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In recent years, optical pump-probe microscopy (PPM) has become a vital technique for spatiotemporally imaging electronic excitations and charge-carrier transport in metals and semiconductors. However, existing methods are limited by mechanical delay lines with a probe time window of only several nanoseconds (ns), or monochromatic pump and probe sources with restricted spectral coverage and temporal resolution, hindering their amenability in studying relatively slow processes. To bridge these gaps, we introduce a dual-hyperspectral PPM setup with a time window spanning from ns to milliseconds and single-ns resolution. Our method features a wide-field probe tunable from 370 nm to 1000 nm and a pump spanning from 330 nm to 16 µm. We apply this PPM technique to study various two-dimensional metal-halide perovskites (2D-MHPs) as representative semiconductors by imaging their transient responses near the exciton resonances under both above-bandgap, electronic pump excitation, and below-bandgap, vibrational pump excitation. The resulting spatially- and temporally-resolved images reveal insights into heat dissipation, film uniformity, distribution of impurity phases, and film-substrate interfaces. In addition, the single-ns temporal resolution enables the imaging of in-plane strain wave propagation in 2D-MHP single crystals. Our method, which offers extensive spectral tunability and significantly improved time resolution, opens new possibilities for the imaging of charge carriers, heat, and transient phase transformation processes, particularly in materials with spatially-varying composition, strain, crystalline structure, and interfaces.
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An oscillator-driven, time-resolved optical pump/NIR supercontinuum probe spectrometer
We present a novel, to the best of knowledge, time-resolved, optical pump/NIR supercontinuum probe spectrometer suitable for oscillators. A NIR supercontinuum probe spectrum (850–1250 nm) is generated in a photonic crystal fiber, dispersed across a digital micromirror device (DMD), and then raster scanned into a single element detector at a 5 Hz rate. Dual modulation of pump and probe beams at disparate frequencies permits simultaneous measurement of both the bare reflectance R and its photoinduced change Δ R through lock-in detection, allowing for continuously self-normalized measurement of Δ R / R . Example data are presented on a germanium wafer sample that demonstrate for signals of order Δ R / R ∼ 10 −3 , a 2.87 nm spectral resolution and ≲ 400 fs temporal resolution pre-recompression, and comparable sensitivity to standard time-resolved, amplifier-based pump–probe techniques.
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- Award ID(s):
- 1945222
- PAR ID:
- 10416032
- Date Published:
- Journal Name:
- Optics Letters
- Volume:
- 48
- Issue:
- 3
- ISSN:
- 0146-9592
- Page Range / eLocation ID:
- 570
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
-
Accepted Manuscript
- Journal Article:
- https://doi.org/10.1364/OL.479061
