Florian Hackl

High Infrared Photoconductivity in Films of Arsenic-Sulfide-Encapsulated Lead-Sulfide Nanocrystals

Highly photoconductive thin films of inorganic-capped PbS nanocrystal quantum dots (QDs) are reported. Stable colloidal dispersions of (NH4)3AsS3-capped PbS QDs were processed by a conventional dip-coating technique into a thin homogeneous film of electronically coupled PbS QDs. Upon drying at 130 °C, (NH4)3AsS3 capping ligands were converted into a thin layer of As2S3, acting as an infrared-transparent semiconducting glue. Photodetectors obtained by depositing such films onto glass substrates with interdigitate electrode structures feature extremely high light responsivity and detectivity with values of more than 200 A/W and 1.2 × 1013 Jones, respectively, at infrared wavelengths up to 1400 nm. Importantly, these devices were fabricated and tested under ambient atmosphere. Using a set of time-resolved optoelectronic experiments, the important role played by the carrier trap states, presumably localized on the arsenic-sulfide surface coating, has been elucidated. Foremost, these traps enable a very high photoconductive gain of at least 200. The trap state density as a function of energy has been plotted from the frequency dependence of the photoinduced absorption (PIA), whereas the distribution of lifetimes of these traps was recovered from PIA and photoconductivity (PC) phase spectra. These trap states also have an important impact on carrier dynamics, which led us to propose a kinetic model for trap state filling that consistently describes the experimental photoconductivity transients at various intensities of excitation light. This model also provides realistic values for the photoconductive gain and thus may serve as a useful tool to describe photoconductivity in nanocrystal-based solids.

The influence of a Si cap on self-organized SiGe islands and the underlying wetting layer

For the prototypical SiGe/Si(001) Stranski-Krastanow (SK) growth system, the influence of intermixing caused by the deposition of a Si cap layer at temperatures Tcap between 300°C and 700°C is studied both for the SiGe wetting layer (WL) and the SiGe islands. Systematic growth experiments were carried out with an ultrahigh resolution of down to 0.005 monolayers (ML) of deposited Ge. The properties of the samples were investigated via photoluminescence (PL) spectroscopy, atomic force microscopy (AFM), and transmission electron microscopy. We studied in detail the influence of Tcap in the three main coverage regions of SiGe SK growth, which are (i) the WL build-up regime, (ii) the island nucleation regime, where most of the Ge is supplied via material transfer from the WL, and (iii) the saturation regime, where the WL thickness remains initially stable. At Tcap = 300°C, we found that both the WL and the island are essentially preserved in composition and shape, whereas at 500°C the WL becomes heavily alloye...

Microphotoluminescence and perfect ordering of SiGe islands on pit-patterned Si(001) substrates

We show that both the morphology and the optoelectronic properties of SiGe islands growing in the pits of periodically pre-patterned Si(001) substrates are determined by the amount of Ge deposited per unit cell of the pattern. Pit-periods (p) ranging from 300 to 900 nm were investigated, and Ge growth was performed by molecular beam epitaxy (MBE) at temperatures of 690 and 760 °C. The ordered SiGe islands show photoluminescence (PL) emission, which becomes almost completely quenched, once a critical island volume is exceeded. By atomic force and transmission electron microscope images we identify the transition from pyramid-shaped to dome-shaped islands with increasing p. Eventually, the nucleation of dislocations in the islands leads to PL quenching. Below a critical Ge coverage a narrowing and a blue shift of the PL emission is observed, as compared to islands grown on a planar reference area of the same sample.

Lasing from Glassy Ge Quantum Dots in Crystalline Si.

Semiconductor light emitters compatible with standard Si integration technology (SIT) are of particular interest for overcoming limitations in the operating speed of microelectronic devices 1-3. Light sources based on group-IV elements would be SIT compatible but suffer from the poor optoelectronic properties of bulk Si and Ge. Here, we demonstrate that epitaxially grown Ge quantum dots (QDs) in a fully coherent Si matrix show extraordinary optical properties if partially amorphised by Ge-ion bombardment (GIB). The GIB-QDs exhibit a quasi-direct-band gap and show, in contrast to conventional SiGe nanostructures, almost no thermal quenching of the photoluminescence (PL) up to room-temperature (RT). Microdisk resonators with embedded GIB-QDs exhibit threshold-behaviour and super-linear increase of the integrated PL-intensity (IPL) with increasing excitation power Pexc which indicates light amplification by stimulated emission in a fully SIT-compatible group-IV nano-system.Semiconductor light-emitters compatible with standard Si integration technology (SIT) are of particular interest for overcoming limitations in the operating speed of microelectronic devices. Light sources based on group IV elements would be SIT-compatible, but suffer from the poor optoelectronic properties of bulk Si and Ge. Here we demonstrate that epitaxially grown Ge quantum dots (QDs) in a defect-free Si matrix show extraordinary optical properties if partially amorphized by Ge-ion bombardment (GIB). In contrast to conventional SiGe nanostructures, these QDs exhibit dramatically shortened carrier lifetimes and negligible thermal quenching of the photoluminescence (PL) up to room temperature. Microdisk resonators with embedded GIB-QDs exhibit threshold behavior as well as a superlinear increase of the integrated PL intensity with concomitant line width narrowing as the pump power increases. These findings demonstrate light amplification by stimulated emission in a fully SIT-compatible group IV nanosystem.

