CVD-Grown Monolayer MoS2 and GaN Thin Film Heterostructure for a Self-Powered and Bidirectional Photodetector with an Extended Active Spectrum.

Photodetector technology has evolved significantly over the years with the emergence of new active materials. However, there remain trade-offs between spectral sensitivity, operating energy, and, more recently, an ability to harbor additional features such as persistent photoconductivity and bidirectional photocurrents for new emerging application areas such as switchable light imaging and filter-less color discrimination. Here, we demonstrate a self-powered bidirectional photodetector based on molybdenum disulfide/gallium nitride (MoS2/GaN) epitaxial heterostructure. This fabricated detector exhibits self-powered functionality and achieves detection in two discrete wavelength bands: ultraviolet and visible. Notably, it attains a peak responsivity of 631 mAW-1 at a bias of 0V. The device's response to illumination at these two wavelengths is governed by distinct mechanisms, activated under applied bias conditions, thereby inducing a reversal in the polarity of the photocurrent. This work underscores the feasibility of self-powered and bidirectional photocurrent detection but also opens new vistas for technological advancements for future optoelectronic, neuromorphic, and sensing applications.

Effects of Floquet Engineering on the Coherent Exciton Dynamics in Monolayer WS2.

Coherent optical manipulation of electronic bandstructures via Floquet Engineering is a promising means to control quantum systems on an ultrafast time scale. However, the ultrafast switching on/off of the driving field comes with questions regarding the limits of the Floquet formalism (which is defined for an infinite periodic drive) through the switching process and to what extent the transient changes can be driven adiabatically. Experimentally addressing these questions has been difficult, in large part due to the absence of an established technique to measure coherent dynamics through the duration of the pulse. Here, using multidimensional coherent spectroscopy we explicitly excite, control, and probe a coherent superposition of excitons in the K and K' valleys in monolayer WS2. With a circularly polarized, red-detuned pump pulse, the degeneracy of the K and K' excitons can be lifted, and the phase of the coherence rotated. We directly measure phase rotations greater than π during the 100 fs driving pulse and show that this can be described by a combination of the AC-Stark shift of excitons in one valley and the Bloch-Siegert shift of excitons in the opposite valley. Despite showing a smooth evolution of the phase that directly follows the intensity envelope of the nonresonant pump pulse, the process is not perfectly adiabatic. By measuring the magnitude of the macroscopic coherence as it evolves before, during, and after the nonresonant pump pulse we show that there is additional decoherence caused by power broadening in the presence of the nonresonant pump. This nonadiabaticity arises as a result of interactions with the otherwise adiabatic Floquet states and may be a problem for many applications, such as manipulating qubits in quantum information processing; however, these measurements also suggest ways such effects can be minimized or eliminated.

Interactions between Fermi polarons in monolayer WS2.

Interactions between quasiparticles are of fundamental importance and ultimately determine the macroscopic properties of quantum matter. A famous example is the phenomenon of superconductivity, which arises from attractive electron-electron interactions that are mediated by phonons or even other more exotic fluctuations in the material. Here we introduce mobile exciton impurities into a two-dimensional electron gas and investigate the interactions between the resulting Fermi polaron quasiparticles. We employ multi-dimensional coherent spectroscopy on monolayer WS2, which provides an ideal platform for determining the nature of polaron-polaron interactions due to the underlying trion fine structure and the valley specific optical selection rules. At low electron doping densities, we find that the dominant interactions are between polaron states that are dressed by the same Fermi sea. In the absence of bound polaron pairs (bipolarons), we show using a minimal microscopic model that these interactions originate from a phase-space filling effect, where excitons compete for the same electrons. We furthermore reveal the existence of a bipolaron bound state with remarkably large binding energy, involving excitons in different valleys cooperatively bound to the same electron. Our work lays the foundation for probing and understanding strong electron correlation effects in two-dimensional layered structures such as moiré superlattices.

Supertransport of excitons in atomically thin organic semiconductors at the 2D quantum limit.

Long-range and fast transport of coherent excitons is important for the development of high-speed excitonic circuits and quantum computing applications. However, most of these coherent excitons have only been observed in some low-dimensional semiconductors when coupled with cavities, as there are large inhomogeneous broadening and dephasing effects on the transport of excitons in their native states in materials. Here, by confining coherent excitons at the 2D quantum limit, we first observed molecular aggregation-enabled 'supertransport' of excitons in atomically thin two-dimensional (2D) organic semiconductors between coherent states, with a measured high effective exciton diffusion coefficient of ~346.9 cm2/s at room temperature. This value is one to several orders of magnitude higher than the values reported for other organic molecular aggregates and low-dimensional inorganic materials. Without coupling to any optical cavities, the monolayer pentacene sample, a very clean 2D quantum system (~1.2 nm thick) with high crystallinity (J-type aggregation) and minimal interfacial states, showed superradiant emission from Frenkel excitons, which was experimentally confirmed by the temperature-dependent photoluminescence (PL) emission, highly enhanced radiative decay rate, significantly narrowed PL peak width and strongly directional in-plane emission. The coherence in monolayer pentacene samples was observed to be delocalised over ~135 molecules, which is significantly larger than the values (a few molecules) observed for other organic thin films. In addition, the supertransport of excitons in monolayer pentacene samples showed highly anisotropic behaviour. Our results pave the way for the development of future high-speed excitonic circuits, fast OLEDs, and other optoelectronic devices.

Persistent coherence of quantum superpositions in an optimally doped cuprate revealed by 2D spectroscopy.

Quantum materials displaying intriguing magnetic and electronic properties could be key to the development of future technologies. However, it is poorly understood how the macroscopic behavior emerges in complex materials with strong electronic correlations. While measurements of the dynamics of excited electronic populations have been able to give some insight, they have largely neglected the intricate dynamics of quantum coherence. Here, we apply multidimensional coherent spectroscopy to a prototypical cuprate and report unprecedented coherent dynamics persisting for ~500 fs, originating directly from the quantum superposition of optically excited states separated by 20 to 60 meV. These results reveal that the states in this energy range are correlated with the optically excited states at ~1.5 eV and point to nontrivial interactions between quantum many-body states on the different energy scales. In revealing these dynamics and correlations, we demonstrate that multidimensional coherent spectroscopy can interrogate complex quantum materials in unprecedented ways.

Revealing and Characterizing Dark Excitons through Coherent Multidimensional Spectroscopy.

Dark excitons are of fundamental importance in a broad range of contexts but are difficult to study using conventional optical spectroscopy due to their weak interaction with light. We show how coherent multidimensional spectroscopy can reveal and characterize dark states. Using this approach, we identify parity-forbidden and spatially indirect excitons in InGaAs/GaAs quantum wells and determine details regarding lifetimes, homogeneous and inhomogeneous linewidths, broadening mechanisms, and coupling strengths. The observations of coherent coupling between these states and bright excitons hint at a role for a multistep process by which excitons in the barrier can relax into the quantum wells.

Isolating quantum coherence using coherent multi-dimensional spectroscopy with spectrally shaped pulses.

We demonstrate how spectral shaping in coherent multidimensional spectroscopy can isolate specific signal pathways and directly access quantitative details. By selectively exciting pathways involving a coherent superposition of exciton states we are able to identify, isolate and analyse weak coherent coupling between spatially separated excitons in an asymmetric double quantum well. Analysis of the isolated signal elucidates details of the coherent interactions between the spatially separated excitons. With a dynamic range exceeding 10(4) in electric field amplitude, this approach facilitates quantitative comparisons of different signal pathways and a comprehensive description of the electronic states and their interactions.