Confinement-induced nonlocality and casimir force in transdimensional systems.

We study within the framework of the Lifshitz theory the long-range Casimir force for in-plane isotropic and anisotropic free-standing transdimensional material slabs. In the former case, we show that the confinement-induced nonlocality not only weakens the attraction of ultrathin slabs but also changes the distance dependence of the material-dependent correction to the Casimir force to go as contrary to the ∼1/l dependence of that of the local Lifshitz force. In the latter case, we use closely packed array of parallel aligned single-wall carbon nanotubes in a dielectric layer of finite thickness to demonstrate strong orientational anisotropy and crossover behavior for the inter-slab attractive force in addition to its reduction with decreasing slab thickness. We give physical insight as to why such a pair of ultrathin slabs prefers to stick together in the perpendicularly oriented manner, rather than in the parallel relative orientation as one would customarily expect.

Thickness-Dependent Drude Plasma Frequency in Transdimensional Plasmonic TiN.

Plasmonic transdimensional materials (TDMs), which are atomically thin metals of precisely controlled thickness, are expected to exhibit large tailorability and dynamic tunability of their optical response as well as strong light confinement and nonlocal effects. Using spectroscopic ellipsometry, we characterize the complex permittivity of ultrathin films of passivated plasmonic titanium nitride with thicknesses ranging from 1 to 10 nm. By measuring passivated TiN, we experimentally distinguish between the contributions of an oxide layer and thickness to the optical properties. A decrease in the Drude plasma frequency and increase in the damping in thinner films is observed due to spatial confinement. We explain the experimental trends using a nonlocal Drude dielectric response theory based on the Keldysh-Rytova (KR) potential that predicts the thickness-dependent optical properties caused by electron confinement in plasmonic TDMs. Our experimental findings are consistent with the KR model and demonstrate quantum-confinement-induced optical properties in plasmonic transdimensional TiN.

Charged Bosons Made of Fermions in Bilayer Structures with Strong Metallic Screening.

Two-dimensional monolayer structures of transition metal dichalogenides (TMDs) have been shown to allow many higher-order excitonic bound states, including trions (charged excitons), biexcitons (excitonic molecules), and charged biexcitons. We report here experimental evidence and the theoretical basis for a new bound excitonic complex, consisting two free carriers bound to an exciton in a bilayer structure. Our experimental measurements on structures made using two different materials show a new spectral line at the predicted energy with two different TMD materials (MoSe2 and WSe2) with both n- and p-doping if and only if all the required theoretical conditions for this complex are fulfilled, in particular, only in the presence of a parallel metal layer that significantly screens the repulsive interaction between the like-charge carriers. Because these four-carrier bound states are charged bosons, they could eventually be the basis for a new path to superconductivity without Cooper pairing.

Monitoring Charge Separation Processes in Quasi-One-Dimensional Organic Crystalline Structures.

We perform the transient absorption spectroscopy experiments to investigate the dynamics of the low-energy collective electron-hole excitations in α-copper phthalocyanine thin films. The results are interpreted in terms of the third-order nonlinear polarization response function. It is found that, initially excited in the molecular plane, the intramolecular Frenkel exciton polarization reorients with time to align along the molecular chain direction to form coupled Frenkel-charge-transfer exciton states, the eigenstates of the one-dimensional periodic molecular lattice. The process pinpoints the direction of the charge separation in α-copper phthalocyanine and similar organic molecular structures. Being able to observe and monitor such processes is important both for understanding the physical principles of organic thin film solar energy conversion device operation and for the development of organic optoelectronics in general.