Element-Specific Ultrafast Lattice Dynamics in Monolayer WSe.

We study monolayer WSe using ultrafast electron diffraction. We introduce an approach to quantitatively extract atomic-site-specific information, providing an element-specific view of incoherent atomic vibrations following femtosecond excitation. Via differences between W and Se vibrations, we identify stages in the nonthermal evolution of the phonon population.

Two-Dimensional Electronic Spectroscopy Reveals Dynamics within the Bright Fine Structure of CdSe Quantum Dots.

Semiconductor quantum dots are characterized by a discrete excitonic structure featuring coarse as well as fine structure. The lowest fine structure states have splittings into bright-dark states which are now well confirmed by single dot spectroscopy. In contrast, the splitting of the lowest coarse exciton into bright-bright fine structure states has not been observed nor the dynamics between these states.

Exciton-polaron interactions in metal halide perovskite nanocrystals revealed via two-dimensional electronic spectroscopy.

Metal halide perovskite nanocrystals have been under intense investigation for their promise in optoelectronic devices due to their remarkable physics, such as liquid/solid duality. This liquid/solid duality may give rise to their defect tolerance and other such useful properties. This duality means that the electronic states are fluctuating in time, on a distribution of timescales from femtoseconds to picoseconds.

Mediterranean springs: Keystone ecosystems and biodiversity refugia threatened by global change.

Mediterranean spring ecosystems are unique habitats at the interface between surface water and groundwater. These ecosystems support a remarkable array of biodiversity and provide important ecological functions and ecosystem services. Spring ecosystems are influenced by abiotic, biotic, and anthropogenic factors such as the lithology of their draining aquifers, their climate, and the land use of their recharge area, all of which affect the water chemistry of the aquifer and the spring discharges.

Perturbed free induction decay obscures early time dynamics in two-dimensional electronic spectroscopy: The case of semiconductor nanocrystals.

Two-dimensional electronic spectroscopy (2DES) has recently been gaining popularity as an alternative to the more common transient absorption spectroscopy due to the combination of high frequency and time resolution of 2DES. In order to advance the reliable analysis of population dynamics and to optimize the time resolution of the method, one has to understand the numerous field matter interactions that take place at an early and negative time. These interactions have historically been discussed in one-dimensional spectroscopy as coherent artifacts and have been assigned to both resonant and non-resonant system responses during or before the pulse overlap.

Direct Observation of Ultrafast Lattice Distortions during Exciton-Polaron Formation in Lead Halide Perovskite Nanocrystals.

The microscopic origin of slow hot-carrier cooling in lead halide perovskites remains debated and has direct implications for applications. Slow hot-carrier cooling of several picoseconds has been attributed to either polaron formation or a hot-phonon bottleneck effect at high excited carrier densities (>10 cm). These effects cannot be unambiguously disentangled with optical experiments alone.

Observation of Multi-Directional Energy Transfer in a Hybrid Plasmonic-Excitonic Nanostructure.

Hybrid plasmonic devices involve a nanostructured metal supporting localized surface plasmons to amplify light-matter interaction, and a non-plasmonic material to functionalize charge excitations. Application-relevant epitaxial heterostructures, however, give rise to ballistic ultrafast dynamics that challenge the conventional semiclassical understanding of unidirectional nanometal-to-substrate energy transfer. Epitaxial Au nanoislands are studied on WSe with time- and angle-resolved photoemission spectroscopy and femtosecond electron diffraction: this combination of techniques resolves material, energy, and momentum of charge-carriers and phonons excited in the heterostructure.

Photoinduced Ultrafast Transition of the Local Correlated Structure in Chalcogenide Phase-Change Materials.

Revealing the bonding and time-evolving atomic dynamics in functional materials with complex lattice structures can update the fundamental knowledge on rich physics therein, and also help to manipulate the material properties as desired. As the most prototypical chalcogenide phase change material, Ge_{2}Sb_{2}Te_{5} has been widely used in optical data storage and nonvolatile electric memory due to the fast switching speed and the low energy consumption. However, the basic understanding of the structural dynamics on the atomic scale is still not clear.

