Single-photon detectors have historically consisted of macroscopic-sized materials but recent experimental and theoretical progress suggests new approaches based on nanoscale and molecular electronics. Here, we present a theoretical study of photodetection in a system composed of a quantum electronic transport channel functionalized by a photon absorber. Notably, the photon field, absorption process, transduction mechanism, and measurement process are all treated as part of one fully coupled quantum system, with explicit interactions. Using nonequilibrium, time-dependent quantum transport simulations, we reveal the unique temporal signatures of the single-photon detection process, and show that the system can be described using optical Bloch equations, with a new nonlinearity as a consequence of time-dependent detuning caused by the back-action from the transport channel via the dynamical Stark effect. We compute the photodetector signal-to-noise ratio and demonstrate that single-photon detection at high count rate is possible for realistic parameters by exploiting a unique nonequilibrium control of back-action.
Bilayer van der Waals (vdW) heterostructures such as MoS2/WS2 and MoSe2/WSe2 have attracted much attention recently, particularly because of their type II band alignments and the formation of interlayer exciton as the lowest-energy excitonic state. In this work, we calculate the electronic and optical properties of such heterostructures with the first-principles GW+Bethe-Salpeter Equation (BSE) method and reveal the important role of interlayer coupling in deciding the excited-state properties, including the band alignment and excitonic properties. Our calculation shows that due to the interlayer coupling, the low energy excitons can be widely tuned by a vertical gate field. In particular, the dipole oscillator strength and radiative lifetime of the lowest energy exciton in these bilayer heterostructures is varied by over an order of magnitude within a practical external gate field. We also build a simple model that captures the essential physics behind this tunability and allows the extension of the ab initio results to a large range of electric fields. Our work clarifies the physical picture of interlayer excitons in bilayer vdW heterostructures and predicts a wide range of gate-tunable excited-state properties of 2D optoelectronic devices.
Metal organic frameworks (MOFs) are extended, nanoporous crystalline compounds consisting of metal ions interconnected by organic ligands. Their synthetic versatility suggest a disruptive class of opto - electronic materials with a high degree of electrical tunability and without the property - degrading disorder of organic conductors. In this project we determined the factors controlling charge and energy transport in MOFs and evaluated their potential for thermoelectric energy conversion. Two strategies for a chieving electronic conductivity in MOFs were explored: 1) using redox active 'guest' molecules introduced into the pores to dope the framework via charge - transfer coupling (Guest@MOF), 2) metal organic graphene analogs (MOGs) with dispersive band structur es arising from strong electronic overlap between the MOG metal ions and its coordinating linker groups. Inkjet deposition methods were developed to facilitate integration of the guest@MOF and MOG materials into practical devices.
Dynamic wavelength tunability has long been the holy grail of photodetector technology. Because of its atomic thickness and unique properties, graphene opens up new paradigms to realize this concept, but so far this has been elusive experimentally. Here we employ detailed quantum transport modeling of photocurrent in graphene field-effect transistors (including realistic electromagnetic fields) to show that wavelength tunability is possible by dynamically changing the gate voltage. We reveal the phenomena that govern the behavior of this type of device and show significant departure from the simple expectations based on vertical transitions. We find strong focusing of the electromagnetic fields at the contact edges over the same length scale as the band-bending. Both of these spatially-varying potentials lead to an enhancement of non-vertical optical transitions, which dominate even in the absence of phonon or impurity scattering. We also show that the vanishing density of states near the Dirac point leads to contact blocking and a gate-dependent modulation of the photocurrent. Several of the effects discussed here should be applicable to a broad range of one-and two-dimensional materials and devices.
The metal organic framework material Ni3(2,3,6,7,10,11 - hexaiminotriphenylene)2, (Ni3(HITP)2) is composed of layers of extended conjugated planes analogous to graphene. We carried out Density functional theory (DFT) calculations to model the electronic structure of bulk and monolayer Ni3(HITP)2. The layered 3D material is metallic, similar to graphene. Our calculations predict that there is appreciable band dispersion not only in-plane, but perpendicular to the stacking planes as well, suggesting that, unlike graphene, the conductivity may be nearly isotropic. In contrast, a 2D monolayer of the material exhibits a band gap, consistent with previously published results. Insight obtained from studies of the evolution of the material from semiconducting to metallic as the material is transitioned from 2D to 3D suggests the possibility of modifying the material to render it semiconducting by changing the metal center and inserting spacer moieties between the layers. Furthermore, the DFT calculations predict that the modified material will be structurally stable and exhibit a band gap.
Oxidation of exfoliated gallium selenide (GaSe) is investigated through Raman, photoluminescence, Auger, and X-ray photoelectron spectroscopies. Photoluminescence and Raman intensity reductions associated with spectral features of GaSe are shown to coincide with the emergence of signatures emanating from the by-products of the oxidation reaction, namely, Ga2Se3 and amorphous Se. Furthermore, photoinduced oxidation is initiated over a portion of a flake highlighting the potential for laser based patterning of two-dimensional heterostructures via selective oxidation.