Field-dependent THz transport nonlinearities in semiconductor nano structures.

Charge transport nonlinearities in semiconductor quantum dots and nanorods are studied. Using a density matrix formalism, we retrieve the field-dependent nonlinear mobility and show the possibility of intra-pulse gain. We further demonstrate that the dynamics of master equations can be captured in an analytical formula for the field-dependent charge carrier mobility, e.g. for two-level systems. This equation extends the linear response theory based Kubo-Greenwood result to nonlinear processes at elevated field strength, easily reached in THz transport spectroscopy. With these tools we analyze the field strength, chirp, temperature and dephasing dependence of the charge carrier mobility in the model system of CdSe quantum dots and wires. Stark broadening and Rabi splitting result in strong alterations of the mobility spectra, pronounced at low temperatures. The mobility spectra are strongly temperature and pulse shape dependent in the nonlinear regime. The findings are of immediate interest e.g. for nonlinear THz generation, conversion and amplification in 6G technology and nano electronics. Our results further enable experimentalists to fit and understand measured charge transport nonlinearities with analytical expressions and to design nanosystems with engineered material properties.

Optical properties of orthorhombic germanium sulfide: unveiling the anisotropic nature of Wannier excitons.

To fully explore exciton-based applications and improve their performance, it is essential to understand the exciton behavior in anisotropic materials. Here, we investigate the optical properties of anisotropic excitons in GeS encapsulated by h-BN using different approaches that combine polarization- and temperature-dependent photoluminescence (PL) measurements, ab initio calculations, and effective mass approximation (EMA). Using the Bethe-Salpeter Equation (BSE) method, we found that the optical absorption spectra in GeS are significantly affected by the Coulomb interaction included in the BSE method, which shows the importance of excitonic effects besides it exhibits a significant dependence on the direction of polarization, revealing the anisotropic nature of bulk GeS. By combining ab initio calculations and EMA methods, we investigated the quasi-hydrogenic exciton states and oscillator strength (OS) of GeS along the zigzag and armchair axes. We found that the anisotropy induces lifting of the degeneracy and mixing of the excitonic states in GeS, which results in highly non-hydrogenic features. A very good agreement with the experiment is observed.

THz mobility and polarizability: impact of transformation and dephasing on the spectral response of excitons in a 2D semiconductor.

We introduce a response theory based transformation for excitonic polarizability into mobility, which allows an in-depth analysis of optical pump-THz probe conductivity experiments, and compare the results with those of a conventional oscillator model. THz spectroscopy is of high interest e.g. for investigations in high bandwidth and low noise nanoelectronics or solar energy harvesting nanomaterials. In contrast to simple ω scaling of estimated static polarizability, suggested in the literature, an appropriate transformation of the spectral response into mobility can be achieved in principle forward and backward due to the presence of dephasing, as we show for the exemplary system of CdSe nanoplatelets. Common analysis approaches capture the excitonic properties only under specific conditions, and do not apply in many cases. We demonstrate that a thermal distribution of excitons and transitions between higher states in general have to be considered and that dephasing has to be taken into account for a proper transformation at all temperatures. The presented in-depth understanding of the exciton mobility in nanoparticles can help improve e.g. solar hydrogen generation, charge extraction efficiencies of solar cells, or light emission performance of LEDs.

Correction: Tuning trion binding energy and oscillator strength in a laterally finite 2D system: CdSe nanoplatelets as a model system for trion properties.

Correction for 'Tuning trion binding energy and oscillator strength in a laterally finite 2D system: CdSe nanoplatelets as a model system for trion properties' by Sabrine Ayari et al., Nanoscale, 2020, 12, 14448-14458, DOI: .

Tuning exciton diffusion, mobility and emission line width in CdSe nanoplatelets via lateral size.

We investigate the lateral size tunability of the exciton diffusion coefficient and mobility in colloidal quantum wells by means of line width analysis and theoretical modeling. We show that the exciton diffusion coefficient and mobility in laterally finite 2D systems like CdSe nanoplatelets can be tuned via the lateral size and aspect ratio. The coupling to acoustic and optical phonons can be altered via the lateral size and aspect ratio of the platelets. Subsequently the exciton diffusion and mobility become tunable since these phonon scattering processes determine and limit the mobility. At 4 K the exciton mobility increases from ∼ 4 × 103 cm2 V-1 s-1 to more than 1.4 × 104 cm2 V-1 s-1 for large platelets, while there are weaker changes with size and the mobility is around 8 × 101 cm2 V-1 s-1 for large platelets at room temperature. In turn at 4 K the exciton diffusion coefficient increases with the lateral size from ∼ 1.3 cm2 s-1 to ∼ 5 cm2 s-1, while it is around half the value for large platelets at room temperature. Our experimental results are in good agreement with theoretical modeling, showing a lateral size and aspect ratio dependence. The findings open up the possibility for materials with tunable exciton mobility, diffusion or emission line width, but quasi constant transition energy. High exciton mobility is desirable e.g. for solar cells and allows efficient excitation harvesting and extraction.

Tuning trion binding energy and oscillator strength in a laterally finite 2D system: CdSe nanoplatelets as a model system for trion properties.

We present a theoretical study combined with experimental validations demonstrating that CdSe nanoplatelets are a model system to investigate the tunability of trions and excitons in laterally finite 2D semiconductors. Our results show that the trion binding energy can be tuned from 36 meV to 18 meV with the lateral size and decreasing aspect ratio, while the oscillator strength ratio of trions to excitons decreases. In contrast to conventional quantum dots, the trion oscillator strength in a nanoplatelet at low temperature is smaller than that of the exciton. The trion and exciton Bohr radii become lateral size tunable, e.g. from ∼3.5 to 4.8 nm for the trion. We show that dielectric screening has strong impact on these properties. By theoretical modeling of transition energies, binding energies and oscillator strength of trions and excitons and comparison with experimental findings, we demonstrate that these properties are lateral size and aspect ratio tunable and can be engineered by dielectric confinement, allowing to suppress e.g. detrimental trion emission in devices. Our results strongly impact further in-depth studies, as the demonstrated lateral size tunable trion and exciton manifold is expected to influence properties like gain mechanisms, lasing, quantum efficiency and transport even at room temperature due to the high and tunable trion binding energies.