Ultrafast Imaging of Molecules with Electron Diffraction

Photoexcited molecules convert light into chemical and mechanical energy through changes in electronic and nuclear structure that take place on femtosecond timescales. Gas phase ultrafast electron diffraction (GUED) is an ideal tool to probe the nuclear geometry evolution of the molecules and complements spectroscopic methods that are mostly sensitive to the electronic state. GUED is a passive probing tool that does not alter the molecular properties during the probing process and is sensitive to the spatial distribution of charge in the molecule, including both electrons and nuclei. Improvements in temporal resolution have enabled GUED to capture coherent nuclear motions in molecules in the excited and ground electronic states with femtosecond and subangstrom resolution. Here we present the basic theory of GUED and explain what information is encoded in the diffraction signal, review how GUED has been used to observe coherent structural dynamics in recent experiments, and discuss the advantages and limitations of the method. Expected final online publication date for the Annual Review of Physical Chemistry, Volume 73 is April 2022. Please see http://www.annualreviews.org/page/journal/pubdates for revised estimates.

High-Resolution Microscopy to Learn the Nuclear Organization of the Living Yeast Cells

The spatial organization of the nucleus is a key determinant in all genome activities. However, the accurate measurement of the nuclear organization is still technically challenging. Here, the technology NucQuant we created previously was utilized to detect the variation of the nuclear organization, including the heterogeneity of the nuclear geometry, the change of the NPC distribution along different cell cycle stages during interphase, and the organization of the nucleolus. The results confirmed that not only the growth rate and the NPC distribution are influenced by the carbon source; the nuclear shape is also impacted by the carbon source. The nuclei lost their spherical geometry gradually when the cell was cultured from the most to a less favorable carbon source. We also discovered that the nucleolus prefers to locate at the nuclear periphery, which was called the “genes poor region,” especially when the cells entered quiescence. Furthermore, the distribution of the NPC along the different stages during the interphase was analyzed. We proposed that with the growth of the cell, the nucleus would grow from the surface of the NE flanking the nucleolus firstly.

Diabatic potential energy curves for the $$^4{\Pi} $$ states of SH

We present a diabatic representation of the potential energy curves (PECs) for the $$^4{{\Pi}} $$ 4 Π states of $$\mathrm {SH}$$ SH . Multireference, configuration interaction (MRCI) calculations were used to determine high-accuracy adiabatic PECs of both $$\mathrm {SH}$$ SH and $${\mathrm {SH}}^+$$ SH + from which the diabatic representation is constructed for $$\mathrm {SH}$$ SH . The adiabatic PECs exhibit many avoided crossings due to strong Rydberg-valence mixing. We employ the block diagonalization method, an orthonormal rotation of the adiabatic Hamiltonian, to disentangle the valence autoionizing and Rydberg $$^4\Pi $$ 4 Π states of $$\mathrm {SH}$$ SH by constructing a diabatic Hamiltonian. The diagonal elements of the diabatic Hamiltonian matrix at each nuclear geometry render the diabatic PECs and the off-diagonal elements are related to the state-to-state coupling. Care is taken to assure smooth variation and consistency of chemically significant molecular orbitals across the entire geometry domain.

Reduced-dimensional surface hopping with offline–online computations

Molecular dynamics simulations often classically evolve the nuclear geometry on adiabatic potential energy surfaces (PESs), punctuated by random hops between energy levels in regions of strong coupling, in an algorithm...

Search for Long-Range Correlations in Relativistic Heavy-Ion Collisions at SPS Energies

Long-range correlations are searched for by analysing the experimental data on16O-AgBr and32S-AgBr collisions at 200 A GeV/c and the results are compared with the predictions of a multi phase transport (AMPT) model. The findings reveal that the observed forward-backward (F-B) multiplicity correlations are mainly of short range in nature. The range of F-B correlations are observed to extend with increasing projectile mass. The observed extended range of F-B correlations might be due to overall multiplicity fluctuations arising because of nuclear geometry. The findings are not sufficient for making any definite conclusions regarding the presence of long-range correlations.