Carrier interactions in 2D nanostructures are of central importance not only in condensed‐matter physics but also for a wide range of optoelectronic and photonic applications. Here, new insights into the behavior of photoinduced carriers in layered platinum diselenide (PtSe2) through ultrafast time‐resolved pump–probe and nonlinear optical measurements are presented. The measurements reveal the temporal evolution of carrier relaxation, chemical potential and bandgap renormalization in PtSe2. These results imply that few‐layer PtSe2 has a semiconductor‐like carrier relaxation instead of a metal‐like one. The relaxation follows a triple‐exponential decay process and exhibits thickness‐dependent relaxation times. This occurs along with a band‐filling effect, which can be controlled based on the number of layers and may be applied in saturable absorption for generating ultrafast laser pulses. The findings may provide means to study many‐body physics in 2D materials as well as potentially leading to applications in the field of optoelectronics and ultrafast photonics.
Lasers, photovoltaics, and thermoelectrically-pumped light emitting diodes are thermodynamic machines which use excitons (electron-hole pairs) as the working medium. The heat transfers in such devices are highly irreversible, leading to low efficiencies. Here we predict that reversible heat transfers between a quantum-dot exciton and its phonon environment can be induced by laser pulses. We calculate the heat transfer when a quantum-dot exciton is driven by a chirped laser pulse. The reversibility of this heat transfer is quantified by the efficiency of a heat engine in which it forms the hot stroke, which we predict to reach 95% of the Carnot limit. This performance is achieved by using the time-dependent laser-dressing of the exciton to control the heat current and exciton temperature. We conclude that reversible heat transfers can be achieved in excitonic thermal machines, allowing substantial improvements in their efficiency.
Solids can be cooled by driving impurity ions with lasers, allowing them to transfer heat from the lattice phonons to the electromagnetic surroundings. This exemplifies a quantum thermal machine, which uses a quantum system as a working medium to transfer heat between reservoirs. We review the derivation of the Bloch-Redfield equation for a quantum system coupled to a reservoir, and its extension, using counting fields, to calculate heat currents. We use the full form of this equation, which makes only the weak-coupling and Markovian approximations, to calculate the cooling power for a simple model of laser cooling. We compare its predictions with two other time-local master equations: the secular approximation to the full Bloch-Redfield equation, and the Lindblad form expected for phonon transitions in the absence of driving. We conclude that the full Bloch-Redfield equation provides accurate results for the heat current in both the weak- and strong- driving regimes, whereas the other forms have more limited applicability. Our results support the use of Bloch-Redfield equations in quantum thermal machines, despite their potential to give unphysical results.
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