While
the properties of surfaces and interfaces are crucial to
modern devices, they are commonly difficult to explore since the signal
from the bulk often masks the surface contribution. Here we introduce
a methodology based on scanning electron microscopy (SEM) coupled
with a pulsed laser source, which offers the capability to sense the
topmost layer of materials, to study the surface photovoltage (SPV)
related effects. This method relies on a pulsed optical laser to transiently
induce an SPV and a continuous primary electron beam to produce secondary
electron (SE) emission and monitor the change of the SE yield under
laser illumination. We observe contrasting behaviors of the SPV-induced
SE yield change on n-type and p-type semiconductors. We further study
the dependence of the SPV-induced SE yield on the primary electron
beam energy, the optical fluence, and the modulation frequency of
the optical excitation, which reveal the details of the dynamics of
the photocarriers in the presence of the surface built-in potential.
This fast, contactless, and bias-free technique offers a convenient
and robust platform to probe surface electronic phenomena, with great
promise to probe nanoscale effects with a high spatial resolution.
Our result further provides a basis to understand the contrast mechanisms
of emerging time-resolved electron microscopic techniques, such as
the scanning ultrafast electron microscopy.
Organic-inorganic hybrid perovskites exhibiting exceptional photovoltaic and optoelectronic properties are of fundamental and practical interest, owing to their tunability and low manufacturing cost. For practical applications, however, challenges such as material instability and the photocurrent hysteresis occurring in perovskite solar cells under light exposure need to be understood and addressed. While extensive investigations have suggested that ion migration is a plausible origin of these detrimental effects, detailed understanding of the ion migration pathways remains elusive. Here, we report the characterization of photo-induced ion migration in perovskites using in situ laser illumination inside a scanning electron microscope, coupled with secondary electron imaging, energy-dispersive X-ray spectroscopy and cathodoluminescence with varying primary electron energies. Using methylammonium lead iodide and formamidinium lead iodide as model systems, we observed photo-induced long-range migration of halide ions over hundreds of micrometers and elucidated the transport pathways of various ions both near the surface and inside the bulk of the samples, including a surprising finding of the vertical migration of lead ions. Our study provides insights into ion migration processes in perovskites that can aid perovskite material design and processing in future applications.
Understanding the optoelectronic properties of semiconducting polymers under external strain is essential for their applications in flexible devices. Although prior studies have highlighted the impact of static and macroscopic strains, assessing the effect of a local transient deformation before structural relaxation occurs remains challenging. Here, we employ scanning ultrafast electron microscopy (SUEM) to image the dynamics of a photoinduced transient strain in the semiconducting polymer poly(3-hexylthiophene) (P3HT). We observe that the photoinduced SUEM contrast, corresponding to the local change of secondary electron emission, exhibits an unusual ring-shaped profile. We attribute the observation to the electronic structure modulation of P3HT caused by a photoinduced strain field owing to its low modulus and strong electron−lattice coupling, supported by a finite-element analysis. Our work provides insights into tailoring optoelectronic properties using transient mechanical deformation in semiconducting polymers and demonstrates the versatility of SUEM to study photophysical processes in diverse materials.
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