Traversing Double-Well Potential Energy Surfaces: Photoinduced Concurrent Intralayer and Interlayer Structural Transitions in XTe (X = Mo, W).

The microscopic arrangement of atoms and molecules is the determining factor in how materials behave and perform; , the structure determines the property, a traditional paradigm in materials science. Photoexcitation-driven manipulation of the crystal structure and associated electronic properties in quantum materials provides opportunities for the exploration of exotic physics and practical applications; however, a generalized mechanism for such symmetry engineering is absent. Here, by ultrafast electron diffraction, structure factor calculation, and TDDFT-MD simulations, we report the photoinduced concurrent intralayer and interlayer structural transitions in the Td and 1T' phases of XTe (X = Mo, W).

Efficient First-Principles Methodology for the Calculation of the All-Phonon Inelastic Scattering in Solids.

Inelastic scattering experiments are key methods for mapping the full dispersion of fundamental excitations of solids in the ground as well as nonequilibrium states. A quantitative analysis of inelastic scattering in terms of phonon excitations requires identifying the role of multiphonon processes. Here, we develop an efficient first-principles methodology for calculating the all-phonon quantum mechanical structure factor of solids.

Ultrafast lattice dynamics and electron-phonon coupling in platinum extracted with a global fitting approach for time-resolved polycrystalline diffraction data.

Quantitative knowledge of electron-phonon coupling is important for many applications as well as for the fundamental understanding of nonequilibrium relaxation processes. Time-resolved diffraction provides direct access to this knowledge through its sensitivity to laser-induced lattice dynamics. Here, we present an approach for analyzing time-resolved polycrystalline diffraction data.

Accessing the Anisotropic Nonthermal Phonon Populations in Black Phosphorus.

We combine ultrafast electron diffuse scattering experiments and first-principles calculations of the coupled electron-phonon dynamics to provide a detailed momentum-resolved picture of lattice thermalization in black phosphorus. The measurements reveal the emergence of highly anisotropic nonthermal phonon populations persisting for several picoseconds after exciting the electrons with a light pulse. Ultrafast dynamics simulations based on the time-dependent Boltzmann formalism are supplemented by calculations of the structure factor, defining an approach to reproduce the experimental signatures of nonequilibrium structural dynamics.

Nuclear dynamics of singlet exciton fission in pentacene single crystals.

Singlet exciton fission (SEF) is a key process for developing efficient optoelectronic devices. An aspect rarely probed directly, yet with tremendous impact on SEF properties, is the nuclear structure and dynamics involved in this process. Here, we directly observe the nuclear dynamics accompanying the SEF process in single crystal pentacene using femtosecond electron diffraction.

Exchange-Striction Driven Ultrafast Nonthermal Lattice Dynamics in NiO.

We use femtosecond electron diffraction to study ultrafast lattice dynamics in the highly correlated antiferromagnetic (AFM) semiconductor NiO. Using the scattering vector (Q) dependence of Bragg diffraction, we introduce Q-resolved effective temperatures describing the transient lattice. We identify a nonthermal lattice state with preferential displacement of O compared to Ni ions, which occurs within ∼0.

Fifth-order two-quantum absorptive two-dimensional electronic spectroscopy of CdSe quantum dots.

Two-quantum variants of two-dimensional electronic spectroscopy (2DES) have previously been used to characterize multi-exciton interactions in molecules and semiconductor nanostructures though many implementations are limited by phasing procedures or non-resonant signals. We implement 2DES using phase-cycling to simultaneously measure one-quantum and two-quantum spectra in colloidal CdSe quantum dots. In the pump-probe geometry, fully absorptive spectra are automatically acquired by measuring the sum of the rephasing and nonrephasing signals.

Atomic fluctuations in electronic materials revealed by dephasing.

The microscopic origin and timescale of the fluctuations of the energies of electronic states has a significant impact on the properties of interest of electronic materials, with implication in fields ranging from photovoltaic devices to quantum information processing. Spectroscopic investigations of coherent dynamics provide a direct measurement of electronic fluctuations. Modern multidimensional spectroscopy techniques allow the mapping of coherent processes along multiple time or frequency axes and thus allow unprecedented discrimination between different sources of electronic dephasing.

