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Pavel K. Olshin

Publications and source records attributed to Pavel K. Olshin.

4 recordsLinked to original sources

Crossed laser phase plates for transmission electron microscopy

For decades since the development of phase-contrast optical microscopy, an analogous approach has been sought for maximizing the image contrast of weakly-scattering objects in transmission electron microscopy (TEM). The recent development of the laser phase plate (LPP) has demonstrated that an amplified, focused laser standing wave provides stable, tunable phase shift to the high-energy electron beam, achieving phase-contrast TEM. Building on proof-of-concept experimental demonstrations, this paper explores design improvements tailored to biological imaging. In particular, we introduce the approach of crossed laser phase plates (XLPP): two laser standing waves intersecting in the diffraction plane of the TEM, rather than a single beam as in the current LPP. We provide a theoretical model for the XLPP inside the microscope and use simulations to quantify its effect on image formation. Using simulations, we find that the XLPP increases information transfer at low spatial frequencies while also suppressing the ghost images formed by Kapitza-Dirac diffraction of the electron beam by the laser beam. We also present a simple acquisition scheme, enabled by the XLPP, which dramatically suppresses unwanted diffraction effects. Finally, we discuss important practical considerations of XLPP design and show experimental results from a prototype. The results of this study chart the course for future developments of LPP hardware.

physics.optics↗

In Situ Melting and Revitrification as an Approach to Microsecond Time-Resolved Cryo-Electron Microscopy

Proteins typically undergo conformational dynamics on the microsecond to millisecond timescale as they perform their function, which is much faster than the time-resolution of cryo-electron microscopy and has thus prevented real-time observations. Here, we propose a novel approach for microsecond time-resolved cryo-electron microscopy that involves rapidly melting a cryo specimen in situ with a laser beam. The sample remains liquid for the duration of the laser pulse, offering a tunable time window in which the dynamics of embedded particles can be induced in their native liquid environment. After the laser pulse, the sample vitrifies in just a few microseconds, trapping particles in their transient configurations, so that they can subsequently be characterized with conventional cryo-electron microscopy. We demonstrate that our melting and revitrification approach is viable and affords microsecond time resolution. As a proof of principle, we study the disassembly of particles after they incur structural damage and trap them in partially unraveled configurations.

physics.bio-ph↗

Time-resolved inner-shell photoelectron spectroscopy: from a bound molecule to an isolated atom

Due to its element- and site-specificity, inner-shell photoelectron spectroscopy is a widely used technique to probe the chemical structure of matter. Here we show that time-resolved inner-shell photoelectron spectroscopy can be employed to observe ultrafast chemical reactions and the electronic response to the nuclear motion with high sensitivity. The ultraviolet dissociation of iodomethane (CH$_3$I) is investigated by ionization above the iodine 4d edge, using time-resolved inner-shell photoelectron and photoion spectroscopy. The dynamics observed in the photoelectron spectra appear earlier and are faster than those seen in the iodine fragments. The experimental results are interpreted using crystal field and spin-orbit configuration interaction calculations, and demonstrate that time-resolved inner-shell photoelectron spectroscopy is a powerful tool to directly track ultrafast structural and electronic transformations in gas-phase molecules.

physics.chem-ph↗

Coulomb explosion imaging of concurrent CH$_{2}$BrI photodissociation dynamics

The dynamics following laser-induced molecular photodissociation of gas-phase CH$_{2}$BrI at 271.6 nm were investigated by time-resolved Coulomb explosion imaging using intense near-IR femtosecond laser pulses. The observed delay-dependent photofragment momenta reveal that CH$_{2}$BrI undergoes C-I cleavage, depositing 65.6% of the available energy into internal product states, and that absorption of a second UV photon breaks the C-Br bond of CH$_{2}$Br. Simulations confirm that this mechanism is consistent with previous data recorded at 248 nm, demonstrating the sensitivity of Coulomb explosion imaging as a real-time probe of chemical dynamics.

physics.chem-ph↗