Having it all: spatiotemporally discerning charge and heat in energy transduction and nanoscale transport

Weaver, Hannah L.; Went, Cora M.; Jasrasaria, Dipti; Wong, Joeson; Rabani, Eran; Atwater, Harry A.; Ginsberg, Naomi S.

doi:10.1117/12.2633940

Cited by 2 publications

(2 citation statements)

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“…This focused-pump setup can enable more delicate studies of charge and heat flow, complementing previous research focusing on the ps-to-ns time range. 53 We anticipate that the dual-hyperspectral PPM setup introduced in this study will open new avenues for investigating charge, heat, and spin transport in various materials including inorganic and hybrid semiconductors, organic and soft materials, magnetic materials, and 2D heterostructures.…”

Section: ■ Conclusionmentioning

confidence: 96%

Dual-Hyperspectral Optical Pump–Probe Microscopy with Single-Nanosecond Time Resolution

Li,

Xu,

Kocoj

et al. 2024

J. Am. Chem. Soc.

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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 up to 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 nanoseconds to milliseconds and single-nanosecond resolution. Our method features a wide-field probe tunable from 370 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-band gap electronic pump excitation and below-band gap 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-nanosecond 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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Section: ■ Conclusionmentioning

confidence: 96%

Dual-Hyperspectral Optical Pump–Probe Microscopy with Single-Nanosecond Time Resolution

Li,

Xu,

Kocoj

et al. 2024

J. Am. Chem. Soc.

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“…These diffusing species -charge versus heat -give rise to a different sign of the transient signal, which makes it easy to distinguish them (Figure 6a). With the same technique, the thermal diffusivity of hBN-encapsulated MoS 2 [59] and disordered films of gold nanocrystals [60] were measured recently.…”

Section: "Normal" Diffusion Of Phonon and Electron Heatmentioning

confidence: 99%

Spatiotemporal Microscopy: Shining Light on Transport Phenomena

Vazquez,

Morganti,

Block

et al. 2023

Adv Elect Materials

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Transport phenomena like diffusion, convection, and drift play key roles in the sciences and engineering disciplines. They belong to the most omnipresent and important phenomena in nature that describe the motion of entities such as mass, charge or heat. Understanding and controlling these transport phenomena is crucial for a host of industrial technologies and applications, from cooling nuclear reactors to nanoscale heat‐management in the semiconductor industry. For decades, macroscopic transport techniques have been used to access important parameters such as charge mobilities or thermal conductivities. While being powerful, they often require physical contacts, which can lead to unwanted effects. Over the past years, an exciting solution has emerged: a technique called spatiotemporal microscopy (SPTM) that accesses crucial transport phenomena in a contactless, all‐optical, fashion. This technique offers powerful advantages in terms of accessible timescales, down to femtoseconds, and length scales, down to nanometres, and, further, selectively observes different species of interest. This tutorial review discusses common experimental configurations of SPTM and explains how they can be implemented by those entering the field. This review highlights the broad applicability of SPTM by presenting several exciting examples of transport phenomena that were unravelled thanks to this technique.

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Having it all: spatiotemporally discerning charge and heat in energy transduction and nanoscale transport

Cited by 2 publications

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Dual-Hyperspectral Optical Pump–Probe Microscopy with Single-Nanosecond Time Resolution

Dual-Hyperspectral Optical Pump–Probe Microscopy with Single-Nanosecond Time Resolution

Spatiotemporal Microscopy: Shining Light on Transport Phenomena

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