Abstract:Transient absorption (TA) spectroscopy has been extensively used in the study of excited state dynamics of various materials and molecules. The transition from TA spectroscopy to TA microscopy, which enables the space-resolved measurement of TA, is opening new investigations toward a more complete picture of excited state dynamics in functional materials, as well as the mapping of crucial biopigments for precision diagnosis. Here, we review the recent instrumental advancement that is pushing the limit of spati… Show more
“…The charge carrier behavior depends on the local structure and is inhomogeneous in nature for the photocatalysts, typically composed of calcinated particles and aggregates. Many studies have been devoted to studying the spatio-temporal behavior of charge carrier dynamics using TA and photoluminescence microscopy on micro-scales 36 – 38 as well as the photocurrent behavior via microscopic photo-electrochemical measurements 39 , 40 . We also have extended our measurements of the refractive index change to the local mapping of the transient responses of photo-excited charge carriers (pattern-illumination phase microscopy (PI-PM)).…”
Photocatalytic water splitting system using particulate semiconductor materials is a promising strategy for converting solar energy into hydrogen and oxygen. In particular, visible-light-driven ‘Z-scheme’ printable photocatalyst sheets are cost-effective and scalable. However, little is known about the fundamental photophysical processes, which are key to explaining and promoting the photoactivity. Here, we applied the pattern-illumination time-resolved phase microscopy for a photocatalyst sheet composed of Mo-doped BiVO4 and Rh-doped SrTiO3 with indium tin oxide as the electron mediator to investigate photo-generated charge carrier dynamics. Using this method, we successfully observed the position- and structure-dependent charge carrier behavior and visualized the active/inactive sites in the sheets under the light irradiation via the time sequence images and the clustering analysis. This combination methodology could provide the material/synthesis optimization methods for the maximum performance of the photocatalyst sheets.
“…The charge carrier behavior depends on the local structure and is inhomogeneous in nature for the photocatalysts, typically composed of calcinated particles and aggregates. Many studies have been devoted to studying the spatio-temporal behavior of charge carrier dynamics using TA and photoluminescence microscopy on micro-scales 36 – 38 as well as the photocurrent behavior via microscopic photo-electrochemical measurements 39 , 40 . We also have extended our measurements of the refractive index change to the local mapping of the transient responses of photo-excited charge carriers (pattern-illumination phase microscopy (PI-PM)).…”
Photocatalytic water splitting system using particulate semiconductor materials is a promising strategy for converting solar energy into hydrogen and oxygen. In particular, visible-light-driven ‘Z-scheme’ printable photocatalyst sheets are cost-effective and scalable. However, little is known about the fundamental photophysical processes, which are key to explaining and promoting the photoactivity. Here, we applied the pattern-illumination time-resolved phase microscopy for a photocatalyst sheet composed of Mo-doped BiVO4 and Rh-doped SrTiO3 with indium tin oxide as the electron mediator to investigate photo-generated charge carrier dynamics. Using this method, we successfully observed the position- and structure-dependent charge carrier behavior and visualized the active/inactive sites in the sheets under the light irradiation via the time sequence images and the clustering analysis. This combination methodology could provide the material/synthesis optimization methods for the maximum performance of the photocatalyst sheets.
“…The high spectral density of the MPC allows for experiments which were previously impossible. Three examples of measurements where this technique is valuable are materials with a high absorption coefficient 36 , frequency domain interferometry (FDI) 37 , 38 and spatial-resolved transient absorption spectroscopy 39 , 40 . Highly absorbing materials are often restricted to reflection experiments as the transmitted probe is too weak to detect.…”
Ultrafast transient absorption spectroscopy is a powerful tool to reveal excited state dynamics in various materials. Conventionally, probe pulses are generated via bulk supercontinuum generation or (noncollinear) optical parametric amplifiers whilst pump pulses are generated separately using (noncollinear) optical parametric amplifiers. These systems are limited by either their spectral density, stability, spectral range, and/or temporal compressibility. Recently, a new intense broadband light source is being developed, the multi-plate compression, which promises to overcome these limitations. In this paper, we analyze the supercontinuum generated by a single Multiple Plate Compression system to set a benchmark for its use in the field of ultrafast pump-probe spectroscopy. We have compressed the supercontinuum to 3.3 fs using chirp mirrors alone, making it an excellent candidate for pump-probe experiments requiring high temporal resolution. Furthermore, the single light source can be used to generate both probe and pump pulses due to its high spectral density (>14.5 nJ/nm) between 490 and 890 nm. The intensity has an average shot-to-shot relative standard deviation of 4.6 % over 490 to 890 nm, calculated over 2,000 sequential shots. By using only 1,000 shot pairs, a $$\Delta T/T$$
Δ
T
/
T
noise level of $$2.6\times 10^{-4}$$
2.6
×
10
-
4
RMS is achieved. Finally, as a proof of concept, the transient absorption spectrum of a methylammonium lead iodide perovskite film is taken, showing great signal to noise with only 1,000 shot pairs. These results show great potential for the employment of this technique in other spectroscopic techniques such as coherent multidimensional spectroscopy.
“…[12] Despite its tremendous utility,P Ps pectroscopy has its limitations.B ecause signal changes are detected against the bright background of the probe pulse,a ccurate detection is difficult in samples producing weak signals,s uch as highly dilute solutions.T his has also been am ajor limitation of transient absorption microscopy. [13] PP spectroscopy is also problematic in highly scattering samples,asthe scattered light is difficult to suppress,e specially when the pump and probe spectra overlap. [14] In some samples,the excited-state absorption overlaps heavily with the ground-state-transition signals, making the contributions difficult to disentangle.F inally,f or ultrafast dynamics,o ff-resonant signals such as solvent response or cross-phase modulation overlay the system dynamics,t ogether comprising the so-called coherent artifact.…”
Section: Introductionmentioning
confidence: 99%
“…This has also been a major limitation of transient absorption microscopy. [13] PP spectroscopy is also problematic in highly scattering samples, as the scattered light is difficult to suppress, especially when the pump and probe spectra overlap. [14] In some samples, the excited‐state absorption overlaps heavily with the ground‐state‐transition signals, making the contributions difficult to disentangle.…”
We introduce an ew approach to transient spectroscopy, fluorescence-detected pump-probe (F-PP) spectroscopy, that overcomes several limitations of traditional PP.F -PP suppresses excited-state absorption, provides background-free detection, removes artifacts resulting from pump-pulse scattering, from non-resonant solvent response,o rf rom coherent pulse overlap,a nd allows unique extraction of excited-state dynamics under certain conditions.D espite incoherent detection, time resolution of F-PP is given by the duration of the laser pulses,i ndependent of the fluorescence lifetime.W e describe the working principle of F-PP and provide its theoretical description. Then we illustrate specific features of F-PP by direct comparison with PP,t heoretically and experimentally.F or this purpose,w ei nvestigate,w ith both techniques,amolecular squaraine heterodimer,c ore-shell CdSe/ ZnS quantum dots,a nd fluorescent protein mCherry.F -PP is broadly applicable to chemical systems in various environments and in different spectral regimes.
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