Andreas Mischok

Organic narrowband near-infrared photodetectors based on intermolecular charge-transfer absorption

Blending organic electron donors and acceptors yields intermolecular charge-transfer states with additional optical transitions below their optical gaps. In organic photovoltaic devices, such states play a crucial role and limit the operating voltage. Due to its extremely weak nature, direct intermolecular charge-transfer absorption often remains undetected and unused for photocurrent generation. Here, we use an optical microcavity to increase the typically negligible external quantum efficiency in the spectral region of charge-transfer absorption by more than 40 times, yielding values over 20%. We demonstrate narrowband detection with spectral widths down to 36 nm and resonance wavelengths between 810 and 1,550 nm, far below the optical gap of both donor and acceptor. The broad spectral tunability via a simple variation of the cavity thickness makes this innovative, flexible and potentially visibly transparent device principle highly suitable for integrated low-cost spectroscopic near-infrared photodetection.

Polymer:Fullerene Bimolecular Crystals for Near‐Infrared Spectroscopic Photodetectors

Spectroscopic photodetection is a powerful tool in disciplines such as medical diagnosis, industrial process monitoring, or agriculture. However, its application in novel fields, including wearable and biointegrated electronics, is hampered by the use of bulky dispersive optics. Here, solution-processed organic donor-acceptor blends are employed in a resonant optical cavity device architecture for wavelength-tunable photodetection. While conventional photodetectors respond to above-gap excitation, the cavity device exploits weak subgap absorption of intermolecular charge-transfer states of the intercalating poly[2,5-bis(3-tetradecylthiophen-2-yl)thieno[3,2-b]thiophene] (PBTTT):[6,6]-phenyl-C61-butyric acid methyl ester (PCBM) bimolecular crystal. This enables a highly wavelength selective, near-infrared photoresponse with a spectral resolution down to 14 nm, as well as dark currents and detectivities comparable with commercial inorganic photodetectors. Based on this concept, a miniaturized spectrophotometer, comprising an array of narrowband cavity photodetectors, is fabricated by using a blade-coated PBTTT:PCBM thin film with a thickness gradient. As an application example, a measurement of the transmittance spectrum of water by this device is demonstrated.

Dispersion tomography of an organic photonic-wire microcavity

We investigate the complex mode structure in microcavities with multidimensional optical confinement. Our active material is composed of the organic blend Alq3:DCM, embedded into a microcavity containing arrays of photonic wires, facilitating strong lateral confinement. We directly record the energy dispersion for one k→ vector component while the second lateral k→ component is scanned. Thereby, we obtain a detailed dispersion tomogram of the cavity resonances, showing excellent agreement with our optical model. We are able to exceed the lasing threshold and observe stimulated emission not only from the bottom of the cavity parabola, but also from higher order modes.

Photonic confinement in laterally structured metal-organic microcavities

We investigate the formation of optical modes in organic microcavities with an incorporated perforated silver layer. The metal leads to a formation of Tamm-plasmon-polaritons and thus separates the sample into metal-free or metal-containing areas, supporting different resonances. This mode splitting is exploited to confine photons in elliptic holes and triangular cuts, forming distinctive standing wave patterns showing the strong lateral confinement. A comparison with a Maxwell-Bloch based rate equation model clearly shows the nonlinear transition into the lasing regime. The concentration of the electric field density and inhibition of lateral loss channels in turn decreases the lasing threshold by up to one order of magnitude, to 0.1 nJ. By spectroscopic investigation of such a triangular wedge, we observe the transition from the unperturbed cavity state to a strongly confined complex transversal mode. Such a structured silver layer can be utilized in future for charge carrier injection in an electrically driven organic solid state laser.

Fast Organic Near-Infrared Photodetectors Based on Charge-Transfer Absorption

We present organic near-infrared photodetectors based on the absorption of charge-transfer (CT) states at the zinc-phthalocyanine-C60 interface. By using a resonant optical cavity device architecture, we achieve a narrowband detection, centered around 1060 nm and well below (>200 nm) the optical gap of the neat materials. We measure transient photocurrent responses at wavelengths of 532 and 1064 nm, exciting dominantly the neat materials or the CT state, respectively, and obtain rise and fall times of a few nanoseconds at short circuit, independent of the excitation wavelength. The current transients are modeled with time-dependent drift-diffusion simulations of electrons and holes which reconstruct the photocurrent signal, including capacitance and series resistance effects. The hole mobility of the donor material is identified as the limiting factor for the high-frequency response. With this knowledge, we demonstrate a new device concept, which balances hole and electron extraction times and achieves a cutoff frequency of 68 MHz upon 1064 nm CT excitation.

