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A quantitative and predictive theory of quantum light-matter interactions in ultra thin materials involves several fundamental challenges. Any realistic model must simultaneously account for the ultra-confined plasmonic modes and their quantization i n the presence of losses, while describing the electronic states from first principles. Herein we develop such a framework by combining density functional theory (DFT) with macroscopic quantum electrodynamics, which we use to show Purcell enhancements reaching $10^7$ for intersubband transitions in few-layer transition metal dichalcogenides sandwiched between graphene and a perfect conductor. The general validity of our methodology allows us to put several common approximation paradigms to quantitative test, namely the dipole-approximation, the use of 1D quantum well model wave functions, and the Fermis Golden rule. The analysis shows that the choice of wave functions is of particular importance. Our work lays the foundation for practical ab initio-based quantum treatments of light matter interactions in realistic nanostructured materials.
The science and applications of electronics and optoelectronics have been driven for decades by progress in growth of semiconducting heterostructures. Many applications in the infrared and terahertz frequency range exploit transitions between quantiz ed states in semiconductor quantum wells (intersubband transitions). However, current quantum well devices are limited in functionality and versatility by diffusive interfaces and the requirement of lattice-matched growth conditions. Here, we introduce the concept of intersubband transitions in van der Waals quantum wells and report their first experimental observation. Van der Waals quantum wells are naturally formed by two-dimensional (2D) materials and hold unexplored potential to overcome the aforementioned limitations: They form atomically sharp interfaces and can easily be combined into heterostructures without lattice-matching restrictions. We employ near-field local probing to spectrally resolve and electrostatically control the intersubband absorption with unprecedented nanometer-scale spatial resolution. This work enables exploiting intersubband transitions with unmatched design freedom and individual electronic and optical control suitable for photodetectors, LEDs and lasers.
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