By utilizing a nanometer ultrafast electron source in a point projection microscope we demonstrate that images of nanoparticles with spatial resolutions of the order of 100 nanometers can be obtained. The duration of the emission process of the photoemitted electrons used to make images is shown to be of the order of 100 fs using an autocorrelation technique. The compact geometry of this photoelectron point projection microscope does not preclude its use as a simple ultrafast electron microscope, and we use simple analytic models to estimate temporal resolutions that can be expected when using it as a pump-probe ultrafast electron microscope. These models show a significant increase in temporal resolution when comparing to ultrafast electron microscopes based on conventional designs. We also model the microscopes spectroscopic abilities to capture ultrafast phenomena such as the photon induced near field effect.
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http://dx.doi.org/10.1063/1.4827035 | DOI Listing |
J Phys Chem Lett
January 2025
MOE Key Laboratory for Non-equilibrium Synthesis and Modulation of Condensed Matter, School of Physics, Xi'an Jiaotong University, Xi'an 710049, China.
The ultrafast excited-state dynamics of endohedral fullerenes are crucial in their photophysical and photochemical processes when they are employed as photovoltaic devices, photocatalytic devices, and single-molecule devices. In this study, by employing the non-adiabatic molecular dynamics simulations based on the time-dependent Kohn-Sham (TD-KS) method, we theoretically studied the size effect on ultrafast excited-state decay dynamics of the photoexcited Be electron in endohedral fullerenes Be@C (2 = 60, 70, and 80). These excited-state decay dynamics, which involve the charge-transfer process, occur in an ultrafast time scale of about 3 ps.
View Article and Find Full Text PDFNanomaterials (Basel)
January 2025
Hunan Key Laboratory of Super-Microstructure and Ultrafast Process, School of Physics, Central South University, Changsha 410083, China.
Two-dimensional (2D) layered materials have received much attention due to the unique properties stemming from their van der Waals (vdW) interactions, quantum confinement, and many-body interactions of quasi-particles, which drive their exotic optical and electronic properties, making them critical in many applications. Here, we review our past years' findings, focusing on many-body interactions in 2D layered materials, including phonon anharmonicity, electron-phonon coupling (), exciton dynamics, and phonon anisotropy based on temperature (polarization)-dependent Raman spectroscopy and Photoluminescence (PL). Our review sheds light on the role of quasi-particles in tuning the material properties, which could help optimize 2D materials for future applications in electronic and optoelectronic devices.
View Article and Find Full Text PDFACS Nano
January 2025
James Franck Institute, University of Chicago, Chicago, Illinois 60637, United States.
Phonon dynamics and transport determine how heat is utilized and dissipated in materials. In 2D systems for optoelectronics and thermoelectrics, the impact of nanoscale material structure on phonon propagation is central to controlling thermal conduction. Here, we directly observe in-plane coherent acoustic phonon propagation in black phosphorus (BP) using ultrafast electron microscopy.
View Article and Find Full Text PDFPNAS Nexus
January 2025
The Harrison M. Randall Laboratory of Physics, University of Michigan, Ann Arbor, MI 48109-1040, USA.
The direct, ultrafast excitation of polar phonons with electromagnetic radiation is a potent strategy for controlling the properties of a wide range of materials, particularly in the context of influencing their magnetic behavior. Here, we show that, contrary to common perception, the origin of phonon-induced magnetic activity does not stem from the Maxwellian fields resulting from the motion of the ions themselves or the effect their motion exerts on the electron subsystem. Through the mechanism of electron-phonon coupling, a coherent state of circularly polarized phonons generates substantial non-Maxwellian fields that disrupt time-reversal symmetry, effectively emulating the behavior of authentic magnetic fields.
View Article and Find Full Text PDFNanoscale Adv
January 2025
Department of Chemical Sciences, University of Padova via Marzolo 1 35131 Padova Italy
In this study, we used two-dimensional electronic spectroscopy to examine the early femtosecond dynamics of suspensions of colloidal gold nanorods with different aspect ratios. In all samples, the signal distribution in the 2D maps at this timescale shows a distinctive dispersive behavior, which can be explained by the interference between the exciting field and the field produced on the nanoparticle's surface by the collective motion of electrons when the plasmon is excited. Studying this interference effect, which is active only until the plasmon has been dephased, allows for a direct estimation of the dephasing time of the plasmon of an ensemble of colloidal particles.
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