Threshold reduction by multidimensional photonic confinement in metal-organic microcavities

Due to their geometry, optical microcavities allow strong confinement of light between the mirrors and promise single mode operation at lowest possible lasing thresholds. Nevertheless, such devices suffer from losses not only due to parasitic absorption of the active or mirror layers, but especially via outcoupling of leaky and waveguided modes within the active layer. In this work, we present an organic microcavity sandwiched between high quality dielectric distributed Bragg reflectors. A highly conductive silver layer of 40nm thickness is added next to the active layer, leading to the formation of Tamm-Plasmon-Polaritons (TPP), one replacing the original cavity mode and shifting its resonance to the red, another one emerging from the long-wavelength sideband and moving to the blue. To avoid parasitic absorption introduced by such contacts, the silver layer is structured on the micrometer-scale using photolithography, yielding separated areas supporting either original cavity mode or red shifted TPP-resonances. This separation leads to a strong spatial trapping of the modes to only their resonant regions on the sample and can in turn be exploited to achieve complete three-dimensional confinement of photons. In elliptic holes produced in the metal layer, we observe the formation of Mathieu-Modes, leading to a reduction of the lasing threshold by six times. Facilitating triangular cuts in the silver layer, highly confined standing modes develop in the system, allowing a precise optimization of the spatial mode extension and reducing the threshold even further down to one order of magnitude below the threshold of an unstructured organic cavity. These results show that the introduction of absorptive metals, needed for the realization of an electrically driven laser, can in turn be harnessed to improve the characteristics of the device.

Cross-coupled composite-cavity organic microresonators

We report on cross-coupled composite-cavity microresonators consisting of a vertical cavity and a second-order distributed feedback structure which employ the same organic active medium and support surface-normal and in-plane emission at the same time. The optical coupling is due to a first-order light diffraction on a second-order Bragg grating and, in the degenerate case, can be as efficient as the coupling observed in more classical cascade coupled cavities. When the system is non-degenerate, the diffraction efficiency is suppressed because of sub-coherence-length dimensions of the composite-cavity and both resonators tend to operate as independent structures without experiencing substantial losses due to diffraction on the distributed-feedback grating.

Photonic lattices in organic microcavities: Bloch states and control of lasing

Organic microcavities comprising the host:guest emitter system Alq3:DCM offer an interesting playground to experimentally study the dispersion characteristics of laterally patterned microlasers due to the broad emission spectrum and large oscillator strength of the organic dye. By structuring of metallic or dielectric sublayers directly on top of the bottom mirror, we precisely manipulate the mode structure and influence the coherent emission properties of the device. Embedding silver layers into a microcavity leads to an interaction of the optical cavity-state in the organic layer and the neighboring metal which red-shifts the cavity resonance, creating a Tamm-plasmon-polariton state. A patterning of the metal can in turn be exploited to fabricate deep photonic wells of micron-size, efficiently confining light in lateral direction. In periodic arrays of silver wires, we create a Kronig-Penney-like optical potential in the cavity and in turn observe optical Bloch states spanning over several photonic wires. We modify the Kronig-Penney theory to analytically describe the full far-field emission dispersion of our cavities and show the emergence of either zero- , π-, or 2π- phase-locking in the system. By investigating periodic SiO2 patterns, we experimentally observe stimulated emission from the ground and different excited discrete states at room temperature and are able to directly control the laser emission from both extended and confined modes of the photonic wires at room-temperature.

Organic narrowband NIR-detectors (Conference Presentation)

Organic materials offer fascinating properties for realizing optoelectronic devices such as organic light emitting diodes (OLEDs) and solar cells (OSCs). The performance of the latter is mainly determined by the low operating voltage with respect to the optical band gap and the limited absorption properties of organic materials in the near infrared (NIR) spectral region. We utilize the weakly absorbing charge transfer state to fabricate a narrowband optical sensor in the NIR up to 1500 nm. With very high and competitive detectivities, we are not only entering the Indium-Gallium-Arsenide-dominated world but demonstrate an integrated spectroscopic sensor for accurate moisture detection.

Novel hybrid laser modes in composite VCSEL-DFB microcavities (Conference Presentation)

Two of the most successful microcresonator concepts are the vertical cavity surface emitting laser (VCSEL), where light is confined between distributed Bragg reflectors (DBRs), and the distributed feedback (DFB) laser, where a periodic grating provides positive optical feedback to selected modes in an active waveguide (WG) layer. Our work concerns the combination of both into a composite device, facilitating coherent interaction between both regimes and giving rise to novel laser modes in the system. In a first realization, a full VCSEL stack with an organic active layer is evaporated on top of a diffraction grating with a large period (approximately 1 micron), leading to diffraction of waveguided modes into the surface emission of the device. Here, the coherent interaction between VCSEL and WG modes, as observed in an anticrossing of the dispersion lines, facilitates novel hybrid lasing modes with macroscopic in-plane coherence [1]. In further studies, we decrease the grating period of such devices to realise DFB conditions in a second-order Bragg grating which strongly couples photons via first-order light diffraction to the VCSEL. This efficient coupling can be compared to more classical cascade-coupled cavities and is successfully described by a coupled oscillator model [2]. When both resonators are non-degenerate, they are able to function as independent structures without substantial diffraction losses. The realization of such novel devices provides a promising platform for photonic circuits based on organic microlasers. [1] A. Mischok et al., Adv. Opt. Mater., early online, DOI: 10.1002/adom.201600282, (2016) [2] T. Wagner et al., Appl. Phys. Lett., accepted, in production, (2016)