UV nanoimprint lithography for the realization of large-area ordered SiGe/Si(001) island arrays

We use UV nanoimprint lithography for the pit-patterning of silicon substrates. Ordered silicon-germanium islands are grown inside these pits by molecular-beam epitaxy on arrays of 3×3 mm2 and characterized by atomic force microscopy (AFM) and photoluminescence (PL) measurements. AFM-based statistics reveals an extremely uniform size distribution of the islands in the patterned areas. These results are confirmed by very narrow and uniform PL peaks recorded at various positions across the patterned arrays.

Excitation Intensity Driven PL Shifts of SiGe Islands on Patterned and Planar Si(001) Substrates: Evidence for Ge-rich Dots in Islands

For randomly nucleated SiGe/Si(001) islands, a significantly stronger blue-shift of the PL spectra as a function of the excitation intensity is observed when compared to islands grown on patterned substrates side by side within the same run in a solid source molecular beam epitaxy chamber. We ascribe this different PL behavior to the much larger inhomogeneity of the Ge distribution in islands on planar substrates when compared to islands grown on pit-patterned ones, as observed previously. 3D band-structure calculations show that Ge-rich inclusions of approximately 5 nm diameter at the apex of the islands can account for the observed differences in the PL spectra. The existence of such inclusions can be regarded as a quantum dot in an island and is in agreement with recent nano-tomography experiments.

Commensurate germanium light emitters in silicon-on-insulator photonic crystal slabs

We report on the fabrication and characterization of silicon-on-insulator (SOI) photonic crystal slabs (PCS) with commensurately embedded germanium quantum dot (QD) emitters for near-infrared light emission. Substrate pre-patterning defines preferential nucleation sites for the self-assembly of Ge QDs during epitaxial growth. Aligned two-dimensional photonic crystal slabs are then etched into the SOI layer. QD ordering enhances the photoluminescence output as compared to PCSs with randomly embedded QDs. Rigorously coupled wave analysis shows that coupling of the QD emitters to leaky modes of the PCS can be tuned via their location within the unit cell of the PCS.

Excitation intensity dependence of photoluminescence spectra of SiGe quantum dots grown on prepatterned Si substrates: evidence for biexcitonic transition

The pumping intensity (I) dependence of the photoluminescence (PL) spectra of perfectly laterally two-dimensionally ordered SiGe quantum dots on Si(001) substrates was studied. The PL results from recombinations of holes localized in the SiGe quantum dots and electrons localized due to the strain field in the surrounding Si matrix. The analysis of the spectra revealed several distinct bands, attributed to phonon-assisted recombination and no-phonon recombination of the excitonic ground state and of the excited excitonic states, which all exhibit a linear I dependence of the PL intensity. At approximately I larger than 3 W cm-2, additional bands with a nearly quadratic I dependence appear in the PL spectra, resulting from biexcitonic transitions. These emerging PL contributions shift the composite no-phonon PL band of the SiGe quantum dots to higher energies. The experimentally obtained energies of the no-phonon transitions are in good agreement with the exciton and biexciton energies calculated using the envelope function approximation and the configuration interaction method.

Enhanced Telecom Emission from Single Group-IV Quantum Dots by Precise CMOS-Compatible Positioning in Photonic Crystal Cavities

Efficient coupling to integrated high-quality-factor cavities is crucial for the employment of germanium quantum dot (QD) emitters in future monolithic silicon-based optoelectronic platforms. We report on strongly enhanced emission from single Ge QDs into L3 photonic crystal resonator (PCR) modes based on precise positioning of these dots at the maximum of the respective mode field energy density. Perfect site control of Ge QDs grown on prepatterned silicon-on-insulator substrates was exploited to fabricate in one processing run almost 300 PCRs containing single QDs in systematically varying positions within the cavities. Extensive photoluminescence studies on this cavity chip enable a direct evaluation of the position-dependent coupling efficiency between single dots and selected cavity modes. The experimental results demonstrate the great potential of the approach allowing CMOS-compatible parallel fabrication of arrays of spatially matched dot/cavity systems for group-IV-based data transfer or quantum optical systems in the telecom regime.

Laser Level Scheme of Self-Interstitials in Epitaxial Ge Dots Encapsulated in Si

Recently, it was shown that lasing from epitaxial Ge quantum dots (QDs) on Si substrates can be obtained if they are partially amorphized by Ge ion bombardment (GIB). Here, we present a model for the microscopic origin of the radiative transitions leading to enhanced photoluminescence (PL) from such GIB-QDs. We provide an energy level scheme for GIB-QDs in a crystalline Si matrix that is based on atomistic modeling with Monte Carlo (MC) analysis and density functional theory (DFT). The level scheme is consistent with a broad variety of PL experiments performed on as-grown and annealed GIB-QDs. Our results show that an extended point defect consisting of a split-[110] self-interstitial surrounded by a distorted crystal lattice of about 45 atoms leads to electronic states at the Γ-point of the Brillouin zone well below the conduction band minimum of crystalline Ge. Such defects in Ge QDs allow direct transitions of electrons localized at the split-interstitial with holes confined in the Ge QD. We identify the relevant growth and annealing parameters that will let GIB-QDs be employed as an efficient laser active medium.