Anisotropic Nonequilibrium Lattice Dynamics of Black Phosphorus.

Black phosphorus has recently attracted significant attention for its highly anisotropic properties. A variety of ultrafast optical spectroscopies has been applied to probe the carrier response to photoexcitation, but the complementary lattice response has remained unaddressed. Here we employ femtosecond electron diffraction to explore how the structural anisotropy impacts the lattice dynamics after photoexcitation.

Investigating the electronic structure of confined multiexcitons with nonlinear spectroscopies.

Strong confinement in semiconductor quantum dots enables them to host multiple electron-hole pairs or excitons. The excitons in these materials are forced to interact, resulting in quantum-confined multiexcitons (MXs). The MXs are integral to the physics of the electronic properties of these materials and impact their key properties for applications such as gain and light emission.

Two-dimensional electronic spectroscopy reveals liquid-like lineshape dynamics in CsPbI perovskite nanocrystals.

Lead-halide perovskites have attracted tremendous attention, initially for their performance in thin film photovoltaics, and more recently for a variety of remarkable optical properties. Defect tolerance through polaron formation within the ionic lattice is a key aspect of these materials. Polaron formation arises from the dynamical coupling of atomic fluctuations to electronic states.

Investigating exciton structure and dynamics in colloidal CdSe quantum dots with two-dimensional electronic spectroscopy.

Two-Dimensional Electronic Spectroscopy (2DES) is performed on CdSe colloidal quantum dots. These experiments reveal new observations on exciton structure and dynamics in quantum dots, expanding upon prior transient absorption measurements of excitonics in these systems. The 2DES method enables the separation of line broadening mechanisms, thereby better revealing the excitonic lineshapes and biexcitonic interactions.

Pre-pregnancy and early pregnancy dietary behavior in relation to maternal and newborn health in the Norwegian Fit for Delivery study - a post hoc observational analysis.

Background: Randomized controlled trials targeting maternal dietary and physical activity behaviors during pregnancy have generally failed to accomplish reductions in the prevalence of adverse maternal and neonatal outcomes. Interventions carried out during pregnancy could thus be missing the mark in maximizing intervention health benefit.

Objective: To investigate whether and dietary behavior as reported at inclusion into the Norwegian Fit for Delivery (NFFD) trial was associated with maternal and neonatal outcomes irrespective of subsequent randomization assignment.

Seeing Multiexcitons through Sample Inhomogeneity: Band-Edge Biexciton Structure in CdSe Nanocrystals Revealed by Two-Dimensional Electronic Spectroscopy.

The electronic structure of multiexcitons significantly impacts the performance of nanostructures in lasing and light-emitting applications. However, these multiexcitons remain poorly understood due to their complexity arising from many-body physics. Standard transient-absorption and photoluminescence spectroscopies are unable to unambiguously distinguish effects of sample inhomogeneity from exciton-biexciton interactions.

Coherent multi-dimensional spectroscopy at optical frequencies in a single beam with optical readout.

Ultrafast coherent multi-dimensional spectroscopies form a powerful set of techniques to unravel complex processes, ranging from light-harvesting, chemical exchange in biological systems to many-body interactions in quantum-confined materials. Yet these spectroscopies remain complex to implement at the high frequencies of vibrational and electronic transitions, thereby limiting their widespread use. Here we demonstrate the feasibility of two-dimensional spectroscopy at optical frequencies in a single beam.

Evaluation of implementing a community-based exercise intervention during pregnancy.

Objective: to evaluate the implementation of a community-based exercise intervention (the Norwegian Fit for Delivery study) during pregnancy.

Design: descriptive, explorative.

Setting: healthcare clinics in southern Norway, including urban and rural settings.

Simple fiber-based solution for coherent multidimensional spectroscopy in the visible regime.

We report on a setup for coherent multidimensional spectroscopy based on visible continuum generation obtained by propagating 130 fs, <600  μJ pulses centered at 800 nm in a 2.5 m long hollow-core fiber. We find that with these modest input pulse requirements, the fiber can produce a stable, high brightness continuum spanning the 520-900 nm region, moreover in a single propagation step.