Johannes Haase

Stable Single-Photon Emission by Quantum Dot/Polymer Hybrid Particles

Colloidal quantum dots are well-established probes for quantum optical experiments. However, they possess a limited stability toward their environment. Herein, the generation of hybrid particles composed of a high optical quality quantum dot centered in a polymer particle by means of a miniemulsion polymerization procedure is reported. This embedding strongly enhances emission intensity and photochemical stability of these single-photon emitters. At the same time, their colloidal mobile nature is not compromised.

Coupling of Excitons and Discrete Acoustic Phonons in Vibrationally Isolated Quantum Emitters

The photoluminescence emission by mesoscopic condensed matter is ultimately dictated by the fine-structure splitting of the fundamental exciton into optically allowed and dipole-forbidden states. In epitaxially grown semiconductor quantum dots, nonradiative equilibration between the fine-structure levels is mediated by bulk acoustic phonons, resulting in asymmetric spectral broadening of the excitonic luminescence. In isolated colloidal quantum dots, spatial confinement of the vibrational motion is expected to give rise to an interplay between the quantized electronic and phononic degrees of freedom. In most cases, however, zero-dimensional colloidal nanocrystals are strongly coupled to the substrate such that the charge relaxation processes are still effectively governed by the bulk properties. Here we show that encapsulation of single colloidal CdSe/CdS nanocrystals into individual organic polymer shells allows for systematic vibrational decoupling of the semiconductor nanospheres from the surroundings. In contrast to epitaxially grown quantum dots, simultaneous quantization of both electronic and vibrational degrees of freedom results in a series of strong and narrow acoustic phonon sidebands observed in the photoluminescence. Furthermore, an individual analysis of more than 200 compound particles reveals that enhancement or suppression of the radiative properties of the fundamental exciton is controlled by the interaction between fine-structure states via the discrete vibrational modes. For the first time, pronounced resonances in the scattering rate between the fine-structure states are directly observed, in good agreement with a quantum mechanical model. The unambiguous assignment of mediating acoustic modes to the observed scattering resonances complements the experimental findings. Thus, our results form an attractive basis for future studies on subterahertz quantum opto-mechanics and efficient laser cooling at the nanoscale.

Ultra-strong coupling with spin-split heavyhole cyclotron resonances in sGe QWs (Conference Presentation)

We study the ultra-strong coupling (USC) of Landau level transitions in strained Germanium quantum wells (sGe QW) to THz metasurfaces. The spin-splitting of the heavy-hole cyclotron resonance in sGe QWs due to the Rashba spin-orbit interaction in magnetic field offers an excellent platform to investigate ultra-strong coupling to a non-parabolic system. THz split ring resonators can be tuned to coincide with the single cyclotron transition (around 0.4 THz and a magnetic field of 1.5 T) or the spin-resolved transitions of the sGe QWs (at 1.3 THz and 4.5 T). Coupling to the single cyclotron yields a normalized USC rate of 25%, resulting from fitting with a Hopfield-like Hamiltonian model. Coupling to two or three cyclotron resonances in sGe QWs lead to the observation of multiple polaritons branches, one polariton branch for each oscillator involved in the system. An adaption of the theory allows to also describe this multiple-oscillator system and to determine the coupling strengths. The different Rabi-splittings for the multiple cyclotrons coupling to the same resonator mode relate to the underlying differences in the material. Furthermore, the visibility of an additional transition, possibly a light hole transition with very low carrier density, is strongly enhanced due to the coupling to the LC-resonance with a normalized strong coupling ratio of 4.7%. Future perspectives include controlling spin-flip transitions in USC and studying the impact of non-parabolicity on the ultra-strong coupling physics.

Strong coupling of THz surface plasmon polaritons to complementary metasurfaces (Conference Presentation)

We study the transmission of complementary THz split ring resonator (cSRR) arrays with THz time domain spectroscopy. Utilizing complementary THz metasurfaces and, varying the inter meta-atom separation, a regime of resonant coupling to surface plasmon polaritons (SPPs) is entered. The effective medium condition valid for the direct metasurface is not applicable anymore in the complementary case because of the high THz dielectric constant of gold. We observe a normalized strong coupling of 3.5% to the lattice SPP mode when tuned into resonance with the LC-mode of the cSRR at a frequency of 1.07 THz. The lattice constant is varied from 40 um to 160 um. Finite element simulations with CST MWS show the characteristic field distribution of the two modes and the intermixing of the LC-mode with the SPP-mode very clearly. Analytical modeling with a simple two oscillator model well describes the coupling. An effective relative permittivity of 11.6 for the coupled system was extracted. For broader linewidths, an apparent modulation of the effective Quality-factor can be observed which is of crucial importance for designing metasurfaces for applications. Measurements of the broader lambda/2 mode in orthogonal excitation direction reveal instead a Fano-like interaction. Rectangular array configuration reveal the excitation direction of the SPP modes being along the polarization of the exciting THz pulse. We demonstrate that the understanding of the SPP modes is fundamental for research and applications in which the metasurface has to be designed for special needs.

Femtosecond hole relaxation and biexcitonic transient absorption in single CdSe/ZnSe quantum dots

Femtosecond few-fermion dynamics in single CdSe/ZnSe quantum dots is studied by two-color pump-probe measurements. We observe sub-picosecond hole relaxation and induced absorption into biexciton states when pumping p-p and d-s transitions.