Broadband micro-transient absorption spectroscopy enabled by improved lock-in amplification.

Recent breakthroughs in material development have increased the demand for characterization methods capable of probing nanoscale features on ultrafast time scales. As the sample reduces to atomically thin levels, an extremely low-level signal limits the feasibility of many experiments. Here, we present an affordable and easy-to-implement solution to expand the maximum sensitivity of lock-in detection systems used in transient absorption spectroscopy by multiple orders of magnitude. By implementation of a tuned RC circuit to the output of an avalanche photodiode, electric pulse shaping allows for vastly improved lock-in detection. Furthermore, a carefully designed "peak detector" circuit provides additional pulse shaping benefits, resulting in even more lock-in detection signal enhancement. We demonstrate the improvement of lock-in detection with each of these schemes by performing benchmark measurements of a white-light continuum signal and micro-transient absorption spectroscopy on a few-layer transition metal dichalcogenide sample. Our results show the practicality of ultrafast pump-probe spectroscopy for many high-sensitivity experimental schemes.

Reversible Photoluminescence Tuning by Defect Passivation via Laser Irradiation on Aged Monolayer MoS2.

Atomically thin (1L)-MoS2 emerged as a direct band gap semiconductor with potential optical applications. The photoluminescence (PL) of 1L-MoS2 degrades due to aging-related defect formation. The passivation of these defects leads to substantial improvement in optical properties. Here, we report the enhancement of PL on aged 1L-MoS2 by laser treatment. Using photoluminescence and Raman spectroscopy in a gas-controlled environment, we show that the enhancement is associated with efficient adsorption of oxygen on existing sulfur vacancies preceded by removal of adsorbates from the sample's surface. Oxygen adsorption depletes negative charges, resulting in suppression of trions and improved neutral exciton recombination. The result is a 6- to 8-fold increase in PL emission. The laser treatment in this work does not cause any measurable damage to the sample as verified by Raman spectroscopy, which is important for practical applications. Surprisingly, the observed PL enhancement is reversible by both vacuum and ultrafast femtosecond excitation. While the former approach allows switching a designed micropattern on the sample ON and OFF, the latter provides a controllable mean for accurate PL tuning, which is highly desirable for optoelectronic and gas sensing applications.

Dense Electron-Hole Plasma Formation and Ultralong Charge Lifetime in Monolayer MoS2 via Material Tuning.

Many-body interactions in photoexcited semiconductors can bring about strongly interacting electronic states, culminating in the fully ionized matter of electron-hole plasma (EHP) and electron-hole liquid (EHL). These exotic phases exhibit unique electronic properties, such as metallic conductivity and metastable high photoexcitation density, which can be the basis for future transformative applications. However, the cryogenic condition required for its formation has limited the study of dense plasma phases to a purely academic pursuit in a restricted parameter space. This paradigm can potentially change with the recent experimental observation of these phases in atomically thin MoS2 and MoTe2 at room temperature. A fundamental understanding of EHP and EHL dynamics is critical for developing novel applications on this versatile layered platform. In this work, we studied the formation and dissipation of EHP in monolayer MoS2. Unlike previous results in bulk semiconductors, our results reveal that electromechanical material changes in monolayer MoS2 during photoexcitation play a significant role in dense EHP formation. Within the free-standing geometry, photoexcitation is accompanied by an unconstrained thermal expansion, resulting in a direct-to-indirect gap electronic transition at a critical lattice spacing and fluence. This dramatic altering of the material's energetic landscape extends carrier lifetimes by 2 orders of magnitude and allows the density required for EHP formation. The result is a stable dense plasma state that is sustained with modest optical photoexcitation. Our findings pave the way for novel applications based on dense plasma states in two-dimensional semiconductors.