The duration of transient absorption spectroscopy measurements typically limits the types of systems for which the excited state dynamics can be measured. We present a single-shot transient absorption (SSTA) instrument with a spatially encoded 60 ps time delay range and a 100 nm spectral range that is capable of acquiring a transient spectrum in 20 s. We describe methods to spatially overlap the flat-top pump and probe beams at the sample plane, calibrate the spatially encoded time delay, and correct for non-uniform excitation density. SSTA measurements of organic materials in solution and film demonstrate this technique.
more »
« less
Single-shot transient absorption spectroscopy of an organic film
ABSTRACT We report single-shot transient absorption (SSTA) measurements of an organic film of 3,3’-Diethyloxatricarbocyanine iodide (DOTCI). In SSTA, the pump-probe time delay is spatially encoded by using a tilted pump pulse. Translation of the sample during SSTA measurements averages over any spatial heterogeneity in the film. We demonstrate that exciton dynamics measured with the single-shot technique agrees with traditional transient absorption measurements of the same film. A signal-to-noise ratio of ∼40 is achieved in 10 s. The ability to measure exciton dynamics in organic films will enable future SSTA measurements of exciton dynamics during the molecular aggregation events that result in film formation.
more »
« less
- Award ID(s):
- 1752129
- PAR ID:
- 10086522
- Date Published:
- Journal Name:
- MRS Advances
- Volume:
- 3
- Issue:
- 59
- ISSN:
- 2059-8521
- Page Range / eLocation ID:
- 3453 to 3457
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
A significant advantage of organic semiconductors over many of their inorganic counterparts is solution processability. However, solution processing commonly yields heterogeneous films with properties that are highly sensitive to the conditions and parameters of casting and processing. Measuring the key properties of these materials in situ, during film production, can provide new insight into the mechanism of these processing steps and how they lead to the emergence of the final organic film properties. The excited-state dynamics is often of import in photovoltaic, electronic, and light-emitting devices. This review focuses on single-shot transient absorption, which measures a transient spectrum in a single shot, enabling the rapid measurement of unstable chemical systems such as organic films during their casting and processing. We review the principles of instrument design and provide examples of the utility of this spectroscopy for measuring organic films during their production.more » « less
-
Understanding excitonic dynamics in two-dimensional semiconducting transition metal dichalcogenides is important for developing their optoelectronic applications. Recently, transient absorption techniques based on resonant excitonic absorption have been used to study various aspects of excitonic dynamics in these materials. The transient absorption in such measurements originates from phase-space state filling, bandgap renormalization, or screening effects. Here we report a new method to probe excitonic dynamics based on exciton intraband absorption. In this Drude-like process, probe photons are absorbed by excitons in their intraband excitation to higher energy states, causing a transient absorption signal. Although the magnitude of the transient absorption is lower than that of the resonant techniques, the new method is less restrictive on the selection of probe wavelength, has a larger linear range, and can provide complementary information on photocarrier dynamics. Using the WS 2 monolayer and bulk samples as examples, we show that the new method can probe exciton–exciton annihilation at high densities and reveal exciton formation processes. We also found that the exciton intraband absorption cross section of the WS 2 monolayer is on the order of 10 −18 cm 2 .more » « less
-
null (Ed.)Two-dimensional transition metal dichalcogenides (2D-TMDs) hold a great potential to platform future flexible optoelectronics. The beating hearts of these materials are their excitons known as XA and XB, which arise from transitions between spin-orbit split (SOS) levels in the conduction and valence bands at the K-point. The functionality of 2D-TMD-based devices is determined by the dynamics of these excitons. One of the most consequential channels of exciton decay on the device functionality is the defect-assisted recombination (DAR). Here, we employ steady-state absorption and emission spectroscopies, and pump density-dependent femtosecond transient absorption spectroscopy to report on the effect of DAR on the lifetime of excitons in monolayers of tungsten disulfide (2D-WS2) and diselenide (2D-WSe2). These pump-probe measurements suggested that while exciton decay dynamics in both monolayers are driven by DAR, in 2D-WS2, defect states near the XB exciton fill up before those near the XA exciton. However, in the 2D-WSe2 monolayer, the defect states fill up similarly. Understanding the contribution of DAR on the lifetime of excitons and the partition of this decay channel between XA and XB excitons may open new horizons for the incorporation of 2D-TMD materials in future optoelectronics.more » « less