xenon-doped helium nanodroplets
Diffraction imaging of light induced dynamics in xenon-doped helium nanodroplets Open
We have explored the light induced dynamics in superfluid helium nanodroplets with wide-angle scattering in a pump-probe measurement scheme. The droplets are doped with xenon atoms to facilitate the ignition of a nanoplasma through irradia…
View article: Attosecond coherent electron motion in Auger-Meitner decay
Attosecond coherent electron motion in Auger-Meitner decay Open
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 per…
View article: Relaxation dynamics in excited helium nanodroplets probed with high resolution, time-resolved photoelectron spectroscopy
Relaxation dynamics in excited helium nanodroplets probed with high resolution, time-resolved photoelectron spectroscopy Open
The ultrafast relaxation dynamics of excited helium nanodroplets were studied using time-resolved photoelectron spectroscopy. We observed an efficient population of triplet atomic states as well as the formation of the first excimer state …
View article: Ultrafast molecular dynamics in ionized 1- and 2-propanol: from simple fragmentation to complex isomerization and roaming mechanisms
Ultrafast molecular dynamics in ionized 1- and 2-propanol: from simple fragmentation to complex isomerization and roaming mechanisms Open
Photoexcitation of 1- and 2-propanol initiates a variety of molecular dynamics such as fragmentation, hydrogen migration, and even possible methyl roaming (only in 2-propanol).
View article: Enhancement of Above Threshold Ionization in Resonantly Excited Helium Nanodroplets
Enhancement of Above Threshold Ionization in Resonantly Excited Helium Nanodroplets Open
Clusters and nanodroplets hold the promise of enhancing high-order nonlinear optical effects due to their high local density. However, only moderate enhancement has been demonstrated to date. Here, we report the observation of energetic el…
View article: Collective enhancement of above threshold ionization by resonantly excited helium nanodroplets
Collective enhancement of above threshold ionization by resonantly excited helium nanodroplets Open
Clusters and nanodroplets hold the promise of enhancing high-order nonlinear optical effects due to their high local density. However, only moderate enhancement has been demonstrated to date. Here, we report the observation of energetic el…
View article: Ultrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics
Ultrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics Open
Interatomic processes play a crucial role in weakly bound complexes exposed to ionizing radiation;
\ntherefore, gaining a thorough understanding of their efficiency is of fundamental importance. Here, we
\ndirectly measure the timescale of…
View article: Ultrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics
Ultrafast Resonant Interatomic Coulombic Decay Induced by Quantum Fluid Dynamics Open
Interatomic processes play a crucial role in weakly bound complexes exposed to ionizing radiation; therefore, gaining a thorough understanding of their efficiency is of fundamental importance. Here, we directly measure the timescale of int…
View article: Time-resolved quantum beats in the fluorescence of helium resonantly excited by XUV radiation
Time-resolved quantum beats in the fluorescence of helium resonantly excited by XUV radiation Open
We report on the observation of time-resolved quantum beats in the helium fluorescence from the transition 1 s 3 p → 1 s 2 s , where the initial state is excited by XUV free electron laser radiation. The quantum beats originate from the Ze…
View article: Time-resolved study of resonant interatomic Coulombic decay in helium nanodroplets
Time-resolved study of resonant interatomic Coulombic decay in helium nanodroplets Open
When weakly-bound complexes are multiply excited by intense electromagnetic radiation, energy can be exchanged between neighboring atoms through a type of resonant interatomic Coulombic decay (ICD). This decay mechanism due to multiple exc…
View article: Autoionization dynamics of helium nanodroplets resonantly excited by intense XUV laser pulses
Autoionization dynamics of helium nanodroplets resonantly excited by intense XUV laser pulses Open
The ionization dynamics of helium droplets irradiated by intense, femtosecond extreme ultraviolet (XUV) pulses is investigated in detail by photoelectron spectroscopy. Helium droplets are resonantly excited to atomic-like 2p states with a …
View article: Real-time observation of water radiolysis and hydrated electron formation induced by extreme-ultraviolet pulses
Real-time observation of water radiolysis and hydrated electron formation induced by extreme-ultraviolet pulses Open
The earliest stages of hydrated electron formation are revealed by femtosecond extreme ultraviolet photoelectron imaging.
View article: Electron transfer mediated decay of alkali dimers attached to He nanodroplets
Electron transfer mediated decay of alkali dimers attached to He nanodroplets Open
Double ionization of alkali dimers attached to He nanodroplets by electron transfer mediated decay (ETMD).
View article: Charge Exchange Dominates Long-Range Interatomic Coulombic Decay of Excited Metal-Doped Helium Nanodroplets
Charge Exchange Dominates Long-Range Interatomic Coulombic Decay of Excited Metal-Doped Helium Nanodroplets Open
Atoms and molecules attached to rare-gas clusters are ionized by an interatomic autoionization process traditionally termed "Penning ionization" when the host cluster is resonantly excited. Here we analyze this process in the light of the …
View article: Charge-exchange dominates long-range interatomic Coulombic decay of excited metal-doped He nanodroplets
Charge-exchange dominates long-range interatomic Coulombic decay of excited metal-doped He nanodroplets Open
Atoms and molecules attached to rare gas clusters are ionized by an interatomic autoionization process traditionally termed 'Penning ionization' when the host cluster is resonantly excited. Here we analyze this process in the light of the …
View article: Deep neural networks for classifying complex features in diffraction images
Deep neural networks for classifying complex features in diffraction images Open
Intense short-wavelength pulses from free-electron lasers and high-harmonic-generation sources enable diffractive imaging of individual nanosized objects with a single x-ray laser shot. The enormous data sets with up to several million dif…
View article: Real-Time Dynamics of the Formation of Hydrated Electrons upon Irradiation of Water Clusters with Extreme Ultraviolet Light
Real-Time Dynamics of the Formation of Hydrated Electrons upon Irradiation of Water Clusters with Extreme Ultraviolet Light Open
Free electrons in a polar liquid can form a bound state via interaction with the molecular environment. This so-called hydrated electron state in water is of fundamental importance, e.g., in cellular biology or radiation chemistry. Hydrate…
View article: Autoionization dynamics of He nanodroplets resonantly excited by intense XUV laser pulses
Autoionization dynamics of He nanodroplets resonantly excited by intense XUV laser pulses Open
The ionization dynamics of helium droplets in a wide size range from 220 to 10^6 He atoms irradiated with intense femtosecond extreme ultraviolet (XUV) pulses of 10^9 ÷ 10^{12} W/cm2 power density is investigated in detail by photoelectron…
View article: Penning Ionization of Acene Molecules by Helium Nanodroplets
Penning Ionization of Acene Molecules by Helium Nanodroplets Open
Acene molecules (anthracene, tetracene, pentacene) and fullerene (C60) are embedded in He nanodroplets (HeN) and probed by EUV synchrotron radiation. When resonantly exciting the He nanodroplets, the embedded molecules M are efficiently io…
View article: Interatomic Coulombic decay in helium nanodroplets
Interatomic Coulombic decay in helium nanodroplets Open
Interatomic Coulombic decay (ICD) is induced in helium (He) nanodroplets by\nphotoexciting the n=2 excited state of He^+ using XUV synchrotron radiation. By\nrecording multiple coincidence electron and ion images we find that ICD occurs\ni…
View article: Fano resonances observed in helium nanodroplets
Fano resonances observed in helium nanodroplets Open
Doubly-excited Rydberg states of helium (He) nanodroplets have been studied using synchrotron radiation. We observed Fano resonances related to the atomic N = 2,0 series as a function of droplet size. Although similar qualitatively to thei…